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基于响应面法的蜂窝陶瓷催化剂载体预处理工艺优化实验设计OA

Optimization experiment of the pretreatment process for cordierite honeycomb ceramic catalyst support using response surface methodology

中文摘要英文摘要

针对质子交换膜燃料电池电极催化剂受 CO 毒化的问题,研究富氢气中的CO选择性催化氧化脱除技术中蜂窝陶瓷载体预处理工艺对催化性能的影响:采用单因素实验与响应面法结合,分析酸处理(时间、浓度)和焙烧处理(温度、时间)对载体表面形貌及催化活性的影响.研究结果表明,单因素实验结果与响应面法构建的模型预测值吻合:1 mol/L的硝酸浓度、2~3 h的酸处理时长、400℃的焙烧温度,以及1 h的焙烧时间均为各自单因素条件下的较优参数,能改善孔隙结构与表面化学状态、提升涂层负载率;而响应面法分析表明,除焙烧时间与其他因素交互作用不显著外,其他因素协同都会影响催化剂活性.该研究为同类催化化学体系的工艺开发提供了可借鉴的教学化思路和方法,有利于培养学生的多因素耦合分析能力.

[Objective]Proton exchange membrane fuel cells are pivotal to the global energy transition,however,their catalysts exhibit high sensitivity to CO poisoning.CO preferential oxidation(CO-PROX)serves as the core technology for hydrogen purification,and honeycomb ceramics are ideal supports for CO-PROX catalysts.However,raw cordierite honeycomb ceramics(2MgO·2Al2O3·5SiO2)have drawbacks,including a low specific surface area and poor coating adhesion,which limit catalytic performance.Oriented toward cultivating scientific thinking in teaching practice,this study investigates how pretreatment of honeycomb ceramic supports affects catalytic performance in CO-PROX under hydrogen-rich conditions.It aims to enhance support performance through pretreatment optimization and establish an experimental teaching paradigm that progresses from single-factor to multiparameter optimization.[Methods]Single-factor experiments were first conducted to screen the reasonable operating ranges of key parameters as a basis for systematic optimization of the pretreatment process.Employing the coating loading rate and catalytic activity(correlated with subsequent T50/T90 indicators)as evaluation criteria,this study investigated the independent effects of acid treatment time(1-3 h),nitric acid concentration(1-3 mol/L),calcination temperature(300-500℃),and calcination time(1-3 h).This step excluded support structure damage and ineffective modifications caused by excessive parameter values,and the study then determined the effective range for subsequent multifactor optimization.Based on the results,a response surface methodology(RSM)model was constructed using a four-variable central composite rotatable design.A total of 30 experiments were designed,comprising 16 full-factor points covering different level combinations of the 4 parameters,8 axial points to expand the response at the parameter boundaries,and 6 center repeat points to evaluate experimental errors.The temperatures at which CO conversion reached 50%(T50)and 90%(T90)were used as response values.The RSM model's visual analysis function enabled intuitive identification of parameter interactions and facilitated determination of the parameter combination that minimized T50 and T90 to optimal levels.The model fitting effect was verified to ensure consistency between the experimental data and the predicted results.Finally,the pretreatment process parameters were systematically optimized and verified,and model fitting was used to analyze synergistic effects between acid treatment time,acid concentration,calcination temperature,and calcination time to determine the optimal process parameters.[Results]The single-factor experiments revealed that treating the supports with 1 mol/L nitric acid for 2-3 h effectively optimized their specific surface area and surface roughness,thereby improving coating loading rate.Additionally,calcination at 400℃for 1 h enhanced the pore structure and modified the surface chemical state.The RSM-based model demonstrated strong agreement between predicted and experimental values.The optimal process parameters were identified as a 2.5 h treatment with 1 mol/L nitric acid,followed by calcination at 400℃for 1 h,which significantly enhanced catalytic activity.The analysis of the RSM model revealed that acid treatment time,acid concentration,and calcination temperature exhibit notable synergistic effects on catalytic performance,whereas calcination time shows negligible interactions and can thus be optimized independently.[Conclusions]This study offers a reference for process development in catalytic chemical systems and presents an instructional framework to enhance students'capabilities in multifactor coupling analysis.

脱永笑;金薪;王晴;朱传勇;段欣悦;冯翔

中国石油大学(华东) 石大山能新能源学院,山东 青岛 266580中国石油大学(华东) 石大山能新能源学院,山东 青岛 266580中国石油大学(华东) 化学化工学院,山东 青岛 266580中国石油大学(华东) 石大山能新能源学院,山东 青岛 266580中国石油大学(华东) 石大山能新能源学院,山东 青岛 266580中国石油大学(华东) 化学化工学院,山东 青岛 266580

化学化工

响应面法蜂窝陶瓷酸处理焙烧处理CO选择性氧化

response surface methodologyhoneycomb ceramicacid treatmentcalcination treatmentCO preferential oxidation

《实验技术与管理》 2026 (1)

66-76,11

中国石油大学(华东)研究生课程建设项目(UPCYKS-2025-10)教育部产学合作协同育人项目(231101283223008)中国高等教育学会2022年度高等教育科学研究规划课题(22WL0310)

10.16791/j.cnki.sjg.2026.01.009

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