火焰喷雾热解制Pd-Pt/CeO_(2)催化甲烷燃烧的性能研究  

Methane catalytic combustion over flame spray pyrolysis-synthesized Pd-Pt/CeO_(2) catalyst

作　　者：武琳渊 王乙 陈召英 田庆玲 王琳茹 付紫君 赵宁[5] 王晓波 黄鑫 WU Linyuan;WANG Yi;CHEN Zhaoying;TIAN Qingling;WANG Linru;FU Zijun;ZHAO Ning;WANG Xiaobo;HUANG Xin(College of Safety and Emergency Management Engineering,Taiyuan University of Technology,Taiyuan 030024,China;Shanxi Lu’an Chemical Group Co.,Ltd.,Changzhi 046200,China;State Key Laboratory of Coal and CBM Co-mining,Jincheng 048012,China;Jinneng Holding Equipment Manufacturing Group Co.,Ltd.,Jincheng 048006,China;Institute of Coal Chemistry,Chinese Academy of Sciences,Taiyuan 030001,China)

机构地区：[1]太原理工大学安全与应急管理工程学院,山西太原030024 [2]山西潞安化工集团有限公司,山西长治046200 [3]煤与煤层气共采国家重点实验室,山西晋城048012 [4]晋能控股装备制造集团有限公司,山西晋城048006 [5]中国科学院山西煤炭化学研究所,山西太原030001

出　　处：《燃料化学学报（中英文）》2024年第5期725-734,共10页Journal of Fuel Chemistry and Technology

基　　金：煤与煤层气共采国家重点实验室开放基金(2022KF12);山西省科技成果转化引导专项(202204021301010);山西省科技创新人才团队项目(202204051002025);国家自然科学基金(52004177)资助。

摘　　要：火焰喷雾热解法(FSP)是一种简单、快速、可规模化制备纳米催化剂的技术。通过火焰喷雾热解法合成CeO_(2)和Pt-CeO_(2)载体、Pd-Pt-CeO_(2)催化剂,采用浸渍法在CeO_(2)和Pt-CeO_(2)载体分别沉积Pd-Pt和Pd而制得Pd-Pt双金属催化剂,并考察其甲烷催化燃烧性能。利用ICP、XRD、TEM、BET、H_(2)-TPR、XPS和Raman对催化剂的物化性质进行分析。TEM结果表明,Pd-Pt/CeO_(2)催化剂中Pd和Pt物种高分散于CeO_(2)载体。相比于一步法(one step)制得的Pd-Pt-CeO_(2)(OS-FSP)催化剂,共浸渍法制得Pd-Pt/CeO_(2)(0.25)-WI的催化活性更高,其t_(50)降低了60℃,且稳定运行60 h而没有明显失活。这归因于Pd-Pt/CeO_(2)(0.25)-WI催化剂表面上Pd^(0)/Pd^(2+)和Ce^(3+)/Ce^(4+)物质的量比更高、晶格氧更多,进而导致其具有良好的甲烷催化燃烧性能。Flame spray pyrolysis(FSP)is a versatile,rapid,and scalable preparation technique for the nanocatalysts.CeO_(2) and Pt-CeO_(2) carriers,Pd-Pt-CeO_(2) catalyst were synthesized by flame spray pyrolysis,and then Pd-Pt bimetallic catalysts were prepared by impregnation method,and as-obtained Pd-Pt catalysts were tested in the methane combustion.The physicochemical properties of the catalysts were characterized by ICP,XRD,TEM,BET,H_(2)-TPR,XPS,and Raman.TEM results showed that Pd and Pt species were highly dispersed in CeO_(2) carriers in Pd-Pt/CeO_(2) catalysts.Compared with the Pd-Pt-CeO_(2)(OS-FSP)catalyst prepared by one-step flame spray pyrolysis,the catalytic activity of the Pd-Pt/CeO_(2)(0.25)-WI prepared by co-impregnation was higher,with its t_(50) reduced by 60℃,and no deactivation was seen for 60 h.It is attributed to the fact that the Pd-Pt/CeO_(2)(0.25)-WI catalyst has a higher molar ratio of Pd^(0)/Pd^(2+)and Ce^(3+)/Ce^(4+)on the surface of the catalyst and more lattice oxygen,resulting in an excellent performance during the methane combustion.

关 键 词：甲烷催化燃烧 火焰喷雾热解 浸渍法 钯 稳定性 

分 类 号：O643[理学—物理化学]