Artificial hydrogenases

被引：80

作者：

Barton, Bryan E. ^{[1
]}

Olsen, Matthew T. ^{[1
]}

Rauchfuss, Thomas B. ^{[1
]}

机构：

[1] Univ Illinois, Sch Chem Sci, Urbana, IL 61801 USA

来源：

CURRENT OPINION IN BIOTECHNOLOGY | 2010年 / 21卷 / 03期

基金：

美国国家卫生研究院;

关键词：

ACTIVE-SITE MODELS; DE-NOVO DESIGN; H-2; PRODUCTION; STRUCTURAL-PROPERTIES; ELECTRONIC-PROPERTIES; MOLECULAR-HYDROGEN; IRON HYDROGENASE; COMPLEXES; CATALYSIS; DIHYDROGEN;

D O I：

10.1016/j.copbio.2010.03.003

中图分类号：

Q5 [生物化学];

学科分类号：

071010 ; 081704 ;

摘要：

Decades of biophysical study on the hydrogenase (H(2)ase) enzymes have yielded sufficient information to guide the synthesis of analogs of their active sites. Three families of enzymes serve as inspiration for this work: the [FeFe]-H(2)ases, [NiFe]-H(2)ases, and [Fe]-H(2)ases, all of which feature iron centers bound to both CO and thiolate. Artificial H(2)ases affect the oxidation of H-2 and the reverse reaction, the reduction of protons. These reactions occur via the intermediacy of metal hydrides. The inclusion of amine bases within the catalysts is an important design feature that is emulated in related bioinspired catalysts. Continuing challenges are the low reactivity of H-2 toward biomimetic H(2)ases.

引用

页码：292 / 297

页数：6

共 52 条

[1] [Anonymous], 2004, Basic Research Needs for the Hydrogen Economy: Report of the Basic Energy Sciences Workshop on Hydrogen Production, Storage, and Use, V2nd
[2] Some general principles for designing electrocatalysts with hydrogenase activity
Artero, V
Fontecave, M
[J]. COORDINATION CHEMISTRY REVIEWS, 2005, 249 (15-16) : 1518 - 1535
[3] Terminal hydride in [FeFe]-hydrogenase model has lower potential for H2 production than the isomeric bridging hydride
Barton, Bryan E.
Rauchfuss, Thomas B.
[J]. INORGANIC CHEMISTRY, 2008, 47 (07) : 2261 - 2263
[4] Nickel-Iron Dithiolato Hydrides Relevant to the [NiFe]-Hydrogenase Active Site
Barton, Bryan E.
Whaley, C. Matthew
Rauchfuss, Thomas B.
Gray, Danielle L.
[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2009, 131 (20) : 6942 - +
[5] Aza- and Oxadithiolates Are Probable Proton Relays in Functional Models for the [FeFe]-Hydrogenases
Barton, Bryan E.
Olsen, Matthew T.
Rauchfuss, Thomas B.
[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2008, 130 (50) : 16834 - +
[6] Hydrogen evolution by cobalt tetraimine catalysts adsorbed on electrode surfaces
Berben, Louise A.
Peters, Jonas C.
[J]. CHEMICAL COMMUNICATIONS, 2010, 46 (03) : 398 - 400
[7] Cammack R., 2001, Hydrogen as a Fuel Learning from Nature
[8] Modeling [Fe-Fe] hydrogenase: evidence for bridging carbonyl and distal iron coordination vacancy in an electrocatalytically competent proton reduction by an iron thiolate assembly that operates through Fe(0)-Fe(II) levels
Cheah, Mun Hon
Tard, Cedric
Borg, Stacey J.
Liu, Xiaoming
Ibrahim, Saad K.
Pickett, Christopher J.
Best, Stephen P.
[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2007, 129 (36) : 11085 - 11092
[9] COBALT-CATALYZED EVOLUTION OF MOLECULAR-HYDROGEN
CONNOLLY, P
ESPENSON, JH
[J]. INORGANIC CHEMISTRY, 1986, 25 (16) : 2684 - 2688
[10] The roles of the first and second coordination spheres in the design of molecular catalysts for H2 production and oxidation
DuBois, M. Rakowski
DuBois, Daniel L.
[J]. CHEMICAL SOCIETY REVIEWS, 2009, 38 (01) : 62 - 72

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