Sekine Yasushi, Manabe Ryo
Waseda University, 3-4-1, Okubo, Shinjuku, Tokyo, Japan 1698555.
Faraday Discuss. 2021 May 1;229:341-358. doi: 10.1039/c9fd00129h. Epub 2021 Feb 26.
The process of combining heterogeneous catalysts and direct current (DC) electric fields can achieve high catalytic activities, even under mild conditions (<500 K) with relatively low electrical energy consumption. Hydrogen production by steam reforming of methane, aromatics and alcohol, dehydrogenation of methylcyclohexane, dry reforming of methane, and ammonia synthesis are known to proceed at low temperatures in an electric field. In situ/operando analyses are conducted using IR, Raman, X-ray absorption fine structure, electrochemical impedance spectroscopy, and isotopic kinetic analyses to elucidate the reaction mechanism for these reactions at low temperatures. The results show that surface proton hopping by a DC electric field, called surface protonics, is important for these reactions at low temperatures because of the higher surface adsorbate concentrations at lower temperatures.
将多相催化剂与直流(DC)电场相结合的过程,即使在温和条件(<500 K)下且电能消耗相对较低的情况下,也能实现高催化活性。已知通过甲烷、芳烃和醇的蒸汽重整制氢、甲基环己烷的脱氢、甲烷的干重整以及氨合成在电场中可在低温下进行。使用红外光谱(IR)、拉曼光谱、X射线吸收精细结构、电化学阻抗谱和同位素动力学分析进行原位/操作分析,以阐明这些反应在低温下的反应机理。结果表明,直流电场引起的表面质子跳跃,即表面质子学,由于在较低温度下表面吸附物浓度较高,对于这些低温反应很重要。