期刊
NATURE COMMUNICATIONS
卷 10, 期 -, 页码 -出版社
NATURE PUBLISHING GROUP
DOI: 10.1038/s41467-019-12788-0
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资金
- Ontario Research Fund Research-Excellence Program
- Natural Sciences and Engineering Research Council (NSERC) of Canada
- CIFAR Bio-Inspired Solar Energy program
- U.S. DOE [DE-AC02-06CH11357]
- Canadian Light Source
- National Natural Science Foundation of China [21431006]
- Foundation for Innovative Research Groups of the National Natural Science Foundation of China [21521001]
- NSERC E.W.R Steacie Memorial Fellowship
- Banting Postdoctoral Fellowships program
- NSERC Postdoctoral Fellowships program
- Southern Ontario Smart Computing Innovation Platform (SOSCIP)
- Niagara supercomputer at the SciNet HPC Consortium
- Federal Economic Development Agency of Southern Ontario
- Province of Ontario
- IBM Canada Ltd.
- Ontario Centres of Excellence
- Mitacs and 15 Ontario academic member institutions
- Canada Foundation for Innovation
- Government of Ontario
- Ontario Research Fund-Research Excellence
- University of Toronto
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.
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