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Selective CO-to-acetate electroreduction via intermediate adsorption tuning on ordered Cu–Pd sites
Nature Catalysis ( IF 42.8 ) Pub Date : 2022-03-28 , DOI: 10.1038/s41929-022-00757-8
Yali Ji 1 , Zheng Chen 1 , Chao Yang 1 , Anxiang Guan 1 , Xin Xu 1 , Gengfeng Zheng 1 , Ruilin Wei 2 , Yaoyue Yang 2 , Yuhang Wang 3 , Jie Xu 3 , Hao Zhang 4 , Jun Luo 4 , Jiatang Chen 5 , Tsun-Kong Sham 5
Affiliation  

Electrochemical reduction of carbon monoxide (CO) has recently emerged as a potential approach for obtaining high-value, multicarbon products such as acetate, while the activity and selectivity for prodution of acetate have remained low. Herein, we develop an atomically ordered copper–palladium intermetallic compound (CuPd) composed of a high density of Cu–Pd pairs that feature as catalytic sites to enrich surface *CO coverage, stabilize ethenone as a key acetate path intermediate and inhibit the hydrogen evolution reaction, thus substantially promoting acetate formation. The CuPd electrocatalyst enables a high Faradaic efficiency of 70 ± 5% for CO-to-acetate electroreduction and a high acetate partial current density of 425 mA cm−2. Under membrane electrode assembly conditions, the CuPd electrocatalyst demonstrated a 500 h CO-to-acetate conversion at 500 mA cm−2 with a stable acetate Faradaic efficiency of ~50%.



中文翻译:

通过在有序 Cu-Pd 位点上的中间吸附调节选择性 CO 到乙酸的电还原

一氧化碳 (CO) 的电化学还原最近已成为获得高价值、多碳产品(如乙酸盐)的潜在方法,而生产乙酸盐的活性和选择性仍然很低。在此,我们开发了一种原子有序的铜-钯金属间化合物 (CuPd),该化合物由高密度的 Cu-Pd 对组成,作为催化位点以丰富表面*CO 覆盖,稳定乙烯酮作为关键的醋酸途径中间体并抑制析氢反应,从而大大促进乙酸盐的形成。CuPd 电催化剂实现了 70 ± 5% 的高法拉第效率,用于 CO 转化为乙酸盐的电还原和 425 mA cm -2的高乙酸盐分电流密度. 在膜电极组装条件下,CuPd 电催化剂在 500 mA cm -2下表现出 500 小时 CO 到乙酸盐的转化,稳定的乙酸盐法拉第效率约为 50%。

更新日期:2022-03-28
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