Wang Shengyao, associate professor from the College of Science of HZAU, has made new progress in solar-driven reduction of CO2 into chemical fuels, with Prof. Ye Jinhua from National Institute for Materials Science in Japan. The findings were published in the Journal of the American Chemical Society under the title of “Facile Top-Down Strategy for Direct Metal Atomization and Coordination Achieving a High Turnover Number in CO2 Photoreduction”.
The solar-driven reduction of CO2 into chemical fuels is an approach to mitigate CO2 emission and supply alternative energy. However, the considerable barrier that exists in both thermodynamics and kinetics is a significant obstacle preventing the activation of CO2 from exceeding that of green plants. Therefore, developing robust active sites is crucial to activating and converting CO2 efficiently. As one of the recently emerging catalysts, the single-atom-modified carbon-based materials are very attractive because of their unusual electronic and level structures having characteristics with extraordinary catalytic properties, flexible selectivity and high stability. To date, four nitrogen coordinated metal sites (denoted as M-N4) are the most widely reported active sites catalyzing various reactions among diverse isolated species on N-rich carbon (NC). The M-N4 moiety presents a stable coordination structure for the isolated metals; however, it limits the regulation of electronic structure in metal sites to achieve better catalytic performance.
In this regard, they developed a facile top-down strategy for direct metal atomization and coordination. Gaseous acid produced in situ could downsize the large metal particles into corresponding ions, which subsequently anchored onto the surface defects of a nitrogen-rich carbon (NC) matrix. Additionally, the low-temperature treatment-induced C═O motifs within the interlayer of NC could bond with the discrete Fe sites in a perpendicular direction and finally create stabilized Fe–N4O species with high valence status (Fe3+) on the shallow surface of the NC matrix. Benefiting from the particular Fe–N4O species and its near-surface enrichment feature, the optimized Fe–NO/NC with single Fe–N4O species delivers an outstanding co-catalytic visible-light-driven CO2 reduction performance when it was integrated with homogeneous and heterogeneous photocatalysts, which achieves a superb Turnover Number TON of 1494 and 825 in 1 hour, respectively. This study may exert huge influence on the exploration and design of high-performance single-atom catalysts for efficient solar-energy-driven conversion.
The first author of this paper is Dr. Li Yunxiang from the Hokkaido University, with Wang and Ye as the co-corresponding authors. Wang made the findings during his stay in Japan as a visiting scholar sponsored by the International Young Scholar Program of HZAU.
It is reported Wang has carried out a series of innovative research on the spectral absorption expansion of the photocatalytic carbon dioxide reduction system, the regulation of carrier migration, and the design of catalytic active sites. The relevant results were published in the Nature Communications, Journal of the American Chemical Society and Applied Catalysis B: Environment, which attracted great attention at home and abroad.
Article: https://pubs.acs.org/doi/10.1021/jacs.0c09060
https://www.nature.com/articles/s41467-020-18350-7
https://www.nature.com/articles/s41467-020-14851-7
https://doi.org/10.1016/j.apcatb.2020.119096
Source: http://news.hzau.edu.cn/2020/1102/58645.shtml
Translated by: Li Ying & Liu Nianyi
Proofread by: Guo Haiyan
