期刊
ENERGY & ENVIRONMENTAL MATERIALS
卷 5, 期 3, 页码 892-898出版社
WILEY
DOI: 10.1002/eem2.12203
关键词
metal doping; hydrogen-bonding ligand; density functional theory; electrochemical CO2 reduction; C-2 oxygenates selectivity
资金
- National Natural Science Foundation of China [22033002, 21525311, 21773027]
- Scientific Research Foundation of Graduate School of Southeast University [YBPY1920]
- China Postdoctoral Science Foundation [2020M681450]
- China Scholarship Council (CSC) [201906090150]
By introducing a second metal and a functional ligand, a design strategy is proposed to achieve high selectivity of C-2 oxygenates and effectively inhibit the HER on the Cu(100) surface. This approach provides a new method to improve the electrocatalytic reduction of CO2.
Effectively controlling the selectivity of C-2 oxygenates is desirable for electrocatalytic CO2 reduction. Copper catalyst has been considered as the most potential for reducing CO2 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 simultaneously. Seven 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 *CHO. In 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 oxygenates. Therefore, this heterogeneous electrocatalyst can effectively reduce CO2 to ethanol and ethylene glycol with an ultra-low limiting potential of -0.43 V. This study provides a new strategy for effectively improving the selectivity of C-2 oxygenates and inhibiting HER to achieve advanced electrocatalytic CO2 reduction.
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