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Highly efficient electrochemical reforming of CH4/CO2 in a solid oxide electrolyser.
Science Advances ( IF 11.7 ) Pub Date : 2018-Mar-01 , DOI: 10.1126/sciadv.aar5100
Jinhai Lu 1 , Changli Zhu 1 , Changchang Pan 1 , Wenlie Lin 2 , John P. Lemmon 3 , Fanglin Chen 4 , Chunsen Li 2 , Kui Xie 1
Affiliation  

Reforming CH4 into syngas using CO2 remains a fundamental challenge due to carbon deposition and nanocatalyst instability. We, for the first time, demonstrate highly efficient electrochemical reforming of CH4/CO2 to produce syngas in a solid oxide electrolyser with CO2 electrolysis in the cathode and CH4 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 CO2 at a transition state between a CO2 molecule and a carbonate ion. Carbon removal at the interfaces is highly favorable with electrochemically provided oxygen species, even in the presence of H2 or H2O. 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 CH4 into syngas using CO2.

中文翻译:

固体氧化物电解槽中CH4 / CO2的高效电化学重整。

由于碳沉积和纳米催化剂的不稳定性,使用CO 2将CH 4重整为合成气仍然是一个基本挑战。我们首次展示了CH 4 / CO 2的高效电化学重整,以在固体氧化物电解槽中产生合成气,其中阴极为CO 2电解,阳极为CH 4氧化。钙钛矿电极上锚固金属/氧化物界面的原位析出可显着提高抗焦化性和催化剂稳定性。原位傅立叶变换红外表征与第一原理计算相结合,揭示了在CO之间的过渡态下CO 2的界面活化2个分子和一个碳酸根离子。即使在H 2或H 2 O存在的情况下,通过电化学方法提供的氧也非常有利于界面处的碳去除。这种新颖的策略可提供最佳性能,并且在高温运行300小时和10个氧化还原循环后不会出现明显的降解。使用CO 2将CH 4转化为合成气的可靠方法。
更新日期:2018-03-31
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