Methane Oxidation to Methanol in Water
نویسندگان
چکیده
ConspectusMethane represents one of the most abundant carbon sources for fuel or chemical production. However, remote geographical locations and high transportation costs result in a substantial proportion being flared at source. The selective oxidation methane to methanol remains grand challenge catalytic chemistry due large energy barrier initial C–H activation prevention overoxidation CO2. Indirect methods such as steam reforming produce CO H2 building blocks, but they consume amounts over multistage processes. This makes development low-temperature highly desirable explains why it has remained an active area research last 50 years.The thermodynamically favorable would ideally use only molecular oxygen. Nature effects this transformation with enzyme monooxygenase (MMO) aqueous solution ambient temperature addition 2 equiv reducing cofactor. MMO sites are Fe Cu oxoclusters, incorporation these metals into zeolitic frameworks can biomimetic activity. Most approaches using metal-doped zeolites oxygen N2O; however, demonstrations cycles without catalyst regeneration limited. Over 10 years, we have developed Fe-Cu-ZSM-5 materials under conditions °C H2O2 oxidant (effectively O2 + equiv), which compete terms To date, among catalysts mild condition, industrially, is expensive production methanol.This observation activity led new utilize oxidant. Supported precious metal nanoparticles been shown be range reactions H2O2, rapid decomposition surfaces limits efficiency. We identified that could minimized by removing support material carrying out reaction colloidal AuPd nanoparticles. efficiency consumption was increased 4 orders magnitude, crucially demonstrated first time incorporated produced 91% selectivity. understanding gained from two provides valuable insight possible routes will presented here context our own area.
منابع مشابه
Methane oxidation by aqueous osmium tetroxide and sodium periodate: inhibition of methanol oxidation by methane.
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ژورنال
عنوان ژورنال: Accounts of Chemical Research
سال: 2021
ISSN: ['1520-4898', '0001-4842']
DOI: https://doi.org/10.1021/acs.accounts.1c00129