Applied Catalysis B: Environment and Energy ( IF 20.2 ) Pub Date : 2021-05-11 , DOI: 10.1016/j.apcatb.2021.120342 Ke Ye , Tianfu Liu , Yanpeng Song , Qi Wang , Guoxiong Wang
Electrochemical CO2 reduction reaction (CO2RR) offers an appealing route to simultaneously store intermittent renewable energy as value-added chemicals and close carbon cycle. Silver (Ag) catalyst is a promising candidate for the electrochemical conversion of CO2 to CO, but the electrocatalytic properties are still insufficient for practical applications. Herein, we put forward a strategy to in situ reconstruct a heterogeneous Ag2S/Ag interface structure, in which their strong interactions facilitate CO2RR performance. The in situ reconstructive Ag2S/Ag catalyst achieves a large current density of 421.7 ± 14.4 mA cm–2 at –0.70 V vs. reversible hydrogen electrode (RHE) and maintains steadily at a current density of 244.5 ± 31.8 mA cm–2 and CO Faradaic efficiency of 99.1 ± 0.8 % at –0.49 V vs. RHE for 50 h, superior to state-of-the-art CO-selective Ag-based catalysts. Density functional theory calculations reveal that the in situ reconstructive Ag2S/Ag interface active sites stabilize the *COOH intermediate during CO2RR process.
中文翻译:
量身定制异质Ag 2 S / Ag界面的相互作用,以实现有效的CO 2电还原
电化学CO 2还原反应(CO 2 RR)提供了一种吸引人的途径,可以同时存储间歇性可再生能源,作为增值化学品并关闭碳循环。银(Ag)催化剂是将CO 2电化学转化为CO的有前途的候选物,但电催化性能仍不足以用于实际应用。本文中,我们提出了一种原位重建异质Ag 2 S / Ag界面结构的策略,其中它们的强相互作用促进了CO 2 RR性能。在原位重建的Ag 2 S /银催化剂实现的421.7±14.4毫安厘米的大电流密度-2在-0.70 V VS。可逆氢电极(RHE),在–0.49 V vs.时稳定地保持在244.5±31.8 mA cm –2的电流密度和99.1±0.8%的CO法拉第效率。RHE历时50小时,优于最先进的CO选择性银基催化剂。密度泛函理论计算表明,在CO 2 RR过程中,原位重建的Ag 2 S / Ag界面活性位点稳定了* COOH中间体。