Biphasic water splitting by osmocene

被引:40
作者
Ge, Peiyu [1 ]
Todorova, Tanya K. [2 ]
Patir, Imren Hatay [1 ]
Olaya, Astrid J. [1 ]
Vrubel, Heron [3 ]
Mendez, Manuel [1 ]
Hu, Xile [3 ]
Corminboeuf, Clemence [2 ]
Girault, Hubert H. [1 ]
机构
[1] Ecole Polytech Fed Lausanne, Lab Phys & Analyt Electrochem, CH-1015 Lausanne, Switzerland
[2] Ecole Polytech Fed Lausanne, Lab Computat Mol Design, CH-1015 Lausanne, Switzerland
[3] Ecole Polytech Fed Lausanne, Lab Inorgan Synth & Catalysis, CH-1015 Lausanne, Switzerland
基金
瑞士国家科学基金会; 欧洲研究理事会;
关键词
DENSITY-FUNCTIONAL THEORY; GAUSSIAN-BASIS SETS; ARTIFICIAL PHOTOSYNTHESIS; OXYGEN REDUCTION; OXIDATION; HYDROGEN; RUTHENOCENE; COMPLEXES; KINETICS;
D O I
10.1073/pnas.1203743109
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
The photochemical reactivity of osmocene in a biphasic water-organic solvent system has been investigated to probe its water splitting properties. The photoreduction of aqueous protons to hydrogen under anaerobic conditions induced by osmocene dissolved in 1,2-dichloroethane and the subsequent water splitting by the osmocenium metal-metal dimer formed during H-2 production were studied by electrochemical methods, UV-visible spectrometry, gas chromatography, and nuclear magnetic resonance spectroscopy. Density functional theory computations were used to validate the reaction pathways.
引用
收藏
页码:11558 / 11563
页数:6
相关论文
共 40 条
[1]   Systematically convergent basis sets for transition metals.: I.: All-electron correlation consistent basis sets for the 3d elements Sc-Zn -: art. no. 064107 [J].
Balabanov, NB ;
Peterson, KA .
JOURNAL OF CHEMICAL PHYSICS, 2005, 123 (06)
[2]   ARTIFICIAL PHOTOSYNTHESIS - SOLAR SPLITTING OF WATER TO HYDROGEN AND OXYGEN [J].
BARD, AJ ;
FOX, MA .
ACCOUNTS OF CHEMICAL RESEARCH, 1995, 28 (03) :141-145
[3]   Mediator-assisted water oxidation by the ruthenium "blue dimer" cis,cis-[(bpy)2(H2O)RuORu(OH2)(bpy)2]4+ [J].
Concepcion, Javier J. ;
Jurss, Jonah W. ;
Templeton, Joseph L. ;
Meyer, Thomas J. .
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2008, 105 (46) :17632-17635
[4]   Solar Energy Supply and Storage for the Legacy and Non legacy Worlds [J].
Cook, Timothy R. ;
Dogutan, Dilek K. ;
Reece, Steven Y. ;
Surendranath, Yogesh ;
Teets, Thomas S. ;
Nocera, Daniel G. .
CHEMICAL REVIEWS, 2010, 110 (11) :6474-6502
[5]  
Cramer, 2004, ESSENTIALS COMPUTATI
[6]   SELF-CONSISTENT PERTURBATION-THEORY OF DIAMAGNETISM .1. GAUGE-INVARIANT LCAO METHOD FOR NMR CHEMICAL-SHIFTS [J].
DITCHFIELD, R .
MOLECULAR PHYSICS, 1974, 27 (04) :789-807
[7]   HIGHER OXIDATION-STATE CHEMISTRY OF OSMOCENE - DIMERIC NATURE OF THE OSMOCENIUM ION [J].
DROEGE, MW ;
HARMAN, WD ;
TAUBE, H .
INORGANIC CHEMISTRY, 1987, 26 (08) :1309-1315
[9]   UBER AROMATENKOMPLEXE VON METALLEN .29. DI-CYCLOPENTADIENYL-OSMIUM [J].
FISCHER, EO ;
GRUBERT, H .
CHEMISCHE BERICHTE-RECUEIL, 1959, 92 (09) :2302-2309
[10]  
Frisch M. J., 2016, Gaussian 03 Revision B.03