Facile synthesis of porous hybrid materials based on Calix-3 dye and TiO2 for high photocatalytic water splitting performance with excellent stability
Facile synthesis of porous hybrid materials based on Calix-3 dye and TiO2 for high photocatalytic water splitting performance with excellent stability
复制标题
基于 Calix-3 染料和 TiO2 的多孔杂化材料的轻松合成，具有高光催化水分解性能和优异的稳定性
DOI：
10.1039/c8ta10633a
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发表时间：
2019-02-21
影响因子：
11.9
通讯作者：
Su, Cheng-Yong
中科院分区：
文献类型：
--
作者：
Huang, Jian-Feng;Liu, Jun-Min;Su, Cheng-Yong
首次采用溶胶-凝胶法合成了杯芳烃染料Calix-3与二氧化钛共价键合的杂化材料Calix-3-TiO 2。该材料不仅具有微孔/介孔结构和大的比表面积，而且具有两个明显的带隙：窄的1.7 eV带隙和宽的3.1 eV带隙，分别归属于Calix-3和Gel-TiO 2。当Pt纳米粒子作为助催化剂引入到杂化物上时，优化的Pt/Calix-3-TiO 2催化剂表现出较高的产氢活性（2444 mmol g（-1）h（-1），基于Pt质量），并且即使在循环10次后也表现出优异的稳定性（50小时后的营业额为24 920），该催化体系的催化活性上级于类似的敏化Pt/Gel-TiO 2/Calix-3体系，是已报道的在可见光下催化活性最高的多相催化体系之一。光效率和稳定性的提高可以归因于更稳定的Ti-O-Calix-3键和Calix-3与TiO 2之间更有效的电子转移。杂化材料中的微孔/介孔TiO 2保护染料，促进反应物/产物的转移，同时作为电子传输介质和储存器。本研究为新型多功能有机-无机杂化体系的设计和应用提供了启示。
A highly robust hybrid material consisting of calixarene dye Calix-3 linked covalently to titanium dioxide, denoted as Calix-3-TiO2, is synthesized by a facile sol-gel method for the first time. The material not only has a micro/mesoporous structure and a large surface area, but also owns two clear band gaps: a narrow 1.7 eV and a wide 3.1 eV band gap, which can be ascribed to Calix-3 and Gel-TiO2, respectively. When Pt nanoparticles as co-catalysts are introduced onto the hybrid, the optimized Pt/Calix-3-TiO2 catalyst exhibits high hydrogen production activity (2444 mmol g(-1) h(-1) based on Pt mass) and performs with excellent stability even after recycling 10 times (a turnover number of 24 920 after 50 h), which is superior to that of the analogous sensitized Pt/Gel-TiO2/Calix-3 system and represents one of the highest among those reported heterogeneous catalytic systems under visible-light. The enhancement in efficiency and stability could be attributed to the more stable Ti-O-Calix-3 linkage and more efficient electron transfer between Calix-3 and TiO2. The micro/mesoporous TiO2 in the hybrid protects the dye, facilitates reactant/product transfer, and works as an electron transporting mediator and a reservoir simultaneously. The current study offers an inspiration for the design and application of new multi-functional organic-inorganic hybrid systems in efficient photocatalysis.