The development of novel nano‐single‐atom‐site catalysts with optimized electron configurations and active water adsorption (*H2O) to release hydrogen protons (*H) is paramount for photocatalytic hydrogen evolution (PHE), a multi‐step reaction process involving two electrons. In this study, an atom‐confinement and thermal reduction strategy is introduced to achieve synergistic Ag single‐atoms (Ag1) and nanoparticles (AgNPs) confined within carbon nitride nanotubes (Ag1+NPs‐CN) for enhanced photocatalytic hydrogen evolution. Mechanistic investigations reveal that H2O adsorption/dissociation predominantly occurs at Ag1 sites, while AgNPs sites notably facilitate H2 release, indicating the synergistic effect between Ag1 and AgNPs in the H2 evolution reaction. Furthermore, the effective confining of Ag species is beneficial for trapping electrons in highly active reaction regions, while the “electronic metal‐support interactions” (EMSIs) of AgNPs and Ag1‐C2N sites regulate the d‐band centers and effectively optimize the adsorption/desorption of intermediates in photocatalytic hydrogen evolution, leading to enhanced H2 production performance. This work demonstrates the potential of the construction of synergistic photocatalysts for efficient energy conversion and storage; Hydrogen production; Nanoparticles; Photocatalysis; Single atom; and Synergistic effect.

中文翻译：

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揭示限制在氮化碳纳米管内的 Ag 单原子和纳米粒子的多功能位点，用于协同光催化析氢


开发具有优化电子构型和活性水吸附 （*H2O） 的新型纳米单原子位点催化剂以释放氢质子 （*H） 对于光催化析氢 （PHE） 至关重要，PHE 是一种涉及两个电子的多步反应过程。在本研究中，引入了一种原子限制和热还原策略，以实现限制在氮化碳纳米管 （Ag1+NPs-CN） 内的协同 Ag 单原子 （Ag1） 和纳米颗粒 （AgNPs），以增强光催化析氢。机理研究表明，H2O 吸附/解离主要发生在 Ag1 位点，而 AgNPs 位点显着促进 H2 释放，表明 Ag1 和 AgNPs 在 H2 进化反应中的协同作用。此外，Ag 物种的有效限制有利于将电子捕获在高活性反应区域，而 AgNPs 和 Ag1‐C2N 位点的“电子金属-支持相互作用”（EMSI） 调节 d 波段中心，有效优化光催化析氢中中间体的吸附/解吸，从而提高 H2 生产性能。这项工作展示了构建协同光催化剂在高效能量转换和储存方面的潜力;氢气生产;纳米颗粒;光 催化;单原子;和 协同效应。