Photocatalytic hydrogen evolution (PHE) is a promising way to generate hydrogen driven by solar light. Noble metallic Pt is usually used as a co–catalyst to catalyze this reaction. However, Pt can also act as an active center for H₂ and O₂ recombination reverse reaction, which results in the low photocatalytic efficiency for H₂ generation. Herein, the H₂ and O₂ recombination can remarkably be inhibited by incorporating amide–functionalized groups onto graphene surface and edge, which act as the oxygen adsorbent site and reduce migration of O₂ molecules in the dye–sensitized PHE system. Theoretical studies verify that the adsorption energy of oxygen change remarkable due to orbital hybridization by N 2p in amide group with O 2p in O₂ molecule, leading to redistribution the electron structure of graphene, and change of electrical properties of sensitized matrix. By amide–functionalized graphene (AF–RGO), we achieved high H₂ evolution activity over AF–RGO/Pt nanohybrid catalyst under visible light irradiation. The quantum efficiency of AF–RGO/Pt (AF–RGO prepared at 140 °C) achieved 36.4% at 430 nm. This superior photocatalytic performance can be attributed to the repression of H₂ and O₂ recombination and the synergy of electrical properties. This work is helpful to design high active catalyst for solar hydrogen generation.

光催化放氢（PHE）是一种有前途的产生由太阳光驱动的氢的方法。贵金属铂通常用作催化该反应的助催化剂。然而，Pt还可以充当H ₂和O ₂重组逆反应的活性中心，这导致H ₂生成的光催化效率低。在此，通过将酰胺官能化的基团掺入石墨烯的表面和边缘，可以显着抑制H ₂和O _2的重组，这些基团充当氧吸附位点并减少O _2的迁移染料敏化的PHE系统中的分子。理论研究证明，由于酰胺基团中的N 2p与O ₂分子中的O 2p发生轨道杂交，氧的吸附能发生显着变化，导致石墨烯的电子结构重新分布，敏化基质的电学性质发生变化。通过酰胺官能化的石墨烯（AF-RGO），在可见光照射下，我们在AF-RGO / Pt纳米杂化催化剂上实现了很高的H ₂析出活性。AF-RGO / Pt（在140°C下制备的AF-RGO）的量子效率在430 nm处达到36.4％。这种优异的光催化性能可以归因于H ₂和O ₂的抑制重组和电性能的协同作用。这项工作有助于设计用于太阳能制氢的高活性催化剂。