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学者姓名：谈鑫
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Abstract ：
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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Electrocatalytic nitrate reduction is an attractive route for sustainable hydroxylamine synthesis, but its selectivity is limited by over-reduction and competing hydrogen evolution, highlighting the need for in-depth mechanistic understanding to guide catalyst design. Here, we systematically investigate the electrochemical synthesis of hydroxylamine via a formaldehyde-mediated method on titanium oxides. An electrochromic rutile array prepared via a wet-chemical route achieved a Faradaic efficiency (FE) of 92.6% (for formaldehyde oxime) and a corresponding yield rate of up to 2085 mu mol cm-2 h-1 under ambient conditions. Mechanistic studies reveal that the electrochromism is a macroscopic manifestation of the protonation of Ob (bridging oxygen) sites and the formation of Ov (oxygen vacancies) and Ti3+, which act as proton "sponges" and electron reservoirs. Formaldehyde not only serves as the capturing agent but also helps to stabilize *NH2OH through molecular tuning, thereby achieving high selectivity. Through formaldehyde-nitrate electro-reforming, hydrogen, formic acid, and hydroxylamine can be coproduced at 200 mA cm-2 under an ultralow cell voltage of 0.78 V. This work links the catalytic performance of hydroxylamine electrosynthesis to the dynamic surface of titanium oxides, offering insights into selectivity control in nitrate electroreduction and providing a green, cost-effective alternative to conventional hydroxylamine synthesis.
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| GB/T 7714 | Zhang, Jiaqi , Zhao, Erbo , Hsueh, Chou-Hung et al. Electrochromic Rutile with Dynamically Tailored Surfaces in Formaldehyde-Mediated Hydroxylamine Electrosynthesis [J]. | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY , 2025 , 147 (24) : 20559-20570 . |
| MLA | Zhang, Jiaqi et al. "Electrochromic Rutile with Dynamically Tailored Surfaces in Formaldehyde-Mediated Hydroxylamine Electrosynthesis" . | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 147 . 24 (2025) : 20559-20570 . |
| APA | Zhang, Jiaqi , Zhao, Erbo , Hsueh, Chou-Hung , Cheong, Weng-Chon Max , Tan, Xin , Liu, Chuhao et al. Electrochromic Rutile with Dynamically Tailored Surfaces in Formaldehyde-Mediated Hydroxylamine Electrosynthesis . | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY , 2025 , 147 (24) , 20559-20570 . |
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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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The two-electron oxygen reduction reaction (2e- ORR) is a pivotal pathway for the distributed production of hydrogen peroxide (H2O2). In nature, enzymes containing manganese (Mn) centers can convert reactive oxygen species into H2O2. However, Mn-based heterogeneous catalysts for 2e- ORR are scarcely reported. Herein, we developed a nature-inspired single-atom electrocatalyst comprising N, O co-coordinated Mn sites, utilizing carbon dots as the modulation platform (Mn CD/C). As-synthesized Mn CD/C exhibited exceptional 2e- ORR activity with an onset potential of 0.786 V and a maximum H2O2 selectivity of 95.8 %. Impressively, Mn CD/C continuously produced 0.1 M H2O2 solution at 200 mA/cm2 for 50 h in the flow cell, with negligible loss in activity and H2O2 faradaic efficiency, demonstrating practical application potential. The enhanced activity was attributed to the incorporation of Mn atomic sites into the carbon dots. Theoretical calculations revealed that the N, O co-coordinated structure, combined with abundant oxygen-containing functional groups on the carbon dots, optimized the binding strength of intermediate *OOH at the Mn sites to the apex of the catalytic activity volcano. This work illustrates that carbon dots can serve as a versatile platform for modulating the microenvironment of single-atom catalysts and for the rational design of nature-inspired catalysts.
Keyword ：
carbon dots carbon dots electrocatalysis electrocatalysis hydrogen peroxide hydrogen peroxide interfacial regulation interfacial regulation single-atom catalysts single-atom catalysts
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| GB/T 7714 | Zeng, Yuan , Tan, Xin , Zhuang, Zewen et al. Nature-Inspired N, O Co-Coordinated Manganese Single-Atom Catalyst for Efficient Hydrogen Peroxide Electrosynthesis [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 , 64 (4) . |
| MLA | Zeng, Yuan et al. "Nature-Inspired N, O Co-Coordinated Manganese Single-Atom Catalyst for Efficient Hydrogen Peroxide Electrosynthesis" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 64 . 4 (2024) . |
| APA | Zeng, Yuan , Tan, Xin , Zhuang, Zewen , Chen, Chen , Peng, Qing . Nature-Inspired N, O Co-Coordinated Manganese Single-Atom Catalyst for Efficient Hydrogen Peroxide Electrosynthesis . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2024 , 64 (4) . |
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