磷酸改性CeO2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 CeO2 nanorod supported Pt catalyst for propane combustion
金声势 1刘凯杰 2刘秋文 2张一波 1杨向光1
作者信息
- 1. 中国科学技术大学稀土学院,安徽合肥 230026;中国科学院赣江创新研究院,江西赣州 341000
- 2. 中国科学院赣江创新研究院,江西赣州 341000
- 折叠
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/CeO2-yPOx催化剂,发现磷酸改性之后丙烷催化燃烧T50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Pt2+和Pt4+比,有利于丙烷在催化剂表面吸附和反应.H2-TPR和NH3-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.
Abstract
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/CeO2-yPOx catalysts were synthesized by acid modification with cerium oxide nanorods as carrier.It was found that the T50 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 Pt2+/Pt4+ ratio,which was beneficial to the adsorption and reaction of propane on the cata-lyst surface.H2-TPR and NH3-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Key words
cerium-based catalyst/phosphoric acid modification/propane oxidation/precious metals/rare earth catalysts引用本文复制引用
基金项目
国家自然科学基金项目(22072141)
国家自然科学基金项目(22176185)
中国科学院青年创新促进会人才项目(2018263)
江西省双千计划(青年)项目(jxsq2020101047)
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)
出版年
2024
NETL
NSTL
万方数据