Mechanisms for Methane and Ammonia Oxidation by Particulate Methane Monooxygenase
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作者:
Siegbahn, Per E. M.
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Stockholm Univ, Dept Organ Chem, Arrhenius Lab, SE-10691 Stockholm, SwedenStockholm Univ, Dept Organ Chem, Arrhenius Lab, SE-10691 Stockholm, Sweden
Siegbahn, Per E. M.
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[1] Stockholm Univ, Dept Organ Chem, Arrhenius Lab, SE-10691 Stockholm, Sweden
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JOURNAL OF PHYSICAL CHEMISTRY B
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2024年
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128卷
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24期
Particulate MMO (pMMO) catalyzes the oxidation of methane to methanol and also ammonia to hydroxylamine. Experimental characterization of the active site has been very difficult partly because the enzyme is membrane-bound. However, recently, there has been major progress mainly through the use of cryogenic electron microscopy (cryoEM). Electron paramagnetic resonance (EPR) and X-ray spectroscopy have also been employed. Surprisingly, the active site has only one copper. There are two histidine ligands and one asparagine ligand, and the active site is surrounded by phenyl alanines but no charged amino acids in the close surrounding. The present study is the first quantum chemical study using a model of that active site (Cu-D). Low barrier mechanisms have been found, where an important part is that there are two initial proton-coupled electron transfer steps to a bound O-2 ligand before the substrate enters. Surprisingly, this leads to large radical character for the oxygens even though they are protonated. That result is very important for the ability to accept a proton from the substrates. Methods have been used which have been thoroughly tested for redox enzyme mechanisms.
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Southwest Petr Univ, Natl Key Lab Oil & Gas Reservoir Geol & Exploitat, Chengdu 610500, Peoples R China
Southwest Petr Univ, Sch New Energy & Mat, Chengdu 610500, Peoples R ChinaSouthwest Petr Univ, Natl Key Lab Oil & Gas Reservoir Geol & Exploitat, Chengdu 610500, Peoples R China
Han, Chunqiu
Cao, Yuehan
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Southwest Petr Univ, Natl Key Lab Oil & Gas Reservoir Geol & Exploitat, Chengdu 610500, Peoples R China
Southwest Petr Univ, Sch New Energy & Mat, Chengdu 610500, Peoples R ChinaSouthwest Petr Univ, Natl Key Lab Oil & Gas Reservoir Geol & Exploitat, Chengdu 610500, Peoples R China
Cao, Yuehan
Huang, Chuan
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Southwest Petr Univ, Sch New Energy & Mat, Chengdu 610500, Peoples R ChinaSouthwest Petr Univ, Natl Key Lab Oil & Gas Reservoir Geol & Exploitat, Chengdu 610500, Peoples R China
Huang, Chuan
Lv, Weifeng
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Southwest Petr Univ, Sch New Energy & Mat, Chengdu 610500, Peoples R ChinaSouthwest Petr Univ, Natl Key Lab Oil & Gas Reservoir Geol & Exploitat, Chengdu 610500, Peoples R China
Lv, Weifeng
Zhou, Ying
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Southwest Petr Univ, Natl Key Lab Oil & Gas Reservoir Geol & Exploitat, Chengdu 610500, Peoples R China
Southwest Petr Univ, Sch New Energy & Mat, Chengdu 610500, Peoples R ChinaSouthwest Petr Univ, Natl Key Lab Oil & Gas Reservoir Geol & Exploitat, Chengdu 610500, Peoples R China
机构:
Jeonbuk Natl Univ, Dept Chem, Jeonju 54896, South KoreaJeonbuk Natl Univ, Dept Chem, Jeonju 54896, South Korea
Lee, Chaemin
Hwang, Yunha
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Jeonbuk Natl Univ, Dept Chem, Jeonju 54896, South KoreaJeonbuk Natl Univ, Dept Chem, Jeonju 54896, South Korea
Hwang, Yunha
Kang, Hyun Goo
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Jeonbuk Natl Univ, Res Inst Clin Med, Dept Neurol, Jeonju 54907, South Korea
Jeonbuk Natl Univ Hosp, Biomed Res Inst, Jeonju 54907, South KoreaJeonbuk Natl Univ, Dept Chem, Jeonju 54896, South Korea