Li Shoujie, Dong Xiao, Zhao Yonghui, Mao Jianing, Chen Wei, Chen Aohui, Song Yanfang, Li Guihua, Jiang Zheng, Wei Wei, Sun Yuhan
Low-Carbon Conversion Science and Engineering Center, Shanghai Advanced Research Institute, Chinese Academy of Sciences, 100 Haike Road, Shanghai, 201210, P. R. China.
School of Physical Science and Technology, ShanghaiTech University, 393 Middle Huaxia Road, Shanghai, 201203, P. R. China.
Angew Chem Int Ed Engl. 2022 Oct 17;61(42):e202210432. doi: 10.1002/anie.202210432. Epub 2022 Sep 19.
Electrochemical conversion of CO into valuable feedstocks is a promising strategy for carbon neutrality. However, it remains a challenge to possess a large current density, a high faradaic efficiency and excellent stability for practical applications of CO utilization. Herein, we report a facile tactic that enables exceedingly efficient CO electroreduction to CO by virtue of low-coordination chloride ion (Cl ) adsorption on a silver hollow fiber (Ag HF) electrode. A CO faradaic efficiency of 92.3 % at a current density of one ampere per square centimeter (1 A cm ) in 3.0 M KCl with a sustained performance observed during a 150-hour test was achieved, which is better than state-of-the-art electrocatalysts. The electrochemical results and density functional theory (DFT) calculations suggested a low-coordination Cl adsorption on surface of Ag HF, which not only suppressed the competitive hydrogen evolution reaction (HER), but also facilitated the CO reduction kinetics.
将CO电化学转化为有价值的原料是实现碳中和的一种很有前景的策略。然而，对于CO利用的实际应用而言，要同时具备大电流密度、高法拉第效率和出色的稳定性仍然是一项挑战。在此，我们报告了一种简便的策略，通过低配位氯离子（Cl⁻）吸附在银中空纤维（Ag HF）电极上，能够极其高效地将CO电还原为CO。在3.0 M KCl中，当电流密度为每平方厘米1安培（1 A cm⁻²）时，实现了92.3%的CO法拉第效率，并且在150小时的测试中观察到了持续的性能，这优于目前最先进的电催化剂。电化学结果和密度泛函理论（DFT）计算表明，低配位Cl⁻吸附在Ag HF表面，这不仅抑制了竞争性析氢反应（HER），还促进了CO还原动力学。
