Substituted Ti(IV) in Ce-UiO-66-NH2 Metal–Organic Frameworks Increases H2 and O2 Evolution under Visible Light

IF 8.2 2区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

ACS Applied Materials & Interfaces Pub Date : 2023-01-07 DOI:10.1021/acsami.2c18389

Wenqing Hou, Chen Chen, Diya Xie and Yiming Xu*,

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引用次数: 6

Abstract

Metal–organic frameworks (MOFs) as photocatalysts have received increasing attention. In this work, a dual metal-substituted UiO-66-NH₂ (Ti/Ce-MOF) containing different Ti/Ce mole ratios (x = 0–2.46) has been prepared via post-synthetic exchange between Ce-UiO-66 and TiCl₄, followed by amination. The solid had a high surface area (828–937 m²/g) and a large pore volume (0.451–0.507 m³/g). Under visible light, Ti/Ce-MOF showed x-dependent activity for H₂O reduction and oxidation on a film electrode, respectively. However, such a change for H₂ evolution in a Na₂S/Na₂SO₃ aqueous solution was observed only after CdS loading. In combination with the photoluminescence and band parameters, we propose that the photoactivity of Ti/Ce-MOF for redox reaction is determined by its ability for electron transfer. Furthermore, there is an interfacial electron transfer from Ti/Ce-MOF to CdS and a hole transfer from CdS to Ti/Ce-MOF, respectively, significantly improving the efficiency of charge separation for redox reactions. This work offers a new insight that Ti substitution benefits the performance of Ce-based MOF.

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Ce-UiO-66-NH2金属有机骨架中取代Ti(IV)增加了可见光下H2和O2的析出

金属有机骨架(MOFs)作为光催化剂越来越受到人们的关注。本文通过合成后Ce- uio -66与TiCl4交换，胺化制备了不同Ti/Ce摩尔比(x = 0-2.46)的双金属取代UiO-66-NH2 (Ti/Ce- mof)。该固体具有较高的比表面积(828 ~ 937 m2/g)和较大的孔隙体积(0.451 ~ 0.507 m3/g)。在可见光下，Ti/Ce-MOF在膜电极上分别表现出x依赖性的H2O还原活性和氧化活性。然而，在Na2S/Na2SO3水溶液中，只有在cd加载后才会观察到这种H2演化的变化。结合光致发光和能带参数，我们提出Ti/Ce-MOF在氧化还原反应中的光活性是由其电子转移能力决定的。此外，界面电子从Ti/Ce-MOF转移到CdS，空穴从CdS转移到Ti/Ce-MOF，显著提高了氧化还原反应的电荷分离效率。这项工作提供了一个新的见解，即Ti取代有利于ce基MOF的性能。

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

ACS Applied Materials & Interfaces 工程技术-材料科学：综合

CiteScore

16.00

自引率

6.30%

发文量

4978

审稿时长

1.8 months

期刊介绍： ACS Applied Materials & Interfaces is a leading interdisciplinary journal that brings together chemists, engineers, physicists, and biologists to explore the development and utilization of newly-discovered materials and interfacial processes for specific applications. Our journal has experienced remarkable growth since its establishment in 2009, both in terms of the number of articles published and the impact of the research showcased. We are proud to foster a truly global community, with the majority of published articles originating from outside the United States, reflecting the rapid growth of applied research worldwide.