用于 CO2 电还原的单原子催化剂和双原子催化剂：竞争还是合作？,Small

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用于 CO2 电还原的单原子催化剂和双原子催化剂：竞争还是合作？
Small ( IF 13.0 ) Pub Date : 2023-06-02 , DOI: 10.1002/smll.202303446
Yueyue Shao _{1,

2} , Qunhui Yuan ₃ , Jia Zhou _{1,

2}

Affiliation

开发用于电化学还原CO ₂的高活性和选择性电催化剂可以减少环境污染和温室气体排放。由于原子利用率最大化，原子分散催化剂被广泛应用于CO ₂还原反应(CO ₂ RR)。与单原子催化剂（SAC）相比，双原子催化剂（DAC）具有更灵活的活性位点、独特的电子结构和协同原子间相互作用，可能具有提高催化性能的巨大潜力。然而，大多数现有的电催化剂由于其高能垒而具有较低的活性和选择性。在此，探索了15种将贵金属（Cu、Ag和Au）活性位点嵌入金属有机杂化物（MOH）中用于高性能CO ₂ RR的电催化剂，并通过第一性原理计算研究了SAC和DAC之间的关系。结果表明DACs具有优异的电催化性能，单原子中心和双原子中心之间的适度相互作用可以提高CO ₂ RR的催化活性。15种催化剂中的4种，包括(CuAu)、(CuCu)、Cu(CuCu)和Cu(CuAu) MOHs继承了抑制竞争性析氢反应的能力，并具有有利的CO过电势。这项工作不仅揭示了基于MOHs的双原子CO ₂ RR电催化剂的优秀候选者，而且为合理设计2D金属电催化剂提供了新的理论见解。

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Single-Atom Catalysts and Dual-Atom Catalysts for CO2 Electroreduction: Competition or Cooperation?

Developing highly active and selective electrocatalysts for electrochemical reduction of CO₂ can reduce environmental pollution and mitigation of greenhouse gas emission. Owing to maximal atomic utilization, the atomically dispersed catalysts are broadly adopted in CO₂ reduction reaction (CO₂RR). Dual-atom catalysts (DACs), with more flexible active sites, distinct electronic structures, and synergetic interatomic interactions compared to single-atom catalysts (SACs), may have great potential to enhance catalytic performance. Nevertheless, most of the existing electrocatalysts have low activity and selectivity due to their high energy barrier. Herein, 15 electrocatalysts are explored with noble metallic (Cu, Ag, and Au) active sites embedded in metal–organic hybrids (MOHs) for high-performance CO₂RR and studied the relationship between SACs and DACs by first-principles calculation. The results indicated that the DACs have excellent electrocatalytic performance, and the moderate interaction between the single- and dual-atomic center can improve catalytic activity in CO₂RR. Four among the 15 catalysts, including (CuAu), (CuCu), Cu(CuCu), and Cu(CuAu) MOHs inherited a capability of suppressing the competitive hydrogen evolution reaction with favorable CO overpotential. This work not only reveals outstanding candidates for MOHs-based dual-atom CO₂RR electrocatalysts but also provides new theoretical insights into rationally designing 2D metallic electrocatalysts.

更新日期：2023-06-02

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