Porous Hybrid Materials Based on Mesotetrakis(Hydroxyphenyl) Porphyrins and TiO2for Efficient Visible-Light-Driven Hydrogen Production
Porous Hybrid Materials Based on Mesotetrakis(Hydroxyphenyl) Porphyrins and TiO2for Efficient Visible-Light-Driven Hydrogen Production
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DOI：
10.3390/catal10060656
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发表时间：
2020-06-01
期刊：
影响因子：
3.9
通讯作者：
Liu, Jun-Min
中科院分区：
文献类型：
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作者：
Huang, Li-Yuan;Huang, Jian-Feng;Liu, Jun-Min
首次采用溶胶-凝胶法制备了一系列基于meso-四（4-羟基苯基）卟啉（M = H，Pd，Zn）和二氧化钛（THPP-TiO 2，THPP-Pd-TiO 2和THPP-Zn-TiO 2）的高稳定性纳米-微米杂化材料。当Pt纳米粒子被引入到这些杂化物中时，Pt/THPP-Pd-TiO（2）实现了良好的产氢活性（2025.4 μ mol g（-1）h（-1）和12.03 μ mol m（-2）h（-1）），比Pt/THPP-Zn-TiO 2催化剂的催化活性高（1239.8 μ mol g（-1）h（-1）和7.46 μ mol m（-2）h（-1））和Pt/THPP-TiO_2（576.8 μ mol g（-1）h（-1）和4.02 μ mol m（-2）h（-1））。Pt/THPP-Pd-TiO（2）催化剂的最佳催化活性是由于Pd金属离子和Pt纳米粒子的双中心催化作用，而Pt/THPP-Zn-TiO（2）催化剂的活性高于Pt/THPP-TiO（2）催化剂，这可能是由于THPP-Zn和TiO（2）之间更有效的捕光和电子转移。此外，杂化Pt/THPP-Pd-TiO（2）催化剂循环使用10次后仍表现出稳定的产氢性能（50 h后的累积转化数为5111），远上级表面敏化的Pt/THPP-Pd/TiO（2）催化剂，这是由于杂化体系中卟啉中的四种酚与TiO（2）之间存在更稳定的Ti-O键。本研究提供了一个有前途的方法，构建稳定的有机-无机杂化系统具有独特的层次结构，有效的光吸收和电子转移。
A series of highly robust nano-micro hybrid materials based on meso-tetra(4-hydroxyphenyl) porphyrins (M = H, Pd, Zn) and titanium dioxide (denoted as THPP-TiO2, THPP-Pd-TiO2, and THPP-Zn-TiO2) have been prepared by a facile sol-gel method for the first time. When Pt nanoparticles are incorporated in these hybrids, Pt/THPP-Pd-TiO(2)achieves good H(2)production activity (2025.4 mu mol g(-1)h(-1)and 12.03 mu mol m(-2)h(-1)), higher than that of Pt/THPP-Zn-TiO2(1239.8 mu mol g(-1)h(-1)and 7.46 mu mol m(-2)h(-1)) and Pt/THPP-TiO2(576.8 mu mol g(-1)h(-1)and 4.02 mu mol m(-2)h(-1)), owing to the different central metal ions in porphyrins. The best activity of Pt/THPP-Pd-TiO(2)would be attributed to the two-center catalysis from coordination Pd metal ions and Pt nanoparticles, while the higher activity of Pt/THPP-Zn-TiO(2)than Pt/THPP-TiO(2)could be ascribed to the more effective light harvesting and electron transfer between THPP-Zn and TiO2. In addition, the hybridized Pt/THPP-Pd-TiO(2)catalyst exhibits unattenuated hydrogen production stability even after recycling the experiment 10 times (cumulative turnover number of 5111 after 50 h), far superior to that of the surface-sensitized Pt/THPP-Pd/TiO(2)catalyst with analogous components, due to the more stable Ti-O bonds between four phenols in porphyrins and TiO(2)for the hybrid system. The present study provides a promising approach for constructing stable organic-inorganic hybrid systems with unique hierarchical structures for efficient light absorption and electron transfer.