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首页> 外文期刊>Applied Catalysis, B. Environmental: An International Journal Devoted to Catalytic Science and Its Applications >Charge-regulated sequential adsorption of anionic catalysts and cationic photosensitizers into metal-organic frameworks enhances photocatalytic proton reduction
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Charge-regulated sequential adsorption of anionic catalysts and cationic photosensitizers into metal-organic frameworks enhances photocatalytic proton reduction

机译：将阴离子催化剂和阳离子光敏剂的充电顺序吸附到金属 - 有机骨架中增强了光催化质子

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摘要

We have developed a simple, general, and efficient method for constructing photocatalytic active metal-organic framework (MOF)-based composite materials for visible light-driven hydrogen production. Here, several transition metal-substituted Wells - Dawson-type polyoxometalates (POMs) were successfully immobilized into a Cr-MOF of the MIL-101 structure, resulting in a series of POM@MOF composite materials [POM = K8HP2W15V3O62 center dot 9H(2)O (P2W15V3), K8P2W17(NiOH2)O-61 center dot 17H(2)O (P2W17Ni),K8P2W17(CoOH2)O-61 center dot 16H(2)O ((P)2W(17)Co)]. We adjust the charge of MIL-101 framework by introducing Wells - Dawson-type POM anions with highly negative charge into the MOF. The MIL-101 framework absorbs the anionic POM, while the charge overcompensation in the POM@MOF composites allow them to efficiently adsorb cationic dyes. These composite materials accommodate and enrich cationic photosensitizer (PS) ruthenium(II) tris(bipyridyl) (Ru(bpy)(3)(2+)) from the solution, allowing the PSs to surround the POM proton reduction catalysts, resulting in a heterogeneous catalytic device POM@PSs@MOF with much higher photocatalytic activity than that of the corresponding homogeneous catalytic system. POM@MIL-101 could also be readily recycled and reused in catalytic reaction. Furthermore, this strategy was extended to sequential adsorption of anionic Mo2S122- and cationic PSs to lead to highly active photocatalytic proton reduction system with a H-2 evolution rate of up to 25578 mu mol h(-1) g(-1) (corresponding to Mo2S122- catalyst) in 8 h under visible light irradiation.
机译：我们开发了一种简单，一般，高效，可用于构建光催化活性金属 - 有机框架（MOF）的基于复合材料，用于可见光氢气产生。这里，将几种过渡金属取代的孔 - Dawson型多氧化钙（POMS）成功地固定到MIL-101结构的CR-MOF中，得到一系列POM @ MOF复合材料[POM = K8HP2W15V3O62中心点9H（2 ）O（P2W15V3），K8P2W17（NIOH2）O-61中心点17H（2）O（P2W17NI），K8P2W17（COOH2）O-61中心点16H（2）O（（P）2W（17）CO）]。我们通过引入井 - 道森型POM阴离子来调整MIL-101框架的电荷，该井型在MOF中具有高负电荷。 MIL-101框架吸收阴离子POM，而POM @ MOF复合材料中的电荷过度补偿允许它们有效吸附阳离子染料。这些复合材料可容纳并富含阳离子光敏剂（PS）钌（II）三（双吡啶基）（ru（BPY）（3）（3））（3）），允许PSS围绕POM质子还原催化剂，从而产生a非均相催化装置POM @ PSS @ MOF具有比相应均相催化系统更高的光催化活性。 POM @ MIL-101也可以在催化反应中容易地再循环并重复使用。此外，该策略扩展到阴离子MO2S122和阳离子PS的顺序吸附，导致高度活性的光催化质子还原系统，其H-2进化率高达25578μmolH（-1）G（-1）（对应）在可见光照射下8小时的MO2S122-催化剂。

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  • 作者

    Li He; Yao Shuang; Wu Hong-Li; Qu Jing-Yan; Zhang Zhi-Ming; Lu Tong-Bu; Lin Wenbin; Wang En-Bo;

  • 作者单位

    Northeast Normal Univ Dept Chem Minist Educ Key Lab Polyoxometalate Sci Changchun 130024 Jilin Peoples R China;

    Tianjin Univ Technol Tianjin Key Lab Organ Solar Cells &

    Photochem Con Inst New Energy Mat &

    Low Carbon Technol 391 Binshuixi Rd Tianjin 300384 Peoples R China;

    Northeast Normal Univ Dept Chem Minist Educ Key Lab Polyoxometalate Sci Changchun 130024 Jilin Peoples R China;

    Northeast Normal Univ Dept Chem Minist Educ Key Lab Polyoxometalate Sci Changchun 130024 Jilin Peoples R China;

    Northeast Normal Univ Dept Chem Minist Educ Key Lab Polyoxometalate Sci Changchun 130024 Jilin Peoples R China;

    Tianjin Univ Technol Tianjin Key Lab Organ Solar Cells &

    Photochem Con Inst New Energy Mat &

    Low Carbon Technol 391 Binshuixi Rd Tianjin 300384 Peoples R China;

    Univ Chicago Dept Chem 929 East 57th St Chicago IL 60637 USA;

    Northeast Normal Univ Dept Chem Minist Educ Key Lab Polyoxometalate Sci Changchun 130024 Jilin Peoples R China;

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  • 正文语种 eng
  • 中图分类 催化;
  • 关键词

    Polyoxometalate; Metal-organic framework; Composite materials; Hydrogen production;

    机译：聚毒素;金属有机框架;复合材料;氢气生产;

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