TY - JOUR
T1 - Dry reforming of methane on bimetallic Pt-Ni@CeO2catalyst
T2 - A in situ DRIFTS-MS mechanistic study
AU - Chen, Huanhao
AU - Chansai, Sarayute
AU - Xu, Shaojun
AU - Xu, Shanshan
AU - Mu, Yibing
AU - Hardacre, Christopher
AU - Fan, Xiaolei
N1 - Publisher Copyright:
© 2021 The Royal Society of Chemistry.
PY - 2021/8/7
Y1 - 2021/8/7
N2 - Bimetallic Pt-Ni catalysts can promote catalytic dry reforming of methane (DRM) with improved activity and deactivation resistance compared to the relevant monometallic catalysts. Further development of Pt-Ni catalysts requires mechanistic insights into the catalytic system. Herein, a mechanistic study of DRM over Pt-Ni supported on cerium oxide catalysts (i.e., Pt-Ni@CeO2) was performed using in situ coupled diffuse reflectance infrared Fourier-transform spectroscopy and mass spectrometry (DRIFTS-MS). Specifically, a comparative study of DRM over Pt-Ni@CeO2 and control materials under continuous temperature ramping, isothermal steady-state and fast cycling transient conditions was conducted to gain information on the key surface active intermediates. As compared with the Ni@CeO2 monometallic catalyst, the bimetallic Pt-Ni@CeO2 catalyst showed significantly enhanced performance regarding activity, H2/CO ratio and long-term stability. In situ DRIFTS measurements revealed that CH4 decomposition on the surface of monometallic Ni phases readily caused serious coke deposition and deactivation. Conversely, the Pt phase in the bimetallic catalyst could improve CO2 dissociation, thus producing adsorbed oxygen species, which are beneficial for oxidising surface carbon species (derived from CH4 decomposition) to reduce coke formation. Meanwhile, the existence of Pt sites in the bimetallic catalyst could significantly improve metal dispersion, and thus facilitate the decomposition of CH4.
AB - Bimetallic Pt-Ni catalysts can promote catalytic dry reforming of methane (DRM) with improved activity and deactivation resistance compared to the relevant monometallic catalysts. Further development of Pt-Ni catalysts requires mechanistic insights into the catalytic system. Herein, a mechanistic study of DRM over Pt-Ni supported on cerium oxide catalysts (i.e., Pt-Ni@CeO2) was performed using in situ coupled diffuse reflectance infrared Fourier-transform spectroscopy and mass spectrometry (DRIFTS-MS). Specifically, a comparative study of DRM over Pt-Ni@CeO2 and control materials under continuous temperature ramping, isothermal steady-state and fast cycling transient conditions was conducted to gain information on the key surface active intermediates. As compared with the Ni@CeO2 monometallic catalyst, the bimetallic Pt-Ni@CeO2 catalyst showed significantly enhanced performance regarding activity, H2/CO ratio and long-term stability. In situ DRIFTS measurements revealed that CH4 decomposition on the surface of monometallic Ni phases readily caused serious coke deposition and deactivation. Conversely, the Pt phase in the bimetallic catalyst could improve CO2 dissociation, thus producing adsorbed oxygen species, which are beneficial for oxidising surface carbon species (derived from CH4 decomposition) to reduce coke formation. Meanwhile, the existence of Pt sites in the bimetallic catalyst could significantly improve metal dispersion, and thus facilitate the decomposition of CH4.
UR - http://www.scopus.com/inward/record.url?scp=85112365952&partnerID=8YFLogxK
U2 - 10.1039/d1cy00382h
DO - 10.1039/d1cy00382h
M3 - Article
AN - SCOPUS:85112365952
SN - 2044-4753
VL - 11
SP - 5260
EP - 5272
JO - Catalysis Science and Technology
JF - Catalysis Science and Technology
IS - 15
ER -