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Activating Inert Sites in Cobalt Silicate Hydroxides for Oxygen Evolution through Atomically Doping
Energy & Environmental Materials ( IF 13.0 ) Pub Date : 2021-05-24 , DOI: 10.1002/eem2.12219 Jiexin Zhu 1 , Lixue Xia 2 , Wenxuan Yang 1 , Ruohan Yu 1 , Wei Zhang 1 , Wen Luo 1 , Yuhang Dai 1 , Wei Wei 1 , Liang Zhou 1, 3 , Yan Zhao 2 , Liqiang Mai 1, 3
Energy & Environmental Materials ( IF 13.0 ) Pub Date : 2021-05-24 , DOI: 10.1002/eem2.12219 Jiexin Zhu 1 , Lixue Xia 2 , Wenxuan Yang 1 , Ruohan Yu 1 , Wei Zhang 1 , Wen Luo 1 , Yuhang Dai 1 , Wei Wei 1 , Liang Zhou 1, 3 , Yan Zhao 2 , Liqiang Mai 1, 3
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Metal silicate hydroxides have been recognized as efficient oxygen evolution reaction (OER) electrocatalysts, yet tailoring of their intrinsic activity remains confused. Herein, Fe had been incorporated into cobalt silicate hydroxide nanosheets and the resulted material achieves a competitive OER catalytic activity. It is found that the doping state obviously affects the electrical transport property. Specifically, highly dispersed Fe atoms (low-concentration Fe doping) trigger slight electron transfer to Co atoms while serried Fe (high-concentration Fe doping) attract vast electrons. By introducing 6 at.% Fe doping, partial relatively inert Co sites are activated by atomically dispersed Fe, bearing an optimal metal 3d electronic occupation and adsorption capacity to oxygen intermediate. The introduced Co−O−Fe unit trigger the π-donation effect and decrease the number of electrons in π*-antibonding orbitals, which enhance the Fe−O covalency and the structural stability. As a result, the sample delivers a low overpotential of 293 mV to achieve a current density of 10 mA cm−2. This work clarifies the superiority of atomically dispersed doping state, which is of fundamental interest to the design of doped catalyst.
中文翻译：
Activating Inert Sites in Cobalt Silicate Hydroxides for Oxygen Evolution through Atomically Doping,通过原子掺杂激活硅酸钴中的惰性位点用于析氧
Metal silicate hydroxides have been recognized as efficient oxygen evolution reaction (OER) electrocatalysts, yet tailoring of their intrinsic activity remains confused. Herein, Fe had been incorporated into cobalt silicate hydroxide nanosheets and the resulted material achieves a competitive OER catalytic activity. It is found that the doping state obviously affects the electrical transport property. Specifically, highly dispersed Fe atoms (low-concentration Fe doping) trigger slight electron transfer to Co atoms while serried Fe (high-concentration Fe doping) attract vast electrons. By introducing 6 at.% Fe doping, partial relatively inert Co sites are activated by atomically dispersed Fe, bearing an optimal metal 3d electronic occupation and adsorption capacity to oxygen intermediate. The introduced Co−O−Fe unit trigger the π-donation effect and decrease the number of electrons in π*-antibonding orbitals, which enhance the Fe−O covalency and the structural stability. As a result, the sample delivers a low overpotential of 293 mV to achieve a current density of 10 mA cm−2. This work clarifies the superiority of atomically dispersed doping state, which is of fundamental interest to the design of doped catalyst.,金属硅酸盐氢氧化物已被公认为有效的析氧反应 (OER) 电催化剂，但对其内在活性的定制仍存在混淆。在此，Fe 已掺入氢氧化硅酸钴纳米片中，所得材料具有竞争性的 OER 催化活性。发现掺杂状态明显影响电传输性能。具体来说，高度分散的 Fe 原子（低浓度 Fe 掺杂）触发轻微的电子转移到 Co 原子，而串联的 Fe（高浓度 Fe 掺杂）吸引大量电子。通过引入 6 at.% 的 Fe 掺杂，部分相对惰性的 Co 位点被原子分散的 Fe 激活，具有最佳金属 3 d氧中间体的电子占有和吸附能力。引入的Co-O-Fe单元触发了π-捐赠效应并减少了π *-反键轨道中的电子数，从而增强了Fe-O的共价性和结构稳定性。结果，样品提供了 293 mV 的低过电位，以实现 10 mA cm -2的电流密度。这项工作阐明了原子分散掺杂态的优越性，这对掺杂催化剂的设计具有根本意义。
更新日期：2021-05-24
中文翻译：
Activating Inert Sites in Cobalt Silicate Hydroxides for Oxygen Evolution through Atomically Doping,通过原子掺杂激活硅酸钴中的惰性位点用于析氧
Metal silicate hydroxides have been recognized as efficient oxygen evolution reaction (OER) electrocatalysts, yet tailoring of their intrinsic activity remains confused. Herein, Fe had been incorporated into cobalt silicate hydroxide nanosheets and the resulted material achieves a competitive OER catalytic activity. It is found that the doping state obviously affects the electrical transport property. Specifically, highly dispersed Fe atoms (low-concentration Fe doping) trigger slight electron transfer to Co atoms while serried Fe (high-concentration Fe doping) attract vast electrons. By introducing 6 at.% Fe doping, partial relatively inert Co sites are activated by atomically dispersed Fe, bearing an optimal metal 3d electronic occupation and adsorption capacity to oxygen intermediate. The introduced Co−O−Fe unit trigger the π-donation effect and decrease the number of electrons in π*-antibonding orbitals, which enhance the Fe−O covalency and the structural stability. As a result, the sample delivers a low overpotential of 293 mV to achieve a current density of 10 mA cm−2. This work clarifies the superiority of atomically dispersed doping state, which is of fundamental interest to the design of doped catalyst.,金属硅酸盐氢氧化物已被公认为有效的析氧反应 (OER) 电催化剂，但对其内在活性的定制仍存在混淆。在此，Fe 已掺入氢氧化硅酸钴纳米片中，所得材料具有竞争性的 OER 催化活性。发现掺杂状态明显影响电传输性能。具体来说，高度分散的 Fe 原子（低浓度 Fe 掺杂）触发轻微的电子转移到 Co 原子，而串联的 Fe（高浓度 Fe 掺杂）吸引大量电子。通过引入 6 at.% 的 Fe 掺杂，部分相对惰性的 Co 位点被原子分散的 Fe 激活，具有最佳金属 3 d氧中间体的电子占有和吸附能力。引入的Co-O-Fe单元触发了π-捐赠效应并减少了π *-反键轨道中的电子数，从而增强了Fe-O的共价性和结构稳定性。结果，样品提供了 293 mV 的低过电位，以实现 10 mA cm -2的电流密度。这项工作阐明了原子分散掺杂态的优越性，这对掺杂催化剂的设计具有根本意义。
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