中北大学学报（自然科学版）2025，Vol.46Issue(4)：469-479,11.DOI:10.62756/jnuc.issn.1673-3193.2024.11.0014
超重力法制备铈锆固溶体及其催化CO2合成DMC的性能研究
Preparation of Cerium-Zirconium Solid Solution by High-Gravity Method and Its Performance in Catalysing the Synthesis of DMC from CO2
摘要
Abstract
In order to improve the problems of serious agglomeration,large particle size and uneven distribution of nanoparticles in cerium-zirconium solid solution(CeZrO2)prepared by co-precipitation method,CeZrO2 was prepared by coupling high-gravity technology with polyvinylpyrrolidone(PVP)modification.It was applied to catalyze the direct conversion of carbon dioxide(CO2)and methanol into dimethyl carbonate(DMC),and its catalytic activity was studied.The effects of PVP mass fraction,high gravity factor β and impact initial velocity u on the activity and particle size distribution of CeZrO2 were investigated.The optimal operating conditions of the impinging stream-rotating packed bed(IS-RPB)were determined as PVP mass fraction is 6%,β is 105.81 and u is 5.31 m/s.The optimum performance of CeZrO2 was obtained under these operating conditions,and the yield of generated DMC was 5.54 mmol/g.The CeZrO2 prepared under the optimum conditions was later characterized by XRD,FTIR,DLS,SEM and EPR.The crystalline structure of the catalyst can be determined by XRD,the results showed that CeZrO2 was successfully prepared with cubic fluorite structure,chemical composition was analyzed by FTIR,the results showed that PVP was successfully doped into the catalyst but did not change the structure of the catalyst,according to the DLS hydraulic particle size distribution and it was clear from the particle size distribution graphs that the catalysts prepared by IS-RPB had uniform particle size.SEM was used for morphology analysis,and the results showed that the morphology of catalysts produced in IS-RPB was significantly better than that of stirred-tank reactor,and the average particle size was about 30 nm,and EPR was used to characterize the oxygen vacancies and the Ce3+content on the surface of the catalysts,and the results showed that IS-RPB significantly increased the Ce3+content of catalysts surface.Compared with the DMC yield in the literature,the catalytic performance of IS-RPB-CZ prepared in this paper is at an upper level.关键词
共沉淀法/撞击流-旋转填料床/CeZrO2/PVP改性/CO2利用Key words
co-precipitation/impinging stream-rotating packed bed/CeZrO2/PVP modification/CO2 utilization分类
化学工程引用本文复制引用
王雅宁,李宁,郭豫晋,何景婷,祁贵生..超重力法制备铈锆固溶体及其催化CO2合成DMC的性能研究[J].中北大学学报（自然科学版）,2025,46(4):469-479,11.基金项目
山西省科技成果转化引导专项(202204021301047) （202204021301047）
山西省基础研究计划青年科学研究项目(202203021212134) （202203021212134）
