Department of Electrical and Computer Engineering, University of Toronto, 10 King's College Road, Toronto, ON, M5S 3G4, Canada.
Key Laboratory of Luminescence and Optical Information, Beijing Jiaotong University, Ministry of Education, Beijing, 100044, China.
Nat Commun. 2018 Sep 20;9(1):3828. doi: 10.1038/s41467-018-06311-0.
Copper-based materials are promising electrocatalysts for CO reduction. Prior studies show that the mixture of copper (I) and copper (0) at the catalyst surface enhances multi-carbon products from CO reduction; however, the stable presence of copper (I) remains the subject of debate. Here we report a copper on copper (I) composite that stabilizes copper (I) during CO reduction through the use of copper nitride as an underlying copper (I) species. We synthesize a copper-on-nitride catalyst that exhibits a Faradaic efficiency of 64 ± 2% for C products. We achieve a 40-fold enhancement in the ratio of C to the competing CH compared to the case of pure copper. We further show that the copper-on-nitride catalyst performs stable CO reduction over 30 h. Mechanistic studies suggest that the use of copper nitride contributes to reducing the CO dimerization energy barrier-a rate-limiting step in CO reduction to multi-carbon products.
基于铜的材料是一种很有前途的 CO 还原电催化剂。先前的研究表明,催化剂表面铜(I)和铜(0)的混合物可以增强 CO 还原的多碳产物;然而,铜(I)的稳定存在仍然存在争议。在这里,我们报告了一种铜铜(I)复合材料,它通过使用氮化铜作为底层铜(I)物种,在 CO 还原过程中稳定铜(I)。我们合成了一种铜氮化物催化剂,其 C 产物的法拉第效率为 64±2%。与纯铜相比,我们将 C 与竞争 CH 的比例提高了 40 倍。我们进一步表明,铜氮化物催化剂在 30 小时内能够稳定地进行 CO 还原。机理研究表明,使用氮化铜有助于降低 CO 二聚能垒——这是 CO 还原为多碳产物的限速步骤。