数据分析法应用于撬装式甲烷水蒸气重整制氢的工艺优化  

Optimization of the process of skid-mounted methane steam reforming hydrogen production by data analysis method

作　　者：于丽华 刘冬雨 南军 于人可 黄欣 赵翰清 彭孝铭 刘亭亭 连奕新[1] YU Lihua;LIU Dongyu;NAN Jun;YU Renke;HUANG Xin;ZHAO Hanqing;PENG Xiaoming;LIU Tingting;LIAN Yixin(College of Chemistry and Chemical Engineering,Xiamen University,Xiamen 361005,China;CNOOC Tianjin Chemical Research and Design Institute Co.,Ltd.,Tianjin 300131,China;Zhejiang Provincial Innovation Center of Green Petrochemical Technology,Ningbo 315000,China)

机构地区：[1]厦门大学化学化工学院,福建厦门361005 [2]中海油天津化工研究设计院有限公司,天津300131 [3]浙江省绿色石化技术创新中心,浙江宁波315000

出　　处：《厦门大学学报(自然科学版)》2025年第1期146-155,共10页Journal of Xiamen University:Natural Science

摘　　要：[目的]对甲烷水蒸气重整反应的工艺参数进行关联性分析和优化,为工业催化剂的研发和撬装天然气制氢装置设计提供可靠的理论依据.[方法]以传统的15Ni/Al_(2)O_(3)为甲烷水蒸气重整反应催化剂,在不同反应温度、水碳比、压力、空速的条件下进行一系列活性评价,利用所得实验数据结合热力学分析和人工智能(AI)+大数据降维技术进行数据分析,对甲烷水蒸气重整工艺条件进行优化,并探究其工艺条件与最终反应结果的相关性.[结果]温度、水碳比和压力通过影响体系中的甲烷水蒸气重整反应、水煤气变换反应和甲烷二氧化碳重整反应,进而影响最终反应结果;空速通过改变反应物与催化剂的接触时间影响最终结果.甲烷转化率与反应温度、水碳比呈显著正相关,与压力呈负相关,且温度和压力对其影响最大;对产物H2体积分数影响的相关性大小为温度>压力>空速≈水碳比,其中温度、水碳比与其呈正相关;对产物CO体积分数影响的相关性大小为温度>空速>压力>水碳比.[结论]高温、高水碳比、低压和低空速更有利于甲烷水蒸气重整反应,AI+大数据降维分析得出甲烷水蒸气重整中高温、高水碳比、适当压力(约0.5 MPa)为高效工作区,可为小型撬装制氢装置选择合适的工艺操作参数提供理论依据.[Objective]Small skid-mounted natural gas reforming hydrogen production is currently the most promising method of hydrogen production at stations.However,its process is limited by the integration degree,generally allowing only a single stage conversion.Therefore,the selection of appropriate process conditions has a great impact on the depth of the reforming reaction and the configuration and integration of three-stage process equipment.With the help of artificial intelligence(AI)+big data dimension reduction technology,this study aims to optimize the process conditions of methane steam reforming through experimental data,obtain the best process area,and provide a reliable theoretical basis for the development of catalysts and the design of operating parameters in industrial plants.[Methods]15Ni/Al_(2)O_(3) was used as the catalyst for methane steam reforming.After a reduction at 450℃in the atmosphere of V(H_(2))∶V(N_(2))=1∶9 for 4 h,a series of activity evaluations were conducted under the conditions of different reaction temperatures,water-carbon ratios,pressures and space velocity.[Results]The experimental data and the analysis of HSC Chemistry 9 show that excess water vapor in the process of methane steam reforming can inhibit the methanation reaction of CO and CO_(2),but is conducive to the steam reforming reaction of CH_(4) and the transformation reaction of CO.Temperature,water-carbon ratio and pressure mainly affect the results of methane steam reforming(1)and(2),water-gas shift reaction(3)and methane-carbon dioxide reforming(4).Raising the temperature can promote the progress of reactions(1),(2),and(4),but inhibit reaction(3).Therefore,the conversion rate of CH_(4) and selectivity of CO increase with temperature.As the water-carbon ratio increase,the reaction(1),(2)and(3)promote,increasing the conversion rate of CH_(4),but decreasing the selectivity of CO.Increasing pressure is not conducive to the forward reaction of reactions(1),(2)and(4),but has no great effect on reaction(3).Therefore,the conver

关 键 词：甲烷重整 撬装天然气制氢 数值分析 热力学分析 人工智能 大数据降维 

分 类 号：TQ116.2[化学工程—无机化工]