Theoretical Insights into the Limitation of Photocatalytic Overall Water Splitting Performance of VIA Group Elements Doped Polymeric Carbon Nitride: A DFT Calculation Predicting Solar-to-Hydrogen Efficiency
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ArticleDate
2021-03-10Online Publication Date
2021-03-10Print Publication Date
2021-06Embargo End Date
2022-02-26Submitted Date
2020-10-07Permanent link to this record
http://hdl.handle.net/10754/667690
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Polymeric carbon nitride (p-C3N4) is thermodynamically feasible for photocatalytic overall water splitting. Element doping has been proved effective in enhancing the photocatalytic performance of p-C3N4. The effect of doping is usually interpreted from the angle of electronic structures by first-principles density functional theory (DFT) calculations. However, the information on electronic structures is insufficient for understanding and predicting the ultimate criterion of solar-to-hydrogen (STH) efficiency. Herein, we provided a DFT calculation method to investigate and predict the STH of VIA group elements doped p-C3N4 by calculating the efficiencies of both light absorption and carrier utilization. Particularly, significant efforts were made to calculating the energy barriers for surface hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) to determine the carrier utilization efficiency. Moreover, the chemisorption energies of the reactant intermediates were calculated to quantify the intermediates affinity for HER and OER on the surface. Among the VIA elements, oxygen was discovered as the most effective dopant in promoting the STH because that oxygen-doped p-C3N4 has the lowest energy barriers for OER and the largest chemisorption energy for intermediates absorption. The calculation results highlight the importance of the surface reaction properties for efficient photocatalytic overall water splitting.Citation
Wang, Y., Zhao, D., Deng, H., Li, M., Chen, J., & Shen, S. (2021). Theoretical Insights into the Limitation of Photocatalytic Overall Water Splitting Performance of VIA Group Elements Doped Polymeric Carbon Nitride: A DFT Calculation Predicting Solar-to-Hydrogen Efficiency. Solar RRL. doi:10.1002/solr.202000630Publisher
WileyJournal
Solar RRLAdditional Links
https://onlinelibrary.wiley.com/doi/10.1002/solr.202000630ae974a485f413a2113503eed53cd6c53
10.1002/solr.202000630