Dopant-tuned stabilization of intermediates promotes electrosynthesis of valuable C3 products.
Tao-Tao ZhuangDae-Hyun NamZiyun WangHui-Hui LiChristine M GabardoYi LiZhi-Qin LiangJun LiXiao-Jing LiuBin ChenWan Ru LeowRui WuXue WangFengwang LiYanwei LumJoshua WicksColin P O'BrienTao PengAlexander H IpTsun-Kong ShamShu-Hong YuDavid SintonEdward H SargentPublished in: Nature communications (2019)
The upgrading of CO2/CO feedstocks to higher-value chemicals via energy-efficient electrochemical processes enables carbon utilization and renewable energy storage. Substantial progress has been made to improve performance at the cathodic side; whereas less progress has been made on improving anodic electro-oxidation reactions to generate value. Here we report the efficient electroproduction of value-added multi-carbon dimethyl carbonate (DMC) from CO and methanol via oxidative carbonylation. We find that, compared to pure palladium controls, boron-doped palladium (Pd-B) tunes the binding strength of intermediates along this reaction pathway and favors DMC formation. We implement this doping strategy and report the selective electrosynthesis of DMC experimentally. We achieve a DMC Faradaic efficiency of 83 ± 5%, fully a 3x increase in performance compared to the corresponding pure Pd electrocatalyst.