Citation: Linhui Li, Suitian Lai, Hongyan Lin, Xinyun Zhao, Xin Li, Xi Chen, Junjun Liu, Guangfu Yang, Changguo Zhan. QM/MM study on the O₂ activation reaction of 4-hydroxylphenyl pyruvate dioxygenase reveals a common mechanism for α-ketoglutarate dependent dioxygenase[J]. Chinese Chemical Letters, ;2023, 34(5): 107803. doi: 10.1016/j.cclet.2022.107803 shu

QM/MM study on the O₂ activation reaction of 4-hydroxylphenyl pyruvate dioxygenase reveals a common mechanism for α-ketoglutarate dependent dioxygenase

Linhui Li ^{a, 1} ,
Suitian Lai ^{c, 1} ,
Hongyan Lin ^{b, 1} ,
Xinyun Zhao ^a ,
Xin Li ^a ,
Xi Chen ^{a, *,} ,
Junjun Liu ^{c, *,} ,
Guangfu Yang ^{b, *,} ,
Changguo Zhan ^d

a.
College of Chemistry and Material Science, South-Central Minzu University, Wuhan 430074, China
b.
Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, College of Chemistry, Central China Normal University, Wuhan 430079, China
c.
School of Pharmacy, Tongji Medical College, Huazhong University of Science and Technology, Wuhan 430030, China
d.
Department of Pharmaceutical Sciences, College of Pharmacy, University of Kentucky, Lexington, KY 40536, United States

chen@mail.scuec.edu.cn

junjun.liu@hust.edu.cn

gfyang@mail.ccnu.edu.cn

Received Date: 16 June 2022
Revised Date: 2 September 2022
Accepted Date: 2 September 2022
Available Online: 6 September 2022

Figures(4)

The dioxygen activation catalyzed by 4-hydorxylphenyl pyruvate dioxygenase (HPPD) were reinvestigated by using hybrid quantum mechanics/molecular mechanics (QM/MM) approaches at the B3LYP/6-311++G(d, p): AMBER level. These studies showed that this reaction consisted of two steps including the dioxygen addition/decarboxylation and hetero OO bond cleavage, where the first step was found to be rate-determining. The former step initially runs on a septet potential energy surface (PES), then switches to a quintet PES after crossing a septet/quintet minimum energy crossing point (MECP) ^5-7M2, whereas the rest step runs on the quintet PES. The reliability of our theoretical predictions is supported by the excellent agreement of the calculated free-energy barrier value of 16.9 kcal/mol with available experimental value of 16–17 kcal/mol. The present study challenges the widely accepted view which holds that the O₂ activation catalyzed by α-keto glutamate (α-KG) dioxygenase mainly runs on the quintet PES and provides new insight into the catalytic mechanism of α-KG dioxygenase and/or other related Fe(Ⅱ)-dependent oxygenase.
- 4-Hydroxylphenyl pyruvate dioxygenase,
- O₂ activation,
- QM/MM,
- Mechanism,
- Minimum energy crossing point
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通讯作者: 陈斌, bchen63@163.com

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沈阳化工大学材料科学与工程学院沈阳 110142

QM/MM study on the O2 activation reaction of 4-hydroxylphenyl pyruvate dioxygenase reveals a common mechanism for α-ketoglutarate dependent dioxygenase

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通讯作者: 陈斌, bchen63@163.com

QM/MM study on the O₂ activation reaction of 4-hydroxylphenyl pyruvate dioxygenase reveals a common mechanism for α-ketoglutarate dependent dioxygenase