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Pd-Rh/TiO2光催化CO2氧化乙烷脱氢研究
引用本文:李倩倩,唐思扬,岳海荣,刘长军,马奎,钟山,梁斌.Pd-Rh/TiO2光催化CO2氧化乙烷脱氢研究[J].化工学报,2020,71(8):3556-3564.
作者姓名:李倩倩  唐思扬  岳海荣  刘长军  马奎  钟山  梁斌
作者单位:1.四川大学化学工程学院,低碳技术与化学反应工程研究室,四川 成都 610065;2.四川大学新能源与低碳技术学院,四川 成都 610207
摘    要:采用浸渍还原方法制备Pd-Rh/TiO2催化剂用于常温光催化CO2氧化乙烷脱氢制C2H4。研究不同Pd/Rh比催化剂的光反应性能,利用XRD、EDX-mapping、TEM、HRTEM、XPS技术表征催化剂表面和电子特性,通过UV-Vis、PL技术考察催化剂光响应性能,采用原位红外光谱技术分析Pd-Rh/TiO2光催化CO2氧化乙烷脱氢反应机理。研究表明,Pd-Rh双金属体系可有效提高光反应活性,光照下Pd和Rh金属之间存在内部电子转移的作用,降低了Pd表面的电子云密度,促进光生电子和空穴的分离,同时促进了C2H6和CO2在材料表面的吸附。Ar替换CO2的对比实验证明,反应中的CO2消耗H2,可消除催化剂表面积碳,促进C2H4生成。

关 键 词:催化  烷烃  二氧化碳  氧化  脱氢  二氧化钛      
收稿时间:2020-02-24
修稿时间:2020-05-22

Study on the photocatalytic oxidative dehydrogenation of ethane with CO2 over Pd-Rh /TiO2 catalyst
LI Qianqian,TANG Siyang,YUE Hairong,LIU Changjun,MA Kui,ZHONG Shan,LIANG Bin.Study on the photocatalytic oxidative dehydrogenation of ethane with CO2 over Pd-Rh /TiO2 catalyst[J].Journal of Chemical Industry and Engineering(China),2020,71(8):3556-3564.
Authors:LI Qianqian  TANG Siyang  YUE Hairong  LIU Changjun  MA Kui  ZHONG Shan  LIANG Bin
Affiliation:1.School of Chemical Engineering, Sichuan University, Chengdu 610065, Sichuan, China;2.Institute of New Energy and Low Carbon Technology, Sichuan University, Chengdu 610207, Sichuan, China
Abstract:Pd-Rh/ TiO2 catalyst was prepared by impregnation reduction method for photocatalytic CO2 oxidative dehydrogenation of ethane to C2H4 at room temperature. Effects of different Pd/Rh ratio of the catalysts on the photocatalytic performances were studied. Morphology characteristics of the catalysts were examined by XRD, EDX-mapping, TEM, HRTEM and XPS. The photocatalytic performances of the catalysts were measured by UV-Vis and PL. The mechanism of oxidative dehydrogenation of ethane was examined with in situ FTIR. The internal electrons transfer between Pd cluster and Rh cluster effectively improves the photocatalytic performance. It reduces the electron density of the Pd surface, and promotes the separation of e- and h+. It also improves the adsorption of C2H4 and CO2 on the surface of the catalyst. The contrast experiments of CO2 and Ar prove that CO2 does help to eliminate carbon deposed on the catalyst and to promote ethylene generating with itself reduced by H2.
Keywords:catalysis  alkane  carbon dioxide  oxidation  dehydrogenation  titanium dioxide  palladium  rhodium  
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