Syngas production via CO2 reforming of CH4 over Ni-based SBA-15: Promotional effect of promoters (Ce, Mg, and Zr)

被引:60
作者
Chong, Chi Cheng [1 ]
Teh, Lee Peng [2 ]
Setiabudi, Herma Dina [1 ,3 ]
机构
[1] Univ Malaysia Pahang, Fac Chem & Nat Resources Engn, Kuantan 26300, Pahang, Malaysia
[2] Univ Kebangsaan Malaysia, Fac Sci & Technol, Ctr Adv Mat & Renewable Resources, Ukm Bangi 43600, Selangor, Malaysia
[3] Univ Malaysia Pahang, Ctr Excellence Adv Res Fluid Flow, Kuantan 26300, Pahang, Malaysia
关键词
Cerium; Magnesium; Zirconium; Ni/SBA-15; CO2 reforming of CH4; ASSISTED IMPREGNATION METHOD; MESOPOROUS SILICA; SYNTHESIS GAS; NI/SBA-15; CATALYSTS; COKE RESISTANCE; METHANE; TEMPERATURE; STEAM; DEHYDROGENATION; NANOPARTICLES;
D O I
10.1016/j.mtener.2019.04.001
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
The promotional effect of different types of metals (Ce, Mg, and Zr) over Ni/SBA-15 which synthesized using ultrasonic co-impregnation technique were scientifically evaluated via CO2 reforming of CH4 (CRM). Characterizations including XRD, BET, FTIR, CO2-TPD were done to examine their physical attributes, metal-support interactions, and basicity properties. XRD results suggested that NiO particles were not distributed homogeneously within the confined framework of SBA-15 for Ni-Ce/SBA-15. Nevertheless, Mg and Zr promoters could effectively improve Ni dispersion over the SBA-15's siliceous framework and controlled the NiO crystallize sizes. The smallest NiO crystallite size of 9.3 nm was obtained by Ni-Zr/SBA-15. BET results verified the alteration of pore structure without changing the ordered structure of SBA-15 upon promoter addition. FTIR results suggested the partial transformation of Si-OH groups to the Si-O-X bond (X = Ce, Mg and Zr), whereas, CO2-TPD results confirmed the moderate basic sites present in Ni-Zr/SBA-15. H-2-TPR evidenced the strongest metal-support interaction in Ni-Zr/SBA-15 owing to its high temperature reduction behaviour. At operating condition of P = 1.0 bar and WHSV = 15,000 mLg(-1)h(-1), catalytic performance and stability ascended the trend of un-promoted < Ce-promoted < Mg-promoted < Zr-promoted Ni/SBA-15, in which Zr-promoted Ni/SBA-15 manifested the best catalytic activity (CO2 conversion = 93.8%; CH4 conversion = 88.3%; H-2/CO ratio = 0.82). The ascendency catalytic activity and stability of Ni-Zr/SBA-15 catalyst were attributed to its favourable properties such as strong Si-O-Zr bond formation, smallest NiO crystallite size and a moderate amount of basic sites, which crucial for sintering restriction of NiO particles and carbon deposition, thus facilitated CRM reaction. (C) 2019 Elsevier Ltd. All rights reserved.
引用
收藏
页码:408 / 417
页数:10
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