A functionalised nickel cyclam catalyst for CO2 reduction: electrocatalysis, semiconductor surface immobilisation and light-driven electron transfer

被引:54
作者
Neri, Gaia [1 ]
Walsh, James J. [1 ]
Wilson, Calum [1 ]
Reynal, Anna [2 ]
Lim, Jason Y. C. [2 ]
Li, Xiaoe [2 ]
White, Andrew J. P. [2 ]
Long, Nicholas J. [2 ]
Durrant, James R. [2 ]
Cowan, Alexander J. [1 ]
机构
[1] Univ Liverpool, Stephenson Inst Renewable Energy, Dept Chem, Liverpool L69 7ZF, Merseyside, England
[2] Univ London Imperial Coll Sci Technol & Med, Dept Chem, London SW7 2AZ, England
基金
英国工程与自然科学研究理事会;
关键词
COMPLEX HYBRID PHOTOCATALYST; CARBON-DIOXIDE REDUCTION; METAL-COMPLEX; PHOTOELECTROCHEMICAL CELLS; PHOTOCHEMICAL REDUCTION; SELECTIVE REDUCTION; TIO2; ELECTRODES; WATER; PHOTOREDUCTION; CONVERSION;
D O I
10.1039/c4cp04871g
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 immobilisation of electrocatalysts for CO2 reduction onto light harvesting semiconductors is proposed to be an important step towards developing more efficient CO2 reduction photoelectrodes. Here, we report a low cost nickel cyclam complex covalently anchored to a metal oxide surface. Using transient spectroscopy we validate the role of surface immobilisation on enhancing the rate of photoelectron transfer. Furthermore [Ni(1,4,8,11-tetraazacyclotetradecane-6-carboxylic acid)](2+) (2) is shown to be a very active electrocatalyst in solution.
引用
收藏
页码:1562 / 1566
页数:5
相关论文
共 37 条
[1]   DOES A MACROCYCLIC EFFECT EXIST IN BLUE-TO-YELLOW CONVERSION OF NICKEL(II) COMPLEXES WITH TETRA-AZA LIGANDS [J].
ANICHINI, A ;
FABBRIZZI, L ;
PAOLETTI, P ;
CLAY, RM .
INORGANICA CHIMICA ACTA, 1977, 24 (02) :L21-L23
[2]   Solar CO2 reduction using H2O by a semiconductor/metal-complex hybrid photocatalyst: enhanced efficiency and demonstration of a wireless system using SrTiO3 photoanodes [J].
Arai, Takeo ;
Sato, Shunsuke ;
Kajino, Tsutomu ;
Morikawa, Takeshi .
ENERGY & ENVIRONMENTAL SCIENCE, 2013, 6 (04) :1274-1282
[3]   Photoelectrochemical reduction of CO2 in water under visible-light irradiation by a p-type InP photocathode modified with an electropolymerized ruthenium complex [J].
Arai, Takeo ;
Sato, Shunsuke ;
Uemura, Keiko ;
Morikawa, Takeshi ;
Kajino, Tsutomu ;
Motohiro, Tomoyoshi .
CHEMICAL COMMUNICATIONS, 2010, 46 (37) :6944-6946
[4]   Selective Visible-Light-Driven CO2 Reduction on a p-Type Dye-Sensitized NiO Photocathode [J].
Bachmeier, Andreas ;
Hall, Samuel ;
Ragsdale, Stephen W. ;
Armstrong, Fraser A. .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2014, 136 (39) :13518-13521
[5]   FLASH-PHOTOLYSIS OBSERVATION OF THE ABSORPTION-SPECTRA OF TRAPPED POSITIVE HOLES AND ELECTRONS IN COLLOIDAL TIO2 [J].
BAHNEMANN, D ;
HENGLEIN, A ;
LILIE, J ;
SPANHEL, L .
JOURNAL OF PHYSICAL CHEMISTRY, 1984, 88 (04) :709-711
[6]   NICKEL(II) CYCLAM - AN EXTREMELY SELECTIVE ELECTROCATALYST FOR REDUCTION OF CO2 IN WATER [J].
BELEY, M ;
COLLIN, JP ;
RUPPERT, R ;
SAUVAGE, JP .
JOURNAL OF THE CHEMICAL SOCIETY-CHEMICAL COMMUNICATIONS, 1984, (19) :1315-1316
[7]   ELECTROCATALYTIC REDUCTION OF CO2 BY NI CYCLAM2+ IN WATER - STUDY OF THE FACTORS AFFECTING THE EFFICIENCY AND THE SELECTIVITY OF THE PROCESS [J].
BELEY, M ;
COLLIN, JP ;
RUPPERT, R ;
SAUVAGE, JP .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1986, 108 (24) :7461-7467
[8]   COMPLEXES OF NICKEL(2) WITH A CYCLIC TETRADENTATE SECONDARY AMINE [J].
BOSNICH, B ;
TOBE, ML ;
WEBB, GA .
INORGANIC CHEMISTRY, 1965, 4 (08) :1109-&
[9]   P-TYPE SILICON BASED PHOTO-ELECTROCHEMICAL CELLS FOR OPTICAL-ENERGY CONVERSION - ELECTROCHEMISTRY OF TETRAAZOMACROCYCLIC METAL-COMPLEXES AT ILLUMINATED P-TYPE SILICON SEMICONDUCTING ELECTRODES [J].
BRADLEY, MG ;
TYSAK, T .
JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 1982, 135 (01) :153-157
[10]   Effects of ligand structure on the adsorption of nickel tetraazamacrocyclic complexes and electrocatalytic CO2 reduction [J].
Bujno, K ;
Bilewicz, R ;
Siegfried, L ;
Kaden, TA .
JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 1998, 445 (1-2) :47-53