Construction of single-atom copper-loaded iron-based MOF/carbon nitride nanosheet heterojunction for enhanced N₂ photofixation under visible light

Abstract

The utilization of photocatalytic nitrogen fixation, a process celebrated for its environmental friendliness and sustainability, has emerged as a promising avenue for ammonia synthesis. The rational design of photocatalysts containing single atoms and heterojunctions has been a long-standing challenge for achieving efficient nitrogen fixation. This study innovatively constructs composite catalysts integrating single-atom copper within metal–organic frameworks (Fe-MOF, NH₂-MIL-101) and carbon nitride nanosheet (CNNS). The nitrogen fixation efficiency of the Cu@MIL-CNNS heterojunction was 8 and 12 times those of the original MOF and CNNSs, respectively. Through detailed characterization, we unveil a unique charge transfer pathway facilitated by the synergy between single-atom copper and heterojunctions, highlighting the critical function of copper centers as potent active sites. Our findings underscore the transformative potential of single atomic sites in amplifying charge transfer efficiency, propelling advancements in the photocatalyst design.

Graphical abstract

Keywords

single atom copper / photocatalytic nitrogen fixation / metal–organic framework / carbon nitride nanosheet

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Authors’ contributions

Xinshan Rong: conceptualization, supervision, and writing — review & editing; Yuqing He: data curation and original draft writing; Ping Gao: methodology and visualization; Ting Sun: data curation and visualization; Xiangtong Zhou: methodology; Zhiren Wu: methodology and visualization.

Declaration of competing interests

The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.

Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (Grant No. 22005125) and the Jiangsu Collaborative Innovation Center of Technology and Material of Water Treatment.

Data availability statement

The authors confirm that the data supporting the findings of this study are available within the article.

Online appendix

Electronic supplementary material (ESM) can be found in the online version at https://doi.org/10.1007/s11706-024-0702-z and https://journal.hep.com.cn/foms/EN/10.1007/s11706-024-0702-z that includes Table S1 and Figs. S1–S6.

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