Harnessing the synergistic interactions between adjacent bimetallic atoms, dual-atom catalysts (DACs) emerge as promising candidates for the CO2 reduction reaction (CO2RR). However, precise regulation of neighboring effects at dual-atom sites to optimize and enhance CO2RR performance remains highly challenging. This review focuses on Fe-, Co-, Ni-, and Cu-based DACs, systematically elucidating how proximity effects modulate reaction intermediates and product selectivity in both homonuclear and heteronuclear systems. The distinct electronic configurations of homonuclear and heteronuclear DACs lead to diversified CO2RR pathways and product distributions. When the two metal atoms are spatially separated, the weakened electronic coupling primarily lowers the energy barrier for C1 intermediates, thereby improving the selectivity toward C1 products. In contrast, a reduced metal–metal distance strengthens interatomic electronic interactions through the formation of N/O-coordinated or direct metal–metal structures, facilitating C─C coupling and thus enhancing C2 product formation. A mechanistic understanding of C─C coupling serves as a fundamental basis for directing CO2RR toward multi-carbon products with higher energy density and practical relevance. Additionally, theoretical investigations provide valuable insights into structure–activity relationships, offering guidelines for the rational design of efficient DACs for CO2RR.
Organic materials are highly compelling candidates for next-generation electrodes. However, low mass-loading and poor cycle stability in aqueous electrolyte during repetitive charge-discharge process significantly undermine its practical deployment. Here, indanthrone (IDT), characterized with extended conjugated π-system and rigid planar structure, was developed as a high-performance proton-storage material. Electrochemical analyses and theoretical calculations identify two carbonyl (C=O) and two imine (C = N) groups as the active proton-hosting sites. Importantly, two additional carbonyls flanking the imines remain inactive owing to intramolecular hydrogen bonds, which enhance the chemical and electrochemical robustness of IDT and underpin extended cycling. As a result, a full MnO2@GF//IDT cell delivers ultra-stable operation for over 20,000 cycles at a high mass loading of 8 mg cm-2, demonstrating durable performance and practical relevance. These results establish a structure-function blueprint for organic proton batteries and highlight IDT as a promising, scalable proton-storage material.
Heteroatom modification effectively tailors the electronic structure of the p-block metal for CO2 reduction reaction, but the p-orbital hybridization of sulfur-induced in the electroreduction process remains unclear. Here, an in-situ electrochemical modification approach is developed to tailor bismuth catalysts coordinated with sulfur atoms. The pronounced interaction between bismuth and sulfur p orbital optimizes the electronic states for efficient CO2 electroreduction, achieving high Faradaic efficiency of 95.5% for formate and near 100% selectivity for C1 products, while maintaining 93% formate Faradaic efficiency under pH-universal electrolytes. In-situ characterization and theoretical calculations reveal a descriptor-based design principle, wherein tuning the sulfur atom configuration modulates bismuth p-orbital delocalization with an optimized p-band center, thereby reducing energy barrier for formate generation. Based on the fundamental insights, a solar-driven CO2-H2O electrolyzer was constructed with a FEformate of 93.7% and an energy conversion efficiency of 13.9%. This work establishes an electronic structure design strategy based on p-orbital delocalization modulation, offering theoretical insights and practical guidance for developing advanced main-group metal electrocatalysts.
Freshwater scarcity and industrial wastewater pollution present dual challenges that severely hinder sustainable development. Solar-driven interfacial evaporation (SDIE) strategy, combined with heavy metal ion removal, offers a cost-effective solution for wastewater purification by harnessing solar energy. Herein, inspired by the integration of photothermal conversion and adsorption capabilities, a multifunctional aerogel (r-WCTOA) evaporator was engineered by introducing oxygen vacancies in WO3 (r-WO3-x) to enhance its photothermal conversion efficiency, followed by compositing with wastepaper-derived cellulose. The enhanced localized surface plasmon resonance (LSPR) of r-WO3-x particles, coupled with the porous structure of a cellulose fiber substrate exhibiting excellent mechanical integrity, enables efficient light absorption up to 92.89%. The r-WCTOA evaporator achieves an average water evaporation rate of 1.812 kg m-2 h-1 with a desalination efficiency of 99.8% under one sun irradiation. Additionally, r-WCTOA evaporator demonstrates superior heavy metal removal capacity with a maximum Pb2+ adsorption performance of 171.86 mg g-1, producing purified water that meets WHO drinking water standards. Notably, the freshwater recovered from evaporated leachate could be directly reused for subsequent irrigation, ensuring a sustainable and resource-efficient remediation cycle. This multifunctional r-WCTOA evaporator with porous structures synergistically achieves efficient wastewater purification and heavy metal removal during solar-driven evaporation, providing a scalable, cost-effective and eco-friendly solution for solar water treatment systems.
We report the defect-related luminescence properties and non-powered UV detection capabilities of Sm3+ and Pr3+-doped Ca2SnO4 (CSO:RE, RE = Sm and Pr) phosphors. Under UV excitation, CSO:RE exhibits distinct orange and deep-red emissions due to characteristic 4f–4 f transitions of RE3+ ions. Comprehensive long-persistent luminescence (LPL), thermoluminescence (TL), and optically stimulated luminescence (OSL) measurements confirm the presence of thermally and optically responsive trap states. Notably, our samples demonstrated highly stable OSL signals even after 504 h of storage in a dark environment, evidencing excellent information storage retention. Finally, leveraging these properties, we demonstrate battery-free UV-dose detectors that operate under ambient sunlight and enable optical readout. Our approach requires zero operational energy, avoids battery- and wiring e-waste, and minimizes maintenance. Furthermore, robust oxide host combined with elastomeric encapsulation ensures outdoor durability and solid validation on solar-exposure mapping.
The trade-off effect of polymer membranes induced by molecular chains entanglement and tight packing remains a key bottleneck restricting their widespread application in the carbon capture field. This study fabricates a novel facilitated transport mixed matrix membrane by employing polyethylene oxide (PEO) as the continuous phase and poly (p-phenylenediamine) (PpPD) as the dispersed phase through an in-situ polymerization strategy. Low-concentration of PpPD nanoparticles can be uniformly dispersed in the PEO cross-linked network, which not only modulates the PEO chains packing, restricting its segmental motion, but also significantly enhances the CO2/N2 separation performance of the membrane via CO2-philic amino groups in PpPD. This strategy effectively avoids the interfacial defect between PpPD fillers and PEO matrix in traditional technology, and the optimized membrane of IP/PEO achieves CO2 permeability of 721.5 Barrer and CO2/N2 selectivity of 49.0, which exceeds the 2008 Robeson upper bound.
Understanding the microscopic mechanism of interfacial charge transfer is crucial for optimizing the performance of triboelectric nanogenerators (TENGs). Here, a combined first-principles density-functional theory and experimental study reveals how polymer polarity and chemical composition regulate charge transfer at PVDF/polymer interfaces, including Nylon, PDMS, PVC, PE, PTFE, and FEP. The results demonstrate that polar β-PVDF/polymer heterostructures exhibit substantially stronger interfacial charge transfer than nonpolar systems, driven by the intrinsic built-in electric field of β-PVDF. The transferred charges primarily originate from the functional groups of the polymers, and the charge transfer magnitude follows the sequence β-PVDF/Nylon > β-PVDF/PDMS > β-PVDF/PVC > β-PVDF/PE > β-PVDF/PTFE > β-PVDF/FEP, corresponding to electron flow from low work function polymers toward the high work function β-PVDF. Furthermore, these theoretical trends are supported by experimental results, which confirm that β-PVDF-based TENGs deliver higher electrical outputs than α-PVDF-based systems and follow the same material-dependent sequence. This work elucidates the polarization-driven and material-dependent mechanisms of interfacial charge redistribution, providing design principles for high-output and controllable TENGs.
Catalytic CO2 hydrogenation to light olefins and single hydrocarbons represents a crucial pathway for achieving carbon neutrality and sustainable chemical production. Oxide–zeolite (OX-ZEO) catalysts have shown remarkable potential due to their high selectivity for target products. However, a systematic understanding of their active sites remains notably underdeveloped. This review provides a comprehensive analysis of the active sites in OX-ZEO catalytic systems for CO2 hydrogenation to light olefins and single hydrocarbons. For the oxide components, we critically examine the controversial nature of active sites in metal oxide, including oxygen vacancies, special electronic state metal ions and dual-site synergy, with special focus on the debated ZnZrOx system. For zeolite, we analyze the relationship between zeolite properties and product distribution, including acid location and acid property. Significantly, we emphasize the interactions between oxide and zeolite components and their influence on catalytic behavior. Finally, we point out that future catalyst design should focus on understanding and utilizing the interactions between active sites.
The global freshwater crisis, intensified by population growth and climate change, has spurred the demand for sustainable desalination technologies. Traditional desalination methods are hindered by high energy consumption and operational costs, whereas solar-driven interfacial evaporation (SIE) technology offers a green and efficient alternative by localizing solar energy at the gas–liquid interface for water evaporation. This review systematically summarizes the working mechanisms of SIE, including photothermal conversion materials and water transport/evaporation processes. The review first summarizes design strategies of SIE systems, encompassing high-performance photothermal materials, water transport materials, and matrix structures, along with key performance metrics such as evaporation rate, photothermal efficiency, and long-term stability. It then explores the practical applications of SIE in seawater desalination, wastewater treatment, and emerging fields like steam sterilization and agricultural irrigation. Finally, it addresses current technical challenges, including efficiency limits of photothermal conversion, long-term stability in harsh environments, and cost-effective scaling, and outlines future trends in novel material development, multifunctional system integration, and intelligent optimization. This work provides a comprehensive perspective on the development of SIE technology as a promising approach to alleviating water scarcity.
Silicon–carbon (Si/C) anodes, as an attractive alternative to traditional anode materials, have been extensively studied for lithium-ion batteries (LIBs). Nevertheless, their widespread application still faces several key obstacles, including low initial Coulombic efficiency (ICE) and a fast capacity decay rate. Pre-lithiation as an effective strategy has been widely used to address these issues through compensating for active lithium loss. This review comprehensively analyzes the failure mechanisms of Si/C anodes during cycling, including structural degradation, SEI instability, and kinetic constraints. The recent pre-lithiation progresses are evaluated in three categories based on the different manufacturing stages: pre-lithiation during active material synthesis, pre-lithiation during electrode fabrication, and pre-lithiation after full-cell assembly. This classification integrates pre-lithiation strategies and industrial production workflows, enabling a systematic evaluation of the relationships between cost, lithium utilization efficiency, and battery performance. Novel techniques such as dry pre-lithiation, bifunctional electrolyte additives, and topological intercalation are also investigated for their contributions to improved ICE, cycling stability, and energy density. Although significant progress has been made, obstacles related to the degree of pre-lithiation, lithiation uniformity, and process compatibility continue to restrict the large-scale application of Si/C anodes. Finally, a detailed analysis of these challenges in Si/C anodes is provided, and future development prospects are discussed for next-generation LIBs with enhanced performance and expanded commercial viability.
Moisture-electric generation (MEG) holds promise for sustainable energy, but it usually suffers from low output and poor stability. Herein, we report a high-performance MEG device fabricated by depositing aminated carbon dots (CDs) onto a flexible fabric substrate. A key improvement involves a thermal-induced crosslinking strategy, where heat treatment triggers covalent bonding between aminated CDs and the substrate. This process creates a stable network that enhances interfacial adhesion, removes inactive groups, and inhibits CDs migration, thereby promoting sustained moisture adsorption and efficient hydroxide ion transport, collectively boosting electrical output and device stability. Consequently, the thermal treated device delivers a markedly increased output voltage of 0.90 V, surpassing the 0.56 V of the untreated control. Moreover, the device exhibits outstanding flexibility, wash fastness, and long-term durability, maintaining stable electrical output for up to 120 h. We further demonstrate that multiple devices can be integrated into a scalable power system via series/parallel circuits, highlighting their practical potential for real-world energy harvesting.
The selectivity of the oxygen reduction reaction (ORR) is critical for energy transformation efficiency of metal–air batteries or the synthesis of hydrogen peroxide. Hence, we report a coordination-engineering strategy for cobalt single-atom (CoSA) catalysts anchored on carbon nanotubes, which enables accurate adjustment of the coordination structure of Co centers via sulfur doping. By modulating the first coordination shell (Co─NxSy), the two-electron reduction ORR pathway on CoSA can be facilitated. Specifically, the Co─N2S2–coordinated catalyst (CoS@CoSA/NS-CNT/CC) achieves an onset potential of 0.73 V with average Faraday efficiency (FE) of H2O2 for 88% within the 0.35–0.55 V potential window. In contrast, the catalyst with Co─NS3 coordination (CoS2@CoSA/NS-CNT/CC) exhibits a higher onset potential of 0.78 V but a lower FE of H2O2 for only 48%. Through combined theoretical and experimental analyses, including XAS and in situ ATR-FTIR, we demonstrate that sulfur doping modulates the electronic configuration of CoSA, thereby optimizing the adsorption behavior of the *OOH intermediate, leading to > 90% H2O2 selectivity and showcasing performance that compares favorably with the top-tier catalysts known for acidic electrosynthesis of H2O2.
The proton exchange membrane fuel cell (PEMFC) converts clean hydrogen's chemical energy into electricity and is vital for carbon neutrality. However, its development is limited by low volumetric power density and high cost. Thickness-reduced composite bipolar plates (CBPs) offer a promising solution to boost power density and reduce costs. CBPs are critical PEMFC components, comprising 70%–80% of the stack's volume and weight, and function for current collection, gas separation, and mechanical support. On this basis, this review explores strategies to achieve thickness reduction in CBPs from the perspectives of material, structure, and manufacturing processes, analyzes the primary factors influencing CBP thickness and key performance metrics starting from the theoretical minimum thickness limitation, and proposes enhancement approaches to improve the electrical conductivity, mechanical properties, and gas barrier properties of CBP following thickness reduction. The conductivity is improved by optimizing carrier transport, and the influence of material interface modification on gas permeability is analyzed. The design innovation of novel biomimetic structures optimizes the mechanical properties. By synthesizing these perspectives, this review offers valuable insights for reducing thickness and optimizing the performance of CBPs.
Enzymes are widely employed in bioprocesses as catalysts to enhance biofuel and value-added compound (VACs) production. To improve product yield in these processes, researchers are working on various methods. Among them, nanobiocatalysts (NBCs) are promising, in which enzymes are immobilized onto a nanocarriers. This facilitates improvements in the activity, stability, and recyclability of the immobilized enzymes and reduces the cost of the treatment process. Different nanocarriers, such as organic, inorganic, hybrid, and functionalized materials, have gained attention for immobilizing single and multiple enzymes. Exploiting NBCs to improve hydrolysis, fermenting the substrate to produce biofuels such as bioethanol and biohydrogen, and enhancing the transesterification process for biodiesel are discussed. The role of NBCs in the bioconversion of various substrates to generate VACs and the use of single and multienzyme cascade systems for biotransformation are discussed. The review critically evaluates the efficiency of current nanobiocatalytic systems and highlights strategies to enhance their performance for practical applications. Finally, the review concludes by highlighting the challenges NBCs face in real-time implementations and outlining possible areas for NBC applications in biorefineries.
Solar photocatalysis emerges as a promising solution for sustainable energy conversion and valuable chemical production. However, its efficiency remains limited by three fundamental challenges: suboptimal light harvesting, rapid charge recombination, and sluggish surface redox kinetics. Recent breakthroughs have established electron spin control as a transformative paradigm, achieved through controllable modulation of intrinsic photocatalyst properties (e.g., elemental doping), heterojunction construction, and external fields induction (e.g., magnetic field). These approaches primarily enhance charge separation via spin polarization and improve surface reaction kinetics, thereby improving photocatalytic performances. This minireview systematically outlines the fundamental principles of spin-dependent processes in photocatalysis, with a focus on recent advances in spin effects across various applications, including photocatalytic water splitting, CO2 conversion, environmental remediation, organic synthesis, and H2O2 production. The underlying mechanisms linking electron spin to enhanced photocatalytic activities are discussed in detail. Finally, this review concludes with a summary and future perspectives on spin-mediated photocatalysis, aiming to provide a comprehensive understanding of the spin effect and its regulation for improved photocatalytic applications.
With environmental issues intensifying, such as global warming and ocean acidification, the development of low-carbon energy has become an urgent imperative. Hydrogen, as an ideal zero-carbon energy source, has received widespread attention. Among various hydrogen production processes, water electrolysis is a promising way for large-scale green hydrogen production. As a key half-reaction in water electrolysis, the hydrogen evolution reaction (HER) requires efficient electrocatalysts to maintain hydrogen production efficiency under the harsh conditions. Transition metal phosphides (TMPs) have emerged as crucial candidates to replace noble metal platinum-based catalysts due to their low cost, abundant reserves, tunable electronic structure, excellent electrical conductivity, and performance comparable to that of noble metals. However, TMPs face several bottlenecks in alkaline media, such as sluggish water dissociation kinetics and mismatched adsorption energy of hydrogen intermediates. Therefore, this review summarizes the synthesis methods and regulation strategies of TMPs, offering critical insights into overcoming the core challenges of TMP-based electrocatalysts for alkaline HER, which can accelerate the development of cost-effective green hydrogen production technologies.
Achieving fast and reversible sodiation/desodiation in MXene materials remains an eye-catching yet unresolved challenge. This work introduces a benzaldehyde-welded Ti3C2 MXene (Ti3C2–BD) as a high-performance anode material for sodium-ion batteries (SIBs). This functionalization boosts electrochemical activity and structural stability while directly addressing key limitations like interlayer stacking and rapid performance degradation. With these advantages, the Ti3C2–BD anode delivers a specific capacity of 54.5 mAh g-1 at 10 A g-1 and retains 51.1 mAh g-1 after 2500 cycles at 5 A g-1, demonstrating exceptional rate capability and cycling stability. In full-cell systems, Ti3C2–BD achieves an energy density of 205.3 Wh kg-1. Structural and kinetic analyses reveal its stable architecture, superior Na+ ion adsorption, and favorable diffusion kinetics. This study offers a strategic approach for designing MXene-based anodes with high capacity, rate capability, and long-term stability, providing both theoretical and practical advancements in SIBs technology.
MnO2 has been considered as a promising cathode for aqueous zinc-ion batteries (AZIBs) due to its environmental benignity, low cost, and high theoretical capacity. However, the severe Mn2+ dissolution and sluggish interfacial reaction kinetics of MnO2 dramatically impede its practical applications. Herein, the phytic acid anion-functionalized MnO2 (PCA-MO) cathode with electron-rich surface is reported for high-performance AZIBs. Specifically, phytic acid anion with lone pairs of electrons can increase surface charge density and form stronger interactions with Zn2+, achieving interfacial Zn2+ enrichment and promoting charge transfer. Moreover, the phytic acid anion layer acts as a protective barrier, preventing direct contact between the electrode and the electrolyte, thereby effectively suppressing Mn2+ dissolution. Therefore, the PCA-MO delivers high specific capacity (332 mAh g-1 at 0.2 A g-1), superior rate performance (111 mAh g-1 at 5.0 A g-1), and long-term cycling stability for 1000 cycles at 2.0 A g-1. This work provides new insights into developing high-performance Mn-based cathodes for aqueous batteries.
There is a pressing need for efficient, stable, and low-cost electrocatalysts to overcome the core bottleneck associated with the sluggish kinetics of electrochemical energy conversion processes. In response to this challenge, molten-salt synthesis (MSS) has emerged as a powerful, versatile, and scalable strategy for the rational construction of advanced electrocatalysts. Benefiting from its unique liquid-phase reaction environment, MSS enables rapid mass transport and homogeneous reaction conditions. This allows precise regulation of catalyst crystal structure, composition, and electronic properties, while simultaneously facilitating atomic-level dispersion of active species, controllable defect engineering, and well-defined interface construction. These features are crucial for optimizing catalytic activity, selectivity, and stability. In addition, the inherent scalability of MSS makes this approach particularly attractive for the large-scale preparation of functional electrocatalysts. This review systematically summarizes recent advances in the synthesis of various advanced electrocatalysts via MSS, including carbon-based materials, metal oxides, layered double hydroxides, and two-dimensional transition metal dichalcogenides. The catalytic performances of these materials in key electrochemical reactions, such as the hydrogen evolution reaction, oxygen evolution reaction, oxygen reduction reaction, and other related applications, are critically evaluated, with particular emphasis on the underlying structure–performance relationships. Finally, current research gaps, major challenges, and future opportunities in the field are highlighted to provide insights for the rational design and scalable development of next-generation electrocatalysts.
Protonic ceramic electrolysis cells (PCECs) have emerged as a transformative technology for low-cost, large-scale green hydrogen production, owing to their intrinsic high energy conversion efficiency and unique advantages of mid-temperature operation. However, systematic discussion is still lacking regarding the unique characteristics of PCEC systems and the specific implications of these characteristics for material design and operational condition optimization. This review provides a comprehensive and critical assessment of milestone innovative achievements across the entire development chain of PCECs, from fundamental laboratory research to large-scale energy applications. Specifically, it highlights the critical roles of compositional regulation, structural design, and fabrication process optimization in breaking through the core technical bottlenecks, systematically analyzes the physicochemical stability, interface bonding strength, and electrochemical–thermal coupling behavior of electrolyte and electrode components under practical operating conditions, thoroughly explores the engineering application potential from single-cell scale-up, stack design to system integration, and finally discusses the key challenges and future development prospects in the industrial scaling-up process.
Cathodic oxygen reduction for the electrosynthesis of hydrogen peroxide (H2O2) offers a green and decentralized alternative to the energy-intensive anthraquinone process. However, its development has been largely confined to alkaline electrolytes, limiting practical application. Designing active and selective catalysts for neutral media is therefore crucial. Herein, we report a facile phosphate-activation method to convert low-cost, amino acid-rich soybeans into N, P, O co-doped porous carbon (NPODC). Electrochemical tests in 0.1 M K2SO4 reveal that NPODC-600 exhibits exceptional selectivity for the two-electron oxygen reduction pathway. Structural analysis, in situ characterization, and theoretical calculations confirm the synergistic role of multi-heteroatom doping (N, P, O) and defect structures in optimizing intermediate adsorption. In practical applications, NPODC-600 demonstrated outstanding electro-synthesis of H2O2 ability, with a production rate reaching 8089 mg L-1 h-1. Importantly, after continuous operation in a solid-state electrolytic cell, 7.5 wt% pure H2O2 accumulation was achieved, and rapid synthesis was realized under solar energy drive. This work not only provides a reference for the high-value utilization of biomass but also fully demonstrates the great potential of the two-electron oxygen reduction system in clean energy utilization and H2O2 production.
Developing low-cost and highly efficient S-scheme heterojunction photocatalysts is still a significant challenge towards enhancing the activity of photocatalytic hydrogen evolution (PHE). This study created an S-scheme heterojunction by in situ growing inorganic Al-doped SrTiO3 (ASTO), which possesses superior oxidation capability, on a substrate of the covalent organic framework (TpPa-1-COF), which has great reduction capacity, using a solvothermal method. With the advantages of stronger redox capacity, quicker electron transport, and more potent carrier separation, the optimal 5% ASTO/TpPa-1 S-scheme heterojunction achieved remarkable photocatalytic performance in ascorbic acid (AsA) solution when exposed to simulated solar light, with a hydrogen production rate of 4.12 mmol g-1 h-1, which is 14.2 and 11.4 times higher than that of pure TpPa-1 and ASTO, respectively. This performance outperforms most recently reported SrTiO3-based and TpPa-1-COF-based heterojunctions under similar conditions. Notably, an intense interfacial internal electric field (IEF) in ASTO/TpPa-1 heterojunction was formed resulting from the free electron consumption in TpPa-1 and accumulation in ASTO, which could speed up the transfer dynamics of photoinduced electrons from the conduction band (CB) of ASTO to the valence band (VB) of TpPa-1 via an interfacial electron-transfer channel that follows the directed S-scheme migration process. Moreover, the direction of the IEF is from TpPa-1 to ASTO, which could accelerate charge separation and migration, thereby prolonging the lifetimes of charge carriers. The dynamic behavior of photoinduced carriers was confirmed by femtosecond transient absorption spectroscopy (fs-TAS). Overall, this study provides valuable guidance for the rational design of an innovative organic/inorganic hybrid S-scheme heterojunction.
Mixed-halide (I/Br) wide-bandgap perovskites have emerged as promising top-cell candidates for tandem photovoltaics due to their tunable bandgap and excellent optoelectronic properties. However, halide phase segregation poses a critical challenge to their commercialization, as initially homogeneous perovskite films spontaneously demix into iodide-rich and bromide-rich domains under illumination or electrical bias. This phenomenon leads to severe open-circuit voltage (VOC) losses, efficiency degradation, and compromised device stability. This comprehensive review systematically examines the fundamental origins of halide phase segregation from thermodynamic, kinetic, and defect chemistry perspectives, with particular emphasis on the oxidation-driven irreversible degradation pathways. We survey advanced characterization techniques including transmission electron microscopy (TEM), Kelvin probe force microscopy (KPFM), conductive atomic force microscopy (c-AFM), photoluminescence (PL), and cathodoluminescence (CL) that have provided unprecedented insights into the spatiotemporal dynamics of phase segregation. Furthermore, we critically evaluate multidimensional mitigation strategies encompassing compositional engineering, grain boundary passivation, and interface optimization. This review aims to provide a holistic understanding of halide phase segregation and guide the development of next-generation stable perovskite photovoltaics.
With the rapid deployment of sodium (Na)-ion batteries (NIBs), recycling spent batteries is essential for reducing system cost and improving sustainability. Hard carbon (HC) anodes are particularly valuable recycling targets because of their complex synthesis and high production cost. Here, combined spectroscopic and structural analyses reveal that HC failure strongly associated with irreversible Na accumulation, continuous solid electrolyte interphase (SEI) growth/decomposition, and degradation of closed-pore microstructures. Regeneration of spent HC is therefore intrinsically challenging, because it requires not only complete removal of electrochemically inactive Na-containing residues and parasitic species, but also precise reconstruction of the disordered closed-pore carbon framework that governs Na storage, while avoiding further disruption of its microstructure. Guided by these insights, we develop a green recycling strategy integrating oxalic acid treatment with thermal processing. This approach removes surface deposits and parasitic species, while oxalic acid induces oxygen-containing functionalities and C–O–C linkages that promote carbon framework rearrangement and pore restoration. As a result, the regenerated HC delivers a reversible capacity of 302.6 mAh g-1 with markedly restored rate capability. This work provides a practical pathway for the sustainable regeneration of HC anodes for large-scale NIB applications.
In the last decade, the lithium-rich layered oxides (LLOs) as cathode materials of lithium-ion batteries (LIBs) have attracted considerable research interest owing to the high specific capacity (> 300 mAh g-1), elevated operating voltage, and cost-effectiveness. However, these oxide materials suffer from severe interfacial degradation, capacity fading, and voltage decay, primarily attributed to the poor reversibility of anionic redox reactions. To address these limitations, we proposed a dual-functional modification paradigm combining the surface piezoelectric interphase layer of lithium gallium oxide (LiGaO2) with gradient Ga3+ bulk doping to synergistically suppress lattice oxygen evolution in LLOs. Combined with simulation calculations, multiscale characterization, and electrochemical performance evaluation, this study unambiguously elucidates the underlying mechanism by which the engineered interface suppresses lattice oxygen release. This piezoelectric interphase spontaneously generated a persistent built-in electric field through stress-induced piezoelectric polarization during cycling, thereby dynamically restraining oxygen release at high operating voltages. Moreover, Ga-doping into the subsurface lattice modulated the local electronic configuration and thus enhanced the reversibility of anionic redox reactions, avoiding the limitation of single-strategy approaches that merely address symptoms rather than root causes. Benefitting from these advantages, the piezoelectric interphase modified cathode demonstrated significantly an improved cycling stability with 81.5% capacity retention after 300 cycles at 200 mA g-1, coupled with a substantially mitigated average voltage decay rate of 1.03 mV per cycle (vs. 1.43 mV per cycle for the pristine sample). This work presents the first demonstration of piezoelectric interphase engineering for oxygen redox regulation, providing a new pathway for developing high-energy-density LLOs with a much extended cycling span.
Perovskite solar cells (PSCs) have drawn great attention due to their excellent photovoltaic performance for next-generation photovoltaics on account of their excellent optoelectrical properties, for example, high defect tolerance, strong absorption coefficient, easy processability, and low cost. Although the performance of small-area PSCs has achieved over 27% certified efficiency, approaching that of silicon solar cells, large-scale modules often come with serious issues in device performance and stability reduction. To address these challenges, significant investigations have been made in the development of scale-up fabrication techniques to enhance large-area film uniformity and crystalline properties. In this review, the progress on stabilizing the perovskite structure, optimizing device structure, and encapsulation is discussed to give a deep understanding of film decomposition and device degradation mechanisms. Besides, this review provides an overview of strategies aiming at the delicate fabrication of large-area perovskite films and relevant PSCs and modules while simultaneously improving their stability. The comprehensive understanding of the mechanism of large-area perovskite film deposition and device degradation paves the way for future commercialization of perovskite photovoltaics.
Proton exchange membrane fuel cells (PEMFCs) offer a clean pathway for electricity generation. However, their widespread adoption is hindered by the high cost and insufficient durability of platinum (Pt)-based cathode catalysts. Although non-precious metal single-atom catalysts (SACs) have emerged as promising alternatives, their activity and stability still lag behind practical requirements. An effective strategy to bridge this gap is the construction of hybrid catalysts that couple Pt nanoparticles (NPs) with SACs. This approach simultaneously addresses cost and durability challenges; however, the fundamental mechanisms behind the synergistic enhancement remain unclear, impeding rational design. This review systematically summarizes recent advances in Pt-based NPs/clusters combined with non-platinum single-atom site catalysts/hybrid catalysts (Pt/M@SACs), focusing on how the integration of SACs enhances the sintering resistance, durability, poisoning tolerance, and intrinsic activity of Pt sites. This review focuses on elucidating the underlying mechanisms, including charge transfer, modulation of intermediate adsorption, and alteration of reaction pathways. Finally, we provide perspectives on future research directions, aiming to guide the rational design of next-generation, high-performance, and low-Pt fuel cell catalysts.
The rapid and selective removal of carcinogenic hexavalent chromium (Cr(VI)) from water remains a critical challenge for sustainable environmental remediation. This work reports the elaborate design of oxygen-vacancy-rich MnFe2O4@ZnFe2O4 (MZFO-VO) heterojunction microspheres for highly efficient microwave-assisted Cr(VI) reduction under mild conditions. At an initial pH of ~7, with a catalyst dosage of 2 g L-1 and a temperature of 100°C, the MZFO-VO heterojunction composite achieved complete removal of Cr(VI) from a 50 mg L-1 solution within 35 min under microwave irradiation. Density-functional theory calculations revealed that the introduced vacancies reduced the work function to 4.66 eV, suggesting a lowered energy barrier for bulk-to-surface electron migration. Moreover, Fe–O anchoring sites were identified as the active centers that enable efficient adsorption and reduction of dichromate ions, which is accompanied by significant charge transfer from Fe to the adsorbate. The synergistic coupling of defect-induced polarization and conduction losses, and efficient microwave absorption collectively underpins the high activity and operational stability of MZFO-VO. These findings establish a clear design route for next-generation microwave catalysts and highlight the practical potential of vacancy-modulated ferrite heterostructures for rapid, energy-efficient treatment of Cr(VI)-contaminated water.