Tunable titanium metal-organic frameworks with infinite 1D Ti-O rods for efficient visible-light-driven photocatalytic H2 evolution
Tunable titanium metal-organic frameworks with infinite 1D Ti-O rods for efficient visible-light-driven photocatalytic H2 evolution
复制标题
具有无限一维 Ti-O 棒的可调谐钛金属有机框架，用于高效可见光驱动光催化析氢
DOI：
10.1039/c9ta01942a
复制
发表时间：
2019-05-21
影响因子：
11.9
通讯作者：
Chen, Banglin
中科院分区：
文献类型：
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作者：
Li, Changqing;Xu, Hui;Chen, Banglin
无限一维Ti-O棒基金属有机框架（MOFs）具有高光学响应和良好的光氧化还原性能和稳定性，是很有前途的水分解光催化剂，但尚未得到探索。在本研究中，成功地构建了三种等网格多孔一维棒状Ti-MOFs ZSTU-1，ZSTU-2和ZSTU-3，它们由无限的[Ti-6（（3）-O）（6）（（2）-OH）（6）]（n）二级结构单元（SBU）和三位羧酸酯连接基4，4，4-次氮基三苯甲酸（H（3）TCA），1，3，5-三（4-羧基苯基）苯（H3 BTB）和三（4-羧基联苯）胺（H（3）BTCA）。它们的孔隙率随着更大和更长的有机连接体而系统地增加。由三苯胺基配体构建的两种MOFs ZSTU-1和ZSTU-3可以吸收可见光，表现出比ZSTU-2更好的光催化性能，如ZSTU-1和ZSTU-3的H-2产生速率比ZSTU-2高3-4倍。ZSTU-1、ZSTU-2和ZSTU-3的光催化产氢速率分别为1060 mol g（-1）h（-1）、350 mol g（-1）h（-1）和1350 mol g（-1）h（-1）。ZSTU-3的优异光催化活性归因于其可见光吸收、大的比表面积和良好的电荷分离。
Infinite 1D Ti-O rod-based metal-organic frameworks (MOFs) are promising photocatalysts for water splitting due to their high optical response and favourable photo-redox properties and stability, but have not been explored yet. In this study, three isoreticular porous 1D rod-based Ti-MOFs ZSTU-1, ZSTU-2 and ZSTU-3 are successfully constructed from infinite [Ti-6((3)-O)(6)((2)-OH)(6)](n) secondary building units (SBUs) and tritopic carboxylate linkers 4,4,4-nitrilotribenzoic acid (H(3)TCA), 1,3,5-tris(4-carboxyphenyl)benzene (H3BTB) and tris(4-carboxybiphenyl)amine (H(3)BTCA), respectively. Their porosities systematically increase with the larger and longer organic linkers. The two MOFs ZSTU-1 and ZSTU-3 built from the triphenylamino-based ligands can absorb visible light, exhibiting much better photocatalytic performance than ZSTU-2 as shown by the H-2 production rate of ZSTU-1 and ZSTU-3 being 3-4 times higher than that of ZSTU-2. The photocatalytic H-2 production rates for ZSTU-1, ZSTU-2, and ZSTU-3 are 1060 mol g(-1) h(-1), 350 mol g(-1) h(-1) and 1350 mol g(-1) h(-1), respectively. The extraordinary photocatalytic activity of ZSTU-3 is attributed to its visible light absorption, large surface area, and favorable charge separation.