水蒸汽处理温度对Ni-Ga/γ-Al_(2)O_(3)催化剂乙烷氧化脱氢性能的影响  

The Influence of Water Vapor Treating Temperature on Ni-Ga/γ-Al_(2)O_(3)for Oxidative Dehydrogenation of Ethane to Ethylene

作　　者：李庆慧 赵华华[1] 杨建[1] 赵军[1] 闫亮[1] 宋焕玲[1] 丑凌军[1] LI Qinghui;ZHAO Huahua;YANG Jian;ZHAO Jun;YAN Liang;SONG Huanling;CHOU Lingjun(State Key Laboratory of Low Carbon Catalysis and Carbon Dioxide Utilization,Lanzhou Institute of Chemical Physics,Chinese Academy of Sciences,Lanzhou 730000,China;University of Chinese Academy of Sciences,Beijing 100049,China)

机构地区：[1]中国科学院兰州化学物理研究所低碳催化与二氧化碳利用全国重点实验室,甘肃兰州730000 [2]中国科学院大学,北京100049

出　　处：《分子催化(中英文)》2025年第1期1-13,I0001,共14页Journal of Molecular Catalysis(China)

基　　金：国家自然科学基金委重大研究计划(92045301);甘肃省科技重大专项(22ZD6GA003);中国科学院“西部之光”计划(2022);中国科学院兰州化学物理研究所重点实验室自主部署项目(CHGZ-202209)。

摘　　要：本文采用湿浸渍法制备Ni-Ga/γ-Al_(2)O_(3)催化剂,并在不同温度下(150~550℃)对该催化剂进行水蒸汽处理后用于乙烷氧化脱氢制乙烯反应(ODHE).采用XRD、H2-TPR、quasi in-situ XPS、FTIR以及Py-IR等表征手段探究不同水蒸汽处理温度对催化剂组成、结构、氧化还原性、电子转移以及酸性的影响.结果表明,低温水蒸汽处理(≤350℃)更有利于游离NiO物种的生成,该物种有利于提高乙烷的转化率.进一步提高水蒸汽处理温度(≥450℃),催化剂中金属-载体相互作用增强,LAS酸浓度增加,有利于提高乙烯的选择性.水蒸汽处理催化剂可以促进催化剂中Ni、Ga和Al间电子转移,且高温水蒸汽处理有利于活性组分和载体的稳定,使得乙烯收率下降比例减小.Ni-Ga/γ-Al_(2)O_(3)catalyst was prepared by wet impregnation method and then treated by water vapor at different temperatures(150~550℃)for the ethane oxidative dehydrogenation to ethylene reaction(ODHE).Based on the analysis of XRD,H2-TPR,quasi in-situ XPS,FTIR and Py-IR,the effects of different water vapor treatment temperatures on the composition,structure,redox properties,electronic transfer and acidity of the catalysts were explored.Low-temperature water vapor treatment(≤350℃)was more conducive to the generation of free NiO,which was beneficial for improving the conversion of ethane.Further increasing of the water vapor treatment temperature(≥450℃)strengthened the interaction between metal and support,increased the LAS concentration of catalysts and favored the improvement of ethylene selectivity.Water vapor treatment could promote the electron transfer among Ni,Ga and Al,and the high-temperature water vapor treatment was conducive to stabilizing of the active components and support,resulting in a decreased percentage of ethylene yield.

关 键 词：乙烷 氧化脱氢 乙烯 水蒸汽处理 金属-载体相互作用 

分 类 号：O643.36[理学—物理化学]