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CO2 Conversion on Ligand-Protected Au25 Nanoparticle: The Role of Structural Inhomogeneity in the Promotion of the Electrocatalytic Process
Physica Status Solidi (B) - Basic Solid State Physics ( IF 1.6 ) Pub Date : 2020-09-15 , DOI: 10.1002/pssb.202000387
Dominic R. Alfonso 1
Affiliation  

The possibility of direct integration with renewable electric sources adds more potential to the electrochemical method as a promising route for CO2 conversion. Previous experimental breakthrough reveals that Au25(SR)18 nanoclusters having 25 gold atoms and 18 protecting thiolate ligands can be utilized as catalysts for CO2 electroreduction to CO. The reason for its observed activity toward CO2 conversion is of fundamental importance that needs to be explained. Herein, the progress made in the first-principles mechanistic studies of the reduction process is described. Contrary to long-standing assumptions, the fully ligand protected version is not the active catalyst because of the weak adsorption of the relevant intermediates. Instead, the calculations based on computational hydrogen electrode method reveal that the reduction process is facilitated by a thermodynamically stable yet structurally inhomogeneous active site. This reaction center binds the intermediates in such a way that the process can occur at low overpotentials. The results point to the role of inhomogeneity in the surface region for this class of materials as a critical factor promoting the CO2 conversion process under electrochemical environment.

中文翻译:

配体保护的 Au25 纳米颗粒上的 CO2 转化:结构不均匀性在促进电催化过程中的作用

与可再生能源直接集成的可能性为电化学方法增加了更多潜力,作为 CO 2转化的有前途的途径。先前的实验突破表明,具有 25 个金原子和 18 个保护硫醇盐配体的Au 25 (SR) 18 -纳米团簇可用作 CO 2电还原为 CO 的催化剂。观察到其对 CO 2活性的原因转换具有根本的重要性,需要加以解释。在此,描述了在还原过程的第一性原理机制研究中取得的进展。与长期存在的假设相反,完全配体保护的版本不是活性催化剂,因为相关中间体的吸附较弱。相反,基于计算氢电极方法的计算表明,热力学稳定但结构不均匀的活性位点促进了还原过程。该反应中心以这样一种方式结合中间体,使得该过程可以在低过电位下发生。结果表明,这类材料表面区域的不均匀性是促进 CO 2 电化学环境下的转化过程。
更新日期:2020-09-15
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