Self-Supported Nickel Single Atoms Overwhelming the Concomitant Nickel Nanoparticles Enable Efficient and Selective CO2 Electroreduction,Advanced Materials Interfaces

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Self-Supported Nickel Single Atoms Overwhelming the Concomitant Nickel Nanoparticles Enable Efficient and Selective CO2 Electroreduction
Advanced Materials Interfaces ( IF 4.3 ) Pub Date : 2021-09-23 , DOI: 10.1002/admi.202101542
Shujin Shen ₁ , Cheng Han ₁ , Bing Wang ₁ , Yingde Wang ₁

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Self-supported metal/nitrogen-doped carbon (M-N-C) catalysts with unitary single-atom (SA) sites are highly desired to facilitate the electrocatalysis industrialization. Nevertheless, the concomitance of metal nanoparticles (NPs) enclosed by graphene layers is commonly inevitable and results in structure heterogeneity. Herein, an electronic structure modulation strategy of inactivating nickel (Ni) NPs to maximize Ni SAs for highly efficient and selective carbon dioxide reduction reaction (CO₂RR) within a facilely prepared self-supported Ni NPs/SAs-containing catalyst is reported. The side effect of Ni NPs is effectively inhibited by finely tuning the encapsulating graphene layers thickness to block electrons penetration. The optimized catalyst exhibits a nearly 100% selectivity of CO production under moderate working potentials of −0.6– −0.8 V (vs reversible hydrogen electrode) and produces a partial current density of 341 mA cm⁻² when directly used as a gas diffusion electrode for CO₂RR. The authors’ discoveries provide fresh insights into the design and scalable preparation of self-supported M-N-C catalysts with unitary single-atom active sites for CO₂RR aiming at industrialization.

中文翻译：

自支撑镍单原子压倒伴随的镍纳米颗粒实现高效和选择性的 CO2 电还原

非常需要具有单一单原子（SA）位点的自支撑金属/氮掺杂碳（MNC）催化剂以促进电催化工业化。然而，石墨烯层包围的金属纳米粒子 (NPs) 的伴随通常是不可避免的，并导致结构异质性。在此，一种使镍 (Ni) NPs 失活以最大化 Ni SAs 的电子结构调节策略，用于高效和选择性的二氧化碳还原反应 (CO ₂RR) 在一种容易制备的自支撑 Ni NPs/SAs 含催化剂中被报道。通过微调封装石墨烯层的厚度以阻止电子渗透，可以有效抑制 Ni NPs 的副作用。优化后的催化剂在 -0.6– -0.8 V（相对于可逆氢电极）的中等工作电位下表现出近 100% 的 CO 生成选择性，当直接用作气体扩散电极时，产生的部分电流密度为 341 mA cm ^-2 CO ₂ RR。作者的发现为以工业化为目标的具有单一单原子活性位点的自支撑 MNC 催化剂的设计和可扩展制备提供了新的见解，用于 CO ₂ RR。

更新日期：2021-10-22

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