催化作用
二氧化碳重整
氧气
X射线光电子能谱
甲烷
烧结
漫反射红外傅里叶变换
空位缺陷
化学
分解
镍
合成气
材料科学
无机化学
光化学
化学工程
光催化
结晶学
有机化学
工程类
作者
Ye Wang,Li Li,Guiying Li,Qing Zhao,Xue shuang Wu,Yannan Wang,Yifei Sun,Changwei Hu
标识
DOI:10.1021/acscatal.2c06412
摘要
Low-temperature dry reforming of methane (DRM) can avoid the sintering of nickel and reduce the cost of the process. However, inefficient activation of CO2 and oxidization of Ni0 hamper the catalytic performance of Ni-based catalysts at low temperatures. Herein, a Ni/ZrO2 catalyst was prepared and used in the DRM reaction, which exhibited stable activity at low temperatures (400, 320 and 300 °C) for 10 h, with CH4 and CO2 turnover frequencies of 0.26 and 0.18 s–1 at 320 °C, respectively. The presence of Ni0 species and oxygen vacancies promotes the activation of CO2 at 300 °C, proved by CO2 temperature-programmed oxidation (CO2-TPO). Combined with O2 temperature-programmed decomposition (O2-TPD), C18O2-DRM, in situ X-ray photoelectron spectroscopy (XPS), and diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) results, after CH4 decomposition on the Ni0 site, the resultant C would react with nearby surface oxygen species and lattice oxygen species of ZrO2, forming CO and an oxygen vacancy. The oxygen vacancy nearby Ni0 species with more electron transfer would promote the activation of CO2. This work highlights the importance of CO2 activation and emphasizes the key role of the synergistic effect between Ni0 species and the oxygen vacancy in enhancing the stability of catalysts over low-temperature DRM reactions.
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