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Functionalized Ag with Thiol Ligand to Promote Effective CO2 Electroreduction
ACS Nano ( IF 15.8 ) Pub Date : 2022-09-12 , DOI: 10.1021/acsnano.2c03512
Junmei Chen 1 , Xiaoqing Liu 2 , Shibo Xi 3 , Tianyu Zhang 1 , Zhihe Liu 1 , Jiayi Chen 1 , Lei Shen 2 , Sibudjing Kawi 1 , Lei Wang 1
Affiliation  

It is challenging while critical to develop efficient catalysts that can achieve both high current density and high energy efficiency for electrocatalytic CO2 reduction (CO2R). Herein, we report a strategy of tailoring the surface electronic structure of an Ag catalyst via thiol ligand modification to improve its intrinsic activity, selectivity, and further energy efficiency toward CO2R. Specifically, interconnected Ag nanoparticles with residual thiol ligands on the surface were prepared through electrochemical activation of a thiol-ligand-based Ag complex. When it was used as a catalyst for CO2R, the thiol-ligand modified Ag exhibited high CO selectivity (>90%) throughout a wide electrode-potential range; furthermore, high cathodic energy efficiencies of >90% and >70% were obtained for CO formation at high current densities of 150 and 750 mA cm–2, respectively, outperforming the state-of-the-art Ag-based electrocatalysts for CO2 to CO conversion. The first-principle calculations on the reaction energetics suggest that the binding energies of the key intermediate −*COOH on Ag are optimized by the adsorbed thiol ligand, thus favoring CO formation while suppressing the competing H2 evolution. Our findings provide a rational design strategy for CO2 reduction electrocatalyst by electronic modulation through surface-adsorbed ligands.

中文翻译:

具有硫醇配体的功能化银促进有效的 CO2 电还原

开发能够同时实现高电流密度和高能量效率的高效催化剂具有挑战性,同时也很关键,用于电催化 CO 2还原 (CO 2 R)。在此,我们报告了一种通过硫醇配体修饰来调整 Ag 催化剂表面电子结构的策略,以提高其对 CO 2 R 的内在活性、选择性和进一步的能量效率。具体而言,表面上具有残留硫醇配体的互连 Ag 纳米颗粒是通过电化学活化硫醇-配体基银复合物制备。当它用作CO 2的催化剂时R,硫醇-配体修饰的银在很宽的电极电位范围内表现出高的 CO 选择性(>90%);此外,在 150 和 750 mA cm –2的高电流密度下,CO 生成的高阴极能量效率分别为 >90% 和 >70% ,优于最先进的银基 CO 2电催化剂转化为 CO。对反应能量学的第一性原理计算表明,关键中间体-*COOH 在 Ag 上的结合能被吸附的硫醇配体优化,从而有利于 CO 的形成,同时抑制了竞争的 H 2释放。我们的研究结果为 CO 2提供了合理的设计策略通过表面吸附配体的电子调制还原电催化剂。
更新日期:2022-09-12
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