期刊
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
卷 -, 期 -, 页码 -出版社
AMER CHEMICAL SOC
DOI: 10.1021/acssuschemeng.2c04801
关键词
CO2 reduction; silver nanoclusters; formate; photocatalysis; formate dehydrogenase
资金
- National Key Research and Development Program of China [2020YFA0907300]
- National Natural Science Foundation of China [22077069]
- Natural Science Foundation of Tianjin [19JCZDJC33400]
- Fundamental Research Funds for the Central Universities, Nankai University [63201111]
This study demonstrates the efficient and stable conversion of CO2 into formate using a photocatalytic assembly. The key role of silver nanoclusters in enhancing durability and efficiency is highlighted.
(Photo)Electrochemical CO2 transformation to produce valuable chemicals or biofuels is one of the essential technologies for the carbon-neutral economy to store clean and renewable energy in chemical bonds. Herein, we show an efficient photocatalytic assembly formed by coupling formate dehydrogenase from Clostridium ljungdahliia (ClFDH), silver nanoclusters (AgNCs), TiO2, and graphitic carbon nitride (g-C3N4). The resulting integrated system is stable and can convert CO2 into formate with a turnover frequency of 1 s-1 and a turnover number of over 10,000 in 4 h. We highlight the key roles AgNCs have played to achieve such durability and high efficiency, which include (1) increasing the overall loading of biocatalysts and optimizing the orientation of enzyme molecules upon semiconductors by the Ag-cysteine interaction; (2) as the electron mediator, facilitating the interfacial electron transfer; and (3) scavenging the enzyme-deactivating reactive oxygen species. Our results provide a paradigm of selective CO2- capturing reaction under ambient conditions.
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