Insights into the Enhanced Catalytic Activity of Cytochrome c When Encapsulated in a Metal-Organic Framework

被引：93

作者：

Chen, Yijing ^{[1
]}

Jimenez-Angeles, Felipe ^{[2
]}

Qiao, Baofu ^{[2
]}

Krzyaniak, Matthew D. ^{[1
,3
]}

Sha, Fanrui ^{[1
]}

Kato, Satoshi ^{[1
]}

Gong, Xinyi ^{[1
,4
]}

Buru, Cassandra T. ^{[1
]}

Chen, Zhijie ^{[1
]}

Zhang, Xuan ^{[1
]}

Gianneschi, Nathan C. ^{[5
,6
,7
]}

Wasielewski, Michael R. ^{[3
,8
]}

de la Cruz, Monica Olvera ^{[11
,12
]}

Farha, Omar K. ^{[9
,10
]}

机构：

[1] Northwestern Univ, Dept Chem, Evanston, IL 60208 USA

[2] Northwestern Univ, Dept Mat Sci & Engn, Evanston, IL 60208 USA

[3] Northwestern Univ, Inst Sustainabil & Energy Northwestern, Evanston, IL 60208 USA

[4] Northwestern Univ, Int Inst Nanotechnol IIN, Evanston, IL 60208 USA

[5] Northwestern Univ, Dept Chem, Dept Mat Sci & Engn, Int Inst Nanotechnol IIN, Evanston, IL 60208 USA

[6] Northwestern Univ, Simpson Querrey Inst, Evanston, IL 60208 USA

[7] Northwestern Univ, Dept Med, Evanston, IL 60208 USA

[8] Northwestern Univ, Dept Chem, Int Inst Nanotechnol IIN, Evanston, IL 60208 USA

[9] Northwestern Univ, Dept Chem, Int Inst Nanotechnol IIN, Inst Sustainabil & Energy Northwestern, Evanston, IL 60208 USA

[10] Northwestern Univ, Dept Chem & Biol Engn, Evanston, IL 60208 USA

[11] Northwestern Univ, Dept Chem, Dept Mat Sci & Engn, Dept Chem & Biol Engn, Evanston, IL 60208 USA

[12] Northwestern Univ, Dept Phys & Astron, Evanston, IL 60208 USA

来源：

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY | 2020年 / 142卷 / 43期

基金：

美国国家科学基金会;

关键词：

PARTICLE MESH EWALD; ENZYME ENCAPSULATION; IMMOBILIZATION; WATER; TRANSITION;

D O I：

10.1021/jacs.0c07870

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

The encapsulation of enzymes within porous materials has shown great promise, not only in protecting the enzymes from denaturation under nonbiological environments, but also, in some cases, in facilitating their enzymatic reaction rates at favorable reaction conditions. While a number of hypotheses have been developed to explain this phenomenon, the detailed structural changes of the enzymes upon encapsulation within the porous material, which are closely related to their activity, remain largely elusive. Herein, the structural change of cytochrome c (Cyt c) upon encapsulation within a hierarchical metal-organic framework, NU-1000, is investigated through a combination of experimental and computational methods, such as electron paramagnetic resonance, solid-state ultraviolet- visible spectroscopy, and all-atom explicit solvent molecular dynamics simulations. The enhanced catalytic performance of Cyt c after being encapsulated within NU-1000 is supported by the physical and in silico observations of a change around the heme ferric active center.

引用

页码：18576 / 18582

页数：7

共 58 条

[1] EPR SIGNALS FROM CYTOCHROME-C OXIDASE [J].