Gao Jing, Li Jun, Liu Yuhang, Xia Meng, Finfrock Y Zou, Zakeeruddin Shaik Mohammed, Ren Dan, Grätzel Michael
Laboratory of Photonics and Interfaces, École Polytechnique Fédérale de Lausanne, 1015, Lausanne, Switzerland.
Structural Biology Center, X-ray Science Division, Argonne National Laboratory, Lemont, IL, 60439, USA.
Nat Commun. 2022 Oct 6;13(1):5898. doi: 10.1038/s41467-022-33049-7.
Copper catalysts modified with tin have been demonstrated to be selective for the electroreduction of carbon dioxide to carbon monoxide. However, such catalysts require the precise control of tin loading amount. Here, we develop a copper/tin-oxide catalyst with dominant tin oxide surface being formed via a spontaneous exchange reaction between sputtered tin and copper oxide. Even though the surface of this catalyst is tin-rich, it achieves an excellent performance towards carbon monoxide production in a flow cell. This contrasts with copper/tin-oxide prepared via atomic layer deposition since it yields selectivity towards carbon monoxide only on a copper-rich surface. Mechanism studies reveal that the tin sites on the tin-rich copper/tin-oxide surface achieve a suitable binding with adsorbed carbon monoxide under the presence of copper. Powered by a triple-junction solar cell, the copper/tin-oxide based electrolyzer sets a new benchmark solar-to-chemical energy conversion efficiency of 19.9 percent with a Faradaic efficiency of 98.9 percent towards carbon monoxide under simulated standard air mass 1.5 global illumination.
已证明用锡改性的铜催化剂对二氧化碳电还原为一氧化碳具有选择性。然而,这种催化剂需要精确控制锡的负载量。在此,我们开发了一种铜/氧化锡催化剂,通过溅射的锡与氧化铜之间的自发交换反应形成以氧化锡为主的表面。尽管该催化剂表面富含锡,但它在流动池中对一氧化碳的产生具有优异的性能。这与通过原子层沉积制备的铜/氧化锡形成对比,因为后者仅在富铜表面产生对一氧化碳的选择性。机理研究表明,在铜的存在下,富铜/氧化锡表面的锡位点与吸附的一氧化碳实现了合适的结合。由三结太阳能电池供电,基于铜/氧化锡的电解槽在模拟标准空气质量1.5全球光照下,创下了19.9%的太阳能到化学能转换效率新基准,对一氧化碳的法拉第效率为98.9%。