Organic Linker Defines the Excited-State Decay of Photocatalytic MIL-125(Ti)-Type Materials

被引：102
|
作者：
Santaclara, Jara G. [1 ]
Nasalevich, Maxim A. [1 ]
Castellanos, Sonia [1 ]
Evers, Wiel H. [2 ,3 ]
Spoor, Frank C. M. [2 ]
Rock, Kamila [4 ]
Siebbeles, Laurens D. A. [2 ]
Kapteijn, Freek [1 ]
Grozema, Ferdinand [2 ]
Houtepen, Arjan [2 ]
Gascon, Jorge [1 ]
Hunger, Johannes [4 ]
van der Veen, Monique A. [1 ]
机构：
[1] Delft Univ Technol, Dept Chem Engn, Catalysis Engn, Julianalaan 136, NL-2628 BL Delft, Netherlands
[2] Delft Univ Technol, Dept Chem Engn, Optoelect Mat, Julianalaan 136, NL-2628 BL Delft, Netherlands
[3] Delft Univ Technol, Kavli Inst Nanosci, Lorentzweg 1, NL-2628 CJ Delft, Netherlands
[4] Max Planck Inst Polymer Res, Ackermannweg 10, D-55128 Mainz, Germany
来源：
CHEMSUSCHEM | 2016年 / 9卷 / 04期
关键词：
amines; metal-organic frameworks; photochemistry; titanium; water splitting; ELECTRON-TRANSFER; RADICAL CATIONS; AROMATIC-AMINES; WATER OXIDATION; PHOTOSYSTEM-II; TRIPLET-STATES; CO2; REDUCTION; FRAMEWORKS; ANILINE; TITANIUM(IV);
D O I：
10.1002/cssc.201501353
中图分类号：
O6 [化学];
学科分类号：
0703 ;
摘要：
Recently, MIL-125(Ti) and NH2-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), NH2-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 NH2-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 NH2-MIL-125(Ti), the electron donation of which extends the lifetime of the photoexcited state substantially.
引用
收藏
页码：388 / 395
页数：8
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