催化作用
化学
光化学
甲烷
X射线光电子能谱
辐照
离解(化学)
紫外线
拉曼光谱
化学工程
物理化学
材料科学
光电子学
有机化学
光学
物理
工程类
核物理学
作者
Tao Xie,Tao Zhang,Ruikun Wang,Bo Yu,Ziyu Tang,Hao-Ye Zheng,Dan He,Tao Xie,Zhun Hu
标识
DOI:10.1016/j.jcat.2022.07.028
摘要
Driving the dry reforming of methane (DRM) reaction via integrating the photo and thermal catalysis is a promising strategy to release the greenhouse effect caused by greenhouse gases (CH4/CO2). However, existing photo-thermal catalysts have limited response range to light (ultraviolet region), and broadening light response region to reaching high-performance is quite critical for DRM reaction. Here, the Pt-Au/P25 photo-thermal catalyst was proposed. The catalyst showed obvious enhancement of response range that widened to visible light region. The catalytic performance of catalyst was improved by the SPR effect. The structure–activity relationship was determined by XRD, XPS, Raman, UV–vis and PL spectra. Pt-Au/P25 catalytic performance was evaluated in different light irradiation intensity and reaction temperature. It was found that light irradiation greatly increased the catalytic performance of DRM reaction. The formation rate of H₂ was 85.38 mmol·gcat−1·h−1 and 201.92 mmol·gcat−1·h−1 for CO at 500 °C under 4.6 W·cm−2 light irradiation intensity, which were 3.09 times for H2 and 2.08 times for CO compared with dark conditions. Moreover, The DRM reaction mechanism was investigated by in situ DRIFTS test. It was found that among the intermediate species (CHx, HCOO*, H* and so on), HCOO* was critical species for the DRM reaction to proceed. During the photo-thermal DRM reaction process, activation/dissociation of CH4 and CO2 and formation of H2 steps were strengthened due to photoelectric and SPR effect by light irradiation.
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