Lu Jinhai, Zhu Changli, Pan Changchang, Lin Wenlie, Lemmon John P, Chen Fanglin, Li Chunsen, Xie Kui
Key Laboratory of Design and Assembly of Functional Nanostructures, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian 350002, China.
State Key Laboratory of Structure Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian 350002, China.
Sci Adv. 2018 Mar 30;4(3):eaar5100. doi: 10.1126/sciadv.aar5100. eCollection 2018 Mar.
Reforming CH into syngas using CO remains a fundamental challenge due to carbon deposition and nanocatalyst instability. We, for the first time, demonstrate highly efficient electrochemical reforming of CH/CO to produce syngas in a solid oxide electrolyser with CO electrolysis in the cathode and CH oxidation in the anode. In situ exsolution of an anchored metal/oxide interface on perovskite electrode delivers remarkably enhanced coking resistance and catalyst stability. In situ Fourier transform infrared characterizations combined with first principle calculations disclose the interface activation of CO at a transition state between a CO molecule and a carbonate ion. Carbon removal at the interfaces is highly favorable with electrochemically provided oxygen species, even in the presence of H or HO. This novel strategy provides optimal performance with no obvious degradation after 300 hours of high-temperature operation and 10 redox cycles, suggesting a reliable process for conversion of CH into syngas using CO.
由于积碳和纳米催化剂的不稳定性，利用一氧化碳将甲烷重整为合成气仍然是一个基本挑战。我们首次展示了在固体氧化物电解槽中，通过阴极的一氧化碳电解和阳极的甲烷氧化，将甲烷/一氧化碳高效电化学重整以生产合成气。在钙钛矿电极上原位析出锚定的金属/氧化物界面，显著提高了抗结焦性和催化剂稳定性。原位傅里叶变换红外光谱表征结合第一性原理计算，揭示了在一氧化碳分子和碳酸根离子之间的过渡态下一氧化碳的界面活化。即使在存在氢或水的情况下，通过电化学提供的氧物种，界面处的碳去除也非常有利。这种新策略在300小时的高温运行和10次氧化还原循环后没有明显降解，提供了最佳性能，表明这是一种将甲烷利用一氧化碳转化为合成气的可靠工艺。
