Highly Efficient and Selective Photocatalytic CO2 Reduction to CO in Water by a Cobalt Porphyrin Molecular Catalyst

被引：192

作者：

Call, Arnau ^{[1
,2
]}

Cibian, Mihaela ^{[1
,2
]}

Yamamoto, Keiya ^{[1
,2
]}

Nakazono, Takashi ^{[1
,2
]}

Yamauchi, Kosei ^{[1
,2
]}

Sakai, Ken ^{[1
,2
,3
]}

机构：

[1] Kyushu Univ, Fac Sci, Dept Chem, Nishi Ku, Motooka 744, Fukuoka, Fukuoka 8190395, Japan

[2] Kyushu Univ, Int Inst Carbon Neutral Energy Res WPI I2CNER, Nishi Ku, Motooka 744, Fukuoka, Fukuoka 8190395, Japan

[3] Kyushu Univ, CMS, Nishi Ku, Motooka 744, Fukuoka, Fukuoka 8190395, Japan

来源：

ACS CATALYSIS | 2019年 / 9卷 / 06期

关键词：

CO2; reduction; cobalt porphyrin; photocatalysis; selectivity; molecular catalysis; BINUCLEAR RUTHENIUM(II) COMPLEX; VISIBLE-LIGHT; CARBON-DIOXIDE; PHOTOCHEMICAL REDUCTION; ELECTROCHEMICAL REDUCTION; HYDROGEN EVOLUTION; QUANTUM DOTS; IRON; CONVERSION; MECHANISM;

D O I：

10.1021/acscatal.8b04975

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

The performance of a water-soluble cobalt porphyrin ([{meso-tetra(4-sulfonatophenyl)porphyrinato}cobalt(III)], CoTPPS) as a catalyst for the photoreduction of CO2 in fully aqueous media has been investigated under visible light irradiation using [Ru(bpy)(3)](2+) as a photosensitizer and ascorbate as a sacrificial electron donor. CO is selectively produced (>82%) with high efficiency (926 TONCO; TONCO = turnover number for CO). Upon optimization, selectivities of at least 91% are achieved. Efficiencies up to 4000 TONCO and 2400 h(-1) TOFCO (TOFCO = turnover frequency for CO) are reached at low catalyst loadings, albeit with loss in selectivity. This work successfully demonstrates the ability of CoTPPS to perform highly efficient photoreduction of CO2 in water while retaining its high selectivity for CO formation.

引用

页码：4867 / 4874

页数：15

共 56 条

[1] Mechanism of a one-photon two-electron process in photocatalytic hydrogen evolution from ascorbic acid with a cobalt chlorin complex [J].