Zhang Renjie, Zhang Jianling, Wang Sha, Tan Zhonghao, Yang Yisen, Song Yi, Li Meiling, Zhao Yingzhe, Wang Hao, Han Buxing, Duan Ran
Beijing National Laboratory for Molecular Sciences, CAS Laboratory of Colloid and Interface and Thermodynamics, CAS Research/Education Center for Excellence in Molecular Sciences, Center for Carbon Neutral Chemistry, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190, China.
School of Chemical Sciences, University of Chinese Academy of Sciences, Beijing, 100049, China.
Angew Chem Int Ed Engl. 2024 Jul 22;63(30):e202405733. doi: 10.1002/anie.202405733. Epub 2024 Jun 21.
n-propanol is an important pharmaceutical and pesticide intermediate. To produce n-propanol by electrochemical reduction of CO is a promising way, but is largely restricted by the very low selectivity and activity. How to promote the coupling of *C and *C intermediates to form the *C intermediate for n-propanol formation is challenging. Here, we propose the construction of bicontinuous structure of CuO/Cu electrocatalyst, which consists of ultra-small CuO nanodomains, Cu nanodomains and large amounts of grain boundaries between CuO and Cu nanodomains. The n-propanol current density is as high as 101.6 mA cm at the applied potential of -1.1 V vs. reversible hydrogen electrode in flow cell, with the Faradaic efficiency up to 12.1 %. Moreover, the catalyst keeps relatively stable during electrochemical CO reduction process. Experimental studies and theoretical calculations reveal that the bicontinuous structure of CuO/Cu can facilitate the *CO formation, *CO-*CO coupling and *CO-*OCCO coupling for the final generation of n-propanol.
正丙醇是一种重要的医药和农药中间体。通过电化学还原CO制备正丙醇是一种很有前景的方法，但很大程度上受到极低的选择性和活性的限制。如何促进C和C中间体的偶联以形成用于生成正丙醇的C中间体具有挑战性。在此，我们提出构建CuO/Cu电催化剂的双连续结构，其由超小的CuO纳米域、Cu纳米域以及CuO和Cu纳米域之间的大量晶界组成。在流动池中相对于可逆氢电极施加-1.1 V的电位时，正丙醇电流密度高达101.6 mA cm，法拉第效率高达12.1%。此外，该催化剂在电化学CO还原过程中保持相对稳定。实验研究和理论计算表明，CuO/Cu的双连续结构可促进CO的形成、*CO-CO偶联以及CO-*OCCO偶联，最终生成正丙醇。
