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Synergistic Effect of Metal Doping and Tethered ligand Promoted High-Selectivity Conversion of CO_(2)to C_(2)Oxygenates at Ultra-Low Potential

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Energy & Environmental Materials 2022年第3期5卷 892-898页

作者： Xiaowan Bai Li Shi Qiang Li Chongyi Ling Yixin Ouyang Shiyan Wang Jinlan Wang School of Physics Southeast UniversityNanjing 211189China

Effectively controlling the selectivity of C_(2) oxygenates is desirable for electrocatalytic CO_(2) *** catalyst has been considered as the most potential for reducing CO_(2) to C_(2) products,but it still suffers from low C_(2) selectivity,high overpotential,and competitive hydrogen evolution reaction(HER).Here,we propose a design strategy to introduce a second metal that weakly binds to H and a functional ligand that provides hydrogen bonds and protons to achieve high selectivity of C_(2)oxygenates and effective suppression of HER on the Cu(100)surface *** metals and eleven ligands are screened using first-principles calculations,which shows that Sn is the most efficient for inhibiting HER and cysteamine(CYS)ligand is the most significant in reducing the limiting potential of^(*)CO hydrogenation to^(*)*** the post C-C coupling steps,a so-called“pulling effect”that transfers H in the CYS ligand as a viable proton donor to the C_(2)intermediate to form an H bond,can further stabilize the OH group and facilitate the selection of C_(2)products toward ***,this heterogeneous electrocatalyst can effectively reduce CO_(2)to ethanol and ethylene glycol with an ultra-low limiting potential of-0.43 *** study provides a new strategy for effectively improving the selectivity of C_(2)oxygenates and inhibiting HER to achieve advanced electrocatalytic CO_(2)reduction.

关键词： metal doping hydrogen-bonding ligand density functional theory electrochemical CO_(2)reduction C_(2)oxygenates selectivity

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