光催化
离域电子
石墨氮化碳
密度泛函理论
材料科学
可见光谱
氢
光化学
吸收(声学)
化学物理
电子结构
纳米技术
催化作用
化学
计算化学
光电子学
有机化学
复合材料
作者
Yingying Qin,Jian Lü,Xinyu Zhao,Xinyu Lin,Yue Hao,Pengwei Huo,Minjia Meng,Yongsheng Yan
标识
DOI:10.1016/j.cej.2021.131844
摘要
The precise molecular tunability strategy is deemed to have great potential to improve the photocatalytic performance of metal-free photocatalysts for applying in hydrogen evolution but remains a formidable task. We herein cover a logical design for integrating N defect engineering and π-conjugation structure into g-C3N4. The photocatalytic hydrogen evolution rate of up to 1541.6 μmol g−1 h−1 is acquired over the optimum DCN350, which has 7.5-fold increase over primal g-C3N4 (205.9 μmol g−1 h−1). The experimental study and density functional theory (DFT) investigations confirm that DCN350 with N defects not only can shorten band gaps for expanding the light absorption range via optimizing the electronic band structure, but also act as active sites for facilitating hydrogen evolution reaction. Besides, the –C≡N as strong electron-withdrawing functional group can make the isolated valence electrons delocalized to drive the charge spatial separation. Therefore, the light absorption capacity and charge separation/transfer of g‐C3N4 can be flexibly mastered via changing calcination temperature of g-C3N4 and NaBH4. Overall, this study provides an opportunity for having a deep understanding the role of structural defects on ameliorating the photocatalytic evolution hydrogen activity.
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