Interfacial coordination bonds accelerate charge separation for unprecedented hydrogen evolution over S-scheme heterojunction

IF 15.7 1区 化学 Q1 CHEMISTRY, APPLIED Chinese Journal of Catalysis Pub Date : 2024-10-01 DOI:10.1016/S1872-2067(24)60108-7
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Abstract

Inspired by natural photosynthesis, fabricating high-performance S-scheme heterojunction is regarded as a successful tactic to address energy and environmental issues. Herein, NH2-MIL-125(Ti)/Zn0.5Cd0.5S/NiS (NMT/ZCS/NiS) S-scheme heterojunction with interfacial coordination bonds is successfully synthesized through in-situ solvothermal strategy. Notably, the optimal NMT/ZCS/NiS S-scheme heterojunction exhibits comparable photocatalytic H2 evolution (PHE) rate of about 14876.7 μmol h−1 g−1 with apparent quantum yield of 24.2% at 420 nm, which is significantly higher than that of recently reported MOFs-based photocatalysts. The interfacial coordination bonds (Zn–N, Cd–N, and Ni–N bonds) accelerate the separation and transfer of photogenerated charges, and the NiS as cocatalyst can provide more catalytically active sites, which synergistically improve the photocatalytic performance. Moreover, theoretical calculation results display that the construction of NMT/ZCS/NiS S-scheme heterojunction also optimize the binding energy of active site-adsorbed hydrogen atoms to enable fast adsorption and desorption. Photoassisted Kelvin probe force microscopy, in-situ irradiation X-ray photoelectron spectroscopy, femtosecond transient absorption spectroscopy, and theoretical calculations provide sufficient evidence of the S-scheme charge migration mechanism. This work offers unique viewpoints for simultaneously accelerating the charge dynamics and optimizing the binding strength between the active sites and hydrogen adsorbates over S-scheme heterojunction.
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表面配位键加速电荷分离,使 S 型异质结实现前所未有的氢演化
受自然光合作用的启发,制造高性能 S 型异质结被认为是解决能源和环境问题的一种成功策略。本文通过原位溶热策略成功合成了具有界面配位键的 NH2-MIL-125(Ti)/Zn0.5Cd0.5S/NiS(NMT/ZCS/NiS)S 型异质结。值得注意的是,最佳的 NMT/ZCS/NiS S 型异质结在 420 纳米波长下的光催化 H2 进化(PHE)率约为 14876.7 μmol h-1 g-1,表观量子产率为 24.2%,明显高于最近报道的基于 MOFs 的光催化剂。界面配位键(Zn-N、Cd-N 和 Ni-N 键)加速了光生电荷的分离和转移,NiS 作为协同催化剂可以提供更多的催化活性位点,从而协同提高光催化性能。此外,理论计算结果表明,NMT/ZCS/NiS S 型异质结的构建还优化了活性位点吸附氢原子的结合能,从而实现了快速吸附和解吸。光助开尔文探针力显微镜、原位辐照 X 射线光电子能谱、飞秒瞬态吸收光谱和理论计算为 S-scheme电荷迁移机制提供了充分的证据。这项工作为同时加速电荷动力学和优化 S 型异质结上活性位点与氢吸附剂之间的结合强度提供了独特的视角。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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来源期刊
Chinese Journal of Catalysis
Chinese Journal of Catalysis 工程技术-工程:化工
CiteScore
25.80
自引率
10.30%
发文量
235
审稿时长
1.2 months
期刊介绍: The journal covers a broad scope, encompassing new trends in catalysis for applications in energy production, environmental protection, and the preparation of materials, petroleum chemicals, and fine chemicals. It explores the scientific foundation for preparing and activating catalysts of commercial interest, emphasizing representative models.The focus includes spectroscopic methods for structural characterization, especially in situ techniques, as well as new theoretical methods with practical impact in catalysis and catalytic reactions.The journal delves into the relationship between homogeneous and heterogeneous catalysis and includes theoretical studies on the structure and reactivity of catalysts.Additionally, contributions on photocatalysis, biocatalysis, surface science, and catalysis-related chemical kinetics are welcomed.
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