Issue 10, 2021

Single-atom nickel terminating sp2 and sp3 nitride in polymeric carbon nitride for visible-light photocatalytic overall water splitting

Abstract

Polymeric carbon nitride (PCN) has been widely used as a metal-free photocatalyst for solar hydrogen generation from water. However, rapid charge carrier recombination and sluggish water catalysis kinetics have greatly limited its photocatalytic performance for overall water splitting. Herein, a single-atom Ni terminating agent was introduced to coordinate with the heptazine units of PCN to create new hybrid orbitals. Both theoretical calculation and experimental evidence revealed that the new hybrid orbitals synergistically broadened visible light absorption via a metal-to-ligand charge transfer (MLCT) process, and accelerated the separation and transfer of photoexcited electrons and holes. The obtained single-atom Ni terminated PCN (PCNNi), without an additional cocatalyst loading, realized efficient photocatalytic overall water splitting into easily-separated gas-product H2 and liquid-product H2O2 under visible light, with evolution rates reaching 26.6 and 24.0 μmol g−1 h−1, respectively. It was indicated that single-atom Ni and the neighboring C atom served as water oxidation and reduction active sites, respectively, for overall water splitting via a two-electron reaction pathway.

Graphical abstract: Single-atom nickel terminating sp2 and sp3 nitride in polymeric carbon nitride for visible-light photocatalytic overall water splitting

Supplementary files

Article information

Article type
Edge Article
Submitted
30 dec 2020
Accepted
17 jan 2021
First published
26 jan 2021
This article is Open Access

All publication charges for this article have been paid for by the Royal Society of Chemistry
Creative Commons BY-NC license

Chem. Sci., 2021,12, 3633-3643

Single-atom nickel terminating sp2 and sp3 nitride in polymeric carbon nitride for visible-light photocatalytic overall water splitting

Y. Li, Y. Wang, C. Dong, Y. Huang, J. Chen, Z. Zhang, F. Meng, Q. Zhang, Y. Huangfu, D. Zhao, L. Gu and S. Shen, Chem. Sci., 2021, 12, 3633 DOI: 10.1039/D0SC07093A

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