Jun-Jun Sun,Wei Li,Fen-Fen Ma,Jian-Liang Cao,Hui-Jun Li,Yan Wang
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引用次数: 0
摘要
多金属氧酸盐衍生的光催化剂具有独特的类半导体性能和丰富的催化位点,在光催化领域具有广阔的应用前景。然而,多金属氧酸盐基光催化化合物载体的合成步骤繁琐、结构复杂,对其光催化性能提出了重大挑战。在这项研究中,我们报道了两种异结构多金属氧酸衍生的光催化剂[M(H2O)4(TeMo6O24)][M(Hpca)(H2O)5]2·6H2O [M = Co (1), Zn(2)],以异烟酸(pca)为有机配体,以anderson型多金属氧酸[TeMo6O24]6-为无机嵌段,原位合成,可以实现多相光催化制氢(3207.1 μmol g-1 h-1),远远优于大多数报道的多金属氧酸基多相体系。此外,化合物1作为光催化剂,表现出优异的光催化可回收性和稳定性。密度泛函理论计算表明,钴(II)配体的存在促进了析氢反应过程,而M(Hpca)(H2O)5的掺入进一步促进了反应。这项工作提出了一种通用的策略来设计先进的多金属氧酸盐基光催化剂,用于可持续的光催化制氢。
In Situ Assembly of Recyclable Polyoxometalate-Derived Photocatalysts for Sustainable Photocatalytic H2 Generation.
Polyoxometalate-derived photocatalysts with unique semiconductor-like performance and abundant catalytic sites are promising in photocatalysis. However, the cumbersome synthesis steps and complex structures of polyoxometalate-based compound carriers for photocatalysis pose significant challenges. In this study, we report two isostructural polyoxometalate-derived photocatalysts [M(H2O)4(TeMo6O24)][M(Hpca)(H2O)5]2 · 6H2O [M = Co (1), Zn (2)], in situ synthesized via iso-nicotinic acid (pca) as the organic ligand and Anderson-type polyoxometalate [TeMo6O24]6- as the inorganic block, which enable heterogeneous photocatalytic H2 production (3207.1 μmol g-1 h-1), far superior to most reported polyoxometalate-based heterogeneous systems. Moreover, compound 1, as a photocatalyst, displays excellent photocatalytic recyclability and stability. Density functional theory calculation reveals that the presence of the cobalt(II) ligand facilitates the H2 evolution reactions process, and the incorporation of M(Hpca)(H2O)5 further promotes the reaction. This work presents a versatile strategy for designing advanced polyoxometalate-based photocatalysts for sustainable photocatalytic H2 generation.
期刊介绍:
Inorganic Chemistry publishes fundamental studies in all phases of inorganic chemistry. Coverage includes experimental and theoretical reports on quantitative studies of structure and thermodynamics, kinetics, mechanisms of inorganic reactions, bioinorganic chemistry, and relevant aspects of organometallic chemistry, solid-state phenomena, and chemical bonding theory. Emphasis is placed on the synthesis, structure, thermodynamics, reactivity, spectroscopy, and bonding properties of significant new and known compounds.