Mixed halide perovskites exhibit great potential as materials for the future generation of photovoltaic devices. Yet, their reaction to moisture remains uncertain, necessitating further exploration. While prolonged exposure to moisture can lead to degradation, it can also passivate traps at an optimal moisture level. Here, we use scanning probe microscopy to perform nanoscale moisture-dependent photovoltaic characterizations of open and compressed grain boundary (GB) structures of wide bandgap (FAPbI3)0.3(FAPbBr3)0.7 perovskites. The investigation reveals a decrease in the potential barrier at compact GBs with increasing moisture levels, contrasting with the behavior observed in open GBs. Moreover, the photocurrent distribution over both samples proportionally increases when relative humidity (RH) is raised from 10% to 60%. Notably, following a 24-h exposure at RH 60%, the compact-GB sample demonstrates: i) a reduction in the density of charged trap states at GBs, ii) higher photocurrent, accompanied by a noticeable decrease in current hysteresis compared to the open GB sample, and iii) further enhancement in device efficiency and crystallinity compared to devices with open GBs. These findings suggest that optimizing humidity conditions in engineering the GB chemistry can enhance the optoelectrical properties of GBs, ultimately leading to improved device performance.
Fenton technology has garnered significant attention for the deep removal of low-concentration emerging contaminants due to its remarkable oxidation performance. However, the traditional mineralization process for emerging contaminants requires a substantial amount of hydroxyl radicals (HO˙), leading to excessive consumption of H2O2. Through interfacial engineering of Fe–Zr bimetallic catalysts (FeZrOx), this study demonstrates synergistic enhancement of phenolic pollutant removal at heterojunction interfaces while achieving an 80% reduction in H2O2 dosage compared to traditional Fe2O3 systems. The chemical states of Fe and Zr at the (104)/(111) heterojunction interface in FeZrOx exhibit marked modifications relative to their monometallic Fe2O3 and ZrO2 counterparts. The elevated charge density at interfacial Fe sites in FeZrOx promotes HO˙ generation, while optimized antibonding orbital composition below the Fermi level in bisphenol A adsorbed on Zr sites enhances hydrogen abstraction and subsequent polymerization. This Fe–Zr synergy at the (104)/(111) heterojunction concurrently suppresses HO˙ diffusion losses and directs phenolic pollutant (e.g., phenol and bisphenol A) polymerization within the reactive interface, thereby reducing H2O2 consumption compared to monometallic systems.
As a core technology in flexible electronics systems, piezoresistive sensors exhibit significant application value in frontier fields such as medical health monitoring, intelligent human–machine collaboration, and bionic robot perception. A novel flexible piezoresistive sensing material was developed by combining biomass-derived carbon aerogel (CC) with polydimethylsiloxane (PDMS). The composites had excellent fatigue resistance, maintaining more than 90% shape recovery and less than 3.8% residual deformation after 100 000 cycles at 30% strain. Furthermore, combining biomass-derived carbon aerogel with polydimethylsiloxane composites exhibited excellent piezoresistive response characteristics at different temperatures. In the temperature range from −30 °C to 100 °C, its resistance decreased with increasing temperature, while showing a shortened response time. The composite achieved a stable resistance response through the reversible contact of the conductive network under the action of external forces and had a wide linear detection range, high sensitivity, and effective differentiation between static pressure and dynamic deformation signals. This work established the correlation between the microscopic deformation of the carbon skeleton and the macroscopic electrical behavior, and verified the stability and durability of combining biomass-derived carbon aerogel with polydimethylsiloxane composites under complex stress conditions. The collaborative design strategy provides an innovative platform for the development of sustainable, high-performance flexible sensors with important potential applications in health monitoring and intelligent human–machine interfaces.
This work explores the potential of La1-xPrxNiO4+δ thin films fabricated by Pulsed Injection Metal–Organic Chemical Vapor Deposition as oxygen electrodes for low-temperature solid oxide cells. La1-xPrxNiO4+δ materials offer promising mixed ionic and electronic conductivity and high oxygen reduction reaction kinetics. In this study, we focus on the microstructural and electrochemical properties of LaPrNiO4+δ thin films deposited at various temperatures (600–650 °C), revealing that a two-temperature deposition process yields nano-architectured films with a dense bottom film and a porous nano-columnar top layer of the same material. Electrochemical impedance spectroscopy and electrical conductivity relaxation experiments demonstrate enhanced surface exchange coefficients compared to bulk LaPrNiO4+δ and La2NiO4+δ and high performance, with polarization resistances as low as 0.10 Ω cm2 at 600 °C and 1.00 at 500 °C. To better understand the electrochemical behavior of these electrodes, we investigated the limiting mechanisms of oxygen reduction by analyzing the kinetic response to varying oxygen partial pressures and performing detailed impedance analyses. These nano-columnar LaPrNiO4+δ oxygen electrodes were also deposited on commercial half-cells, enabling the resulting full cells to operate successfully in both reversible solid oxide fuel cell and electrolysis cell modes, reaching a performance of 0.34 W cm−2 at 600 °C in reversible solid oxide fuel cell mode. This work underscores the promise of LaPrNiO4+δ thin films for efficient low-temperature-solid oxide cells while addressing challenges in durability and stability.
Natural polymers possess the qualities of abundant resources, low cost, as well as excellent biocompatibility and biodegradability, and are ideal materials for next-generation wearable and portable electronic devices. To further augment the application scope of natural polymer materials, integrating them with functional materials represents a promising approach that is of great value for the sustainable development of triboelectric nanogenerators. Here, we successfully synthesized starch–[CsPbBr3–KBr]–Fe3O4 composite films through the combination of natural polymer materials with magnetic and fluorescent components. It is capable of achieving reversible hydrochromic conversion by exposing or removing water. The combination of fluorescent CsPbBr3–KBr, magnetic Fe3O4, and waterproof starch - [CsPbBr3 - KBr] - Fe3O4-Polydimethylsiloxane leads to the realization of fluorescence and magnetic composite anti-counterfeiting. This composite anti-counterfeiting technology presents a novel and highly effective approach for ensuring the authenticity and security of various types of information. In addition, the Composite film based triboelectric nanogenerator has been assembled, which has a stable output with a short circuit current and open-circuit voltage of 15.1 μA and 170.1 V, respectively. The triboelectric nanogenerator can light 204 red LED lights at the same time, and the electrical output is not reduced even after 4200 mechanical cycles. Furthermore, based on the triboelectric nanogenerator, we have successfully demonstrated a self-powered sensor that can monitor human movement signals in real time. The sensor has shown broad application prospects in the field of health monitoring and motion analysis.
Selective extraction of precious metals from urban mines plays a crucial role in mitigating the risk of depletion of precious metal resources and reducing waste pollution. However, a major obstacle in precious metal extraction lies in the difficulty of distinguishing the subtle differences in the physicochemical characteristics between them, especially gold and palladium. Herein, a proton-driven separation system was presented for cascade recovery of gold and palladium from waste-printed circuit boards (W-PCBs) leachate using poly(amidoxime) (PAO) hydrogel. This exhibits an ultra-high capacity, extra-fast rate, and excellent selectivity for the extraction of Au(III) and Pd(II). Notably, the separation of Au(III) and Pd(II) can be achieved with high selectivity at pH = 0, resulting in a remarkable separation factor of kAu (III)/Pd(II) = 36.5. This was demonstrated to originate from the differential mechanism of PAO hydrogel for the capture of Au(III) and Pd(II) under proton-mediated conditions. Drawing inspiration from the mechanism, the proton-driven cascade recovery system demonstrates remarkable efficiency in sequentially recovering 99.92% of gold and 99.05% of palladium from W-PCBs acid leachate. This research opens up a strategy to precisely separate and recover precious metals from e-waste of urban mines.
Carbon coatings for silicon (Si)-based anode materials are essential for designing high-performance Li-ion batteries (LIBs). The coatings prevent direct contact with the electrolyte and enhance anode performance. However, conventional carbon coatings are limited by their volume expansion and structural degradation, which lead to capacity fading and reduced durability. This study introduces a scalable and practical one-step carbon-coating strategy for directly coating silicon suboxide (SiOx)-based materials using aqueous quasi-defect-free reduced graphene oxide (QrGO) without post-treatment, unlike conventional graphene oxide (GO)-based coating methods. This simple process enables uniform encapsulation with QrGO for a highly adhesive and conductive coating. The QrGO-based composite anode material has several advantages, including reduced cracking due to volume expansion and enhanced charge carrier transport, as well as an increased Si content of 20 wt.% compared to the 5 wt.% in typical commercial Si-based active materials. In particular, the capacity retention of the QrGO-coated Si electrodes dramatically increases at high C-rate. The full cell exhibited long-term stability and capacity that were twice that of commercial SiOx-based cells. Therefore, the QrGO-based one-step coating process represents a scalable, transformative, and commercially viable strategy for developing high-performance LIBs.
Biomass structural materials can effectively address the issues of high energy consumption and environmental degradation brought by traditional engineering structural materials. However, natural structural materials often suffer from drawbacks such as low mechanical performance and flammability. Therefore, this study has developed an ultra-strong fire-resistant bamboo composite (UFBC). Natural bamboo (NB) was used as the raw material. After delignification treatment, bamboo fibers are grafted with epoxy groups through in-situ chemical bonding. Subsequently, polymer chains underwent in-situ chemical cross-linking within the bamboo fiber framework, combined with reinforcement from nano silica, resulting in strengthened cell walls. In addition, the softened and expanded cell walls can facilitate the deposition of phosphate and borate salt on the cell walls, forming an N-P-B flame-retardant system within the system. The tensile strength (463 MPa vs NB 112 MPa) and flexural strength (655 MPa vs NB 157 MPa) of UFBC increased fourfold, with a Limiting Oxygen Index (LOI) of 54.4%. Compared to similar bamboo-based composite materials, UFBC exhibits superior environmental friendliness and sustainability throughout its lifecycle, with all 18 environmental factors being optimized (up to a 92% reduction). This study provides an important reference for the application of high-performance biomass structural materials in construction and industry.
Demonstrating significant achievements in efficiency, perovskite solar cells (PSCs) have acquired unique positions in photovoltaics, offering alternatives to conventional commercial silicon solar cells. While there has been significant progress in enhancing photovoltaic performance, obvious stability problems remain a primary challenge that continues to hinder the commercial viability of PSCs. This present review first comprehensively discusses the main challenges to the commercialization of PSCs, including stability problems, ion migration, toxicity, and complexities in large-scale fabrication. It then effectively presents universal strategies to overcome the mentioned problems. Moreover, this review article examines various printing techniques that can be used to improve PSCs, emphasizing their benefits like low-cost components and procedures. Several printing processes are covered in the discussion, such as slot-die coating, spray coating, inkjet printing, doctor-blade coating, roll-to-roll printing, and screen printing. The potential uses of PSCs for the implementation of greenhouses, building-integrated photovoltaic systems, and indoor light energy harvesting. These uses highlight the adaptability of PSCs and demonstrate their ability to transform energy production technologies. Additionally, this review highlights the special qualities of perovskite materials that present chances to surpass silicon solar cells' efficiency restrictions and get close to the Shockley-Queisser limit. In conclusion, the current review provides a brief overview of recent developments, existing challenges, and opportunities of PSCs. It provides a thorough understanding of the merits of highly efficient PSCs fabricated by adopting printing methods to tackle stability problems along with facile fabrication of PSCs using simplified and cost-effective strategies.
Solid-state lithium batteries are considered one of the most promising next-generation energy storage technologies owing to their safety and high energy density. The key to solid-state lithium battery advancement lies in the design and optimization of suitable solid-state electrolytes. Among various solid-state electrolytes, solid-state composite polymer electrolytes offer the combined benefits of solid inorganic electrolytes and solid polymer electrolytes. In particular, Li1 + xAlxTi2 − x(PO4)3 (LATP)/polymer composite polymer electrolytes exhibit high ionic conductivity due to LATP and improved flexibility from the polymer matrix. These systems also demonstrate robust mechanical properties and excellent electrode contact. While recent reviews have primarily focused on the performance of LATP/polymer composite polymer electrolytes and the general effects of composite polymer electrolyte modifications for solid-state lithium battery applications, this review provides a concise overview of the Li+ transport mechanisms in LATP/polymer composite polymer electrolytes and strategies to enhance ionic conductivity. It highlights several modification approaches, including the use of fillers, additives, and LATP coatings, which markedly influence the performance of composite polymer electrolytes across different polymer matrices. Finally, the review addresses the challenges of LATP/polymer composite polymer electrolytes and outlines key research directions for developing advanced composite polymer electrolytes for high-performance solid-state lithium batteries.
A versatile spectroelectrochemical measurement method of surface-enhanced Raman scattering spectroscopy is developed, and its capability is assessed in an actual electrochemical system. The spectroelectrochemical cell consists of a plasmonic sensor with metal nanoparticles and a wire-type working electrode. The advantages of this method over conventional surface-enhanced Raman scattering methods are as follows: 1) surface-enhanced Raman scattering for electrode materials that show little plasmon resonance; and 2) measurement without undesirable influences on the physical and chemical states of the electrode surface and transport phenomena of reaction species. During the measurement, the sensor contacts the working electrode wire at a single point, allowing the surface-enhanced Raman scattering signal to be obtained from the interfacial area of the working electrode surface without significantly disturbing the mass transfer of the reaction species. As plasmon-active metal nanoparticles are modified on the sensor surface in advance, destructive and complicated pretreatment processes on the working electrode are not required. The method is applied to the in situ analysis of electrolyte decomposition reactions in a Li metal battery to reveal the potential of each decomposition product of an organic solvent containing Li. The obtained surface-enhanced Raman scattering spectrum corresponding to the voltammogram reveals the pathway for obtaining decomposition products, such as Li2CO3. In particular, Li2C2 was clearly detected with our setup. It is also revealed from the setup that the Ni electrode surface, in contrast to the Cu, does not hold a stable Li-containing composite layer. Such in situ chemical information will contribute to the effective interfacial design of high-performance batteries.
Redox-active covalent organic polymers (COPs) have emerged as appealing renewable electrode materials for next-generation Li-ion batteries, but their performance is limited by insufficient redox sites and inadequate Li-ion diffusion. Here, we develop a novel class of mesoporous covalent organic polymer (namely TF-Azo-COP) bearing multiple redox sites and explore its first use as efficient 18-electron-redox anodes for superior Li-ion storage in both coin-type and fiber-type batteries. The newly produced TF-Azo-COP involves three types of active sites including C=N in triazines and imines, N=N in azo, and C6-ring aromatics to enable 18-Li-ion storage on one repeatable segment, while affording extended π-conjugation for fast electron transfer and a pore size of ~2.5 nm for facilitated ion diffusion with a high coefficient up to ~10−10 cm2 s−1—superior to some reported organic electrodes. Meriting from the above, pairing TF-Azo-COP with metal Li endows a coin cell with good cycling stability and a large reversible capacity of 795.4 mAh g−1 at 0.1 A g−1—representing one of the best performances among reported organic electrodes. When coupled with fiber-shaped LiFePO4 cathodes, the assembled fiber cell delivers an excellent combination of linear capacity (0.23 mAh cm−1), energy density (0.55 mWh cm−1), cycling stability (250 cycles), and good flexibility.
As the carrier of charge storage, the electrode determines the efficiency of the energy conversion reaction between the battery and the substance. However, with the continuous development of scientific research, electrode preparation is still facing complex technical problems, and it is difficult to achieve a balance in performance, cost, and technology. Based on the ion dissolution and deposition behavior of Mn2+/MnO2 and Al3+/Al, a novel cathode-free aqueous ion dissolution/deposition battery is designed, which can contribute 15 mAh at 16 cm2 in a voltage window of 0.5–1.8 V. The charge storage and the attenuation mechanism are systematically investigated. The battery model with compensable electrolyte was constructed, and the cycle characteristics of the cathode-free aqueous ion dissolution/deposition battery were optimized, which could achieve 1000 h continuous operation. This system provides a low-cost and high-safety solution for future high-energy density and large-scale energy storage. Future research will focus on optimizing electrolytes, controlling deposition morphology, and improving interface stability to further promote the commercialization of cathode-free batteries.
Aqueous zinc-ion batteries (AZIBs) have emerged as a promising complement to lithium-ion batteries due to their inherent safety benefits. However, the cycle life of AZIBs is severely limited by the poor stability of zinc anodes, manifested in uncontrolled dendritic growth and persistent side reactions, which hinder wider application. Herein, we report an ion-selective separator (UIO-66-4F/GF) achieved by in situ growth of a fluorine-functionalized metal–organic framework (UIO-66-4F) onto commercial glass fiber (GF). The synergistic mechanism, involving electrostatic repulsion between -F groups and anions along with strong interactions between -F and Zn2+ cations, effectively restricts migration, suppresses 2D Zn2+ diffusion across electrode interfaces, and enhances [Zn(H2O)6]2+ desolvation. Furthermore, the -F groups enable precise regulation of interfacial electric fields and Zn2+ concentration gradients, thereby homogenizing ion flux to realize dendrite-free Zn deposition. The UIO-66-4F separator achieves stable Zn||Zn cell operation for 1500 h at 1 mA cm−2 via oriented deposition and sustains long-term cycling over 1000 h at 1 mA cm−2, and delivers a Zn||Cu cell with 99.4% Coulombic efficiency. Moreover, the Zn|UIO-66-4F/GF|NH4V4O10 full cell represents an ultrastable cycling stability with a high capacity retention of 90% after 500 cycles at a current density of 1 A g−1.
This study investigates phase change materials (PCMs) for lithium battery thermal management. A PCM cooling model was developed and experimentally validated, showing ≤1.5 K temperature error and ≤5% PCM melting simulation deviation. A non-uniform battery arrangement was proposed to optimize temperature distribution. Key PCM parameters (melting point, conductivity, latent heat) were analyzed for thermal performance. A hybrid liquid-PCM cooling system was designed and optimized via an entropy-weighted TOPSIS-NSWOA strategy. At 4 C discharge, the optimized system achieved 311.41 K maximum temperature (5.89 K reduction) and 4.71 K temperature difference, meeting 18 650 battery safety standards. The findings guide PCM selection and integrated thermal management design, balancing heat dissipation and temperature uniformity
Global water scarcity and pollution present critical challenges for human society. Solar-driven wastewater treatments, such as photocatalytic degradation of organic pollutants and photothermal conversion water evaporation, offer promising solutions. TiO2 has garnered extensive attention in these fields, but its large bandgap limits light absorption, affecting its performance and broader applications in energy and environmental fields. Consequently, modifying TiO2 to improve its photocatalytic and photothermal conversion performance has become a research hotspot. Among various modification strategies, self-doping with Ti3+ and oxygen vacancies can reduce the bandgap of TiO2, improve sunlight utilization, and increase the separation efficiency of photogenerated electron–hole pairs, thereby significantly enhancing the photocatalytic and photothermal conversion performance. This review focuses on the inorganic chemical reduction methods for preparing Ti3+/oxygen vacancies self-doped TiO2 and their current applications in solar-driven photothermal conversion water evaporation. It highlights the challenges faced during synthesis and application while offering insights into future development prospects. This review is expected to provide a valuable reference for further research on the preparation and application of Ti3+/oxygen vacancies self-doped TiO2.
The uncontrollable growth of zinc metal dendrites and the water-induced parasitic reaction in pure aqueous electrolyte cause the poor cycling stability of zinc ion battery. Herein, a stable electrode/electrolyte interface with a dendrite-free zinc anode is developed by adding acetone into the aqueous electrolyte. The as-formed water/acetone hybrid solvent effectively optimizes the Zn2+ solvation structure (coordinated water changes from 6 to 4) and induces the uniform zinc ion deposition through the high adsorption energy with the Zn (002) surface. It also stabilizes the zinc metal by reducing the corrosion reaction (hydrogen evolution) with water and the formation of a basic zinc salt by-product. As a result, the symmetrical cell with the acetone/water electrolyte exhibits a superior stability of 3700 h (154 days) at 1 mA cm−2. The battery with the Na2V6O16·3H2O cathode delivers an 84.1% capacity retention after 1000 cycles at 1.0 A g−1. The organic/aqueous electrolyte provides a new insight into understanding the relationship between solvation structure, electrode/electrolyte interface, and the performance of the zinc ion battery.
Traditional nanofiltration membranes face challenges such as membrane fouling and difficulties in achieving precise separation of small organic molecules. A promising solution to these issues is the preparation of thin-film nanocomposite membranes. In this study, Cu and Ag bimetals were incorporated into covalent organic frameworks to fabricate thin-film nanocomposite membranes. The hydrophilic monomer 1,3,5-tris(4-aminophenyl) benzene of covalent organic frameworks was introduced as a water phase monomer during interfacial polymerization to enhance the organic–inorganic compatibility. The incorporated covalent organic frameworks within the thin-film nanocomposite membrane loosened the selective layer, resulting in an enhanced permeability of 24.6 LMH bar−1. The membrane exhibited a rejection rate over 99.0% for Congo Red, Xylene Brilliant Cyanine G, and Reactive Blue, while exhibiting relatively low rejection rates of MgCl2 and NaCl. Moreover, the outstanding catalytic capability of the incorporated bimetals led to a 4-nitrophenol conversion rate of 84.38%, enabling simultaneous conversion and separation. The integration of covalent organic frameworks and bimetals also imparted robust antibacterial properties, significantly enhancing operational stability. In conclusion, the covalent organic framework-Cu/Ag-based thin-film nanocomposite membrane demonstrated superior catalytic and separation capabilities, presenting a promising alternative for advanced filtration applications.
Transition metal phosphides exhibit excellent efficiency in the oxygen evolution reaction under alkaline conditions, and they have garnered widespread recognition. Currently, most studies have focused on the evolution and role of metal cations in the oxygen evolution reaction process, while attention to phosphorus elements is relatively scarce. Actually, phosphides possess unique properties that distinguish them from other metal compounds, and the role of phosphorus in them cannot be ignored. This study used nickel phosphide (Ni2P) as a model catalyst to reveal the reconstruction and dynamic behavior of anions under alkaline conditions through cyclic voltammetry. The results indicate that as the cycle progresses, surface phosphides are converted into active oxyhydroxides. It is worth noting that the presence of the P element accelerates the rapid completion of the reconstruction process but also exhibits triple synergistic functions. First, the internal phosphorus nuclei of the active layer act as conductive scaffolds, effectively enhancing the efficiency of electron conduction. Second, the oxygen-containing anions formed in situ on metal hydroxides optimize the adsorption of reaction intermediates. Finally, the phosphorus atoms dissolved in the electrolyte suppress nickel loss, improve stability, and increase the electrochemical activity specific surface area, exposing more active sites. This study elucidates the oxygen evolution reaction mechanism of phosphides from a novel perspective, enhancing comprehension of surface reconstruction phenomena and the characteristics of active sites, guiding the rational design of phosphide pre-catalysts.
Unlike conventional electrochromic devices, Zinc anode-based electrochromic devices (ZECDs) ensure excellent charge balance between the electrochromic layer and Zn anode during the coloring/bleaching by reversible metal deposition/stripping on the Zn anode. Meanwhile, the inherent potential difference between the metal anode and the electrochromic layer can drive the spontaneous coloration/bleaching of ZECDs, featuring energy retrieval functionality. This review discusses the working mechanisms, performance indexes of ZECDs, and the impact of material selection on ZECD performance. Furthermore, we comprehensively summarize the latest research progress of ZECDs in energy storage, smart windows, and multicolor displays. We argue that using high-transparency zinc mesh, additive manufacturing processes, and self-healing electrochromic materials can significantly advance the commercialization of large-area ZECDs. Finally, “electrode-free” device structures, renewable or replaceable electrolytes, and strategies to suppress zinc dendrites are prospected to overcome cost-effectiveness and lifespan issues of ZECDs. This review aims at enabling more efficient and advanced ZECDs for multifunctional applications.
Amorphous metal-based catalysts are highly promising for water splitting due to their abundance of unsaturated active sites. Herein, we report a one-step, surfactant-free synthesis of amorphous nickel nanoparticles (NPs) encapsulated in nitrogen-doped carbon shells (A-Ni@NC) via pulsed laser ablation in liquid (PLAL). The synergistic integration of the amorphous Ni core and a defect-rich N-doped carbon shell markedly enhanced the catalytic activities for both the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), with low overpotentials of 182 mV for HER and 288 mV for OER at 10 mA cm−2 in 1.0 M KOH. Furthermore, the bifunctional catalyst achieved a current density of 10 mA cm−2 at 1.63 V and retained 98.9% of its initial performance after 100 h of operation. The nitrogen-rich carbon shell not only offered abundant active sites and structural protection but also promoted charge transport. Density functional theory (DFT) calculations revealed that N-doping optimized intermediate adsorption energies, while the amorphous Ni core facilitated efficient electron transfer. This green and scalable synthesis strategy provides a promising platform for developing a wide range of transition metal@N-doped carbon hybrid catalysts for sustainable energy conversion applications.
MXene is a promising conductive nanofiller for hydrogels due to its excellent electricity conductivity and water dispersibility. However, MXene is prone to oxidize in the presence of air and water, resulting in a significant loss of conductivity. Polydopamine (PDA) has been coated on MXene to enhance its antioxidation stability via the physical barrier and chemical reducing ability of PDA, which unavoidably causes severe aggregation and a significant decrease in conductivity due to the crosslinking and insulation of PDA. Herein, we propose a facile strategy to construct a highly conductive, stable, and self-healing MXene-based polyvinyl alcohol (PVA) hydrogel by a controlled assembly of PDA and cellulose nanocrystal (CNC). PDA is first formed by oxidation self-polymerization in PVA solution without the presence of CNC and MXene, which can effectively reduce the content of aggregation-inducing groups and avoid the formation of an insulating PDA layer on the surface of MXene. The addition of CNCs results in the easy dispersion of a high content of MXene via hydrogen bonding and electrostatic interactions. The PVA-PDA hydrogel with MXene and CNC as conductive and reinforcing nanofillers (PP-CM) is cross-linked by dynamic borax covalent bonds and shows a conductivity of 7.14 S m−1. The introduction of PDA effectively protects MXene and results in only a 14% decrease in conductivity after 7 days, significantly improving antioxidant stability. This hydrogel also possesses rapid self-healing capabilities, achieving 90.5% self-healing efficiency within 10 min. This versatile approach opens new avenues for the preparation and application of MXene-based conductive hydrogels.
While the instantaneous power of triboelectric nanogenerators (TENGs) has significantly increased, the average power remains unsatisfactory. Achieving a continuous and stable output remains a significant challenge. Herein, a self-excited vibration TENG inspired by woodpeckers is proposed. This structure converts gravitational potential energy into the continuous vibration of a cantilever beam. A dynamic simulation model of the system is established, and the influence of different structural parameters on the motion characteristics and electrical performance is discussed. Meanwhile, the experimental results indicate that the accelerated motion (approximate free-fall motion) is transformed into approximately uniform velocity motion. For a 3 cm2 TENG, the instantaneous power density reaches 2.03 W m−2, and the average power is 127% higher than that of the conventional cantilever beam mode. The proposed self-excited vibration mechanism is a promising approach for enhancing the average power and operational duration of TENGs. It shows great potential in fluid energy harvesting.
Redox mediators (RMs) represent the most promising strategy to address the sluggish kinetics of lithium–oxygen (Li–O2) batteries. To achieve high-energy and cost-effective Li–O2 batteries, carbon materials are typically regarded as ideal cathodes in these systems. However, the impact of their surface properties—which often regulate specific discharge pathways—on the RM-mediated oxygen reduction reaction (ORR) remains unclear. In this study, CNTs electrodes with different surface properties are fabricated. Results suggest that CNTs with more surface defects not only promote the unmediated discharge pathway even in RMs-involved battery systems but also exacerbate the corrosion of carbon cathodes. This, in turn, leads to the undesired accumulation of Li2O2 and Li2CO3 on the cathode surface, which hinders effective and continuous electron transfer between the cathode and RMs, ultimately decreasing the catalytic activity of RMs. As a result, the discharge capacity of the battery is seriously diminished, especially at large current densities. These findings underscore the significance of surface engineering in advancing the performance of RMs-assisted Li–O2 batteries.
This study investigated the efficient conversion of greenhouse gases (GHGs), CO2 and CH4 mixtures, into few-walled carbon nanotubes (FWCNTs) through an optimized single-step and dual-step chemical vapor deposition (CVD) process. In the single-step process for directly synthesizing FWCNTs from greenhouse gases, CO2 concentration, gas flowrates, and H2 addition were identified as factors influencing the growth of FWCNTs. It was demonstrated that minimizing the amounts of CO2 and H2 was essential for achieving complete CO2 conversion because CO2 acts as an oxidizing agent that hinders CNT growth, while an excess of H2 disrupts the chemical equilibrium of the CO2 conversion reaction, leading to side reactions that suppress FWCNTs formation. To overcome these limitations, a dual-step approach incorporating sequential catalytic reactions was developed. In the first step, the Ni/SiO2 catalyst was utilized to facilitate CO2 methanation, reducing CO2 amounts while generating CH4-rich gas. In the second step, CH4 pyrolysis was performed over the FeMo/MgO catalyst, enabling the growth of high-quality FWCNTs. This sequential configuration successfully synthesized FWCNTs under conditions previously unattainable in the single-step process, validating the effectiveness of the dual-step design. The strategic optimization of process parameters and sequential catalytic reactions established a viable route for converting GHGs into valuable FWCNTs.
Micro-sized silicon (mSi) anodes offer high capacity for next-generation lithium-ion batteries but suffer from severe volume changes, causing unstable interphases and poor cycling. Traditional electrolytes derive unstable electrolyte/electrolyte interphases, and flammable solvents pose safety risks. Here, we introduce a non-flammable molten salt electrolyte, which consists of lithium bis(fluorosulfonyl)imide, potassium bis(fluorosulfonyl)amide, and cesium bis(fluorosulfonyl)imide in a mole ratio of 0.3:0.35:0.35 (noted as Li0.3K0.35Cs0.35FSA), that forms an inorganic interphase on mSi, stabilizing the electrode/electrolyte interface. Computational and experimental insights elucidate the FSA− anion decomposition-derived SEI predominantly of LiF, Li3N, Li2O, and Li2S, which exhibits mechanical resilience and low interfacial resistance, effectively accommodating the significant volume expansion of silicon during lithiation/delithiation. As a result, the Li||mSi half-cell achieves 60.7% capacity retention after 100 cycles with 99.5% average Coulombic efficiency. Overall, the Li0.3K0.35Cs0.35FSA electrolyte eliminates flammability concerns while enabling robust cycling performance. This work demonstrates a safe, high-energy battery system by coupling mSi anodes with stable molten salt electrolytes, addressing both interfacial instability and safety challenges in mSi-based lithium-ion batteries.
Anode-free sodium metal batteries hold significant promise for high-energy-density storage but face critical challenges related to sodium deposition dynamics and interfacial instability. Traditional approaches, such as alloy-based current collectors or fluorinated interfaces, often suffer from irreversible volume expansion or corrosive fabrication processes. This study introduces a solvent co-intercalation-mediated in situ sodiophilic interface engineering strategy to overcome these limitations. A graphitized carbon-modified aluminum current collector dynamically regulates interfacial evolution through solvated sodium-ion co-intercalation during initial cycling, prompting the formation of a C-NaF interface with ultralow Na+ adsorption energy. This sodiophilic interface not only facilitates uniform sodium nucleation by providing abundant sodium-philic sites but also encourages the preferential decomposition of anions in the electrolyte, leading to the creation of a robust and NaF-rich solid electrolyte interphase. Consequently, the asymmetric half-cell delivers an ultralow nucleation overpotential (9.7 mV at 0.5 mA cm−2) and maintains an average coulombic efficiency of 99.8% over 400 cycles at 1 mA cm−2. When combined with a Na3V2(PO4)2O2F (NVPOF) cathode, the full cell achieves an energy density of 363 Wh kg−1 with 80% capacity retention after 250 cycles at 0.5 C. This work integrates molecular-level dynamic interfacial engineering with macroscopic electrochemical stability, providing a scalable industrial solution for next-generation battery systems.
Hydrolysis of ammonia borane is deemed as a promising technique for robust hydrogen production, yet its deployment is still restricted due to the sluggish kinetics of the water dissociation step. An appropriate catalyst that can effectively reduce the H2O dissociation barrier is quite desirable for sustainable ammonia borane-to-hydrogen conversion. Herein, an amino pre-coordination confinement strategy is profiled to achieve sub-2 nm ordered PtCo intermetallics uniformly on N-doped hollow mesoporous carbon spheres (O-PtCo/NHMS) for ammonia borane catalytic hydrolysis. Such a confined approach showcases the capacity of preventing nanoparticles from agglomeration and growth for accurate size control and can be extended to other ordered intermetallic systems (e.g. PtFe and PtCu). As for the ammonia borane hydrolysis, the ordered PtCo intermetallics have delivered a five times higher turnover frequency activity of 1264.1 min−1 than that of the disordered PtCo catalyst, together with excellent catalytic durability. Mechanism studies indicate that the ordered PtCo structure promotes the balanced adsorption of H2O and ammonia borane molecules at Co and Pt sites and reduces the energy barrier for the rate-determining H2O dissociation step to boost the ammonia borane hydrolysis. This work provides valuable insights into the rational design of efficient ordered PtM intermetallic catalysts and expands their application in hydrogen production via ammonia borane hydrolysis.
Efficient photocatalytic reduction of CO2 is crucial to decrease the atmospheric concentration of CO2. Pairing this process with H2O2 production is of considerable importance for simultaneously producing value-added chemicals. However, the photocatalysts reported for such a process suffer from a high recombination rate of the surface/bulk charges, as well as inefficient enrichment and activation toward CO2 and O2, resulting in low conversion efficiency even in the presence of organic sacrificial agents and expensive metal co-catalysts. Herein, two 1,3,5-triphenylbenzene-based organic polymers with high ionic density and porosity are prepared through a facile Sonogashira polymerization. The ionic imidazolium sites embedded in the polymeric skeleton provide the two polymers (iCMP-1 and iCMP-2) with adsorptive selectivity for CO2/N2 up to 98–102 at 273 K, facilitating the enrichment of CO2 and O2 molecules around the catalytic centers, thus boosting their catalytic conversion directly from air under solar light (100 mW cm−2). Benefiting from the improved charge separation and broad light absorption, along with high CO2 and O2 uptake, iCMP-2 can deliver excellent CO and H2O2 yields (611.8 and 810.6 μmol h−1 g−1, respectively) under an atmosphere composed of water vapor and air without any co-catalysts.
Perovskite oxides are highly promising catalysts for the combustion removal of volatile organic compounds (VOCs) due to their excellent stability, structural flexibility, and compositional versatility. This study presents a novel perovskite oxide that exhibits enhanced catalytic activity and superior durability for toluene combustion at reduced temperatures. This improvement is achieved by phosphorus doping at the B-site of LaCoO3-δ (LC) perovskite oxide, followed by post-synthesis acid etching for a proper time. The resulting catalyst demonstrates increased specific surface area, higher total pore volume, and enhanced oxygen vacancy concentration both in the bulk and on the surface. Additionally, the activity of surface lattice oxygen species is significantly improved, leading to enhanced catalytic performance in toluene combustion. Notably, the optimized catalyst shows an exceptionally low activation energy (Ea) of 49.3 kJ mol−1, with a T90 reduction of over 214 °C compared to the phosphorus doped LC and 190 °C compared to pristine LC. Phosphorus doping plays a main role in significantly improving the long-term durability, particularly in the presence of CO2 and H2O, while acid etching boosts the catalytic activity. This work introduces a rational and innovative strategy for optimizing VOC oxidation by improving the structure and surface chemical states of perovskite catalysts.
With the growing global energy demand and the pressing need for a clean energy transition, supercapacitors (SCs) have demonstrated significant application potential in electric vehicles, wearable electronics, and renewable energy storage systems owing to their rapid charge–discharge capability, exceptional power density, and prolonged cycle life. The improvement of their overall performance fundamentally depends on the synergistic design of electrode materials and electrolyte systems, as well as the precise regulation of the electrode-electrolyte interface. This review focuses on the key components of supercapacitors, systematically reviewing the design strategies of high-performance electrode materials, outlining recent advances in novel electrolyte systems, and comprehensively discussing the critical roles of interfacial reinforcement and optimization in enhancing device energy density, power performance, and cycling stability. Furthermore, interfacial engineering strategies and innovations in device architecture are proposed to address interfacial degradation in flexible SCs under mechanical stress. Finally, key future research directions are highlighted, including the development of high-voltage and wide-temperature-range electrolyte systems and the integrated advancement of multiscale in situ characterization techniques and theoretical modeling. This review aims to provide theoretical guidance and innovative strategies for material design, contributing toward the realization of next-generation supercapacitors with enhanced energy density and reliability.
Seawater electrolysis has attracted considerable attention in hydrogen production. However, the chloride ions (Cl−) in seawater can corrode metal sites and decrease the lifespans of the oxygen evolution reaction (OER). Herein, we report a reversed-active sites strategy, converting Cl−-affinitive metal sites to Cl−-repellent oxygen sites, for OER in alkaline seawater electrolysis. First, ex/in situ experiments confirm the effectiveness of such a strategy using typical perovskites following the adsorbate evolution mechanism (AEM) or lattice oxygen-mediated mechanism (LOM). Furthermore, the origins of the superior activity and durability of as-prepared La0.3SrCo0.5Fe0.5Ox (La0.3) can be ascribed to higher participation of lattice oxygen in OER, rapid bulk oxygen diffusion, and excellent OH− adsorption kinetics. Hence, an alkaline seawater electrolytic cell with La0.3 as the anode produces 10 mA cm−2 at just 1.57 V and maintains near-constant activity over 150 hours. This work introduces novel concepts for the production of superactive and steady electrocatalysts for the electrolysis of seawater.
Zinc oxide (ZnO) films, as representative piezoelectric semiconductors, have garnered considerable interest in ultrasonic testing. Current research challenges include maintaining the consistency of continuous c-axis orientation and determining the fundamental link between the electrical structure and piezoelectric response. Accordingly, we have proposed ZnO films incorporated with an orientation-inducing layer (OIL), utilizing orientation induction and rapid deposition technology to regulate the growth structure of the ZnO films. Furthermore, the influence of the competitive mechanism between the film growth and lateral diffusion on the film's growth structure has been investigated. Piezoelectric force microscopy (PFM) analysis demonstrated the regulation and enhancement of ZnO piezoelectric polarization by the OIL. The enhancement mechanism of OIL on film performance was revealed via experimental examination of the film structure, morphology, crystallization orientation, oxygen vacancies, carrier concentration, band structure, and density of states based on density functional theory (DFT). Benefiting from the superior electromechanical response of the ZnO OIL sensor, characterized by fast response recovery times of 2.4 ms/7.7 ms and a sensitivity of 1.09 V/N, the device has successfully demonstrated practical applications in both motion pressure detection and bolt axial force measurement. These findings provide new insights into the ultrasonic detection for aerospace applications of ZnO OIL piezoelectric devices and demonstrate significant potential for health monitoring in connection systems.
The photovoltaic performance of metal halide perovskite solar cells often respond divergently to environmental conditions during storage. In particular, light exposure can either enhance or degrade device efficiency, yet the mechanisms underlying these antithetical behaviors are still under investigation. In this study, we explore the modulation of the open-circuit voltage (Voc) in triple-cation mixed-halide perovskite solar cells by systematically controlling storage environments. While light intensity exhibits minimal impact during storage, the spectral composition of illumination selectively enhances Voc comprising reversible and irreversible contributions. Structural characterization reveals that prolonged storage degrades the quality of perovskite crystals in the upper region of the perovskite layer, whereas light storage promotes the relaxation of microstrain at the buried interface with a p-type organic layer. This structural reorganization at the interface, accompanied by lattice expansion, accounts for suppressed nonradiative recombination and a corresponding increase in quasi-Fermi level splitting. Consequently, devices fabricated without chemical defect passivation achieve a power conversion efficiency of higher than 40% under indoor lighting conditions after preconditioned by continuous exposure to ambient light during storage. These findings highlight the critical role of controlled light exposure during storage not only in enhancing efficiency, but also in ensuring reproducibility of perovskite solar cell characterization.
The development of atomically dispersed multi-metallic catalysts is imperative for tailoring catalytic performance and elucidating structure–activity relationships. However, synthesizing such precisely engineered architectures while maintaining atomic dispersion of distinct metal centers remains a formidable challenge due to thermodynamic instability and synthetic complexity. We herein propose a topological confinement pre-anchoring strategy via pre-anchoring spatially resolved Zn/Fe dual-metal sources in a structurally engineered metal–organic framework precursor to synthesize atomically dispersed ZnFe bimetallic single-atom catalysts. Extended X-ray absorption fine structure measurements and X-ray absorption near-edge structure reveal that the atomically dispersed Zn/Fe metal sites and electronic redistribution in ZnFe bimetallic single-atom catalysts. The ultrahigh surface area, hierarchical pore, and synergistic effect between Zn/Fe can greatly favor the exposure of the active site, mass transport, and improvement of intrinsic activity. Consequently, the ZnFe bimetallic single-atom catalyst demonstrates superior oxygen reduction reaction performance, achieving a half-wave potential of 0.86 V and delivering a kinetic current density of 10.1 mA cm−2 at 0.85 V versus RHE in 0.1 M KOH electrolyte. These metrics not only surpass those of commercial Pt/C, but also rival the highest-performing catalysts reported to date. The Zn-air battery built with ZnFe bimetallic single-atom catalyst exhibits high power density (278.5 mW cm−2) and specific discharging capacities (657 mAh g−1). This work provides a new design pathway for constructing atomically dispersed multi-metal electrocatalysts for high-performance energy-related applications.
Renewable electricity-driven production of value-added sulfur and H2 via electrocatalytic H2S decomposition represents a sustainable route to conventional thermocatalysis. Both the electrocatalyst and electrolyte solution strongly impact the H2S decomposition performance. Despite significant progress in developing sophisticated electrocatalysts, a well-designed electrolyte solution in conjunction with industrial catalysts is an attractive strategy to advance the industrialization process of electrocatalytic H2S decomposition, but remains unexplored. Here, for the first time, we design a solid–liquid–gas three-phase indirect electrolysis system based on a kind of CS2-N electrolyte solution and Ni-Mo2C that can efficiently enable H2S decomposition into valuable H2 and sulfur. Specifically, the solid-phase Ni-Mo2C as a heterogeneous redox mediator presents excellent electrocatalytic efficiency for the H2S removal efficiency of up to 99%, and the formation of liquid-phase sulfur product (CS2-N electrolyte solution dissolves sulfur, yield up to 95%) with the generation of gas-phase H2 product (~1.32 mL min−1), resulting in an interesting three-phase indirect electrolysis system. Remarkably, it enables the scale-up production (~6 g in a batch experiment) of sulfur with continuous operation for 120 h without attenuation. This work may inaugurate a new electrocatalytic H2S decomposition avenue to explore porous metal materials and electrolyte systems in simultaneous production of value-added sulfur and H2.
Magnesium batteries are attracting growing interest as next-generation energy storage technology due to their high safety, cost-effectiveness, and resource abundance. However, their development remains limited by sluggish Mg2+ transport kinetics at the electrode/electrolyte interface. Herein, we propose an electrolyte design strategy that modulates the Mg2+ solvation structure by introducing tetrahydrofuran (THF) as a co-solvent into a borate-based electrolyte, Mg[B(hfip)4] (MBF) in dimethoxyethane (DME). THF, selected from a series of linear and cyclic ethers, has a comparable dielectric constant and donor number to DME, but its cyclic structure introduces steric hindrance that induces competitive coordination with Mg2+. This competition weakens Mg2+ − solvent interactions, yielding a more labile solvation structure and enhanced desolvation kinetics. As a result, Mg||Mg cells employing the optimized MBF/1D1T electrolyte (DME: THF = 1:1, v:v) exhibit a significantly reduced Mg plating/stripping overpotential of 120 mV at 10 mA cm−2, compared with 316 mV at 8 mA cm−2 with MBF/DME, along with exceptional cycling stability exceeding 1200 h. Furthermore, representative sulfide cathodes such as CuS and VS4 demonstrate faster activation and improved high-rate performance in the presence of MBF/1D1T.
The irreversible interfacial side reactions of lithium-rich layered oxides at high voltage lead to deterioration of cycling performance. Herein, we construct a Ce3+-rich surface layer on the lithium-rich layered oxides surface. Owing to the strong chemical affinity between rare-earth elements and oxygen, the Ce-rich spinel surface layer is completely encapsulated around the lithium-rich layered oxides particles. Also, an excess of Ce3+ leads to the formation of LixCeO2−y nanoparticles, which are adorned on the surface layer. This surface modification lowers the work function, promoting the formation of a thin, inorganic-rich, and uniform cathode–electrolyte interphase. Consequently, this layer mitigates the dissolution of transition metals and enhances the stability of the surface lattice oxygen. Consequently, the LLO@Ce cathode demonstrates a high-capacity retention of 93.12% at 1 C after 500 cycles. This work presents a promising path for stabilizing the surface of lithium-rich layered oxides, thereby enhancing its cycling performance for high-energy-density lithium-ion batteries.
Electrochemical carbon dioxide reduction reaction (CO2RR), powered by advanced technologies such as solid oxide electrolysis cells (SOEC), is a promising method to convert CO2 into valuable carbon-based products using renewable electricity. The high chemical stability of CO2 requires catalysts to exhibit both high activity and stable electrocatalytic performance. However, catalysts that deliver high performance in CO2RR are rare and still require further improvement. Here, we report a strategy that can efficiently enhance catalyst activity through Zn doping, which introduces active frustrated Lewis pairs (FLP) to improve the catalyst's ability to activate small molecules. A high current density of −1.85 A cm−2 at 800 °C under a bias voltage of 1.5 V was achieved using the Sr2Fe0.8Zn0.2MoO6-δ (SFZn0.2M) cathode with pure CO2 feeding gas, surpassing previously reported results for perovskite oxide cathodes. This SOEC device also demonstrates excellent stability, with negligible degradation over tests lasting up to 110 h.
Capacitor-related energy storage devices with high power density, excellent cycle stability, wide operating temperature range, and environmental friendliness have enjoyed great popularity. However, the relatively poor energy density hinders their practical large-scale application. Electrospun carbon-based materials are ideal candidates owing to their large specific surface area (SSA), affluent porosity, high conductivity, good flexibility, and stable chemical properties. Therefore, this review provides the research progress of electrospun carbon-based materials for conventional and hybrid supercapacitors in recent years. First, the electrospinning technology is briefly introduced, and then the research progress of various electrospun carbon-based materials for conventional and hybrid supercapacitors is reviewed. Finally, the problems faced by electrospinning technology and developing electrospun carbon-based materials for conventional and hybrid supercapacitors are summarized and prospected. It is expected to provide some ideas for developing new high-performance electrospun carbon-based materials for conventional and hybrid supercapacitors.
All-optically controlled artificial synapses for neuromorphic vision offer unique advantages in simplifying circuit design and minimizing power consumption, meeting the application demands of the current artificial intelligence era. However, developing all-optically controlled devices that combine high performance and high reproducibility remains a significant challenge. In this work, we demonstrate an all-optically controlled artificial synapse based on ZnO and Cs2CoCl4 single crystal connected structure, which integrates light information sensing and processing capabilities. Relying on the simple series-connected structure, as well as the positive photoconductance of ZnO and the negative photoconductance of Cs2CoCl4, the optically controlled bidirectional synaptic plasticity is realized under ultraviolet and visible light stimulation without additional voltage modulation in the all-optically controlled synapse. In addition, leveraging its ultraviolet-enhanced feature extraction and visible-suppression capabilities, the all-optically controlled synapse can act as denoising units in bioinformation preprocessing and weight-updating units in feature recognition. The proposed all-optically controlled synapses exhibit excellent information perception, low-level noise reduction, and high-level cognition functions for bioinformation recognition under complex light conditions. We believe that this work can provide structural-level insights and inspirations in the design and fabrication of all-optically controlled synapses to promote the application for efficient neuromorphic vision in the future.
Conductive cotton fabrics have emerged as promising platforms for advanced wearable applications, including strain sensing, electrical heating, and photothermal conversion. However, their widespread adoption is hindered by several critical limitations: dependence on petroleum-based materials, inherent hydrophilicity, and insufficient durability in practical environments. To overcome these challenges, an eco-friendly, mussel-inspired conductive coating system comprising tannic acid, cellulose nanofibers, and carbon nanotubes is developed. Through a facile dip-coating approach followed by in situ tannic acid polymerization-induced surface roughening and octadecylamine modification, a superhydrophobic conductive cotton fabric combining exceptional flexibility, breathability, and environmental stability is fabricated. The resulting superhydrophobic conductive cotton fabric demonstrates outstanding strain-sensing performance, featuring a rapid response time (127 ms) and reliable signal output over 4000 stretching cycles, capable of precisely detecting various human motions even underwater. Furthermore, the superhydrophobic conductive cotton fabric achieves impressive electrothermal (103.9 °C at 15 V) and photothermal (104.2 °C at 350 mW cm−2) conversion efficiencies with excellent temperature controllability. This multifunctional fabric presents a sustainable solution for next-generation wearable electronics and intelligent thermal management systems, addressing both environmental concerns and performance requirements for real-world applications.
Owing to its excellent eco-friendliness and facile water elution properties, aluminum-based lithium adsorbents have attracted a surge of interest for selectively extracting Li+ from Salt Lake brines, which account for more than 60% of the global lithium resources. However, structural collapse, facile deactivation during desorption process, and ultra-low actual adsorption capacity limit its further large-scale application, particularly in low-grade sulfate-type brines. Herein, considering its advantages, limitations, and structural features, the structural collapse of the aluminum-based lithium adsorbent was effectively suppressed by the in situ intercalation of VO3− and V2O74− into the interlayer of [LiAl2(OH)6]+. Evidently, the initial adsorption capacity and of as-configured adsorbents powder are 14.96 mg g−1 and 192.42 in real sulfate-type West Taijinar Salt Lake brines following NaCl salts removal with 800 mg L−1 Li+ and 9.56 g L−1 SO42−. Furthermore, the initial and retained adsorption capacities of these novel adsorbents granulate in brines after 100 adsorption/desorption cycles are 26.68 and 10.36 mg g−1, respectively, which are almost 10 times higher than those of industrially utilized products. Based on experiments and density functional theory calculations, the process and mechanism of anion intercalation control were preliminarily elucidated. Furthermore, research findings indicate that intercalated anions can influence not only interlayer interactions but also the backbone strength of LDH-type adsorbents. This work significantly overcomes the major utilization challenges of aluminum-based lithium adsorbents, thereby enabling the high-efficiency and stable extraction of Li+ from low-grade brines, including sulfate-type brines.
Metal–organic framework (MOF)-derived porous carbon has attracted particular attention in the electrochemical energy storage field, of which the key is the design and preparation of electrode materials with adjustable porosity and defects for supercapacitors. Here, a novel strategy of coating ZIF-8 with coal tar pitch (CTP) is presented to tailor the porosity and defects of derived porous carbon, by which the inward contraction of ZIF-8 is prevented to enlarge the ultra-micropores, and the defects of ZIF-8-derived carbon are repaired to form a continuous conjugated network. The tradeoff between porosity and electrical conductivity endows this novel hard/soft carbon electrode with fast ion/electron diffusion, achieving high yet balanced capacitance and rate performance of a top-level specific area-normalized capacitance (40 μF cm−2) and a capacitance retention of 52.1% at a 1000-fold increased current density. Meanwhile, the novel electrode realizes a high capacitance of 704 F g−1 at 1 A g−1 and capacitance retention of 91.9% after 50 000 cycles in KOH + PPD electrolyte. This study provides an effective approach to designing novel hard/soft carbon with tuned porosity and carbon defects from MOFs and CTP for supercapacitors and other metal-ion batteries.
The promising prospects for all-day building thermal management are driving widespread research into spectrally selective manipulation materials. This article first summarizes the evolution path of metal reversible deposition technology, noting its advantages of cost-effectiveness and scientific rigor. It then highlights the groundbreaking work by Wang et al. (published in ACS Energy Letters, 2025, 10, 3231) on coupling metastructured photothermal conversion electrodes and reversible Cu deposition for all-day energy management. Finally, the commercial viability of Wang et al.'s approach for building energy saving and its potential applicability to other scenarios are elaborated.