Optimizing the band structure of sponge-like S-doped poly(heptazine imide) with quantum confinement effect towards boosting visible-light photocatalytic H2 generation

Yang Gao; Yuxuan Li; Li Shangguan; Zhigang Mou; Hui Zhang; Dachuan Ge; Jianhua Sun; Feifei Xia; Weiwei Lei

doi:10.1016/j.jcis.2023.03.208

Optimizing the band structure of sponge-like S-doped poly(heptazine imide) with quantum confinement effect towards boosting visible-light photocatalytic H₂ generation

J Colloid Interface Sci. 2023 Aug 15:644:116-123. doi: 10.1016/j.jcis.2023.03.208. Epub 2023 Apr 12.

Authors

Yang Gao¹, Yuxuan Li¹, Li Shangguan¹, Zhigang Mou¹, Hui Zhang¹, Dachuan Ge¹, Jianhua Sun², Feifei Xia¹, Weiwei Lei³

Affiliations

¹ School of Chemistry and Chemical Engineering, Institute of Advanced Functional Materials for Energy, Jiangsu University of Technology, Changzhou 213001, Jiangsu Province, PR China.
² School of Chemistry and Chemical Engineering, Institute of Advanced Functional Materials for Energy, Jiangsu University of Technology, Changzhou 213001, Jiangsu Province, PR China. Electronic address: sunjh@jsut.edu.cn.
³ Institute for Frontier Materials, Deakin University, Waurn Ponds, Victoria 3216, Australia. Electronic address: weiwei.lei@deakin.edu.au.

PMID: 37105035
DOI: 10.1016/j.jcis.2023.03.208

Abstract

Simultaneously manipulating the nanostructure and band structure of semiconductors for boosting the photocatalytic performance of photocatalyts is highly desirable. Herein, a series of hierarchical sponge-like S-doped poly(heptazine imide) (HS-SPHI) assembled by ultrathin nanosheets were successfully fabricated via a facile bottom-up supramolecular preassembly approach using melamine (MA) and trithiocyanuric acid (TTCA) as precursors. Benefiting from the synergistic effect of the S-doping and their unique hierarchical porous structure coupled with quantum confinement effect, the as-obtained HS-SPHIs are endowed with extended visible-light response, improved charge separation efficiency, enlarged specific surface area, and enhanced thermodynamic driving force for water reduction. As a result, all the HS-SPHIs exhibit remarkable boosting visible-light (>420 nm) photocatalytic H₂evolution (PHE). The maximum PHE rate achieved by HS-SPHI-650 can be up to 3584.2 μmol g^-1h^-1, with an apparent quantum efficiency (AQE) of 14.67 % at 420 nm, which is about 22.4 times than that of pristine bulk g-C₃N₄ (B-GCN). We believe that this work will provide a significant strategy for optimizing the band structure of PCN in order to improve its photocatalytic performance.

Keywords: Band structure; Carbon nitride; Photocatalytic hydrogen generation; Quantum confinement effect; S-doped.