作者
Tao Zhuang,Yuanjie Pang,Zhi Liang,Ziyun Wang,Yang Li,Chih Shan Tan,Jun Li,Cao-Thang Dinh,Phil De Luna,Pei Lun Hsieh,Thomas Burdyny,Huihui Li,Mengxia Liu,Yuhang Wang,Fengwang Li,Andrew H. Proppe,Andrew Johnston,Dae‐Hyun Nam,Zhen Wu,Ya Rong Zheng,Alexander H. Ip,Hairen Tan,Lih‐Juann Chen,Shengjie Yu,Shana O. Kelley,David Sinton
摘要
The electrosynthesis of higher-order alcohols from carbon dioxide and carbon monoxide addresses the need for the long-term storage of renewable electricity; unfortunately, the present-day performance remains below what is needed for practical applications. Here we report a catalyst design strategy that promotes C3 formation via the nanoconfinement of C2 intermediates, and thereby promotes C2:C1 coupling inside a reactive nanocavity. We first employed finite-element method simulations to assess the potential for the retention and binding of C2 intermediates as a function of cavity structure. We then developed a method of synthesizing open Cu nanocavity structures with a tunable geometry via the electroreduction of Cu2O cavities formed through acidic etching. The nanocavities showed a morphology-driven shift in selectivity from C2 to C3 products during the carbon monoxide electroreduction, to reach a propanol Faradaic efficiency of 21 ± 1% at a conversion rate of 7.8 ± 0.5 mA cm−2 at −0.56 V versus a reversible hydrogen electrode. The production of higher alcohols is very valuable because of their high volumetric energy density. Now, Sargent, Sinton and co-workers report the design of copper nanoparticles with tailored nanocavities that promote n-propanol formation by the coupling of C2 and C1 intermediates inside the cavity.