A hybrid MOFs/Ti-Fe2O3 Z-scheme photoanode with enhanced charge separation and transfer for efficient photoelectrochemical water oxidation

IF 6.5 1区化学 Q2 CHEMISTRY, PHYSICAL Journal of Catalysis Pub Date : 2024-05-27 DOI:10.1016/j.jcat.2024.115573

Kaikai Ba , Yunan Liu , Ping Wang , Yanhong Lin , Dejun Wang , Tengfeng Xie

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Abstract

The construction of Z-scheme charge transfer pathways simulating natural photosynthesis is considered a promising method for improving reaction driving forces. Here, we modified the surface of titanium doped Fe₂O₃ (Ti-Fe₂O₃) nanorods with NH₂-MIL-125(Ti) (Ti-MOFs) and a promising organic-inorganic hybrid Z-scheme NH₂-MIL-125(Ti)/Ti-Fe₂O₃ was successfully prepared. At 1.23 V vs. RHE, the photocurrent density of the composite photoanode reaches 2.67 mA/cm², which is 5 times higher than that of Ti-Fe₂O₃. The results of surface photovoltage, ESR and fs-TAS indicate that this improvement is mainly due to the effective Z-scheme charge transfer mechanism providing a strong driving force for charge separation and transport, greatly suppressing carrier recombination and allowing carriers with strong oxidation ability to participate in water oxidation. Meanwhile, NH₂-MIL-125(Ti) can enhance light absorption and reduce the surface defect state of Ti-Fe₂O₃. This study not only provides a feasible approach for the photoanode water splitting of traditional inorganic semiconductor/MOF based heterostructures, but also provides rich and effective means for revealing Z-scheme charge transfer mechanism in depth.

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具有增强电荷分离和转移功能的 MOFs/Ti-Fe2O3 Z 型混合光阳极，可用于高效光电化学水氧化

构建模拟自然光合作用的 Z 型电荷转移路径被认为是改善反应驱动力的一种可行方法。在这里，我们用 NH2-MIL-125(Ti)（Ti-MOFs）修饰了掺杂钛的 Fe2O3（Ti-Fe2O3）纳米棒的表面，成功制备了一种前景广阔的有机-无机杂化 Z 型 NH2-MIL-125(Ti)/Ti-Fe2O3 纳米棒。在 1.23 V vs. RHE 条件下，复合光阳极的光电流密度达到 2.67 mA/cm2，是 Ti-Fe2O3 的 5 倍。表面光电压、ESR和fs-TAS的研究结果表明，这种提高主要是由于有效的Z-梯度电荷转移机制为电荷分离和传输提供了强大的驱动力，极大地抑制了载流子的重组，使氧化能力强的载流子得以参与水的氧化。同时，NH2-MIL-125(Ti) 还能增强 Ti-Fe2O3 的光吸收并降低其表面缺陷态。该研究不仅为传统的无机半导体/MOF基异质结构的光阳极水分离提供了一种可行的方法，而且为深入揭示Z型电荷转移机制提供了丰富而有效的手段。

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来源期刊

Journal of Catalysis 工程技术-工程：化工

CiteScore

12.30

自引率

5.50%

发文量

447

审稿时长

31 days

期刊介绍： The Journal of Catalysis publishes scholarly articles on both heterogeneous and homogeneous catalysis, covering a wide range of chemical transformations. These include various types of catalysis, such as those mediated by photons, plasmons, and electrons. The focus of the studies is to understand the relationship between catalytic function and the underlying chemical properties of surfaces and metal complexes. The articles in the journal offer innovative concepts and explore the synthesis and kinetics of inorganic solids and homogeneous complexes. Furthermore, they discuss spectroscopic techniques for characterizing catalysts, investigate the interaction of probes and reacting species with catalysts, and employ theoretical methods. The research presented in the journal should have direct relevance to the field of catalytic processes, addressing either fundamental aspects or applications of catalysis.