Department of Electrical Engineering and Electronics, University of Liverpool, Liverpool, L69 3GJ, UK.
State Key Laboratory of Fine Chemicals, School of Chemical Engineering, Dalian University of Technology, Dalian, 116024, P. R. China.
Angew Chem Int Ed Engl. 2017 Oct 23;56(44):13679-13683. doi: 10.1002/anie.201707131. Epub 2017 Sep 19.
The conversion of CO with CH 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 CO and CH at room temperature (30 °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 CH and CO 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.
将 CO 和 CH 一步催化转化为液体燃料和化学品,而无需先合成合成气,这仍然是一个挑战。在这项研究中,首次使用带有水电极的新型等离子体反应器,在室温(30°C)和常压下,将 CO 和 CH 一步转化为液体燃料和化学品(如乙酸、甲醇、乙醇和甲醛)。含氧物的总选择性约为 50-60%,其中乙酸的选择性为 40.2%,是迄今为止报道的乙酸的最高值。有趣的是,CH 和 CO 通过直接等离子体合成乙酸是一个具有 100%原子经济性的理想反应,但由于热力学障碍很大,通过热催化几乎是不可能的。在这个过程中,等离子体和催化剂的结合显示出了在给定过程中控制液体化学品分布的巨大潜力。