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Ultrahigh Electrocatalytic Conversion of Methane at Room Temperature

机译:室温下甲烷的超高电催化转化率

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摘要

Due to the greenhouse effect, enormous efforts are done for carbon dioxide reduction. By contrast, more attention should be paid for the methane oxidation and conversion, which can help the effective utilization of methane without emission. However, methane conversion and utilization under ambient conditions remains a challenge. Here, this study designs a Co3O4/ZrO2 nanocomposite for the electrochemical oxidation of methane gas using a carbonate electrolyte at room temperature. Co3O4 activated the highly efficient oxidation of methane under mild electric energy with the help of carbonate as an oxidant, which is delivered by ZrO2. Based on the experimental results, acetaldehyde is the key intermediate product. Subsequent nucleophilic addition and free radical addition reactions accounted for the generation of 2‐propanol and 1‐propanol, respectively. Surprisingly, this work achieves a production efficiency of over 60% in the conversion of methane to produce these long‐term stable products. The as‐proposed regional electrochemical methane oxidation provides a new pathway for the synthesis of higher alcohols with high production efficiencies under ambient conditions.
机译:由于温室效应,为减少二氧化碳付出了巨大的努力。相比之下,应更多地关注甲烷的氧化和转化,这可以帮助有效地利用甲烷而不产生排放。但是,在环境条件下甲烷的转化和利用仍然是一个挑战。在这里,这项研究设计了一种Co3O4 / ZrO2纳米复合材料,用于在室温下使用碳酸盐电解质对甲烷气体进行电化学氧化。 Co3O4借助碳酸盐作为氧化剂,在温和的电能下激活了甲烷的高效氧化,而ZrO2则可将其作为氧化剂。根据实验结果,乙醛是关键的中间产物。随后的亲核加成反应和自由基加成反应分别占2-丙醇和1-丙醇的生成量。令人惊讶的是,这项工作将甲烷转化为这些长期稳定的产品的生产效率达到了60%以上。提议的区域电化学甲烷氧化为在环境条件下以高生产效率合成高级醇提供了一条新途径。

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