期刊
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
卷 3, 期 10, 页码 1369-1373出版社
AMER CHEMICAL SOC
DOI: 10.1021/jz300419u
关键词
-
类别
资金
- U.S. Department of Energy at Lawrence Livermore National Laboratory [DE-AC52-07NA27344]
- Office of Science of the U.S. Department of Energy [DE-AC02-05CH11231]
Hydrolysis of carbon dioxide is an important reaction for CO2 collection. Using accurate first-principles electronic structure calculations, we predict how the catalytic hydrolysis reaction in carbonic anhydrase (CA) can be mimicked in a metal porphyrin carbon nanotube. The two-step catalytic process can be improved remarkably by controlling the porphyrin oxidation state via the nanotube charge state and by substituting the porphyrin metal atom. The oxidation state and the metal substitution both have profound effects on the reaction energetics for the initial hydration reaction step. For the subsequent product-release reaction step, two different reaction mechanisms could take place. These mechanisms are distinctively sensitive to either the oxidation state change or the metal substitution, but not to both. For the overall catalytic cycle, a significant dependence on the nanotube charge state at low pH and on the metal substitution at high pH is expected.
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