期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 130, 期 33, 页码 11106-11113出版社
AMER CHEMICAL SOC
DOI: 10.1021/ja8027668
关键词
-
资金
- Biotechnology and Biological Sciences Research Council [BB/D52222X, BB/D52222X/1] Funding Source: Medline
- Biotechnology and Biological Sciences Research Council [BB/D52222X/1] Funding Source: researchfish
- Engineering and Physical Sciences Research Council [EP/D047943/1] Funding Source: researchfish
- EPSRC [EP/D047943/1] Funding Source: UKRI
Studies have been carried out to establish the ability of O-2-tolerant membrane-bound [NiFe] hydrogenases (MBH) from Ralstonia sp. to catalyze H-2 production in addition to H-2 oxidation. These hydrogenases are not noted for H-2-evolution activity, and this is partly due to strong product inhibition. However, when adsorbed on a rotating disk graphite electrode the enzymes produce H-2 efficiently, provided the H-2 product is continuously removed by rapidly rotating the electrode and flowing N-2 through the gastight electrochemical cell. Electrocatalytic H-2 production proceeds with minimal overpotential - a significant observation because lowering the overpotential (the electrochemically responsive activation barrier) is seen as crucial in developing small-molecule catalysts for H-2 production. A mutant having a high Km for H-2 oxidation did not prove to be a better H-2 producer relative to the wild type, thus suggesting that weak binding of H-2 does not itself confer a tendency to be a H-2 producer. Inhibition by H-2 is much stronger than inhibition by CO and, most significantly, even O-2. Consequently, H-2 can be produced sustainably in the presence of O2 as long as the H-2 is removed continuously, thereby proving the feasibility for biological H-2 production in air.
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据