期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 60, 期 48, 页码 25485-25492出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202111136
关键词
C2H4; CO2 electroreduction; copper nanoparticle; single atom catalyst; tandem catalysis
资金
- National Key Research and Development Program of China [2018YFA0208600, 2018YFA0704502]
- NSFC [21871263, 22071245, 22033008]
- Youth Innovation Promotion Association, CAS [Y201850]
- Natural Science Foundation of Fujian Provincial Department of Science and Technology [2020J01863]
- Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China [2021ZZ103]
An effective tandem catalysis strategy was developed to improve the selectivity of CO2RR towards C2H4, using multiple distinct catalytic sites in local vicinity. A tandem electrocatalyst PTF(Ni)/Cu was constructed, which significantly enhanced the Faradaic efficiency of C2H4 to 57.3% at -1.1 V versus RHE. Experimental and theoretical results showed that the local high concentration of CO generated by PTF(Ni) sites facilitated the C-C coupling on nearby Cu NP sites to form C2H4.
Herein, an effective tandem catalysis strategy is developed to improve the selectivity of the CO2RR towards C2H4 by multiple distinct catalytic sites in local vicinity. An earth-abundant elements-based tandem electrocatalyst PTF(Ni)/Cu is constructed by uniformly dispersing Cu nanoparticles (NPs) on the porphyrinic triazine framework anchored with atomically isolated nickel-nitrogen sites (PTF(Ni)) for the enhanced CO2RR to produce C2H4. The Faradaic efficiency of C2H4 reaches 57.3 % at -1.1 V versus the reversible hydrogen electrode (RHE), which is about 6 times higher than the non-tandem catalyst PTF/Cu, which produces CH4 as the major carbon product. The operando infrared spectroscopy and theoretic density functional theory (DFT) calculations reveal that the local high concentration of CO generated by PTF(Ni) sites can facilitate the C-C coupling to form C2H4 on the nearby Cu NP sites. The work offers an effective avenue to design electrocatalysts for the highly selective CO2RR to produce multicarbon products via a tandem route.
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