Lorber Kristijan, Zavašnik Janez, Arčon Iztok, Huš Matej, Teržan Janvit, Likozar Blaž, Djinović Petar
National Institute of Chemistry, Hajdrihova 19, 1000 Ljubljana, Slovenia.
University of Nova Gorica, Vipavska 13, SI-5000 Nova Gorica, Slovenia.
ACS Appl Mater Interfaces. 2022 Jul 20;14(28):31862-31878. doi: 10.1021/acsami.2c05221. Epub 2022 Jul 8.
Dry reforming of methane (DRM) is a promising way to convert methane and carbon dioxide into H and CO (syngas). CeO nanorods, nanocubes, and nanospheres were decorated with 1-4 wt % Ni. The materials were structurally characterized using TEM and XANES/EXAFS. The CO activation was analyzed by DFT and temperature-programmed techniques combined with MS-DRIFTS. Synthesized CeO morphologies expose {111} and {100} terminating facets, varying the strength of the CO interaction and redox properties, which influence the CO activation. Temperature-programmed CO DRIFTS analysis revealed that under hydrogen-lean conditions mono- and bidentate carbonates are hydrogenated to formate intermediates, which decompose to HO and CO. In excess hydrogen, methane is the preferred reaction product. The CeO cubes favor the formation of a polydentate carbonate species, which is an inert spectator during DRM at 500 °C. Polydentate covers a considerable fraction of ceria's surface, resulting in less-abundant surface sites for CO dissociation.
甲烷干重整（DRM）是一种将甲烷和二氧化碳转化为H和CO（合成气）的很有前景的方法。用1-4 wt%的Ni修饰CeO纳米棒、纳米立方体和纳米球。使用透射电子显微镜（TEM）和X射线吸收近边结构（XANES）/扩展X射线吸收精细结构（EXAFS）对材料进行结构表征。通过密度泛函理论（DFT）和程序升温技术结合质谱-漫反射红外傅里叶变换光谱（MS-DRIFTS）分析CO的活化情况。合成的CeO形态暴露出{111}和{100}终止面，改变了CO相互作用的强度和氧化还原性质，从而影响CO的活化。程序升温CO DRIFTS分析表明，在贫氢条件下，单齿和双齿碳酸盐被氢化成甲酸中间体，然后分解为HO和CO。在氢气过量的情况下，甲烷是首选的反应产物。CeO立方体有利于多齿碳酸盐物种的形成，该物种在500℃的DRM过程中是惰性旁观者。多齿物种覆盖了相当一部分二氧化铈表面，导致CO解离的表面位点较少。
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