C-C bond formation and cleavage in radical enzymes, a theoretical perspective

被引:46
作者
Himo, F [1 ]
机构
[1] ALBANOVA, Royal Inst Technol, Dept Biotechnol, SE-10691 Stockholm, Sweden
来源
BIOCHIMICA ET BIOPHYSICA ACTA-BIOENERGETICS | 2005年 / 1707卷 / 01期
关键词
density functional theory; pyruvate-formate lyase; spore photoproduct lyase; benzylsuccinate synthase; radical enzyme;
D O I
10.1016/j.bbabio.2004.04.006
中图分类号
Q5 [生物化学]; Q7 [分子生物学];
学科分类号
071010 ; 081704 ;
摘要
Quantum chemical methods are today a viable tool ill the Study of enzyme catalysis. The development of new density functional techniques and the enormous advancement in computer power have made it possible to accurately describe active sites of enzymes. This review gives a brief account of the methods and models used in this field. Three specific enzymes are discussed: pyruvate-formate lyase (PFL), spore photoproduct lyase (SPL), and benzylsuccinate synthase (BSS). What these enzymes have in common is that they use radical chemistry to catalyze C-C bond formation or cleavage reactions. (c) 2004 Elsevier B.V. All rights reserved.
引用
收藏
页码:24 / 33
页数:10
相关论文
共 28 条
[1]  
BAUSCHLICHER CW, 1997, RECENT ADV DENSITY 2, P165
[2]   DENSITY-FUNCTIONAL THERMOCHEMISTRY .1. THE EFFECT OF THE EXCHANGE-ONLY GRADIENT CORRECTION [J].
BECKE, AD .
JOURNAL OF CHEMICAL PHYSICS, 1992, 96 (03) :2155-2160
[3]   DENSITY-FUNCTIONAL THERMOCHEMISTRY .2. THE EFFECT OF THE PERDEW-WANG GENERALIZED-GRADIENT CORRELATION CORRECTION [J].
BECKE, AD .
JOURNAL OF CHEMICAL PHYSICS, 1992, 97 (12) :9173-9177
[4]   DENSITY-FUNCTIONAL THERMOCHEMISTRY .3. THE ROLE OF EXACT EXCHANGE [J].
BECKE, AD .
JOURNAL OF CHEMICAL PHYSICS, 1993, 98 (07) :5648-5652
[5]   DENSITY-FUNCTIONAL EXCHANGE-ENERGY APPROXIMATION WITH CORRECT ASYMPTOTIC-BEHAVIOR [J].
BECKE, AD .
PHYSICAL REVIEW A, 1988, 38 (06) :3098-3100
[6]   X-ray structure of pyruvate formate-lyase in complex with pyruvate and CoA - How the enzyme uses the Cys-418 thiyl radical for pyruvate cleavage [J].
Becker, A ;
Kabsch, W .
JOURNAL OF BIOLOGICAL CHEMISTRY, 2002, 277 (42) :40036-40042
[7]  
Becker A, 1999, NAT STRUCT BIOL, V6, P969
[8]   A quantum chemical approach to the study of reaction mechanisms of redox-active metalloenzymes [J].
Blomberg, MRA ;
Siegbahn, PEM .
JOURNAL OF PHYSICAL CHEMISTRY B, 2001, 105 (39) :9375-9386
[9]   INACTIVATION OF ESCHERICHIA-COLI PYRUVATE FORMATE-LYASE BY HYPOPHOSPHITE - EVIDENCE FOR A RATE-LIMITING PHOSPHORUS HYDROGEN-BOND CLEAVAGE [J].
BRUSH, EJ ;
LIPSETT, KA ;
KOZARICH, JW .
BIOCHEMISTRY, 1988, 27 (06) :2217-2222
[10]   Direct H atom abstraction from spore photoproduct C-6 initiates DNA repair in the reaction catalyzed by spore photoproduct lyase: Evidence for a reversibly generated adenosyl radical intermediate [J].
Cheek, J ;
Broderick, JB .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2002, 124 (12) :2860-2861