Institute of Chemistry, Academia Sinica, Taipei, 115, Taiwan.
Department of Chemistry, National Chung Hsing University, Taichung, 402, Taiwan.
Sci Rep. 2017 Aug 21;7(1):8369. doi: 10.1038/s41598-017-08610-w.
An unprecedented method for the efficient conversion of C-C linear alkanes to their corresponding primary alcohols mediated by the membrane-bound alkane hydroxylase (AlkB) from Pseudomonas putida GPo1 is demonstrated. The X-ray absorption spectroscopy (XAS) studies support that electrons can be transferred from the reduced AlkG (rubredoxin-2, the redox partner of AlkB) to AlkB in a two-phase manner. Based on this observation, an approach for the electrocatalytic conversion from alkanes to alcohols mediated by AlkB using an AlkG immobilized screen-printed carbon electrode (SPCE) is developed. The framework distortion of AlkB-AlkG adduct on SPCE surface might create promiscuity toward gaseous substrates. Hence, small alkanes including propane and n-butane can be accommodated in the hydrophobic pocket of AlkB for C-H bond activation. The proof of concept herein advances the development of artificial C-H bond activation catalysts.
本文展示了一种前所未有的方法,通过假单胞菌 GPo1 中的膜结合烷烃羟化酶 (AlkB) 介导,将 C-C 线性烷烃高效转化为相应的伯醇。X 射线吸收光谱 (XAS) 研究表明,电子可以以两相方式从还原态的 AlkG(烷氧还原酶的氧化还原伴侣)转移到 AlkB。基于这一观察结果,本文开发了一种使用固定化在 AlkG 的丝网印刷碳电极 (SPCE) 介导的 AlkB 从烷烃到醇的电催化转化方法。AlkB-AlkG 加合物在 SPCE 表面的框架变形可能会导致对气态底物的混杂性。因此,包括丙烷和正丁烷在内的小分子烷烃可以容纳在 AlkB 的疏水性口袋中以进行 C-H 键活化。本文的概念验证推进了人工 C-H 键活化催化剂的发展。