Abstract
AbstractMethane (CH4) is the primary component of natural gas and a powerful greenhouse gas. CH4 can be utilized as an important raw material to produce value‐added chemicals via catalytic partial oxidation, oxidative/non‐oxidative coupling, steam reforming, dry reforming, etc. Redox potential is a key thermodynamic quantity in these processes while currently, only standard reduction potentials at 25°C and 1 atm are available. Herein, this is the first time to report the temperature (0–1000°C), pressure (1–100 atm), and adsorption‐dependent redox potentials of 13 CH4 oxidation reactions to generate methyl radical, methanol, methyl hydroperoxide, formaldehyde, formic acid, carbon monoxide, carbon dioxide, ethane, ethylene, ethanol, acetaldehyde, acetic acid, and benzene. It was found that redox potentials of all states (gaseous, aqueous, and adsorption states) decrease with temperature at an accelerated rate but show different responses to pressure change. Namely, while gas‐phase and aqueous‐phase redox potentials increase and decrease with pressure at a gradually declined rate, respectively, adsorption‐state redox potentials are insensitive to pressure. Most importantly, the significant differences up to 1.92 V under varied conditions reveal the necessity of applying operando redox potentials for CH4 oxidation reactions that are enabled by this report as an enriched database for broad applications.
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