期刊
SCIENCE BULLETIN
卷 67, 期 14, 页码 1467-1476出版社
ELSEVIER
DOI: 10.1016/j.scib.2022.06.009
关键词
Solar fuel; Carbon capture and utilization; Operando nanocatalyst synthesis; Photoelectrochemical; Energy conversion efficiency
资金
- National Natural Science Foun-dation of China [51888103, 52006103, 51976090, 52006101]
- Scientific and Technological Innovation Project of Carbon Emission Peak and Carbon Neutrality of Jiangsu Province [BE2022024]
- Nat-ural Science Foundation of Jiangsu Province [BK20200072, BK20200491, BK20200500]
- China Postdoctoral Science Foundation [2020M681603]
We demonstrated an efficient solar photovoltaic-powered electrochemical CO2 reduction device that uses a high-pressure CO2-captured liquid feed. The device takes advantage of high pressure in both catalyst synthesis and the CO2 reduction reaction to achieve high selectivity and energy conversion efficiency.
We demonstrated an efficient solar photovoltaic-powered electrochemical CO2 reduction device with a high-pressure CO2-captured liquid feed. In an air-to-barrel picture, this device holds promise to avoid both high-temperature gaseous CO2 regeneration and high energy-cost gas product separation steps, while these steps are necessary for devices with a gaseous CO2 feed. To date, solar fuel production with a CO2-saturated liquid feed suffers from high over-potential to suppress the hydrogen evolution reaction and consequently, low solar-to-chemical (STC) energy conversion efficiency. Here, we presented a dis-tinct high-pressure operando strategy, i.e., we took extra advantage of the high pressure in catalyst syn-thesis besides in the period of the CO2 reduction reaction (CO2RR). The power of this strategy was demonstrated by a proof-of-concept device in which a representative copper catalyst was first synthe-sized in operando in a high-pressure (50 bar) CO2-saturated KHCO3 solution, and then this high-pressure CO2-captured liquid was converted to solar fuel using the operando synthesized Cu catalyst. This Cu catalyst achieved 95% CO2RR selectivity at the recorded low potential of-0.3 V vs. RHE enabled by the combination of operando facet engineering and oxide derivation. Furthermore, this device achieved a record-high STC efficiency of 21.6% under outdoor illumination, superior to other CO2- saturated liquid-fed devices, and compared favorably to gaseous CO2-fed devices. (C) 2022 Science China Press. Published by Elsevier B.V. and Science China Press. All rights reserved.
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