磷酸改性CeO_(2)纳米棒负载Pt催化剂催化丙烷燃烧性能的研究  

Study on catalytic performance of phosphoric acid modified CeO_(2)nanorod supported Pt catalyst for propane combustion

作　　者：金声势 刘凯杰 刘秋文 张一波 杨向光[1,2] JIN Shengshi;LIU Kaijie;LIU Qiuwen;ZHANG Yibo;YANG Xiangguang(School of Rare Earths,University of Science and Technology of China,Hefei 230026,China;Ganjiang Innovation Academy,Chinese Academy of Sciences,Ganzhou 341000,China)

机构地区：[1]中国科学技术大学稀土学院,安徽合肥230026 [2]中国科学院赣江创新研究院,江西赣州341000

出　　处：《无机盐工业》2024年第1期141-148,共8页Inorganic Chemicals Industry

基　　金：国家自然科学基金项目(22072141、22176185);中国科学院青年创新促进会人才项目(2018263);中国科学院重点部署项目(ZDRW-CN-2021-3);中国科学院赣江创新研究院自主部署项目(E355C001);国家重点研发计划项目(2022YFB3504200);江西省杰出青年基金项目(20232ACB213004)。

摘　　要：机动车和石油化工等污染源排放造成的环境污染日益严重,其中以丙烷为代表的低碳烷烃结构稳定,难以实现低温完全氧化,亟需开发高效低碳烷烃低温催化氧化催化剂。以氧化铈纳米棒为载体,通过酸改性合成不同量磷酸改性的1%Pt/CeO_(2)-y POx催化剂,发现磷酸改性之后丙烷催化燃烧T_(50)降低了60℃。通过XRD、TEM、EDS mapping等表征发现Pt和P均匀分布在氧化铈表面,且在磷酸改性和Pt负载过程后,氧化铈结构保持稳定。XPS和原位CO-DRIFTs表征结果表明磷酸改性之后,Pt在催化剂表面颗粒大小随磷酸改性程度增加而逐渐变大,并存在最优的Pt^(2+)和Pt^(4+)比,有利于丙烷在催化剂表面吸附和反应。H_(2)-TPR和NH_(3)-TPD表征结果表明,磷酸改性之后,催化剂表面产生了大量的酸性位,而磷酸改性并未大幅降低催化剂的氧化还原能力,从而提高了铈基催化剂的丙烷燃烧活性。With the increasingly serious environmental pollution caused by the emission of pollution sources such as motor vehicles and petrochemicals,the structure of low⁃carbon alkanes represented by propane is stable,and it is difficult to achieve complete oxidation at low temperature.Therefore,it is urgent to develop high⁃efficiency low⁃temperature catalytic oxidation catalysts.The different amounts of phosphoric acid modified 1%Pt/CeO_(2)-yPOx catalysts were synthesized by acid modification with cerium oxide nanorods as carrier.It was found that the T_(50)of propane catalytic combustion was reduced by 60℃after phosphoric acid modification.Through XRD,TEM,EDS mapping and other characterization,it was found that Pt and P were evenly distributed on the surface of cerium oxide,and the structure of cerium oxide remained stable after phos⁃phoric acid modification and Pt loading process.XPS and in-situ CO-DRIFTs showed that after phosphoric acid modifica⁃tion,the particle size of Pt on the surface of the catalyst was increased with the increase of the modification degree of phos⁃phoric acid.There was an optimal Pt^(2+)/Pt^(4+)ratio,which was beneficial to the adsorption and reaction of propane on the catalyst surface.H_(2)-TPR and NH_(3)-TPD showed that a large number of acid sites were generated on the surface of the catalyst af⁃ter phosphoric acid modification,while phosphoric acid modification did not significantly reduce the redox ability of the catalyst,thus improving the propane combustion activity of the cerium⁃based catalyst.

关 键 词：铈基催化剂 磷酸改性 丙烷氧化 贵金属 稀土催化剂 

分 类 号：O643.3[理学—物理化学]