PMID- 32361540
OWN - NLM
STAT- MEDLINE
DCOM- 20200716
LR  - 20200716
IS  - 1879-1298 (Electronic)
IS  - 0045-6535 (Linking)
VI  - 254
DP  - 2020 Sep
TI  - Fluoroacetate dehalogenase catalyzed dehalogenation of halogenated carboxylic 
      acids: A QM/MM approach.
PG  - 126803
LID - S0045-6535(20)30996-6 [pii]
LID - 10.1016/j.chemosphere.2020.126803 [doi]
AB  - Dehalogenation is one of the most important reactions in environmental pollution 
      control, for instance, the degradation of persistent organic pollutants (POPs). 
      Recently, fluoroacetate dehalogenase (FAcD) has been reported to catalyze the 
      dehalogenation reactions, which shows great potential in treating halogenated 
      pollutants. Here the dehalogenation mechanism catalyzed by FAcD was fully 
      deciphered with the aid of quantum mechanics/molecular mechanics method. The 
      results show that FAcD catalyzed dehalogenation efficiency follows the order of 
      defluorination > dechlorination > debromination. The corresponding 
      Boltzmann-weighted average barriers are 10.1, 19.7, and 20.9 kcal mol(-1). 
      Positive/negative correlations between activation barriers and structural 
      parameters (e.g. distance and angle) for FAcD catalyzed dechlorination and 
      debromination were established. Based on the structure-energy relationship, we 
      propose that mutation of the binding pocket amino acids (e.g. His155, Trp156, 
      Tyr219) to smaller proton donor amino acids (e.g. Serine, Threonine, Cysteine, 
      Asparagine) may increase the efficiency for dechlorination and debromination. The 
      results may of practical value for the efficient degradation of chlorined and 
      bromined pollutants by harnessing FAcD.
CI  - Copyright (c) 2020 Elsevier Ltd. All rights reserved.
FAU - Yue, Yue
AU  - Yue Y
AD  - Environment Research Institute, Shandong University, Jinan, 250100, PR China.
FAU - Chen, Jinfeng
AU  - Chen J
AD  - School of Life Sciences, Westlake University, Hangzhou, 310000, PR China.
FAU - Bao, Lei
AU  - Bao L
AD  - Environment Research Institute, Shandong University, Jinan, 250100, PR China.
FAU - Wang, Junjie
AU  - Wang J
AD  - Environment Research Institute, Shandong University, Jinan, 250100, PR China.
FAU - Li, Yanwei
AU  - Li Y
AD  - Environment Research Institute, Shandong University, Jinan, 250100, PR China. 
      Electronic address: lyw@sdu.edu.cn.
FAU - Zhang, Qingzhu
AU  - Zhang Q
AD  - Environment Research Institute, Shandong University, Jinan, 250100, PR China.
LA  - eng
PT  - Journal Article
DEP - 20200423
PL  - England
TA  - Chemosphere
JT  - Chemosphere
JID - 0320657
RN  - 0 (Amino Acids)
RN  - 0 (Carboxylic Acids)
RN  - 0 (Environmental Pollutants)
RN  - EC 3.- (Hydrolases)
RN  - EC 3.8.1.3 (haloacetate dehalogenase)
SB  - IM
MH  - Amino Acids/metabolism
MH  - Carboxylic Acids/*chemistry
MH  - Catalysis
MH  - Environmental Pollutants
MH  - Halogenation
MH  - Hydrolases/*chemistry
MH  - Molecular Dynamics Simulation
OTO - NOTNLM
OT  - Brominated carboxylic acids
OT  - Chlorinated carboxylic acids
OT  - Enzymatic dehalogenation
OT  - Quantum mechanics/molecular mechanics
COIS- Declaration of competing interest None.
EDAT- 2020/05/04 06:00
MHDA- 2020/07/17 06:00
CRDT- 2020/05/04 06:00
PHST- 2020/02/01 00:00 [received]
PHST- 2020/04/11 00:00 [revised]
PHST- 2020/04/12 00:00 [accepted]
PHST- 2020/05/04 06:00 [pubmed]
PHST- 2020/07/17 06:00 [medline]
PHST- 2020/05/04 06:00 [entrez]
AID - S0045-6535(20)30996-6 [pii]
AID - 10.1016/j.chemosphere.2020.126803 [doi]
PST - ppublish
SO  - Chemosphere. 2020 Sep;254:126803. doi: 10.1016/j.chemosphere.2020.126803. Epub 
      2020 Apr 23.