Surface engineering of hollow carbon nitride microspheres for efficient photoredox catalysis
Date
2020
Authors
Wang, S.
Zhao, H.
Zhao, X.
Zhang, J.
Ao, Z.
Dong, P.
He, F.
Wu, H.
Xu, X.
Shi, L.
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Journal article
Citation
Chemical Engineering Journal, 2020; 381:122593-1-122593-10
Statement of Responsibility
Shuaijun Wang, Hongfei Zhao, Xiaoli Zhao, Jinqiang Zhang, Zhimin Ao, Pei Dong, Fengting He, Hong Wu, Xinyuan Xu, Lei Shi, Chaocheng Zhao, Shaobin Wang, Hongqi Sun
Conference Name
Abstract
Photocatalysis has attracted extensive interests because of the potential applications in remedying emerging contaminants and easing ever-increasing energy crisis. Towards practical applications of photocatalysis, exploring competing semiconductor materials is a critical challenge. Herein, hollow carbon nitride microspheres (HCNMS) were synthesized via a template-free hydrothermal approach, in which OH groups (OH-HCNMS) were used for further tuning the surface features. Their properties were thoroughly investigated by a number of advanced characterization methods. The as-prepared HCNMS achieved an impressive p-hydroxybenzoic acid (HBA) degradation rate of 0.013 min⁻¹, which was 4.3 times higher than pristine carbon nitride (C₃N₄), even higher than some heterostructured or noble metal modified C₃N₄. The enhanced photooxidation activity of HCNMS was achieved because of the optimized band structure and the deepened valence band edge, as unveiled by both experimental and density functional theory (DFT) calculation results. In addition, OH-HCNMS exhibited an apparent quantum efficiency (AQE) of 3.7% at 420 nm. The improved hydrogen efficiency of OH-HCNMS was ascribed to the surface functionalized OH groups, which react with holes, and release more electrons to participate the water splitting, as well as the modified orbital configuration which facilitates the faster charge carrier transfer.
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