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Boosting Water Dissociation Kinetics on Pt-Ni Nanowires by N-Induced Orbital Tuning.
Xie, Yufang; Cai, Jinyan; Wu, Yishang; Zang, Yipeng; Zheng, Xusheng; Ye, Jian; Cui, Peixin; Niu, Shuwen; Liu, Yun; Zhu, Junfa; Liu, Xiaojing; Wang, Gongming; Qian, Yitai.
Afiliación
  • Xie Y; Hefei National Laboratory for Physical Science at the Microscale, Department of Chemistry, University of Science and Technology of China, Hefei, Anhui, 230026, P. R. China.
  • Cai J; Hefei National Laboratory for Physical Science at the Microscale, Department of Chemistry, University of Science and Technology of China, Hefei, Anhui, 230026, P. R. China.
  • Wu Y; Hefei National Laboratory for Physical Science at the Microscale, Department of Chemistry, University of Science and Technology of China, Hefei, Anhui, 230026, P. R. China.
  • Zang Y; Hefei National Laboratory for Physical Science at the Microscale, Department of Chemistry, University of Science and Technology of China, Hefei, Anhui, 230026, P. R. China.
  • Zheng X; National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, Anhui, 230029, P. R. China.
  • Ye J; National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, Anhui, 230029, P. R. China.
  • Cui P; Key Laboratory of Soil Environment and Pollution Remediation, Institute of Soil Science, The Chinese Academy of Sciences, Nanjing, 210008, P. R. China.
  • Niu S; Hefei National Laboratory for Physical Science at the Microscale, Department of Chemistry, University of Science and Technology of China, Hefei, Anhui, 230026, P. R. China.
  • Liu Y; Hefei National Laboratory for Physical Science at the Microscale, Department of Chemistry, University of Science and Technology of China, Hefei, Anhui, 230026, P. R. China.
  • Zhu J; National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, Anhui, 230029, P. R. China.
  • Liu X; Hefei National Laboratory for Physical Science at the Microscale, Department of Chemistry, University of Science and Technology of China, Hefei, Anhui, 230026, P. R. China.
  • Wang G; Hefei National Laboratory for Physical Science at the Microscale, Department of Chemistry, University of Science and Technology of China, Hefei, Anhui, 230026, P. R. China.
  • Qian Y; Hefei National Laboratory for Physical Science at the Microscale, Department of Chemistry, University of Science and Technology of China, Hefei, Anhui, 230026, P. R. China.
Adv Mater ; 31(16): e1807780, 2019 Apr.
Article en En | MEDLINE | ID: mdl-30811711
Although it is commonly believed that the water-dissociation-related Volmer process is the rate-limiting step for alkaline hydrogen evolution reaction (HER) on Pt-based catalysts, the underlying essence, particularly on the atomic scale, still remains unclear. Herein, it is revealed that the sluggish water-dissociation behavior probably stems from unfavorable orbital orientation and the kinetic issue is successfully resolved via N-induced orbital tuning. Impressively, N modified Pt-Ni nanowires deliver an ultralow overpotential of 13 mV at 10 mA cm-2 , which represents a new benchmark for alkaline HER catalysis. Fine-structural characterization and density functional theory analysis illustrate that the introduced nitrogen can uniquely modulate the electron densities around the Ni sites, and further create empty dz 2 orbitals with superior orientation for water adsorption and activation. More importantly, it is demonstrated that N-induced orbital modulation can generally boost the alkaline HER activities of Pt-Co, Pt-Ni, and Pt-Cu, offering a new perspective for the design of HER catalysts and beyond.
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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: 2019 Tipo del documento: Article Pais de publicación: Alemania
Texto completo
Añadir a Mi BVS
Imprimir
XML
PubMed Links
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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: 2019 Tipo del documento: Article Pais de publicación: Alemania