光激发
光催化
激发态
光化学
材料科学
钛
吸收(声学)
光谱学
化学
原子物理学
物理
催化作用
有机化学
量子力学
复合材料
冶金
作者
Jara G. Santaclara,Maxim A. Nasalevich,Sonia Castellanos,Wiel H. Evers,Frank C. M. Spoor,Kamila Rock,Laurens D. A. Siebbeles,Freek Kapteijn,Ferdinand C. Grozema,Arjan J. Houtepen,Jorge Gascón,Johannes Hunger,Monique A. van der Veen
出处
期刊:Chemsuschem
[Wiley]
日期:2016-02-01
卷期号:9 (4): 388-395
被引量:84
标识
DOI:10.1002/cssc.201501353
摘要
Abstract Recently, MIL‐125(Ti) and NH 2 ‐MIL‐125(Ti), two titanium‐based metal–organic frameworks, have attracted significant research attention in the field of photocatalysis for solar fuel generation. This work reveals that the differences between these structures are not only based on their light absorption range but also on the decay profile and topography of their excited states. In contrast to MIL‐125(Ti), NH 2 ‐MIL‐125(Ti) shows markedly longer lifetimes of the charge‐separated state, which improves photoconversion by the suppression of competing decay mechanisms. We used spectroelectrochemistry and ultrafast spectroscopy to demonstrate that upon photoexcitation in NH 2 ‐MIL‐125(Ti) the electron is located in the Ti‐oxo clusters and the hole resides on the aminoterephthalate unit, specifically on the amino group. The results highlight the role of the amino group in NH 2 ‐MIL‐125(Ti), the electron donation of which extends the lifetime of the photoexcited state substantially.
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