在流动电解槽中由含碳原料电合成乙二醇。
Electrosynthesis of ethylene glycol from C feedstocks in a flow electrolyzer.
作者信息
Xia Rong, Wang Ruoyu, Hasa Bjorn, Lee Ahryeon, Liu Yuanyue, Ma Xinbin, Jiao Feng
机构信息
Key Laboratory for Green Chemical Technology, School of Chemical Engineering and Technology, Tianjin University, Tianjin, 300072, China.
Center for Catalytic Science and Technology, Department of Chemical and Biomolecular Engineering, University of Delaware, Newark, DE, 19716, USA.
出版信息
Nat Commun. 2023 Jul 29;14(1):4570. doi: 10.1038/s41467-023-40296-9.
Ethylene glycol is a widely utilized commodity chemical, the production of which accounts for over 46 million tons of CO emission annually. Here we report a paired electrocatalytic approach for ethylene glycol production from methanol. Carbon catalysts are effective in reducing formaldehyde into ethylene glycol with a 92% Faradaic efficiency, whereas Pt catalysts at the anode enable formaldehyde production through methanol partial oxidation with a 75% Faradaic efficiency. With a membrane-electrode assembly configuration, we show the feasibility of ethylene glycol electrosynthesis from methanol in a single electrolyzer. The electrolyzer operates a full cell voltage of 3.2 V at a current density of 100 mA cm, with a 60% reduction in energy consumption. Further investigations, using operando flow electrolyzer mass spectroscopy, isotopic labeling, and density functional theory (DFT) calculations, indicate that the desorption of a *CHOH intermediate is the crucial step in determining the selectively towards ethylene glycol over methanol.
乙二醇是一种广泛使用的商品化学品，其生产每年排放超过4600万吨二氧化碳。在此，我们报告一种从甲醇生产乙二醇的成对电催化方法。碳催化剂可有效地将甲醛还原为乙二醇，法拉第效率为92%，而阳极的铂催化剂可通过甲醇部分氧化生产甲醛，法拉第效率为75%。采用膜电极组件配置，我们展示了在单个电解槽中由甲醇电合成乙二醇的可行性。该电解槽在电流密度为100 mA cm时的全电池电压为3.2 V，能耗降低了60%。进一步的研究，使用原位流动电解槽质谱、同位素标记和密度泛函理论（DFT）计算，表明*CHOH中间体的解吸是决定对乙二醇而非甲醇选择性的关键步骤。
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