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介孔CuCe/M/CuCe(M=Co,Mn,Zr)催化剂富H_2中优先氧化CO的催化性能
引用本文:王艳,张丞,王雨,赵文怡,李兆强,张旭霞. 介孔CuCe/M/CuCe(M=Co,Mn,Zr)催化剂富H_2中优先氧化CO的催化性能[J]. 工业催化, 2017, 25(9): 35-42. DOI: 10.3969/j.issn.1008-1143.2017.09.007
作者姓名:王艳  张丞  王雨  赵文怡  李兆强  张旭霞
作者单位:1.包头稀土研究院,内蒙古 包头 014030; 2.稀土冶金及功能材料国家工程研究中心,内蒙古 包头014030; 3.白云鄂博稀土资源研究与综合利用国家重点实验室,内蒙古 包头014030
基金项目:内蒙古自治区自然科学基金面上项目(2017MS0209); 北方稀土科技计划项目(2016H1912)
摘    要:优先氧化是去除富H2中CO最有效的方法,铜铈催化剂是该领域的研究热点。以SBA-15为模板剂,采用纳米刻蚀法合成系列介孔Cu Ce/M/Cu Ce(M=Co,Mn,Zr)催化剂,采用XRD、N2吸附-脱附、TEM、H2-TPR和O2-TPD对催化剂结构及形貌进行表征,并对其在富H2中CO优先氧化性能进行研究。结果表明,Mn有利于催化剂表面吸附氧的增加,有助于大量氧空位的产生,进而促进CO优先氧化性能的提高;Zr的加入抑制了Cu O的还原,且其表面氧脱附温度范围过宽,不利于催化剂催化氧化性能的释放。掺杂Co与Mn可以形成Ce-Cu-M-O固溶体,促进了催化剂表面氧和晶格氧之间的相互转化,最终有利于铜铈催化剂CO优先氧化性能的提高。

关 键 词:催化化学  CuCe/M/CuCe催化剂  表面氧  晶格氧  固溶体  CO优先氧化  

Catalytic properties of mesostructured CuCe/M/CuCe(M=Co,Mn,Zr) catalysts for preferential oxidation of CO in H2-rich stream
Wang Yan,Zhang Cheng,Wang Yu,Zhao Wenyi,Li Zhaoqiang,Zhang Xuxia. Catalytic properties of mesostructured CuCe/M/CuCe(M=Co,Mn,Zr) catalysts for preferential oxidation of CO in H2-rich stream[J]. Industrial Catalysis, 2017, 25(9): 35-42. DOI: 10.3969/j.issn.1008-1143.2017.09.007
Authors:Wang Yan  Zhang Cheng  Wang Yu  Zhao Wenyi  Li Zhaoqiang  Zhang Xuxia
Affiliation:1.Baotou Research Institute of Rare Earths,Baotou 014030,Inner Mongolia,China; 2.National Engineering Research Center of Rare Earth Metallurgy and Functional Materials, Baotou 014030,Inner Mongolia,China; 3.State Key Laboratory of Baiyunobo Rare Earth Resource Researches and Comprehensive Utilization, Baotou 014030,Inner Mongolia,China
Abstract:The preferential oxidation of CO is an efficient method to reduce the small amount of CO in H2-rich stream,and CuCe catalysts have been the research hotspots in this field.Using ordered mesoporous silica SBA-15 as a hard template,mesostructured CuCe/M/CuCe(M=Co,Mn,Zr) catalysts were synthesized by nano-etching method,and characterized by XRD,N2 adsorption-desorption,TEM,H2-TPR and O2-TPD.The catalytic performance of the catalysts for the preferential oxidation of CO in H2-rich gases was studied.The results indicated that the addition of Mn was beneficial to the increase of surface adsorbed oxygen species and a great deal of oxygen vacancies over CuCe/Mn/CuCe catalyst,and then promoted the improvement of CO preferential oxidation performance.Zr prevented the reduction of CuO,and the desorption temperature range of surface oxygen was too wide to enhance the catalytic performance.When Co and Mn as addtives were doped,the presence of Ce-Cu-M-O solid solution was favorable for the mutual transformation of surface oxygen and lattice oxygen,therefore the CuCe/Mn/CuCe and CuCe/Co/CuCe catalysts presented good catalytic activity.
Keywords:catalytic chemistry  CuCe/M/CuCe catalyst  surface oxygen  lattice oxygen  solid solution  CO-PROX  
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