Redox cocatalysts play crucial roles in photosynthetic reactions, yet simultaneous loading of oxidative and reductive cocatalysts often leads to enhanced charge recombination that is detrimental to photosynthesis. This study introduces an approach to simultaneously load two redox cocatalysts, atomically dispersed cobalt for improving oxidation activity and anthraquinone for improving reduction selectivity, onto graphitic carbon nitride (C3N4) nanosheets for photocatalytic H2O2 production. Spatial separation of oxidative and reductive cocatalysts was achieved on a two-dimensional (2D) photocatalyst, by coordinating cobalt single atom above the void center of C3N4 and anchoring anthraquinone at the edges of C3N4 nanosheets. Such spatial separation, experimentally confirmed and computationally simulated, was found to be critical for enhancing surface charge separation and achieving efficient H2O2 production. This center/edge strategy for spatial separation of cocatalysts may be applied on other 2D photocatalysts that are increasingly studied in photosynthetic reactions.
|Original language||English (US)|
|Number of pages||7|
|Journal||Proceedings of the National Academy of Sciences of the United States of America|
|State||Published - Mar 11 2020|
Bibliographical noteKAUST Repository Item: Exported on 2022-06-14
Acknowledgements: This work was partially supported by National Science Foundation (NSF) Nanosystems Engineering Research Center for Nanotechnology-Enabled Water Treatment (Grant EEC-1449500). C.C. was financially supported by an Early Postdoctoral Mobility Fellowship, Swiss National Science Foundation (Award P2EZP2_168796) and D.H. was supported by the China Scholarship Council. We thank S. Zhuo and P. Wang at King Abdullah University of Science and Technology for STEM image analysis, J. Karosas at Yale University for ICP-MS analysis, and P. Kelleher at Yale University for help with XAFS sample preparation. We also thank D. Lu at Brookhaven National Laboratory (BNL) Center of Functional Materials for helpful discussions. This research used beamlines 8-BM and 8-ID (ISS) of the NSLS-II, US Department of Energy (DOE) Office of Science User Facilities operated for the DOE Office of Science by BNL under Contract DESC0012704. Computational work used the Extreme Science and Engineering Discovery Environment, supported by NSF (Grant ACI-1548562), through the Bridges high-performance computer at the Pittsburgh Supercomputing Center (Allocation ECD190001).
This publication acknowledges KAUST support, but has no KAUST affiliated authors.
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