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论文类型： 期刊论文

发表时间： 2017-10-23

发表刊物： ANGEWANDTE CHEMIE-INTERNATIONAL EDITION

收录刊物： SCIE、EI、PubMed、Scopus

卷号： 56

期号： 44

页面范围： 13679-13683

ISSN号： 1433-7851

关键字： carbon dioxide; heterogeneous catalysis; methane; plasma chemistry; reforming

摘要： The conversion of CO2 with CH4 into liquid fuels and chemicals in a single-step catalytic process that bypasses the production of syngas remains a challenge. In this study, liquid fuels and chemicals (e.g., acetic acid, methanol, ethanol, and formaldehyde) were synthesized in a one-step process from CO2 and CH4 at room temperature (30 degrees C) and atmospheric pressure for the first time by using a novel plasma reactor with a water electrode. The total selectivity to oxygenates was approximately 50-60%, with acetic acid being the major component at 40.2% selectivity, the highest value reported for acetic acid thus far. Interestingly, the direct plasma synthesis of acetic acid from CH4 and CO2 is an ideal reaction with 100% atom economy, but it is almost impossible by thermal catalysis owing to the significant thermodynamic barrier. The combination of plasma and catalyst in this process shows great potential for manipulating the distribution of liquid chemical products in a given process.