Integration of polyoxometalate into defective UiO-66-NH2(Zr/Hf) for visible-light-driven hydrogen photogeneration

被引:0
|
作者
Dai, Jun [1 ]
Yan, Lulu [2 ]
Yang, Weimian [2 ]
Li, Ruisong [2 ]
Dong, Yan [3 ]
Shen, Yijun [2 ]
机构
[1] Hainan Univ, Sch Chem & Chem Engn, Haikou 570228, Hainan, Peoples R China
[2] Hainan Univ, Sch Marine Sci & Engn, State Key Lab Marine Resource Utilizat South Chin, Haikou 570228, Hainan, Peoples R China
[3] Hainan Univ, Sch Mat Sci & Engn, Haikou 570228, Hainan, Peoples R China
来源
APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY | 2025年 / 362卷
基金
海南省自然科学基金;
关键词
POM@MOF; Charge transfer; Defect engineering; Photocatalysts; Hydrogen evolution; METAL-ORGANIC FRAMEWORK; CATALYSTS; PHOTOCATALYST; EFFICIENT; POROSITY; HAFNIUM; UIO-66; WATER;
D O I
10.1016/j.apcatb.2024.124715
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
UiO-66 plays a crucial role in photocatalytic systems due to its superior stability and tunability. However, the charge transfer from organic ligands to metals is rarely involved in the photo-excitation of the pristine material. Herein, several Keggin-type Cs2.5H0.5PW12O40 (CsPW) were successfully incorporated into a bimetallic metal-organic framework (MOF) using a one-pot, one-step method, resulting in a series of defective CsPW@UNH(Hf-Zr) as optimized photocatalysts for visible-light-driven hydrogen evolution. Further investigations demonstrate that a Z heterojunction mechanism proceeds in the CsPW@UNH(0.65Hf) heterojunction to boost the charge separation via the chemical interaction between the CsPW and UNH(0.65Hf) components. The hydrogen evolution rate for 5 %CsPW@UNH(0.65Hf) is nearly two orders of magnitude greater than that of the bare UNH(Zr). The coexistence of Hf3+ and Zr3+ was observed in defective polyoxometalate-encapsulated MOF (POM@MOF) for the first time during photocatalysis, confirming the successful conjugated pi electrons transition from the amine-containing ligand to bimetallic cluster. This study offers a novel guideline for exploring efficient MOF-based photocatalysts through defect engineering.
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页数:10
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