Linker Engineering of Sandwich-Structured Metal-Organic Framework Composites for Optimized Photocatalytic H2 Production

被引:122
作者
Wang, Siyuan [1 ]
Ai, Zhiwen [1 ]
Niu, Xinwei [2 ]
Yang, Weijie [2 ]
Kang, Rong [1 ]
Lin, Zhongyuan [1 ]
Waseem, Amir [3 ]
Jiao, Long [1 ]
Jiang, Hai-Long [1 ]
机构
[1] Univ Sci & Technol China, Hefei Natl Res Ctr Phys Sci Microscale, Collaborat Innovat Ctr Chem Energy Mat iChEM, Dept Chem, Hefei 230026, Anhui, Peoples R China
[2] North China Elect Power Univ, Sch Energy & Power Engn, Baoding 071003, Hebei, Peoples R China
[3] Quaid I Azam Univ, Dept Chem, Islamabad 45320, Pakistan
基金
中国国家自然科学基金;
关键词
hydrogen production; linker engineering; metal-organic frameworks; photocatalysis;
D O I
10.1002/adma.202302512
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
While the microenvironment around catalytic sites is recognized to be crucial in thermocatalysis, its roles in photocatalysis remain subtle. In this work, a series of sandwich-structured metal-organic framework (MOF) composites, UiO-66-NH2@Pt@UiO-66-X (X means functional groups), is rationally constructed for visible-light photocatalytic H-2 production. By varying the X groups of the UiO-66-X shell, the microenvironment of the Pt sites and photosensitive UiO-66-NH2 core can be simultaneously modulated. Significantly, the MOF composites with identical light absorption and Pt loading present distinctly different photocatalytic H-2 production rates, following the X group sequence of H > Br > NA (naphthalene) > OCH3 > Cl > NO2. UiO-66-NH2@Pt@UiO-66-H demonstrates H-2 production rate up to 2708.2 & mu;mol g(-1) h(-1), & AP;222 times that of UiO-66-NH2@Pt@UiO-66-NO2. Mechanism investigations suggest that the variation of the X group can balance the charge separation of the UiO-66-NH2 core and the proton reduction ability of Pt, leading to an optimal activity of UiO-66-NH2@Pt@UiO-66-H at the equilibrium point.
引用
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页数:7
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