Guo Yan, Zhou Qixin, Nan Jun, Shi Wenxin, Cui Fuyi, Zhu Yongfa
School of Environment, Harbin Institute of Technology, 150090, Harbin, China.
Department of Chemistry, Tsinghua University, 100084, Beijing, China.
Nat Commun. 2022 Apr 19;13(1):2067. doi: 10.1038/s41467-022-29826-z.
Highly efficient hydrogen evolution reactions carried out via photocatalysis using solar light remain a formidable challenge. Herein, perylenetetracarboxylic acid nanosheets with a monolayer thickness of ~1.5 nm were synthesized and shown to be active hydrogen evolution photocatalysts with production rates of 118.9 mmol g h The carboxyl groups increased the intensity of the internal electric fields of perylenetetracarboxylic acid from the perylene center to the carboxyl border by 10.3 times to promote charge-carrier separation. The photogenerated electrons and holes migrated to the edge and plane, respectively, to weaken charge-carrier recombination. Moreover, the perylenetetracarboxylic acid reduction potential increases from -0.47 V to -1.13 V due to the decreased molecular conjugation and enhances the reduction ability. In addition, the carboxyl groups created hydrophilic sites. This work provides a strategy to engineer the molecular structures of future efficient photocatalysts.
利用太阳光通过光催化进行高效析氢反应仍然是一项艰巨的挑战。在此，合成了单层厚度约为1.5nm的苝四羧酸纳米片，并证明其为活性析氢光催化剂，产率为118.9mmol g h 羧基使苝四羧酸从苝中心到羧基边界的内部电场强度增加了10.3倍，以促进电荷载流子分离。光生电子和空穴分别迁移到边缘和平面，以减弱电荷载流子复合。此外，由于分子共轭减少，苝四羧酸还原电位从-0.47V增加到-1.13V，增强了还原能力。此外，羧基产生了亲水位点。这项工作为设计未来高效光催化剂的分子结构提供了一种策略。
