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Role of catalyst support over PdO-NiO catalysts on catalyst activity and stability for oxy-CO2 reforming of methane

机译:PdO-NiO催化剂上的催化剂载体对甲烷氧化-CO2重整的催化剂活性和稳定性的作用

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PdO-NiO catalysts over several commercial metal oxides were synthesized using incipient wet impregnation method. The activities of PdO-NiO catalysts for syngas production via oxy-CO2 reforming of methane were investigated at temperatures ranging from 500 °C to 800°C in a fixed-bed continuous-flow reactor. The PdO-NiO/Y2O3 and PdO-NiO/Al2O3 catalysts show very high CH4 and CO2 conversions due to the formation of metal-support compound on these catalysts. On the PdO-NiO/Y2O3 catalyst, Pd interacts with Y2O3 support to form Pd_xO_yY_z compound while Ni interacts with A12O3 support to form NiAl2O4 spinel compound on the PdO-NiO/Al2O3 catalyst. However, the amount of deposited carbon on the spent PdO-NiO/Y2O3 catalyst is much lower than the one on the PdO-NiO/Al2O3 catalyst due to the presence of surface β-oxygen species and ability of Y2O3 to form oxycarbonate species, resulting in stable catalytic performance without noticeable deactivation during reaction. The surface β-oxygen species are found to promote cracking of C-H bond in CH4 while the oxycarbonate species can oxidize the deposited carbon, respectively, hence leading to the stability of the PdO-NiO/Y2O3 catalyst.
机译:采用初期湿法浸渍法合成了几种工业金属氧化物上的PdO-NiO催化剂。在固定床连续流反应器中,研究了PdO-NiO催化剂通过甲烷的氧化-CO2重整生产合成气的活性,温度范围为500°C至800°C。由于在这些催化剂上形成了金属载体化合物,PdO-NiO / Y2O3和PdO-NiO / Al2O3催化剂显示出很高的CH4和CO2转化率。在PdO-NiO / Y2O3催化剂上,Pd与Y2O3载体相互作用形成Pd_xO_yY_z化合物,而Ni与Al2O3载体相互作用形成PdO-NiO / Al2O3催化剂上的NiAl2O4尖晶石化合物。但是,由于存在表面β-氧物种和Y2O3形成碳酸盐物种的能力,在废PdO-NiO / Y2O3催化剂上沉积的碳量比在PdO-NiO / Al2O3催化剂上的沉积碳量低得多。稳定的催化性能,反应期间不会明显失活。发现表面的β-氧物种促进了CH4中C-H键的裂解,而碳酸盐物种可以分别氧化沉积的碳,因此导致了PdO-NiO / Y2O3催化剂的稳定性。

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