Investigation of the role of Nb on Pd-Zr-Zn catalyst in methanol steam reforming for hydrogen

被引:48
作者
Cai, Fufeng [1 ]
Lu, Peijing [1 ]
Ibrahim, Jessica Juweriah [2 ]
Fu, Yu [1 ]
Zhang, Jun [1 ]
Sun, Yuhan [1 ,3 ]
机构
[1] Chinese Acad Sci, Shanghai Adv Res Inst, CAS Key Lab Low Carbon Convers Sci & Engn, Shanghai 201210, Peoples R China
[2] Chinese Acad Sci, Qingdao Inst Bioenergy & Bioproc Technol, Key Lab Biobased Mat, Qingdao 266101, Shandong, Peoples R China
[3] ShanghaiTech Univ, Sch Phys Sci & Technol, Shanghai 201210, Peoples R China
基金
中国国家自然科学基金;
关键词
Methanol steam reforming; Hydrogen production; Nb-modified Pd-Zr-Zn catalysts; Pd-Zn alloy; Oxygen vacancies; SUPPORTED-PD; OXYGEN VACANCIES; PD/ZNO; ZIRCONIA; WATER; COPRECIPITATION; PERFORMANCE; SELECTIVITY; COMPOSITES; COMBUSTION;
D O I
10.1016/j.ijhydene.2019.03.125
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Methanol steam reforming is regarded as a very promising process to generate H-2 suitable for fuel cells. Typically, the Pd-based catalysts can catalyze efficiently methanol steam reforming for hydrogen production. But their high selectivity to CO, a byproduct of methanol reforming reaction, severely limits their potential application. In this work, a series of Nb-modified Pd-Zr-Zn catalysts with different Nb loadings were prepared to study their catalytic activities with more focus on the role of Nb on Pd-Zr-Zn catalyst for methanol steam reforming. The prepared catalysts were fully analyzed by using various characterization techniques, for example, ICP, BET, SEM, XRD, H-2-TPR, NH3-TPD, HRTEM, CO chemisorption, XPS, and Raman. The experimental results showed that an increase in Nb loading for the Nb-modified Pd-Zr-Zn catalysts led to a decrease of the methanol conversion and H-2 production rate. This was probably due to the decrease in the amount of oxygen vacancies on the catalyst surface. However, introduction of Nb into Pd-Zr-Zn catalyst increased the acid strength on the catalytic surface. The aldehyde species derived from methanol decomposition were readily transformed to HCOOH, thus yielding high selectivity to CO2 for the Nb-modified Pd-Zr-Zn catalysts. Significantly, the addition of Nb to Pd-Zr-Zn catalyst facilitated the incorporation of Pd into the ZnO lattices, which led to the formation of Pd-Zn alloy. Consequently, the Nb-modified Pd-Zr-Zn catalysts exhibited significantly lower CO selectivity and production rate than the Pd-Zr-Zn catalyst. From the results, this work offers a new way to the rational design of selective methanol steam reforming catalysts to decrease the formation of byproduct CO. (C) 2019 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.
引用
收藏
页码:11717 / 11733
页数:17
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