Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 58, Issue 4, Pages 1134-1137Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201810648
Keywords
carbon nitride; carbon vacancies; CO2 reduction; defect engineering; photocatalysis
Categories
Funding
- National Key R&D Program of China [2018YFA0209301]
- National Natural Science Foundation of China [21425309, 21761132002, 21703039, 21861130353]
- 111 Project [D16008]
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Photosynthetic conversion of CO2 into fuel and chemicals is a promising but challenging technology. The bottleneck of this reaction lies in the activation of CO2, owing to the chemical inertness of linear CO2. Herein, we present a defect-engineering methodology to construct CO2 activation sites by implanting carbon vacancies (CVs) in the melon polymer (MP) matrix. Positron annihilation spectroscopy confirmed the location and density of the CVs in the MP skeleton. In situ diffuse reflectance infrared Fourier transform spectroscopy and a DFT study revealed that the CVs can function as active sites for CO2 activation while stabilizing COOH* intermediates, thereby boosting the reaction kinetics. As a result, the modified MP-TAP-CVs displayed a 45-fold improvement in CO2-to-CO activity over the pristine MP. The apparent quantum efficiency of the MP-TAP-CVs was 4.8 % at 420 nm. This study sheds new light on the design of high-efficiency polymer semiconductors for CO2 conversion.
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