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Mechanism of Cations Suppressing Proton Diffusion Kinetics for Electrocatalysis.
Li, Xiao-Yu; Wang, Tao; Cai, Yu-Chen; Meng, Zhao-Dong; Nan, Jing-Wen; Ye, Jin-Yu; Yi, Jun; Zhan, Dong-Ping; Tian, Na; Zhou, Zhi-You; Sun, Shi-Gang.
Afiliación
  • Li XY; State Key Laboratory of Physical Chemistry of Solid Surfaces, Tan Kah Kee Innovation Laboratory, Collaborative Innovation Center of Chemistry for Energy Materials, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, P. R. China.
  • Wang T; State Key Laboratory of Physical Chemistry of Solid Surfaces, Tan Kah Kee Innovation Laboratory, Collaborative Innovation Center of Chemistry for Energy Materials, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, P. R. China.
  • Cai YC; State Key Laboratory of Physical Chemistry of Solid Surfaces, Tan Kah Kee Innovation Laboratory, Collaborative Innovation Center of Chemistry for Energy Materials, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, P. R. China.
  • Meng ZD; State Key Laboratory of Physical Chemistry of Solid Surfaces, Tan Kah Kee Innovation Laboratory, Collaborative Innovation Center of Chemistry for Energy Materials, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, P. R. China.
  • Nan JW; State Key Laboratory of Physical Chemistry of Solid Surfaces, Tan Kah Kee Innovation Laboratory, Collaborative Innovation Center of Chemistry for Energy Materials, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, P. R. China.
  • Ye JY; State Key Laboratory of Physical Chemistry of Solid Surfaces, Tan Kah Kee Innovation Laboratory, Collaborative Innovation Center of Chemistry for Energy Materials, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, P. R. China.
  • Yi J; School of Electronic Science and Engineering, Xiamen University, Xiamen, 361005, P. R. China.
  • Zhan DP; State Key Laboratory of Physical Chemistry of Solid Surfaces, Tan Kah Kee Innovation Laboratory, Collaborative Innovation Center of Chemistry for Energy Materials, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, P. R. China.
  • Tian N; State Key Laboratory of Physical Chemistry of Solid Surfaces, Tan Kah Kee Innovation Laboratory, Collaborative Innovation Center of Chemistry for Energy Materials, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, P. R. China.
  • Zhou ZY; State Key Laboratory of Physical Chemistry of Solid Surfaces, Tan Kah Kee Innovation Laboratory, Collaborative Innovation Center of Chemistry for Energy Materials, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, P. R. China.
  • Sun SG; State Key Laboratory of Physical Chemistry of Solid Surfaces, Tan Kah Kee Innovation Laboratory, Collaborative Innovation Center of Chemistry for Energy Materials, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, P. R. China.
Angew Chem Int Ed Engl ; 62(14): e202218669, 2023 Mar 27.
Article en En | MEDLINE | ID: mdl-36762956
ABSTRACT
Proton transfer is crucial for electrocatalysis. Accumulating cations at electrochemical interfaces can alter the proton transfer rate and then tune electrocatalytic performance. However, the mechanism for regulating proton transfer remains ambiguous. Here, we quantify the cation effect on proton diffusion in solution by hydrogen evolution on microelectrodes, revealing the rate can be suppressed by more than 10 times. Different from the prevalent opinions that proton transport is slowed down by modified electric field, we found water structure imposes a more evident effect on kinetics. FTIR test and path integral molecular dynamics simulation indicate that proton prefers to wander within the hydration shell of cations rather than to hop rapidly along water wires. Low connectivity of water networks disrupted by cations corrupts the fast-moving path in bulk water. This study highlights the promising way for regulating proton kinetics via a modified water structure.
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Texto completo: 1 Colección: 01-internacional Banco de datos: MEDLINE Idioma: En Revista: Angew Chem Int Ed Engl Año: 2023 Tipo del documento: Article

Texto completo: 1 Colección: 01-internacional Banco de datos: MEDLINE Idioma: En Revista: Angew Chem Int Ed Engl Año: 2023 Tipo del documento: Article