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A Generalized Coordination Engineering Strategy for Single-Atom Catalysts toward Efficient Hydrogen Peroxide Electrosynthesis.
Liu, Wei; Chen, Rui; Sang, Zhiyuan; Li, Zhenxin; Nie, Jiahuan; Yin, Lichang; Hou, Feng; Liang, Ji.
Afiliación
  • Liu W; Key Laboratory of Advanced Ceramics and Machining Technology of Ministry of Education School of Materials Science and Engineering, Tianjin University, Tianjin, 300072, P. R. China.
  • Chen R; Key Laboratory of Advanced Ceramics and Machining Technology of Ministry of Education School of Materials Science and Engineering, Tianjin University, Tianjin, 300072, P. R. China.
  • Sang Z; Key Laboratory of Advanced Ceramics and Machining Technology of Ministry of Education School of Materials Science and Engineering, Tianjin University, Tianjin, 300072, P. R. China.
  • Li Z; Key Laboratory of Advanced Ceramics and Machining Technology of Ministry of Education School of Materials Science and Engineering, Tianjin University, Tianjin, 300072, P. R. China.
  • Nie J; Key Laboratory of Advanced Ceramics and Machining Technology of Ministry of Education School of Materials Science and Engineering, Tianjin University, Tianjin, 300072, P. R. China.
  • Yin L; Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Science, Shenyang, 110016, P. R. China.
  • Hou F; Key Laboratory of Advanced Ceramics and Machining Technology of Ministry of Education School of Materials Science and Engineering, Tianjin University, Tianjin, 300072, P. R. China.
  • Liang J; Key Laboratory of Advanced Ceramics and Machining Technology of Ministry of Education School of Materials Science and Engineering, Tianjin University, Tianjin, 300072, P. R. China.
Adv Mater ; 36(38): e2406403, 2024 Sep.
Article en En | MEDLINE | ID: mdl-39036826
ABSTRACT
Designing non-noble metal single-atom catalysts (M-SACs) for two-electron oxygen reduction reaction (2e-ORR) is attractive for the hydrogen peroxide (H2O2) electrosynthesis, in which the coordination configuration of the M-SACs essentially affects the reaction activity and product selectivity. Though extensively investigated, a generalized coordination engineering strategy has not yet been proposed, which fundamentally hinders the rational design of M-SACs with optimized catalytic capabilities. Herein, a generalized coordination engineering strategy is proposed for M-SACs toward H2O2 electrosynthesis via introducing heteroatoms (e.g., oxygen or sulfur atoms) with higher or lower electronegativity than nitrogen atoms into the first sphere of metal-N4 system to tailor their electronic structure and adjust the adsorption strength for *OOH intermediates, respectively, thus optimizing their electrocatalytic capability for 2e-ORR. Specifically, the (O, N)-coordinated Co SAC (Co-N3O) and (S, N)-coordinated Ni SAC (Ni-N3S) are precisely synthesized, and both present superior 2e-ORR activity (Eonset ≈0.80 V versus RHE) and selectivity (≈90%) in alkaline conditions compared with conventional Co-N4 and Ni-N4 sites. The high H2O2 yield rates of 14.2 and 17.5 moL g-1 h-1 and long-term stability over 12 h are respectively achieved for Co-N3O and Ni-N3S. Such favorable 2e-ORR pathway of the catalysts is also theoretically confirmed by the kinetics simulations.
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Adv Mater Asunto de la revista: BIOFISICA / QUIMICA Año: 2024 Tipo del documento: Article Pais de publicación: Alemania
Texto completo
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Adv Mater Asunto de la revista: BIOFISICA / QUIMICA Año: 2024 Tipo del documento: Article Pais de publicación: Alemania