Loading silver nanoclusters onto g-C3N4 by formamide-assisted in-situ strategy to achieve efficient photocatalytic water splitting for hydrogen production

IF 4.7 3区 化学 Q2 CHEMISTRY, PHYSICAL Journal of Photochemistry and Photobiology A-chemistry Pub Date : 2025-05-01 Epub Date: 2025-01-15 DOI:10.1016/j.jphotochem.2025.116275
Zhenbang Xie , Chao Wang , Fuqi Wu , Ruiyuan Hu , Jie Zhang , Hongfei Du , Shouchao Zhang , Yongzhu Zhou
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Abstract

Modification of semiconductor-based photocatalysts with nanoclusters is regarded as a key advancement in photocatalytic hydrogen production. This study successfully prepared g-C3N4-based photocatalysts loaded with small-sized silver nanoclusters (Ag NCs/CN) using formamide as a solvent and reducing agent. Through systematic characterization and density functional theory (DFT) calculations, we demonstrate that silver nanoclusters serve as charge-transfer channels, enhancing the generation and separation of photogenerated carriers and optimizing the surface properties of g-C3N4 to greatly improve its photocatalytic activity. The photocatalytic hydrogen production rate of Ag NCs/CN reaches 1439.77 μmol·g−1·h−1 significantly surpassing that of g-C3N4. Moreover, Ag NCs/CN maintains high photocatalytic activity even after 30 h of continuous cycling. This work reveals the role of silver nanocluster modification in photogenerated electron separation and transport, providing new insights into the application of metal nanocluster composite catalysts.

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甲酰胺辅助原位策略在g-C3N4上负载银纳米团簇实现高效光催化水裂解制氢
用纳米团簇修饰半导体基光催化剂被认为是光催化制氢的关键进展。本研究成功制备了以甲酰胺为溶剂和还原剂负载小尺寸银纳米团簇(Ag NCs/CN)的g- c3n4基光催化剂。通过系统表征和密度泛函理论(DFT)计算,我们证明了银纳米团簇作为电荷转移通道,增强了光生载流子的生成和分离,优化了g-C3N4的表面性质,大大提高了其光催化活性。Ag NCs/CN的光催化产氢速率达到1439.77 μmol·g−1·h−1,显著优于g- c3n4。Ag NCs/CN在连续循环30 h后仍保持较高的光催化活性。这项工作揭示了银纳米团簇修饰在光生电子分离和输运中的作用,为金属纳米团簇复合催化剂的应用提供了新的见解。
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来源期刊
CiteScore
7.90
自引率
7.00%
发文量
580
审稿时长
48 days
期刊介绍: JPPA publishes the results of fundamental studies on all aspects of chemical phenomena induced by interactions between light and molecules/matter of all kinds. All systems capable of being described at the molecular or integrated multimolecular level are appropriate for the journal. This includes all molecular chemical species as well as biomolecular, supramolecular, polymer and other macromolecular systems, as well as solid state photochemistry. In addition, the journal publishes studies of semiconductor and other photoactive organic and inorganic materials, photocatalysis (organic, inorganic, supramolecular and superconductor). The scope includes condensed and gas phase photochemistry, as well as synchrotron radiation chemistry. A broad range of processes and techniques in photochemistry are covered such as light induced energy, electron and proton transfer; nonlinear photochemical behavior; mechanistic investigation of photochemical reactions and identification of the products of photochemical reactions; quantum yield determinations and measurements of rate constants for primary and secondary photochemical processes; steady-state and time-resolved emission, ultrafast spectroscopic methods, single molecule spectroscopy, time resolved X-ray diffraction, luminescence microscopy, and scattering spectroscopy applied to photochemistry. Papers in emerging and applied areas such as luminescent sensors, electroluminescence, solar energy conversion, atmospheric photochemistry, environmental remediation, and related photocatalytic chemistry are also welcome.
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