一例新型二钴取代锑钨酸盐:合成、表征及光催化水氧化性能

doi:10.1016/S1872-2067(19)63358-9

催化学报 ›› 2019, Vol. 40 ›› Issue (6): 953-958.DOI: 10.1016/S1872-2067(19)63358-9

一例新型二钴取代锑钨酸盐:合成、表征及光催化水氧化性能

韩庆^a, 孙頔^c, 赵俊伟^d, 梁向明^a, 丁勇^a,b

a 兰州大学化学化工学院, 甘肃省有色金属重点实验室, 功能有机分子国家重点实验室, 甘肃兰州 730000;
b 中国科学院兰州化学物理研究所羰基合成与选择氧化国家重点实验室, 甘肃兰州 730000;
c 山东大学化学化工学院, 胶体与界面化学教育部重点实验室, 山东济南 250100;
d 河南大学化学化工学院, 河南省多酸化学重点实验室, 分子与晶体研究所, 河南开封 475004

收稿日期:2019-01-23 修回日期:2019-03-25 出版日期:2019-06-18 发布日期:2019-04-26
通讯作者: 丁勇
基金资助:
国家自然科学基金（21773096）；中央高校基本科研业务费专项资金（lzujbky-2018-k08）；甘肃省自然科学基金（17JR5RA186）.

A novel dicobalt-substituted tungstoantimonate polyoxometalate:Synthesis, characterization, and photocatalytic water oxidation properties

Qing Han^a, Di Sun^c, Junwei Zhao^d, Xiangming Liang^a, Yong Ding^a,b

a State Key Laboratory of Applied Organic Chemistry, Key Laboratory of Nonferrous Metals Chemistry and Resources Utilization of Gansu Province, and College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou 730000, Gansu, China;
b State Key Laboratory for Oxo Synthesis and Selective Oxidation, Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences, Lanzhou 730000, Gansu, China;
c Key Laboratory of Colloid and Interface Chemistry, Ministry of Education, School of Chemistry and Chemical Engineering, Shandong University, Jinan 250100, Shandong, China;
d Henan Key Laboratory of Polyoxometalate Chemistry, Institute of Molecule and Crystal Engineering, College of Chemistry and Chemical Engineering, Henan University, Kaifeng 475004, Henan, China

Received:2019-01-23 Revised:2019-03-25 Online:2019-06-18 Published:2019-04-26
Contact: S1872-2067(19)63358-9
Supported by:
This research was financially supported by the National Natural Science Foundation of China (21773096), the Fundamental Research Funds for the Central Universities (lzujbky-2018-k08), and the Natural Science Foundation of Gansu Province (17JR5RA186).

摘要/Abstract

摘要：

太阳能分解水制氢作为解决当前能源危机和环境危机最理想和最有前途的策略之一正受到越来越多的关注.在人工模拟光合作用过程中，水的氧化（2H₂O→4H⁺+O₂+4e^-）是整个反应过程的瓶颈，因此开发高效稳定水氧化催化剂是提高人工光合作用性能的关键.在过去的几十年里，全世界科研工作者已经为设计合成高效稳定的均相和多相水氧化催化剂做了大量工作.在均相水氧化领域，多金属氧酸盐（简称多酸）作为一类结构多样的多金属氧簇化合物，由于其良好的氧化、热、水解稳定性，能够在不改变结构的前提下进行快速、可逆、多电子转移反应，因而受到广泛关注.2009年，Hill课题组首次将四钌多酸用于光驱动水氧化体系.随后，他们报道了不含贵金属的四钴多酸（Co₄（H₂O）₂（PW₉O₃₄）₂]^10-催化水氧化的工作.王恩波团队和我们课题组在该领域也进行了一些深入研究.
值得注意的是，由于Sb³⁺易于在水溶液中水解，这在很大程度上阻碍了锑钨酸盐前驱体与过渡金属离子结合形成多酸簇，所以导致有关过渡金属取代钨锑酸盐的报道非常少.本文采用一锅自组装策略，利用缺位多酸前驱体[B-α-SbW₉O₃₃]^9-与Co²⁺在弱酸性条件下反应，首次合成出一个结构新颖的夹心型锑钨酸盐Na₄[Co₂（H₂O）₆Sb₂（H₂O）₄（B-β-SbW₉O₃₃）₂]·39H₂O（1）.在可见光照射下，可有效催化水氧化反应，在最佳反应条件（Na₂S₂O₈为牺牲电子受体，[Ru（bpy）₃]Cl₂为光敏剂，缓冲溶液pH=8.5）下，反应的转化数和氧气收率最高分别可达193和30.8%，初始量子效率和初始转化频率分别为36.2%和5.3s^–1.紫外-可见吸收光谱、反应前后催化剂的红外光谱、毛细管电泳及甲苯萃取等实验结果表明，该锑钨酸盐1是一个稳定的光催化水氧化催化剂.

关键词: 光驱动水氧化, 锑钨酸盐, 自组装

Abstract:

The one-pot assembly reaction of a trilacunary, lone-pair-containing[B-α-SbW₉O₃₃]^9- precursor with Co²⁺ ions in an aqueous medium led to the isolation of a novel {SbO₃(H₂O)₃} bridging, dicobalt-substituted, sandwich-type tungstoantimonate {Co₂Sb₂(H₂O)₁₀[B-β-SbW₉O₃₃]₂}^4- (1a). This compound was structurally characterized in the solid state by single-crystal X-ray diffraction, elemental analyses, thermogravimetric analysis, and IR spectroscopy. The most remarkable feature was that 1a comprises two trilacunary[B-β-SbW₉O₃₃]^9- fragments trapping a novel, centrally symmetric, rhomb-like {Co₂Sb₂} belt with 10 terminal water molecules. When combined with the photosensitizer [Ru(bpy)₃]²⁺ and the sacrificial electron acceptor S₂O₈^2-, 1a exhibited efficient catalytic activity for water oxidation with a remarkable turnover number (TON) of 193, initial turnover frequency (TOF_initial) of 5.3 s^-1, O₂ yield of 30.8%, and quantum yield (Ф_QY) of 36.2% under light-driven conditions.

Key words: Light-driven water oxidation, Tungstoantimonate, Self-assembly

韩庆, 孙頔, 赵俊伟, 梁向明, 丁勇. 一例新型二钴取代锑钨酸盐:合成、表征及光催化水氧化性能[J]. 催化学报, 2019, 40(6): 953-958.

Qing Han, Di Sun, Junwei Zhao, Xiangming Liang, Yong Ding. A novel dicobalt-substituted tungstoantimonate polyoxometalate:Synthesis, characterization, and photocatalytic water oxidation properties[J]. Chinese Journal of Catalysis, 2019, 40(6): 953-958.

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一例新型二钴取代锑钨酸盐:合成、表征及光催化水氧化性能

A novel dicobalt-substituted tungstoantimonate polyoxometalate:Synthesis, characterization, and photocatalytic water oxidation properties

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