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Tailoring the d‐Band Centers Enables Co4N Nanosheets To Be Highly Active for Hydrogen Evolution Catalysis
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2018-03-23 , DOI: 10.1002/anie.201801834 Zhiyan Chen 1, 2 , Yao Song 1, 2 , Jinyan Cai 1 , Xusheng Zheng 3 , Dongdong Han 1 , Yishang Wu 1, 2 , Yipeng Zang 1 , Shuwen Niu 1 , Yun Liu 1 , Junfa Zhu 3 , Xiaojing Liu 1 , Gongming Wang 1
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2018-03-23 , DOI: 10.1002/anie.201801834 Zhiyan Chen 1, 2 , Yao Song 1, 2 , Jinyan Cai 1 , Xusheng Zheng 3 , Dongdong Han 1 , Yishang Wu 1, 2 , Yipeng Zang 1 , Shuwen Niu 1 , Yun Liu 1 , Junfa Zhu 3 , Xiaojing Liu 1 , Gongming Wang 1
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Endowing materials with specific functions that are not readily available is always of great importance, but extremely challenging. Co4N, with its beneficial metallic characteristics, has been proved to be highly active for the oxidation of water, while it is notoriously poor for catalyzing the hydrogen evolution reaction (HER), because of its unfavorable d‐band energy level. Herein, we successfully endow Co4N with prominent HER catalytic capability by tailoring the positions of the d‐band center through transition‐metal doping. The V‐doped Co4N nanosheets display an overpotential of 37 mV at 10 mA cm−2, which is substantially better than Co4N and even close to the benchmark Pt/C catalysts. XANES, UPS, and DFT calculations consistently reveal the enhanced performance is attributed to the downshift of the d‐band center, which helps facilitate the H desorption. This concept could provide valuable insights into the design of other catalysts for HER and beyond.
中文翻译：
定制d波段中心使Co4N纳米片对氢气析出催化具有很高的活性
赋予具有特定功能的材料不容易获得始终是非常重要的，但是却极具挑战性。Co 4 N具有有益的金属特性，已被证明对水的氧化具有很高的活性，而众所周知，由于其不利的d波段能级，它对催化氢析出反应（HER）的作用极差。在这里，我们通过过渡金属掺杂来调整d谱带中心的位置，从而成功赋予Co 4 N具有出色的HER催化能力。掺V的Co 4 N纳米片在10 mA cm -2处显示37 mV的过电势，这明显好于Co 4N，甚至接近基准Pt / C催化剂。XANES，UPS和DFT计算始终显示出增强的性能归因于d波段中心的降档，这有助于促进H的解吸。这个概念可以为HER以外的其他催化剂的设计提供有价值的见解。
更新日期：2018-03-23
中文翻译：
定制d波段中心使Co4N纳米片对氢气析出催化具有很高的活性
赋予具有特定功能的材料不容易获得始终是非常重要的，但是却极具挑战性。Co 4 N具有有益的金属特性，已被证明对水的氧化具有很高的活性，而众所周知，由于其不利的d波段能级，它对催化氢析出反应（HER）的作用极差。在这里，我们通过过渡金属掺杂来调整d谱带中心的位置，从而成功赋予Co 4 N具有出色的HER催化能力。掺V的Co 4 N纳米片在10 mA cm -2处显示37 mV的过电势，这明显好于Co 4N，甚至接近基准Pt / C催化剂。XANES，UPS和DFT计算始终显示出增强的性能归因于d波段中心的降档，这有助于促进H的解吸。这个概念可以为HER以外的其他催化剂的设计提供有价值的见解。
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