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学者姓名：庄泽文
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Abstract ：
Layered double hydroxide (LDH) materials have been of interest as the noble metal substitutes for oxygen evolution reaction (OER) in alkaline media though their intrinsically inferior electrocatalytic activity. Proper cation vacancy engineering of LDH is an effective approach for improving intrinsic activity during catalytic OER. In this work, the in-situ formation of cation vacancies in LDH nanosheets (NiFeCoZnvac-LDH) is successfully realized by partially Zn etching from medium-entropy NiFeCoZn-LDH precursor. In-situ Raman analysis and DFT calculations uncover that the introduction of metal cation vacancies can significantly lower the generation potential of the surface reconstruction for the formation of abundant high-valence active centers and optimize the adsorption/desorption energy of oxygen-containing intermediates, thereby boosting catalytic OER activity. As a proof of concept, the obtained NiFeCoZnvac-LDH catalyst just requires a low overpotential of 222 mV to reach a current density of 10 mA cm-2 with a small Tafel slope of 37.17 mV dec-1. Furthermore, the NiFeCoZnvac-LDH electrode takes an ultralow potential of 1.48 V at 10 mA cm- 2 in practical anion exchange membrane electrolyzer and operate stably at 100 mA cm- 2 for long period without obvious activity attenuation. The present study enables the development of LDH catalysts for efficient water oxidation using a simple and robust approach.
Keyword ：
Active center Active center Cation vacancy Cation vacancy Layered double hydroxide Layered double hydroxide Oxygen evolution reaction Oxygen evolution reaction Surface reconstruction Surface reconstruction
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| GB/T 7714 | Wang, Kaili , Shuai, Yankang , Deng, Shuqi et al. Cation vacancy engineering in medium-entropy NiFeCoZn layered double hydroxides electrocatalysts for boosting oxygen evolution reaction in water-splitting [J]. | CHEMICAL ENGINEERING JOURNAL , 2025 , 508 . |
| MLA | Wang, Kaili et al. "Cation vacancy engineering in medium-entropy NiFeCoZn layered double hydroxides electrocatalysts for boosting oxygen evolution reaction in water-splitting" . | CHEMICAL ENGINEERING JOURNAL 508 (2025) . |
| APA | Wang, Kaili , Shuai, Yankang , Deng, Shuqi , Lian, Bianyong , Zhao, Zihan , Chen, Jinghong et al. Cation vacancy engineering in medium-entropy NiFeCoZn layered double hydroxides electrocatalysts for boosting oxygen evolution reaction in water-splitting . | CHEMICAL ENGINEERING JOURNAL , 2025 , 508 . |
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The oxygen reduction reaction (ORR) is critical for energy conversion technologies like fuel cells and metal-air batteries. However, advancing efficient and stable ORR catalysts remains a significant challenge. Iron-based single-atom catalysts (Fe SACs) have emerged as promising alternatives to precious metals. However, their catalytic performance and stability remain constrained. Introducing a second metal (M) to construct Fe & horbar;M dual-atom catalysts (Fe & horbar;M DACs) is an effective strategy to enhance the performance of Fe SACs. This review provides a comprehensive overview of the recent advancements in Fe-based DACs for ORR. It begins by examining the structural advantages of Fe & horbar;M DACs from the perspectives of electronic structure and reaction pathways. Next, the precise synthetic strategies for DACs are discussed, and the structure-performance relationships are explored, highlighting the role of the second metal in improving catalytic activity and stability. The review also covers in situ characterization techniques for real-time observation of catalytic dynamics and reaction intermediates. Finally, future directions for Fe & horbar;M DACs are proposed, emphasizing the integration of advanced experimental strategies with theoretical simulations as well as artificial intelligence/machine learning to design highly active and stable ORR catalysts, aiming to expand the application of Fe & horbar;M DACs in energy conversion and storage technologies.
Keyword ：
dual-atom catalysts dual-atom catalysts iron-based electrocatalysts iron-based electrocatalysts oxygen reduction reaction oxygen reduction reaction single-atom catalyst single-atom catalyst
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| GB/T 7714 | You, Shengping , Zhang, Chao , Yu, Mingyu et al. Rational Dual-Atom Design to Boost Oxygen Reduction Reaction on Iron-Based Electrocatalysts [J]. | SMALL , 2025 , 21 (27) . |
| MLA | You, Shengping et al. "Rational Dual-Atom Design to Boost Oxygen Reduction Reaction on Iron-Based Electrocatalysts" . | SMALL 21 . 27 (2025) . |
| APA | You, Shengping , Zhang, Chao , Yu, Mingyu , Tan, Xin , Sun, Kaian , Zheng, Yun et al. Rational Dual-Atom Design to Boost Oxygen Reduction Reaction on Iron-Based Electrocatalysts . | SMALL , 2025 , 21 (27) . |
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The carbon dioxide electroreduction reaction (CO2RR) to ethanol (C2H5OH) represents a sustainable route toward carbon neutrality. Herein, we present the design of enzyme-inspired zirconium-Fe porphyrinic-based metal-organic framework (MOF) nanosheets functionalized with 5-benzimidazolecarboxylic acid (FeTCPP-NSs-BAA) for the CO2RR. Electrochemical performances in a H-cell reveal that FeTCPP-NSs-BAA shows C2H5OH faradaic efficiencies (FEs) of 79.8% under neutral and 89.2% under acidic conditions, with C2H5OH FEs exceeding 60% over wide potential windows of -0.3 to -0.6 V and -0.3 to -0.8 V, respectively. In flow cell tests under acidic conditions, FeTCPP-NSs-BAA delivers the highest C2H5OH partial current density of 8.1 mA cm-2 with pure CO2, and a C2H5OH partial current density of 5.6 mA cm-2 when using 30% low-concentration CO2. In situ spectroscopic characterization and theoretical calculations reveal that the superior C2H5OH performance of FeTCPP-NSs-BAA arises from the enzyme-like non-covalent synergistic effects between FeTCPP and the secondary-sphere functionalities of BAA and Zr6 clusters. Specifically, BAA enhances CO2 enrichment and facilitates the tilted *CO adsorption at Fe centers on FeTCPP, which significantly reduces energy barriers for *CO-CO coupling compared to linearly adsorbed *CO. Meanwhile, the subsequent hydrogenation of *CO-CO to C2H5OH can be further accelerated by proton shuttling mediated through hydrogen-bonding networks introduced by Zr6 clusters.
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| GB/T 7714 | Sun, Kaian , Xie, Shaohui , Guan, Ping et al. A bioinspired electrocatalyst for CO2 electroreduction to ethanol via secondary-sphere synergy in Fe porphyrinic-based metal-organic frameworks [J]. | ENERGY & ENVIRONMENTAL SCIENCE , 2025 , 18 (13) : 6823-6831 . |
| MLA | Sun, Kaian et al. "A bioinspired electrocatalyst for CO2 electroreduction to ethanol via secondary-sphere synergy in Fe porphyrinic-based metal-organic frameworks" . | ENERGY & ENVIRONMENTAL SCIENCE 18 . 13 (2025) : 6823-6831 . |
| APA | Sun, Kaian , Xie, Shaohui , Guan, Ping , Zhuang, Zewen , Tan, Xin , Yan, Wei et al. A bioinspired electrocatalyst for CO2 electroreduction to ethanol via secondary-sphere synergy in Fe porphyrinic-based metal-organic frameworks . | ENERGY & ENVIRONMENTAL SCIENCE , 2025 , 18 (13) , 6823-6831 . |
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| GB/T 7714 | Zhuang, Zewen , Zhang, Chao , Zhang, Jiujun . Single metal, dual sites: Co-P moieties enable efficient and stable electrochemical hydrogen production [J]. | SCIENCE CHINA-CHEMISTRY , 2025 , 68 (5) : 1630-1631 . |
| MLA | Zhuang, Zewen et al. "Single metal, dual sites: Co-P moieties enable efficient and stable electrochemical hydrogen production" . | SCIENCE CHINA-CHEMISTRY 68 . 5 (2025) : 1630-1631 . |
| APA | Zhuang, Zewen , Zhang, Chao , Zhang, Jiujun . Single metal, dual sites: Co-P moieties enable efficient and stable electrochemical hydrogen production . | SCIENCE CHINA-CHEMISTRY , 2025 , 68 (5) , 1630-1631 . |
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High-temperature proton exchange membrane fuel cells (HT-PEMFCs) show broad application perspectives due to their faster reaction kinetics and tolerance to fuel/gas impurities as well as the easy water/heat managements. However, the catalysts and subsequent membrane electrode assemblies (MEAs) are still suffering from performance degradation, which severely restricts HT-PEMFCs' large-scale practical application. To overcome the challenges, developing high-performance catalysts and MEAs with advanced materials and optimized structures to achieve stable and efficient operation of HT-PEMFCs is necessary. To facilitate the research and development of HT-PEMFCs, a comprehensive overview of the latest developments in the design of active and stable catalysts and durable MEAs is presented in this paper. This review systematically summarizes the degradation mechanisms of catalysts, and corresponding mitigation strategies for improving the stability of catalysts and MEAs, aiming to effectively developing high-performance and durable HT-PEMFCs. Furthermore, the main challenges are analyzed and the future research directions for overcoming the challenges are also proposed for developing highactive and stable catalysts and MEAs used in HT-PEMFCs toward practical applications.
Keyword ：
Catalysts Catalysts Degradation mechanisms Degradation mechanisms High-temperature proton exchange membrane fuel cells High-temperature proton exchange membrane fuel cells Membrane electrode assemblies Membrane electrode assemblies Mitigation strategies Mitigation strategies
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| GB/T 7714 | Xu, Chenhui , Wang, Shufan , Zheng, Yun et al. Performance enhancement from catalysts to membrane electrode assemblies for high-temperature proton exchange membrane fuel cells [J]. | NANO ENERGY , 2025 , 139 . |
| MLA | Xu, Chenhui et al. "Performance enhancement from catalysts to membrane electrode assemblies for high-temperature proton exchange membrane fuel cells" . | NANO ENERGY 139 (2025) . |
| APA | Xu, Chenhui , Wang, Shufan , Zheng, Yun , Liu, Haishan , Li, Lingfei , Zhuang, Zewen et al. Performance enhancement from catalysts to membrane electrode assemblies for high-temperature proton exchange membrane fuel cells . | NANO ENERGY , 2025 , 139 . |
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Modulating the electron delocalization of catalysts can improve the activation and conversion capabilities of lithium polysulfides (LiPSs) in lithium-sulfur batteries, while the precise mechanism underlying this enhancement remains unclear. Herein, a p-block In single-atom catalysts (In-N4) is constructed with moderate electron delocalization via axial coordination engineering of gallium nitride (GaN), which exhibits the best adsorption and electrocatalytic activity toward LiPSs. In situ characterization analysis combined with advanced theoretical calculations demonstrate that the axial In-N-Ga coordination induces the electron transfer from In sites toward the N sites of GaN and the unconventional sp3d2 hybridization interactions of In sites. This further helps to optimize adsorption configuration through the orbital hybridization between sp3d2 hybrid orbital of In sites and p orbital of S atoms in LiPSs, namely the sp3d2 - p orbital hybridization, which can weaken S-S covalent bonds of LiPSs and significantly accelerate the sulfur reduction reaction. Accordingly, the capacity decay of lithium-sulfur battery with In-SA/GaN catalyst is only 0.040% per cycle over 800 cycles at 5 C. The stacked pouch cell delivers a reversible capacity of 600 mAh after 100 cycles. This work elaborates on the activity origin of p-block metal catalysts and provides a new perspective on designing advanced catalysts for other catalytic systems.
Keyword ：
electron delocalization electron delocalization orbital hybridization orbital hybridization p-block metal p-block metal single-atom catalyst single-atom catalyst sulfur reduction reaction sulfur reduction reaction
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| GB/T 7714 | Jiao, Xuechao , Lei, Jie , Huang, Zheng et al. Axial Coordination Regulating Electronic Delocalization of p-Block In-N4 Sites to Accelerate Sulfur Reduction Reaction [J]. | ADVANCED FUNCTIONAL MATERIALS , 2025 . |
| MLA | Jiao, Xuechao et al. "Axial Coordination Regulating Electronic Delocalization of p-Block In-N4 Sites to Accelerate Sulfur Reduction Reaction" . | ADVANCED FUNCTIONAL MATERIALS (2025) . |
| APA | Jiao, Xuechao , Lei, Jie , Huang, Zheng , Zuo, Yinze , Zhuang, Zewen , Luo, Yiyuan et al. Axial Coordination Regulating Electronic Delocalization of p-Block In-N4 Sites to Accelerate Sulfur Reduction Reaction . | ADVANCED FUNCTIONAL MATERIALS , 2025 . |
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Single-atomic/cluster metal-based electrocatalysts (M-N-C) is one of the most promising non-noble metal catalysts for the oxygen reduction reaction (ORR), but their practical application is severely hindered by insufficient activity and durability. Herein, charge regulation through rare earth metal oxides (REMOs) for single-atomic/cluster metal based electrocatalysts is proposed for boosting ORR, in which the Co-based catalyst is taken as a representative considering its typicality and universality, and CeO2 is selected as representative after systematic computational screening from more than 10 types of REMOs. As a result, a novel REMO-tailored M-N-C electrocatalyst (REMO-Co-N-C) has been successfully achieved, which demonstrates a remarkably increased activity and superior durability, namely a half-wave potential (E₁/₂) of 0.90 V and only a loss of 8 mV (E₁/₂) after 10,000 cycles. Moreover, in-situ experiments and matched theoretical simulations come together organically to clearly and directly reveal the origin and catalytic behavior of the proposed electrocatalysts. Namely the charge regulation through REMO for M-N-C can effectively modify the electronic structure of the M sites, accelerate the reaction rate, and enhance OH* desorption. This work offers a new insight for promoting M-N-C catalysts through REMO tailoring, that beyond the conventional use of d-block and p-block elements. © 2025 Elsevier B.V.
Keyword ：
Cerium oxide Cerium oxide Electrolysis Electrolysis Electrolytic reduction Electrolytic reduction
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| GB/T 7714 | Wang, Shufan , Li, Lingfei , Zheng, Yun et al. Charge regulation through rare earth metal oxides for single-atomic/cluster Co-based electrocatalysts towards boosting oxygen reduction reaction [J]. | Applied Catalysis B: Environmental , 2025 , 377 . |
| MLA | Wang, Shufan et al. "Charge regulation through rare earth metal oxides for single-atomic/cluster Co-based electrocatalysts towards boosting oxygen reduction reaction" . | Applied Catalysis B: Environmental 377 (2025) . |
| APA | Wang, Shufan , Li, Lingfei , Zheng, Yun , Xu, Chenhui , Zhuang, Zewen , Sun, Kaian et al. Charge regulation through rare earth metal oxides for single-atomic/cluster Co-based electrocatalysts towards boosting oxygen reduction reaction . | Applied Catalysis B: Environmental , 2025 , 377 . |
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High entropy alloys (HEAs) have gained significant attention in electrocatalysis research due to their distinctive multi-element composition, intricate electronic structure, and superior properties. By harnessing multi-component synergy, precise electron regulation, and the high-entropy effect, HEA electrocatalysts exhibit remarkable catalytic activity, selectivity, and stability. These materials demonstrate outstanding catalytic performance in a variety of electrocatalytic small molecule reduction reactions, including oxygen reduction (ORR), hydrogen evolution (HER), and CO2 reduction (CO2RR), making them promising candidates for clean energy conversion and storage applications, including fuel cells, metal-air batteries, water electrolysis, and CO2 conversion technologies. This review highlights recent advancements in HEA electrocatalyst research, focusing on their synthesis, characterization, and applications in electrocatalytic small molecule reduction reactions. It also explores the underlying mechanisms of the high-entropy effect, multi-component synergy, and structural design. Finally, it discusses key challenges that remain in the application of HEAs for electrocatalytic small molecule reduction and outlines potential directions for future development in this field.
Keyword ：
CO2 reduction reaction (CO2RR) CO2 reduction reaction (CO2RR) electrocatalysis electrocatalysis high entropy alloys (HEAs) high entropy alloys (HEAs) hydrogen evolution reaction (HER) hydrogen evolution reaction (HER) oxygen reduction reaction (ORR) oxygen reduction reaction (ORR)
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| GB/T 7714 | Zhang, Chao , You, Shengping , Du, Ang et al. Recent advances in high-entropy alloys for electrochemical hydrogen evolution, oxygen reduction, and CO2 reduction reactions [J]. | FRONTIERS IN ENERGY , 2025 , 19 (4) : 471-499 . |
| MLA | Zhang, Chao et al. "Recent advances in high-entropy alloys for electrochemical hydrogen evolution, oxygen reduction, and CO2 reduction reactions" . | FRONTIERS IN ENERGY 19 . 4 (2025) : 471-499 . |
| APA | Zhang, Chao , You, Shengping , Du, Ang , Zhuang, Zewen , Yan, Wei , Zhang, Jiujun . Recent advances in high-entropy alloys for electrochemical hydrogen evolution, oxygen reduction, and CO2 reduction reactions . | FRONTIERS IN ENERGY , 2025 , 19 (4) , 471-499 . |
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Electrocatalytic nitrate reduction (NO3-RR) holds significant potential for clean NH3 synthesis and the treatment of industrial effluents, effectively converting waste into a valuable resource. However, the catalyst reconstruction mechanism remains ambiguous, and the influence of interfacial hydrogen bonds on NO3-RR performance remains underexplored. Herein, a Cr-doping strategy was developed to regulate the interfacial hydrogen-bonded interactions on Co-based dynamic electrocatalysts to improve electrocatalytic NO3-RR activity. In situ XRD, in situ Raman spectroscopy and theoretical calculations indicated that Cr doping could modulate the reconstruction process of Co-based materials, achieving a dynamic balance between Co(OH)2 and Co. Moreover, molecular dynamics simulations and density functional theory calculations, combined with in situ infrared spectroscopy, revealed that the strong hydrogen-bonding interactions between interfacial H2O and the Cr-doped Co(OH)2 surface could drag more free H2O from the rigid H2O network and facilitate H2O dissociation, forming active hydrogen to accelerate the NO3-RR pathway on metallic Co sites. As a result, the Cr-doped Co-based dynamic electrocatalyst displayed a superior NH3 faradaic efficiency of 97.36% and a high NH3 yield rate of 58.92 mg h-1 cm-2, outperforming the state-of-the-art electrocatalysts. This work can further inspire the design of dynamic electrocatalysts and the modulation of the interfacial microenvironment for promoting effective electrochemical hydrogenation reactions.
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| GB/T 7714 | Wan, Yuchi , Tang, Yixiang , Zuo, Yinze et al. Interfacial hydrogen-bond modulation of dynamic catalysts for nitrate electroreduction to ammonia [J]. | ENERGY & ENVIRONMENTAL SCIENCE , 2025 , 18 (15) : 7460-7469 . |
| MLA | Wan, Yuchi et al. "Interfacial hydrogen-bond modulation of dynamic catalysts for nitrate electroreduction to ammonia" . | ENERGY & ENVIRONMENTAL SCIENCE 18 . 15 (2025) : 7460-7469 . |
| APA | Wan, Yuchi , Tang, Yixiang , Zuo, Yinze , Sun, Kaian , Zhuang, Zewen , Zheng, Yun et al. Interfacial hydrogen-bond modulation of dynamic catalysts for nitrate electroreduction to ammonia . | ENERGY & ENVIRONMENTAL SCIENCE , 2025 , 18 (15) , 7460-7469 . |
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Developing advanced cathode materials plays a positive role in lowering the charge/discharge overpotentials and improving the cycling performance of lithium-oxygen batteries (LOBs). Here we report a direct synthesis strategy to prepare high-dimensional branched PdCoPx series nanostructures, in which the Pd atoms are well dispersed within cobalt phosphide, leading to rich Pd & horbar;Co & horbar;P interfaces and evoking a prominent ligand effect between the elements. The Pd1Co2Px exhibits an excellent and stable activity for oxygen reduction reaction (ORR) in alkaline media, with a mass activity of 1.46 A mgPd-1, far exceeding that of commercial Pd/C (0.12 A mgPd-1) and Pt/C (0.17 A mgPt-1). Using Pd1Co2Px as the cathode, the resulting LOB shows an ultralow discharge/charge overpotential of 0.40 V and could run stably for over 240 cycles, which is a significant improvement compared with the counterparts using CoPx and Pd/C cathodes. Experimental and density functional theory (DFT) calculation results indicate that the dispersed Pd atoms could significantly enhance the ORR kinetics, and the Pd & horbar;Co & horbar;P interfaces could direct the two-dimensional growth of Li2O2, thereby facilitating the formation of more easily decomposable film-like Li2O2 products. This feature successfully elevates both the charge and discharge performances, as well as the stability of the LOB.
Keyword ：
Cathode catalyst Cathode catalyst High-dimensional nanostructures High-dimensional nanostructures Interface engineering Interface engineering Lithium-oxygen batteries Lithium-oxygen batteries Oxygen reduction reaction Oxygen reduction reaction
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| GB/T 7714 | Xu, Zhiyuan , Zhang, Yu , Yu, Hong et al. Interface Engineering of Branched PdCoPx Nanostructures for High-Performance Lithium-Oxygen Batteries [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2025 , 64 (30) . |
| MLA | Xu, Zhiyuan et al. "Interface Engineering of Branched PdCoPx Nanostructures for High-Performance Lithium-Oxygen Batteries" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 64 . 30 (2025) . |
| APA | Xu, Zhiyuan , Zhang, Yu , Yu, Hong , Zhuang, Zewen , Wang, Xingdong , Zhang, Jiaqi et al. Interface Engineering of Branched PdCoPx Nanostructures for High-Performance Lithium-Oxygen Batteries . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2025 , 64 (30) . |
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