Ultrathin sulfur-doped holey carbon nitride nanosheets with superior photocatalytic hydrogen production from water
Ultrathin sulfur-doped holey carbon nitride nanosheets with superior photocatalytic hydrogen production from water
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DOI：
10.1016/j.apcatb.2020.119742
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发表时间：
2021-05-05
影响因子：
22.1
通讯作者：
Tang, Junwang
中科院分区：
文献类型：
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作者：
Luo, Lei;Gong, Zhuyu;Tang, Junwang
表面工程是增强光吸收、促进电荷分离和提高光吸收效率的有效途径。本文以硫代氰尿酸为单一前驱体，通过自模板法制备了硫掺杂的多孔g-C3 N4纳米片。通过巧妙控制前驱体的投料量，合成的掺硫多孔g-C3 N4纳米片具有优异的可见光催化产氢活性。优化后的催化剂在420 nm处的放氢速率为6225.4 umolg（-1）h（-1），表观量子产率为10%。综合表征和理论计算表明，增强的介电常数归因于硫掺杂和超薄二维拓扑结构导致的表面积增大、导带负移和带隙变窄的协同作用。这项工作突出了控制前体剂量和诱导硫掺杂到聚合物中的重要性，提供了一个有前途的和可靠的策略，同时调节g-C3 N4的纳米结构和电子结构，以实现高效的掺杂。
Surface engineering is an efficient way to enhance photoabsorption, promote charge separation and boost photocatalysis. Herein, sulfur-doped holey g-C3N4 nanosheets have been prepared through a universal self-templating approach with thiocyanuric acid as the single-precursor. By subtly controlling the feeding amount of precursor, the synthesized sulfur-doped holey g-C3N4 nanosheets exhibit excellent visible-light driven photocatalytic hydrogen production activity. The optimized catalyst presents a hydrogen evolution rate of 6225.4 umol g(-l) h(-1), with an apparent quantum yield of 10 % at 420 nm. Comprehensive characterizations and theoretical calculations suggest that the enhanced photocatalysis is attributed to the synergy of the enlarged surface area, the negatively-shifted conduction band, and the narrowed bandgap due to sulfur-doping and ultra-thin twodimensional topology. This work highlights the importance of controlling the precursor dosage and inducing sulfur doping into the polymer, providing a promising and reliable strategy to simultaneously regulate the nanostructural and electronic structure of g-C3N4 for highly efficient photocatalysis.