Journal
JOULE
Volume 3, Issue 7, Pages 1703-1718Publisher
CELL PRESS
DOI: 10.1016/j.joule.2019.05.010
Keywords
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Funding
- National Natural Science Foundation of China [21872174]
- International S&T Cooperation Program of China [2017YFE0127800]
- Ontario Research Fund Research-Excellence Program
- Natural Sciences and Engineering Research Council (NSERC) of Canada
- Canadian Institute for Advanced Research
- University of Toronto
- Ministry of Science and Technology of Taiwan
- King Abdullah University of Science and Technology (KAUST)
- Project of Innovation-Driven Plan in Central South University [2017CX003, 20180018050001]
- Hunan Provincial Science and Technology Program [2017XK2026]
- State Key Laboratory of Powder Metallurgy in Central South University
- Shenzhen Science and Technology Innovation Project [JCYJ20180307151313532, JCYJ20180307164633296]
- Thousand Youth Talents Plan of China
- Hundred Youth Talents Program of Hunan
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Defect sites are often proposed as key active sites in the design of catalysts. A promising strategy for improving activity is to achieve a high density of homogeneously dispersed atomic defects; however, this is seldom accomplished in metals. We hypothesize that vacancy-rich catalysts could be obtained through the synthesis of quantum dots (QDs) and their electrochemical reduction during the CO2 reduction reaction (CO2RR). Here, we report that QD-derived catalysts (QDDCs) with up to 20 vol % vacancies achieve record current densities of 16, 19, and 25 mAcm(-2) with high faradic efficiencies in the electrosynthesis of formate, carbon monoxide, and ethylene at low potentials of -0.2, -0.3, and -0.9 V versus reversible hydrogen electrode (RHE), respectively. The materials are stable after 80 hr of CO2RR. These CO2RR performances in aqueous solution surpass those of previously reported catalysts by 2X. Together, X-ray absorption spectroscopy and computational studies reveal that the vacancies produce a local atomic and electronic structure that enhances CO2RR.
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