Electroenzymatic Nitrogen Fixation Using a MoFe Protein System Immobilized in an Organic Redox Polymer

被引：30

作者：

Lee, Yoo Seok ^{[1
]}

Ruff, Adrian ^{[2
]}

Cai, Rong ^{[1
,3
]}

Lim, Koun ^{[1
]}

Schuhmann, Wolfgang ^{[2
]}

Minteer, Shelley D. ^{[1
]}

机构：

[1] Univ Utah, Dept Chem, 315 S 1400 E, Salt Lake City, UT 84112 USA

[2] Ruhr Univ Bochum, Fac Chem & Biochem, Analyt Chem Ctr Electrochem Sci CES, Univ Str 150, D-44780 Bochum, Germany

[3] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA

来源：

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION | 2020年 / 59卷 / 38期

基金：

欧洲研究理事会;

关键词：

ammonia; bioelectrosynthesis; neutral red; nitrogenase; redox polymers; ELECTRON-TRANSFER; BIOELECTROCHEMISTRY; BIOELECTROCATALYSIS; DEHYDROGENASE; REDUCTION; MECHANISM; SUPPORTS; DESIGN;

D O I：

10.1002/anie.202007198

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

We report an organic redox-polymer-based electroenzymatic nitrogen fixation system using a metal-free redox polymer, namely neutral-red-modified poly(glycidyl methacrylate-co-methylmethacrylate-co-poly(ethyleneglycol)methacrylate) with a low redox potential of -0.58 V vs. SCE. The stable and efficient electric wiring of nitrogenase within the redox polymer matrix enables mediated bioelectrocatalysis of N-3(-), NO(2)(-)and N(2)to NH(3)catalyzed by the MoFe protein via the polymer-bound redox moieties distributed in the polymer matrix in the absence of the Fe protein. Bulk bioelectrosynthetic experiments produced 209 +/- 30 nmol NH3 nmol MoFe-1 h(-1)from N(2)reduction.(15)N(2)labeling experiments and NMR analysis were performed to confirm biosynthetic N(2)reduction to NH3.

引用

页码：16511 / 16516

页数：6

共 37 条

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