SiC催化燃烧甲烷性能.pdf

物理化学学报( Wuli luaxue Xuebao
Octobe
Acta Phys.-Chin.Sin.2014,30(10),1941-1946
1941
「 Article
doi:10.3866/PKU.WHXB201408181
www.whxb.pku.edu.cn
Cen Ezr EO2修饰的Ni/SiC、Fe/SiC和Co/SiC催化燃烧甲烷性能
焦志锋2董莉莉郭晓宁靳国强郭向云
王晓敏
(太原理工大学材料科学与工程学院,太原030024;2中国科学院山西牒炭化学研究所牒转化固家重点实验室,大原03000
摘要:以铈锆固溶体(Ce。sZoO2)修饰的高比表面积SiC为载体,采用两步浸法制各了N、Fe和Co基催化剂,
研究了其在煤层气催化燃烧脱氧中的催化活性和稳定性.利用X射线衍射XRD)X射线光电子能谱(XPS)电感
耦合等离子体质谱(CP-MS)高分辨透射电子显微镜( HRTEM)、比表面积(BET)、热重分析(TGA)和H2程序升温
还原(H2-TPR)对催化剂进行了表征.分析结果表明,NI、Fe和Co部分进入 Ceoszrosc2固溶体晶格内部,导致催化
剂体相形成更多的缺陷;同时 Ceaszras o2固浴体有助于加速金属氧化物和金属之间氧化还原过程的进行,促进了
氧吸附、传输和对甲烷的活化.另外,SiC和 Ce,szros O2固熔体良好的抗积碳性能,有效避免了催化剂在富甲烷反
应气氛中因积碳而大活,从而使三种催化剂均其有优良的催化燃烧脱氧活性和稳定性.其中,Co/ Ceaszrosc2/SiC
活性最高,可在320℃活化催化甲烷,并在410C实现完全脱氧.
关键词:高比表面碳化硅;过度金属催化剂;铈锆固溶体;甲烷催化燃烧;煤层气脱氧
中图分类号:O643
Methane Catalytic Combustion over Ni/Sic, Fe/Sic and Co/Sic
Modified by Zros Ceo 502 Solid Solution
JIAO Zhi-feng DONG Li-li GUO Xiao-nir
JIN Guo-qiang
GUO Xiang-yun" WANG Xiao-min
College of Materials Science and Engineering, Taiyuan University of Techmology Taiyuan 030024, P R China
State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, P. R. China)
Abstract: We used Zro s Ce O solid solution modified high specific surface area Sic as the catalyst support
and synthesized N/Ce Z O: /IC, Fe Ce Z o O Sic and Coc Z O Sic catalysts by a two-step impregnation
meto The catal i city and sta ility e investigated in the catalytic combustion deoxidation of coal-bed
gas. The as-prepared catalysts were characterized by X-ray difraction(XRD)x-ay photoelectron spectroscop
(XPS), inductively coupled plasma-mass spectroscopy(.MS) high-resolution transmission electron
microsope(HRTEM runner-emmet-te le(BET measurements, thermal gravimetric analysis(TGA), and
temperature-programmed reuion of H (H TP). The results suggest that partial diffusion of Ni, Fe, and Co
to the Ces Zr O lattice leads to the formation of defects in the catalyst bulk phase. Ces Z oso2 increased the
redox process between metals and their oxides, improving the oxygen storage, mobility capacity, and the
activation of CH In addition. the excellent resistance of both Sic and Ceos O> solid solution to carbor
deposi on e ectively inhibited coke formation on the catalysts during the combustion of rich methane
atmosphere. Hence, these catalysts have good catalytic combustion deoxidation activity and stability. Co
Ce Zr Sic catalyst had the best activity among the three catalysts: CH was activated at 320C and O was
completely removed at 410 C
Received May 14, 2014; Revised: August 11, 2014; Published on Web: August 18, 2014
Corresponding authors. WANG Xiao-min, Email: wangiaomin( tyut.edu.cn. GUO Xiao-ning, Email: guoxiaoningcsicc accn
The project was supported by the Natural Science Foundation of Shanxi Province, China (2013021007-1
山西省白然科学基金(2013021007-1)资助项目
O Editorial office of Acta Physico-chimica Sinica