Homogeneous Catalysts with a Mechanical ("Machine-like") Action

被引:13
作者
Swiegers, Gerhard E. [1 ]
Huang, Junhua [2 ]
Brimblecombe, Robin [3 ]
Chen, Jun [1 ]
Dismukes, G. Charles [4 ,5 ]
Mueller-Westerhoff, Ulrich T. [6 ]
Spiccia, Leone [3 ]
Wallace, Gordon G. [1 ]
机构
[1] Univ Wollongong, ARC Ctr Excellence Electromat Sci, Intelligent Polymer Res Inst, Wollongong, NSW 2522, Australia
[2] CSIRO Energy Technol, Clayton, Vic 3169, Australia
[3] Monash Univ, Sch Chem, Clayton, Vic 3800, Australia
[4] Princeton Univ, Dept Chem, Princeton, NJ 08540 USA
[5] Princeton Univ, Princeton Environm Inst, Princeton, NJ 08540 USA
[6] Univ Connecticut, Dept Chem, Storrs, CT 06268 USA
关键词
biomimetic synthesis; collision frequency; homogeneous catalysis; mechanical reaction; nonequilibrium; ELECTROCATALYTIC 4-ELECTRON REDUCTION; WATER-OXIDIZING COMPLEX; ENZYME CATALYSIS; PROTEIN DYNAMICS; RATE ENHANCEMENT; ALDOL REACTIONS; GROUND-STATE; OXYGEN; ELECTROREDUCTION; PROTONATION;
D O I
10.1002/chem.200802396
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Chemical reactions may be controlled by either: 1)the minimum threshold energy that must be overcome during collisions between reactant molecules/atoms (the activation energy, E(a)) or: 2)the rate at which reactant collisions occur (the collision frequency, A)-for reactions with low E(a). Reactions of type 2 are governed by the physical, mechanical interaction of the reactants. Such mechanical processes are unusual, but not unknown in molecular catalysts. In this work we examine the machine-like nature of the action in various abiological mechanical catalysts and consider the implications for mimicry of biological catalysts.
引用
收藏
页码:4746 / 4759
页数:14
相关论文
共 77 条
[1]   Enzymes: An integrated view of structure, dynamics and function [J].
Agarwal, PK .
MICROBIAL CELL FACTORIES, 2006, 5 (1)
[2]   Role of protein dynamics in reaction rate enhancement by enzymes [J].
Agarwal, PK .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2005, 127 (43) :15248-15256
[3]   Correlated conformational fluctuations during enzymatic catalysis: Implications for catalytic rate enhancement [J].
Alper, KO ;
Singla, M ;
Stone, JL ;
Bagdassarian, CK .
PROTEIN SCIENCE, 2001, 10 (07) :1319-1330
[4]  
ATKINS PW, 1978, PHYS CHEM, P52
[5]  
ATKINS PW, 1978, PHYSICAL CHEM, P897
[6]  
BALANDIN AA, 1958, ADV CATAL, V10, P120
[7]   A perspective on enzyme catalysis [J].
Benkovic, SJ ;
Hammes-Schiffer, S .
SCIENCE, 2003, 301 (5637) :1196-1202
[8]   METALLOCENE BASICITY .3. PROTONATION OF COMPOUNDS CONTAINING TWO FERROCENYL MOIETIES [J].
BITTERWOLF, TE ;
LING, AC .
JOURNAL OF ORGANOMETALLIC CHEMISTRY, 1973, 57 (01) :C15-C18
[9]  
Bond A., UNPUB
[10]  
Bond G.C., 1987, Heterogeneous Catalysis, P62