PMID- 33534993
OWN - NLM
STAT- MEDLINE
DCOM- 20210709
LR  - 20210709
IS  - 1549-960X (Electronic)
IS  - 1549-9596 (Linking)
VI  - 61
IP  - 2
DP  - 2021 Feb 22
TI  - Degradation of a Main Plastic Pollutant Polyethylene Terephthalate by Two 
      Distinct Proteases (Neprilysin and Cutinase-like Enzyme).
PG  - 764-776
LID - 10.1021/acs.jcim.0c00797 [doi]
AB  - In this DFT study, hydrolysis of polyethylene terephthalate (PET), a major cause 
      of plastic pollution, by two distinct enzymes, neprilysin (NEP, a mononuclear 
      metalloprotease) and cutinase-like enzyme (CLE, a serine protease), has been 
      investigated. These enzymes utilize different mechanisms for the degradation of 
      PET. NEP uses either the metal-bound hydroxide attack (MH) mechanism or reverse 
      protonation (RP) mechanism, while CLE utilizes a general acid/base mechanism that 
      includes acylation and deacylation processes. Additionally, the RP mechanism of 
      NEP can proceed through three pathways, RP0, RP1, and RP2. The DFT calculations 
      predict that, among all these mechanisms, the MH mechanism is the energetically 
      most favorable one for the NEP enzyme. In comparison, CLE catalyzes this reaction 
      with a significantly higher barrier. These results suggest that the Lewis acid 
      and nucleophile activations provided by the Zn metal center of NEP are more 
      effective than the hydrogen bonding interactions afforded by the catalytic 
      Ser85-His180-Asp165 triad of CLE. They have provided intrinsic details regarding 
      PET degradation and will pave the way for the design of efficient metal-based 
      catalysts for this critical reaction.
FAU - Hu, Qiaoyu
AU  - Hu Q
AD  - Department of Chemistry, University of Miami, Coral Gables, Florida 33146, United 
      States.
FAU - Jayasinghe-Arachchige, Vindi M
AU  - Jayasinghe-Arachchige VM
AD  - Department of Chemistry, University of Miami, Coral Gables, Florida 33146, United 
      States.
FAU - Prabhakar, Rajeev
AU  - Prabhakar R
AUID- ORCID: 0000-0003-1137-1272
AD  - Department of Chemistry, University of Miami, Coral Gables, Florida 33146, United 
      States.
LA  - eng
PT  - Journal Article
PT  - Research Support, U.S. Gov't, Non-P.H.S.
DEP - 20210203
PL  - United States
TA  - J Chem Inf Model
JT  - Journal of chemical information and modeling
JID - 101230060
RN  - 0 (Environmental Pollutants)
RN  - 0 (Plastics)
RN  - 0 (Polyethylene Terephthalates)
RN  - EC 3.1.1.- (Carboxylic Ester Hydrolases)
RN  - EC 3.1.1.- (cutinase)
RN  - EC 3.4.- (Peptide Hydrolases)
RN  - EC 3.4.24.11 (Neprilysin)
SB  - IM
MH  - Carboxylic Ester Hydrolases
MH  - *Environmental Pollutants
MH  - Neprilysin
MH  - Peptide Hydrolases
MH  - Plastics
MH  - *Polyethylene Terephthalates
EDAT- 2021/02/04 06:00
MHDA- 2021/07/10 06:00
CRDT- 2021/02/03 20:05
PHST- 2021/02/04 06:00 [pubmed]
PHST- 2021/07/10 06:00 [medline]
PHST- 2021/02/03 20:05 [entrez]
AID - 10.1021/acs.jcim.0c00797 [doi]
PST - ppublish
SO  - J Chem Inf Model. 2021 Feb 22;61(2):764-776. doi: 10.1021/acs.jcim.0c00797. Epub 
      2021 Feb 3.