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Electrocatalytic CO2 reduction: role of the cross-talk at nano-carbon interfaces
Energy & Environmental Science ( IF 32.5 ) Pub Date : 2021-10-21 , DOI: 10.1039/d1ee00228g
Michele Melchionna 1 , Paolo Fornasiero 1, 2 , Maurizio Prato 1, 3, 4 , Marcella Bonchio 5
Affiliation  

The electrocatalytic CO2 reduction reaction (CO2RR) is an interfacial process, involving a minimum of three phases at the contact point of gaseous CO2 with the electrodic surface and the liquid electrolyte. As a consequence, surface chemistry at composite interfaces plays a central role for CO2RR selectivity and catalysis. Each interface defines a functional boundary, where active sites are exposed to a unique environment, with respect to distal sites in the bulk of organic and inorganic domains. While the individual role of each component-type is hardly predictable “a-solo”, the interface ensemble works via a strategic interplay of individual effects, including: (i) enhanced electrical conductivity, (ii) high surface area and exposure of the interfacial catalytic sites, (iii) favorable diffusion and feeding of reactants, (iv) complementary interactions for the “on/off” stabilization of cascade intermediates, (v) a secondary sphere assistance to lower the activation energy of bottleneck steps, (vi) a reinforced robustness and long-term operation stability. Selected CO2RR case studies are compared and contrasted to highlight how the organic domains of carbon nanostructures merge with metal and metal-oxide active sites to separate tasks but also to turn them into a cooperative asset of mutual interactions, thus going beyond the classic “Divide et Impera” rule.

中文翻译:

电催化 CO2 还原:纳米碳界面串扰的作用

电催化CO 2还原反应 (CO 2 RR) 是一种界面过程,在气态 CO 2与电极表面和液体电解质的接触点处涉及至少三相。因此,复合界面处的表面化学对 CO 2 RR 选择性和催化作用起着核心作用。每个界面都定义了一个功能边界,其中活性位点暴露于独特的环境中,相对于大部分有机和无机域中的远端位点。虽然每个组件类型的单独角色几乎是不可预测的“a-solo”,但界面集成通过个体效应的战略相互作用,包括:(i) 增强的导电性,(ii) 高表面积和界面催化位点的暴露,(iii) 有利的反应物扩散和进料,(iv) “on/ off”级联中间体的稳定性,(v) 辅助球体帮助降低瓶颈步骤的活化能,(vi) 增强的稳健性和长期操作稳定性。对选定的 CO 2 RR 案例研究进行比较和对比,以突出碳纳米结构的有机域如何与金属和金属氧化物活性位点融合以分离任务,同时将它们变成相互相互作用的合作资产,从而超越经典的“分而治之”的规则。
更新日期:2021-10-22
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