Endowing polymeric carbon nitride photocatalyst with CO2 activation sites by anchoring atomic cobalt cluster

Yaru Shang, Yijie Hou, Xun Cao, Hengjie Liu, Xiaoli Jin, Jiawei Liu, Chunshuang Yan, Yumin Qian*, Li Song, Zeming Qi, Pin Song, Yansong Zhou, Daobin Liu, Zheng Liu, Fengyang Jing, Qingyu Yan, Gang Chen, Chade Lv

*此作品的通讯作者

科研成果: 期刊稿件文章同行评审

7 引用 (Scopus)

摘要

Photocatalytic CO2 reduction to high value-added fuels and chemicals is a promising strategy for alleviating both energy and environmental crises. However, the poor CO2 adsorption and activation ability seriously restrict the CO2 photoreduction activity of metal-free carbon nitride (C3N4), which is an emerging material for photocatalysis applications. In this paper, cobalt (Co) atomic clusters were modified on the surface of hierarchical urchin-like hollow C3N4 nanotubes by NaBH4 reduction, which endowed the as-designed Co atomic cluster-anchored and B-doped C3N4 (Co@B-HCN) catalyst with strong CO2 activation and CO2 photoreduction ability. Theoretical calculations and in situ characterization confirmed that the Co atomic clusters anchoring enabled the change in the bond length/angle of adsorbed CO2 molecules, as well as the change from a linear model to a bending model. This could enhance the CO2 adsorption and activation, which played a vital role in reducing the energy barrier of CO2-to-CO reaction. In addition, the construction of the hierarchical urchin-like nanostructure, the anchoring of Co atomic clusters, and the doping of B favored the surface adsorption and charge separation. Attributed to the above merits, the CO yield of Co@B-HCN photocatalyst reaches 157.51 μmol⋅g−1⋅h−1, which is approximately 22 times that of bulk C3N4. This work provides an insight for the surface engineering of C3N4 photocatalysts to realize high-performance photocatalytic CO2 reduction.

源语言英语
文章编号150306
期刊Chemical Engineering Journal
486
DOI
出版状态已出版 - 15 4月 2024

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