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Powering a CO2 Reduction Catalyst with Visible Light through Multiple Sub-picosecond Electron Transfers from a Quantum Dot
被引:156
作者:

Lian, Shichen
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Northwestern Univ, Dept Chem, 2145 Sheridan Rd, Evanston, IL 60208 USA Northwestern Univ, Dept Chem, 2145 Sheridan Rd, Evanston, IL 60208 USA

Kodaimati, Mohamad S.
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Northwestern Univ, Dept Chem, 2145 Sheridan Rd, Evanston, IL 60208 USA Northwestern Univ, Dept Chem, 2145 Sheridan Rd, Evanston, IL 60208 USA

Dolzhnikov, Dmitriy S.
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Northwestern Univ, Dept Chem, 2145 Sheridan Rd, Evanston, IL 60208 USA Northwestern Univ, Dept Chem, 2145 Sheridan Rd, Evanston, IL 60208 USA

Calzada, Raul
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h-index: 0
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Northwestern Univ, Dept Chem, 2145 Sheridan Rd, Evanston, IL 60208 USA Northwestern Univ, Dept Chem, 2145 Sheridan Rd, Evanston, IL 60208 USA

Weiss, Emily A.
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h-index: 0
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Northwestern Univ, Dept Chem, 2145 Sheridan Rd, Evanston, IL 60208 USA Northwestern Univ, Dept Chem, 2145 Sheridan Rd, Evanston, IL 60208 USA
机构:
[1] Northwestern Univ, Dept Chem, 2145 Sheridan Rd, Evanston, IL 60208 USA
基金:
美国国家科学基金会;
关键词:
SELECTIVE PHOTOCHEMICAL REDUCTION;
PHOTOCATALYTIC REDUCTION;
CARBON-DIOXIDE;
HIGHLY EFFICIENT;
PHOTOELECTROCHEMICAL REDUCTION;
TRANSFER DYNAMICS;
CHARGE-TRANSFER;
IRON;
MECHANISM;
MONOXIDE;
D O I:
10.1021/jacs.7b03134
中图分类号:
O6 [化学];
学科分类号:
0703 ;
摘要:
Photosensitization of molecular catalysts to reduce CO2 to CO is a sustainable route to storable solar fuels. Crucial to the sensitization process is highly efficient transfer of redox equivalents from sensitizer to catalyst; in systems with molecular sensitizers, this transfer is often slow because it is gated by diffusion-limited collisions between sensitizer and catalyst. This article describes the photosensitization of a meso-tetraphenylporphyrin iron(III) chloride (FeTPP) catalyst by colloidal, heavy metal-free CuInS2/ZnS quantum dots (QDs) to reduce CO2 to CO using 450 rim light. The sensitization efficiency (turnover number per absorbed unit of photon energy) of the QD system is a factor of 18 greater than that of an analogous system with a fac-tris(2-phenylpyridine)iridium sensitizer. This high efficiency originates in ultrafast electron transfer between the QD and FeTPP, enabled by formation of QD/FeTPP complexes. Optical spectroscopy reveals that the electron-transfer processes primarily responsible for the first two sensitization steps ((FeTPP)-T-III -> (FeTPP)-T-II, and (FeTPP)-T-II -> (FeTPP)-T-I) both occur in <200 fs.
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页码:8931 / 8938
页数:8
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