Intramolecular modulation of iron-based metal organic framework with energy level adjusting for efficient photocatalytic activity
Intramolecular modulation of iron-based metal organic framework with energy level adjusting for efficient photocatalytic activity
复制标题
铁基金属有机骨架的分子内调节与能级调节以实现高效的光催化活性
DOI：
10.1016/j.apcatb.2021.120823
复制
发表时间：
2021-11-04
影响因子：
22.1
通讯作者：
Wang, Xinxin
中科院分区：
文献类型：
--
作者：
Chen, Haoyun;Yuan, Xingzhong;Wang, Xinxin
高效的光催化活性一直是光催化技术去除有机水污染物的迫切要求。调制本征电子性质是提高光催化效率的最有效途径之一。本文通过硫调制铁基金属有机骨架（S-MIL-53(Fe)）的电子性质，开发了一种很有前途的光催化剂（S-MIL-53(Fe)），其中硫颗粒通过退火工艺插入MIL-53（Fe）的分子内嵌套。构建的S3-MIL-53（Fe）晶体具有规则的纺锤形多面体形态，表观量子效率（AQE）达到27.82%，是纯MIL-53（Fe）晶体（0.903%）的30倍以上，光活性显著增强。通过计算研究揭示了硫调制引起的电子结构变化和电荷转移。实验和计算分析表明，分子内用硫调制MIL-53（Fe）来设计能带结构以促进电荷转移是提高光催化效率的一种很有前途的方法。
Efficient photocatalytic activity is always pressingly expected for photocatalytic technology on removing organic water contaminations. Modulating the intrinsic electronic properties is one of the most effective approaches to improve photocatalytic efficiency. Herein, we developed a promising photocatalyst through modulation electronic properties of iron-based metal organic framework by sulfur (S-MIL-53(Fe)), in which the sulfur particles were intramolecularly in-suite inserted into MIL-53(Fe) through annealing treatment process. The constructed S3-MIL-53(Fe) crystal with regular spindle-shaped polyhedron morphology exhibited superior higher apparent quantum efficiency (AQE) of 27.82% which was over 30 times than that of pure MIL-53(Fe) (0.903%) indicating the significantly enhanced photoactivity. A computational study was conducted to reveal the electronic structure changes and the resulted charge transfer induced by the sulfur modulation. The experimental and computational analyses suggest that intramolecular modulation MIL-53(Fe) with sulfur to engineer band structure for promoting charge transfer is a promising approach to improve the photocatalytic efficiency.