One Model, Two Enzymes: Activation of Hydrogen and Carbon Monoxide.
One Model, Two Enzymes: Activation of Hydrogen and Carbon Monoxide.
复制标题
DOI：
10.1002/anie.201704864
复制
发表时间：
2017-08
影响因子：
--
通讯作者：
S. Ogo;Yuki Mori;T. Ando;Takahiro Matsumoto;Takeshi Yatabe;K. Yoon;H. Hayashi;M. Asano
中科院分区：
文献类型：
--
作者：
S. Ogo;Yuki Mori;T. Ando;Takahiro Matsumoto;Takeshi Yatabe;K. Yoon;H. Hayashi;M. Asano
在一个反应罐中催化H2和CO氧化的能力将是氢技术的主要布恩，因为CO是H2供应的一致污染物。在这里，我们报告了这样的催化剂，具有催化H2和CO中的一个或两个的氧化的能力，基于pH值。该催化剂基于NiIr核，其模拟酸性介质（pH 4-7）中的[NiFe]氢化酶和碱性介质（pH 7-10）中的一氧化碳脱氢酶的化学功能。我们已经将该催化剂应用于示范燃料电池中，使用H2、CO和H2 /CO（1/1）进料作为燃料用于在阳极处的氧化。燃料电池的功率密度取决于燃料电池的介质中的pH值，并且在烧瓶中显示出类似的pH依赖性。我们已经分离和表征了我们提出的催化循环中的所有中间体。
The ability to catalyze the oxidation of both H2 and CO in one reaction pot would be a major boon to hydrogen technology since CO is a consistent contaminant of H2 supplies. Here, we report just such a catalyst, with the ability to catalyze the oxidation of either or both H2 and CO, based on the pH value. This catalyst is based on a NiIr core that mimics the chemical function of [NiFe]hydrogenase in acidic media (pH 4-7) and carbon monoxide dehydrogenase in basic media (pH 7-10). We have applied this catalyst in a demonstration fuel cell using H2 , CO, and H2 /CO (1/1) feeds as fuels for oxidation at the anode. The power density of the fuel cell depends on the pH value in the media of the fuel cell and shows a similar pH dependence in a flask. We have isolated and characterized all intermediates in our proposed catalytic cycles.