Light-assisted catalysis is a promising approach for accelerating the thermally driven catalytic reverse water gas shift (RWGS) reaction, which converts CO2 and H2 into valuable CO. In this work, pure CeO2 nanorods and titanium-modified CeO2 nanorods were functionalized with 1–30 wt.% of copper. The catalyst containing 3 wt.% of copper (3Cu–CeTiO2) was the most active for the light-assisted RWGS reaction. Illuminating the 3Cu–CeTiO2 catalyst with 770 mW cm−2 of visible light resulted in a CO rate, which was up to 57 times higher than that under purely thermal conditions at identical catalyst temperature. Catalyst illumination with wavelengths shorter than 450 nm triggers simultaneous photoexcitation of the Ti-doped CeO2−x support and Cu nanoparticles. This accelerates the RWGS reaction approximately twofold more, compared to excitation of the copper phase alone. Copper is responsible for H2 dissociation, the Cu–Ov–Ce interface active sites enable the catalytic reaction, and titanium doping diminishes emissive recombination, making photoexcitation more efficient. Furthermore, the Ea for CO formation decreased drastically from 92 to 26 kJ mol−1 during the light-assisted reaction, revealing a change of the reaction mechanism and lowered energetics of the rate-determining step. Our kinetic analysis and operando DRIFTS analysis suggest that hydrogen species chemisorb more strongly under illumination, and the most abundant surface species (carbonates and formates) hydrogenate and dissociate faster, resulting in accelerated CO formation.
Amorphous carbon is widely used in energy storage and semiconductor technologies, where surface chemistry critically affects wettability, ion transport, and charge transfer. However, controlling surface oxidation remains challenging, as conventional oxidants indiscriminately modify carbon, degrading the framework and compromising performance. Here, we demonstrate a molecular-level approach to selectively oxidize sp2-rich domains of amorphous carbon using Keggin-type aluminum polyoxometalate (Al-POM)-coated silica nanoparticles. The positively charged Al13(OH)327+ clusters electrostatically interact with sp2 domains and release protons during structural transitions, facilitating proton-coupled oxidation with lower activation energy. This process introduces oxygen-containing groups, enhances interfacial charge transfer, and preserves the carbon framework. Our findings establish Al-POM-coated silica as a molecularly designed strategy for tailoring amorphous carbon interfaces, offering improved performance in both energy and semiconductor applications.
As global energy demand continues to rise, developing sustainable and clean energy technologies has become an urgent priority. Hydrogen production from seawater electrolysis has attracted growing attention as a cost-effective and sustainable approach due to the abundance of seawater as a feedstock. However, during seawater electrolysis, both the oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) are strongly influenced not only by catalyst activity but also by the complex composition of seawater. In particular, the presence of chloride ions and alkaline-earth metal salts such as Ca2+ and Mg2+ reduces efficiency compared with freshwater systems, while the competitive chlorine evolution reaction (ClER) compromises oxygen selectivity and accelerates electrode degradation. To address these challenges, designing corrosion-resistant OER and HER catalysts with high activity and long-term stability is of great importance. This review provides a comprehensive overview of transition metal-based catalysts for seawater electrolysis, emphasizing their reaction mechanisms, degradation pathways, and structural instability caused by poor reaction selectivity. Furthermore, we summarize recent advances in improving catalyst durability through electrolyte modification and electrolyzer design optimization. Finally, we outline key material design principles for developing robust anode and cathode catalysts and present prospects for future research. The insights presented here aim to guide the rational design of highly stable, corrosion-tolerant catalysts for efficient and scalable seawater electrolysis, promoting its practical application in clean energy conversion and storage.
All-solid-state batteries (ASSBs) have emerged as a pivotal direction in next-generation energy storage, driven by their compelling potential for enhanced safety and superior energy density. Among the key enabling materials, solid polymer electrolytes (SPEs) stand out due to their structural tunability, manufacturing scalability, and robust interfacial contact, offering a viable pathway toward practical ASSBs. This review systematically bridges the gap between molecular-level design and macroscopic performance of SPEs. It begins by establishing the structure–property relationships underpinning different SPE categories, and then critically assesses conventional and emerging processing techniques in relation to their electrochemical and mechanical performance. Furthermore, the article synthesizes current challenges and strategic solutions for optimizing SPEs, with an emphasis on integrated approaches that balance ionic conductivity, interfacial stability, and processability. By presenting a coherent technological landscape, this work aims to guide the rational design of SPE materials to accelerate the development of reliable, high-performance ASSBs.
Carbon/silicon (C/Si) heterojunction solar cells have recently achieved power conversion efficiencies exceeding 23% for small-area (6 cm2) devices. The development pathway toward these results highlights the critical requirements for engineering efficient contacts and heterojunction structures in next-generation photovoltaic technologies. If current performance trends continue, C/Si heterojunctions could provide a viable route to affordable, high-efficiency solar cells. This review examines the main carbon allotropes explored for C/Si junctions, that is, amorphous carbon (a-C), C₆₀ fullerene, graphene, and carbon nanotubes (CNTs) and evaluates their optoelectronic properties, deposition strategies, and device performance. The a-C approach enables low-temperature, scalable processing but suffers from high defect densities and limited carrier mobility. Fullerene derivatives offer favorable energy-level alignment for electron extraction, yet their low conductivity and photochemical instability remain obstacles. Graphene provides reasonable optical transparency, mechanical flexibility, and a tunable work function; however, its relatively high sheet resistance, parasitic optical absorption, and interface recombination cast doubt over its use in high-efficiency solar cells. By contrast, CNTs combine outstanding electrical conductivity, one-dimensional carrier transport, and simple solution-based fabrication, supporting efficient charge separation and extraction when integrated with optimized passivation layers. As a result, CNT/Si heterojunctions consistently outperform other carbon-based architectures, positioning CNTs as the leading candidate for future low-cost, high-efficiency C/Si photovoltaic devices. The review concludes by outlining research priorities in interface optimization and scalable large-area processing.
Solid polymer electrolytes (SPEs) show great promise for solid-state lithium metal batteries but face challenges due to inherently slow ion transport and interfacial instability. In this work, we propose a dipole-matching strategy to engineer an SPE with a compact microstructure and stabilized interfaces. Through combined theoretical and experimental studies, we identify a molecular additive, such as 3,5-bis(trifluoromethyl)benzoic acid (N-CFF), that promotes rapid and uniform nucleation and directs phase alignment via dipole interactions with polymer chains, resulting in a compact microstructure conducive to rapid lithium-ion transport and homogeneous deposition. Simultaneously, the dipole-matched N-CFF creates an electron-rich environment that facilitates the formation of a LiF-rich solid electrolyte interphase, effectively suppressing lithium dendrite growth. Employing this strategy, we fabricate Li||LiFePO4 solid-state batteries that deliver ultra-long cycle life (90% capacity retention after 3000 cycles), exceptional low-temperature and rate performance, as well as improved thermal safety. This work offers a comprehensive interface and microstructure co-design approach to promote the development and application of high-performance solid-state batteries.
The occurrence of unexpected Li plating and dendrite growth on graphite anodes poses significant challenges to the practical application of lithium-ion batteries. While existing studies have highlighted the superiority of elevated temperatures in alleviating Li plating and Li dendrite growth. We enable a comprehensive electrochemical-thermal investigation of the Li plating mechanism at an elevated temperature of 60°C, induced by slight over-lithiation on Li|graphite coin cells. By combining voltage evolution with in-situ heat generation, we identify a distinctive exothermic peak corresponding to the Li plating plateau. Intriguingly, we discover a characteristic exothermic peak during the relaxation stage, attributed to the simultaneous occurrence of Li stripping and re-intercalation, which is beyond our regular cognition and serves as a novel indicator of Li plating. The heat contributions analysis further indicates the weakened Li intercalation heat generation once Li plating occurs. Finally, from the post-mortem characterizations, the surface morphologies, chemical composition, and Li content quantification of the lithiated graphite without Li plating and at different Li plating cycles are obtained to reveal the Li nucleation-growth mechanism. The results demonstrate that a total of 0.540 mg metallic Li is plated on a coin cell over the whole cycle. This work provides a new insight into the electrochemical-thermal coupling mechanism of Li plating at elevated temperature.
Polycrystalline SnSe has attracted significant attention due to its facile processing, machinability, and scale-up application. However, n-type polycrystalline SnSe consistently exhibits inferior thermoelectric performance compared to p-type polycrystalline, because SnSe is an intrinsic p-type semiconductor. Here, we promoted the thermoelectric performance of n-type polycrystalline SnSe through manipulating the band structure and dislocations. The band convergence and enhanced density of states in the electronic structure of SnSe promoted by Pb/Ge/Br codoping, lead to significant enhanced Seebeck coefficient. The carrier concentration was simultaneously enhanced through Ge/Pb/Br codoping. The combination of a large Seebeck coefficient and the enhanced electrical conductivity gives rise to a high power factor as high as 7.47 μW cm−1 K−2 at 873 K. Furthermore, we found that dopants induce strong atomic strain disturbance in the SnSe matrix because of large differences in atom radius with host elements, leading to the formation of high-density dislocations. The presence of dislocations and nanoprecipitates forms strong phonon scattering centers, effectively scattering phonons and suppressing lattice thermal conductivity. As a result, a high peak ZT of 1.6 has been obtained in n-type Sn1.04Ge0.02Pb0.02Se0.97Br0.03.
Biomass-based hydrogen production offers a sustainable and carbon-neutral pathway for addressing the growing demand for clean energy. However, conventional biomass-to-hydrogen technologies such as pyrolysis and gasification suffer from high energy consumption, harsh operational conditions, and low hydrogen purity, hindering large-scale deployment. Here, we present a biomass-assisted water electrolysis strategy utilizing pine-derived carbon anodes with hierarchical structures and abundant C─H active sites. These structural features enable rapid OH- transport and enhance carbon oxidation reaction kinetics under high current densities. Specifically, as prepared PA-10 sample delivers 100 mA at only 1.2 V vs. reversible hydrogen electrode, outperforming conventional oxygen evolution reaction catalysts such as RuO2. Mechanistic insights from in situ characterizations and density functional theory calculations confirm that C─H sites act as thermodynamically favorable precursors for carbon radicals, which trigger the generation of reactive oxygen intermediates (ROIs) and stabilize the binding of ROIs to the carbon surface. We further constructed a membrane-free flow electrolyzer, achieving a low levelized cost of hydrogen at 1.56 USD/kg when powered by renewable electricity. This strategy significantly advances biomass-assisted electrolysis as a scalable, low-cost, and sustainable hydrogen production technology.
Developing a highly efficient, stable, and industrially adaptable bifunctional electrode is crucial for green hydrogen production from seawater electrolysis. Herein, 3D nanoneedle-like Fe-doped Ni12P5 arrays anchored on nickel foam (Fe–Ni12P5 NAs@NFF) are in situ fabricated by a facile one-step phosphorization route. Profiting from the favorable electronic configuration and self-supporting structure with superwetting surfaces, this material demonstrates exceptional performance in alkaline seawater, requiring low overpotentials of 369 and 367 mV to achieve 1000 mA cm−2 for oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) and ensuring stable long-term durability of over 2000 h. When applying Fe–Ni12P5 NAs@NFF as both anode and cathode in an anion exchange membrane electrolyzer, it delivers a cell voltage of only 1.87 V at 1000 mA cm−2 and maintains stable operation for over 140 h, outperforming commercial benchmarks. Based on the collective in situ experimental analysis and theoretical calculation, it is demonstrated that the Ni–Fe–P coordination in bimetallic phosphides delivers the favorable electronic structure, facilitates the reconstruction of OER-active species, and ameliorates the hydrogen adsorption energy for HER. Additionally, the superwetting ability in the surface enables efficient gas bubble detachment and active center regeneration, while the free-standing structure prevents catalytically active components from peeling off, endowing robust stability at the industrial-level current. This work provides new insights into designing and synthesizing highly efficient and stable bifunctional catalysts for seawater electrolysis and contributes to the strategy for large-scale production of low-cost renewable hydrogen at industrial current density.
Rechargeable zinc-air batteries are severely limited by the sluggish oxygen evolution reaction (OER), which induces large overpotentials and poor cycle life. Here, we report a high-performance zinc-air/iodide hybrid battery (ZAIHB) that circumvents the OER bottleneck by introducing an efficient iodide/iodate (I−/IO3−) redox couple, integrated with a rationally designed hollow-structured multi-asymmetric Co dual-atom catalyst mediated by selenium (H-CoSe-NC). The atomic-level Co-Se d-p orbital hybridization enables dynamic charge redistribution, forming adaptive adsorption sites that significantly enhance oxygen reduction (0.90 V half-wave potential) and iodide oxidation (1.265 V at 10 mA cm−2), yielding a record-low potential gap of 0.365 V. The resulting ZAIHB delivers exceptional cycling stability exceeding 1150 h with an energy efficiency of 77% at 10 mA cm−2, and superior durability over state-of-the-art hybrid systems. Operando spectroscopy and density functional theory calculations uncover that Se-induced distortion of Co-Co dual sites and electronic reconfiguration modulate the reaction pathways from OOH* to OH*–OH* intermediates and stabilize I*–I* adsorption, effectively lowering activation barriers. This study pioneers a versatile atomic-scale electronic modulation strategy, offering a new paradigm for designing multi-redox battery systems with minimized polarization losses and extended durability.
Efficient thermal management is essential for modern high-power electronics such as photovoltaic panels, lithium-ion batteries, and integrated circuits, where excessive heat severely compromises device performance, reliability, and lifespan. Hererin, we propose a low-cost and energy-free cooling strategy through a porous hygroscopic melamine foam (MF) composite modified with boron nitride (BN) and lithium bromide (LiBr)-containing poly(vinyl alcohol) (PVA) gel. Sonication-assisted hydrolysis produces hydroxylated BN nanosheets that form hydrogen bonds with PVA, enhancing the thermal conductivity and structural stability. LiBr provides strong hygroscopicity, enabling the composite to dynamically absorb moisture during low-power or standby operation and release it through evaporation under high-power working conditions, leveraging the high latent heat of water vaporization for passive cooling. The shape-stabilized composite film with conformal device attachment effectively reduces the simulated chip surface temperature by 37°C during cyclic operation and suppresses the battery peak temperature by up to 26°C at a ultrahigh discharge rate of 8 C. Moreover, it lowers the photovoltaic panel temperature by 15°C under 1000 W m−2 illumination, improving the power output with enhancement of photoelectric conversion efficiency from 13% to 13.5%. This lightweight, scalable, and durable advanced composite material offers a sustainable and maintenance-free approach for next-generation electronic, battery, and energy-harvesting systems.
Wood-based materials, with a naturally intrinsic hierarchical porous structure, are recognized as exceptional water-splitting electrocatalyst supports for green hydrogen production. However, lignin, as the structural binding agent within its native architecture, occludes pores and restricts the anchoring of active sites. Here, controllable delignification pretreatment is used to enable the simultaneous modulation of pore architecture for efficient mass transport and improve the anchoring environment to boost active site density. When the lignin removal rate reaches 65.55%, Ni/Ni(OH)2-DCW-45 shows hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) overpotentials of 147 and 162 mV at 100 mA·cm−2, respectively. These overpotentials are reduced by 49.83% and 34.94% compared to Ni/Ni(OH)2-CW. As a unified cathode/anode in alkaline electrolysis, it drove full water splitting at 1.363 V (10 mA·cm−2) with 48-h stability. Both experimental and DFT calculations reveal that delignification regulates the Ni/Ni(OH)2 ratio, promotes charge transfer, and strengthens the interaction between reaction intermediates and catalytic sites. This electronic modulation lowered the energy barriers of HER and OER, thereby enhancing the overall water-splitting performance. This work exploits wood's structural advantages and validates delignification as a powerful tool for synergistic optimization of mass transport and active site density, providing novel insights for high-performance biomass-based electrocatalyst design.
The performance of protonic ceramic fuel cells (PCFCs) is critically dependent on the surface architecture of cathode materials, yet direct observation of their dynamic evolution under operating conditions remains a formidable challenge. Herein, we employ operando Raman spectroscopy to track, in real-time, the surface reconstruction of a tailored Ba0.5Sr0.5Co0.9Y0.1O3 − δ (BSCY) perovskite cathode. Our results directly capture the exsolution of a BaCoO3 − δ (BCO) secondary phase, which is induced by current and vapor, a process that can be precisely controlled and peaks within 20 min. By combining operando spectroscopic insights with density functional theory calculations, we decipher the synergistic mechanism: the surface-reconstructed BCO phase significantly enhances oxygen adsorption, and the BSCY favors dissociation and product desorption. This coupling delivers remarkable electrochemical performance, achieving a peak power density of 1170 mW cm−2 at 650°C. This work not only establishes an operando characterization platform for visualizing electrode surface dynamics but also provides foundational insights into designing next-generation PCFC cathodes through targeted surface engineering.
Perovskite solar cells have entered intense global competition for commercialization, yet most research heavily relies on solution processing, whereas dry vacuum processes are favored by industry owing to their successful track record in thin-film device manufacturing. This gap reflects the perception that perovskite vacuum growth is difficult to control and intrinsically less efficient. Here, we bridge this gap by reporting a standardized dry vacuum sublimation strategy that utilizes a simple thickness sensor with fully in situ recorded log data during the vacuum deposition process. This enables rigorous comparison of two representative routes, sequential deposition and co-deposition, and provides a basis for presenting the growth mechanism of vacuum-sublimated perovskite films. The perovskite absorbers are fabricated without additives in the bulk, which simplifies processing. Compositional screening shows that sequential deposition yields more compact structures and enhanced optoelectronic quality relative to co-deposition. Devices incorporating the optimized sequential films deliver a champion power conversion efficiency of 25.4%. Crucially, the process demonstrates exceptional reproducibility, with a standard deviation of 0.36% across 90 cells from eight independent runs. These results establish vacuum processing as a competitive route for industrial manufacturing and are expected to accelerate its adoption in laboratory research.
Composite polymer electrolytes (CPEs) are promising for all-solid-state sodium metal batteries but suffer from low ionic conductivity, which stems from limited Na-salt dissociation and narrow polymer amorphous domains, as well as sluggish ion transport caused by discontinuous composite interfacial charge-transfer paths, and poor electrode/electrolyte interfacial stability. This study proposes an original molecular interface engineering strategy: inorganic Zr4+ induces organic phase reconstruction to build continuous high-speed ion channels, simultaneously accelerating Na-salt dissociation and reducing ion migration energy barriers. Zr4+ directs the oriented reorganization of polar groups (─C≡N) to alleviate Na-metal anode interfacial passivation, facilitate NaF/Na3N-rich stable solid electrolyte interphase formation, and enable uniform Na deposition. Moreover, Zr─N═C metal-ligand coordination at the organic/inorganic interface induces interfacial electronic coupling and charge redistribution, promoting fast Na+ migration along continuous coordination pathways. The developed CPEs, denoted as polyacrylonitrile-metal organic framework@polyethylene oxide-Na[N(SO2CF3)2] (PM@PN), show a synergistic interface-bulk effect that significantly enhances electrolyte performance, as evidenced by a reduced apparent activation energy of 0.027 eV (derived from Vogel–Tammann–Fulcher, VTF fitting above Tm), an enhanced ionic conductivity of 3.52 × 10−4 S cm−1, and a Na+ transference number of 0.67 at 60°C, along with an expanded electrochemical window of 5.06 V. The Na|PM@PN|Na symmetric cell demonstrates 0.56 mA cm−2 critical current density and stable Na deposition/stripping over 700 h at 0.4 mA cm−2. Additionally, the assembled Na3V2(PO4)3|PM@PN|Na full cell maintains 93.99% capacity retention after 200 cycles at 0.1 C, confirming PM@PN's applicability in advanced all-solid-state sodium metal batteries.