Stable and improved visible-light photocatalytic hydrogen evolution using copper(II)-organic frameworks: engineering the crystal structures
Stable and improved visible-light photocatalytic hydrogen evolution using copper(II)-organic frameworks: engineering the crystal structures
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使用铜(II)-有机框架稳定和改进可见光光催化析氢：设计晶体结构
DOI：
10.1039/c7ta00095b
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发表时间：
2017
影响因子：
11.9
通讯作者：
Zeng Heping
中科院分区：
文献类型：
--
作者：
Song Ting;Zhang Li;Zhang Piyong;Zeng Jian;Wang Tingting;Ali Atif;Zeng Heping
使用强制性助催化剂或光敏剂的金属-有机骨架（MOF）材料可以表现出相对高的光催化H2产生活性。然而，没有研究集中在使用相同的有机配体和金属离子时，MOF材料的晶体结构对光催化析氢活性的影响。因此，通过将4′-（2，4-二磺酸基苯基）-3，2 ′：6′，3 ′′-三联吡啶（H2 DSPTP）有机配体与CuSO 4·5 H2O连接，得到了（1）和（2）两种不同的MOF光催化剂晶体结构。这些产品，然后分别表征和用于光催化析氢。在没有任何光敏剂和助催化剂的情况下，化合物1和2表现出有效的可见光驱动的光催化H2生产，最大速率为5.77 μmol h-1和6.99 μmol h-1。有趣的是，化合物1和2在近红外光照射下也表现出光催化H2生成。化合物2显示出突出的长期稳定性，如通过超过24小时的八个循环测试所证明的。使用PL，时间分辨PL光谱和光电流测量验证了化合物的电荷分离和转移过程。
Relatively high photocatalytic H2 production activities can be exhibited by metal–organic framework (MOF) materials using a compulsory cocatalyst or photosensitizer. However, no study has focused on the effect of the crystal structures of MOF materials on the photocatalytic H2 evolution activity when using the same organic ligand and metal ion. Therefore, by connecting the 4′-(2,4-disulfophenyl)-3,2′:6′,3′′-terpyridine (H2DSPTP) organic ligand with CuSO4·5H2O, different MOF photocatalyst crystalline structures, (1) and (2), were obtained. These products were then respectively characterized and employed for photocatalytic H2 evolution. In the absence of any photosensitizer and cocatalyst, compounds 1 and 2 exhibited efficient visible-light-driven photocatalytic H2 production at maximum rates of 5.77 μmol h−1 and 6.99 μmol h−1. Interestingly, compounds 1 and 2 also exhibited photocatalytic H2 generation when irradiated with near-infrared light. Compound 2 showed outstanding long-term stability, as evidenced by eight-cycle tests over 24 h. The charge separation and transfer process of the compounds were verified using PL, time-resolved PL spectroscopy, and photocurrent measurements.