Catalytic methane oxidation performance over Pd/γ-Al2O3 catalyst optimized by the synergy of phosphorus and MOx (M = La, Ba and Zr)

Catalytic methane oxidation performance over Pd/γ-Al2O3 catalyst optimized by the synergy of phosphorus and MOx (M = La, Ba and Zr)
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通过磷和 MOx(M = La、Ba 和 Zr)的协同作用优化 Pd/γ-Al2O3 催化剂的催化甲烷氧化性能

DOI:
10.1016/j.fuel.2021.120933
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发表时间:
2021-09
期刊:
影响因子:
7.4
通讯作者:
Lilong Jiang
Lilong Jiang
中科院分区:
工程技术1区
文献类型:
--
作者:
Xiaohua Chen;Jia Lin;Yong Zheng;Yingying Zhan;Wen Zhang;Yihong Xiao;Ying Zheng;Lilong Jiang

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研究了Pd/γ-Al 2 O3催化剂中MOx(M = La、Ba和Zr)和磷助剂对甲烷氧化的协同作用。结果表明,添加MOx作为第二助催化剂对催化剂性能有积极影响。MOx-PdO界面的产生,改变了界面张力,促进了PdO颗粒的晶化,从而改变了钯纳米颗粒的接触角,提高了催化剂的还原性能,同时增加了钯的台阶位,有利于催化剂的上级活性。此外,MOx的给电子效应使催化剂表面氧物种增多,抑制OH/H2O的积累,降低表面酸碱度,提高催化剂的活性和耐湿性。其中,Pd/La-PAl在60小时的反应中表现出最佳的活性和优异的耐久性。经原位反应活化和甲烷气氛处理后,在310 °C左右完全催化甲烷氧化。
The focus of this study was to elucidate the synergy of MOx(M = La, Ba and Zr) and phosphorus additives in Pd/γ-Al2O3catalyst towards methane oxidation. It was revealed that the MOxaddition as a second promoter positively influenced catalyst performance. The generation of extra MOx-PdO interface facilitated the crystallization of PdO grains as a result of the change in the interfacial tension and then the contact angles of palladium nanoparticles, yielding enhanced reducing property jointly with richer palladium step sites, which preferred catalysts with superior activity. Moreover, MOxdopant provided more surface oxygen species over catalysts due to its electron-donating effect, inhibited the OH/H2O accumulation and gave lower surface acidity/basicity ratio, improving both activity and moisture-tolerance. Amongst, Pd/La-PAl manifested the optimum activity and excellent durability during 60-h on-stream reaction. It completely catalyzed methane oxidation at around 310 °C after In situ reaction activation and treatment in methane atmosphere.
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