Amination strategy to boost the CO2 electroreduction current density of M–N/C single-atom catalysts to the industrial application level,Energy & Environmental Science

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Amination strategy to boost the CO2 electroreduction current density of M–N/C single-atom catalysts to the industrial application level
Energy & Environmental Science ( IF 32.4 ) Pub Date : 2021-2-12 , DOI: 10.1039/d0ee04052e
Zhipeng Chen _{1,

2,

3,

4} , Xinxin Zhang _{1,

2,

3,

4} , Wei Liu _{2,

4,

5,

6,

7} , Mingyang Jiao _{1,

2,

3,

4} , Kaiwen Mou _{1,

2,

3,

4} , Xiangping Zhang _{2,

4,

7,

8,

9} , Licheng Liu _{1,

2,

3,

4,

7}

Affiliation

Although the Faraday efficiency (FE) for CO production of single-atom catalysts immobilized on nitrogen-doped carbon supports (M–N/C) for the CO₂ electrocatalytic reduction reaction (CO₂RR) is generally over 90%, M–N/C catalysts demonstrate a poor reaction current density, which is much worse than the current density at the industrial level. Herein, we first report a generalized amination strategy to significantly increase the current density for CO production of M–N/C catalysts (M = Ni, Fe, Zn). Among them, the aminated Ni single-atom catalyst achieves a remarkable CO partial current density of 450 mA cm⁻² (a total current density over 500 mA cm⁻²) with a nearly 90% CO FE at a moderate overpotential of 0.89 V, and particularly CO FE can be maintained over 85% in a wide operating potential range from −0.5 V to −1.0 V. DFT calculations and experimental research demonstrate that the superior activity is attributed to enhanced adsorption energies of CO₂* and COOH* intermediates caused by the regulation of the electronic structure of the aminated catalysts. This work provides an ingenious method for significantly increasing the current density at the industrially-relevant level of single-atom catalysts for the CO₂RR.

中文翻译：

将M–N / C单原子催化剂的CO2电还原电流密度提高到工业应用水平的胺化策略

尽管固定在氮掺杂碳载体上的单原子催化剂的CO生产法拉第效率（FE）（M–N / C）对于CO ₂电催化还原反应（CO ₂ RR）通常超过90％，但M–N / C催化剂显示出较差的反应电流密度，这比工业水平的电流密度差得多。在本文中，我们首先报告了一种广义的胺化策略，以显着提高M / N / C催化剂（M = Ni，Fe，Zn）的CO生产电流密度。其中，胺化的镍单原子催化剂可实现450 mA cm ^-2的显着CO分流密度（总电流密度超过500 mA cm ^-2））的COFE接近90％，在0.89 V的中等过电势下，特别是在-0.5 V至-1.0 V的宽工作电压范围内，CO FE可以保持超过85％.DFT计算和实验研究表明活性归因于由胺化催化剂的电子结构的调节引起的CO ₂ *和COOH *中间体的吸附能的增加。这项工作提供了一种巧妙的方法，可以在与工业相关的水平上大幅提高CO ₂ RR的单原子催化剂的电流密度。

更新日期：2021-03-02

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