期刊
NATURE COMMUNICATIONS
卷 9, 期 -, 页码 -出版社
NATURE PUBLISHING GROUP
DOI: 10.1038/s41467-018-07380-x
关键词
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资金
- National Key Research and Development Program of China [2017YFA0206901, 2018YFA0209401]
- Natural Science Foundation of China [21773036, 21473038]
- Key Basic Research Program of Science and Technology Commission of Shanghai Municipality [17JC1400100]
- Collaborative Innovation Center of Chemistry for Energy Materials [2011-iChem]
- Hui-Chun Chin & Tsung-Dao Lee Chinese Undergraduate Research Endowment
Solar-driven electrochemical carbon dioxide (CO2) reduction is capable of producing value-added chemicals and represents a potential route to alleviate carbon footprint in the global environment. However, the ever-changing sunlight illumination presents a substantial impediment of maintaining high electrocatalytic efficiency and stability for practical applications. Inspired by green plant photosynthesis with separate light reaction and (dark) carbon fixation steps, herein, we developed a redox-medium-assisted system that proceeds water oxidation with a nickel-iron hydroxide electrode under light illumination and stores the reduction energy using a zinc/zincate redox, which can be controllably released to spontaneously reduce CO2 into carbon monoxide (CO) with a gold nanocatalyst in dark condition. This redox-medium-assisted system enables a record-high solar-to-CO photoconversion efficiency of 15.6% under 1-sun intensity, and an outstanding electric energy efficiency of 63%. Furthermore, it allows a unique tuning capability of the solar-to-CO efficiency and selectivity by the current density applied during the carbon fixation.
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