氧化镧掺杂的双孔镍基催化剂甲烷干重整反应性能研究  

Study on catalytic performances of Ni-based catalysts with bimodal porous structure modified by La2O_(3) in dry reforming of methane

作　　者：吴兴亮 王毅婕 吕凌辉 张静[1] 范辉[1] 曾春阳 马清祥[1] 赵天生[1] WU Xingliang;WANG Yijie;LV Linghui;ZHANG Jing;FAN Hui;ZENG Chunyang;MA Qingxiang;ZHAO Tiansheng(State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering,School of Chemistry and Chemical Engineering,Ningxia University,Yinchuan 750021,Ningxia,China;China Petroleum and Chemical Industry Federation,Beijing 1000723,China)

机构地区：[1]宁夏大学化学化工学院省部共建煤炭高效利用与绿色化工国家重点实验室,宁夏银川750021 [2]中国石油和化学工业联合会,北京100723

出　　处：《天然气化工—C1化学与化工》2022年第4期73-82,共10页Natural Gas Chemical Industry

基　　金：宁夏自然科学基金(2020AAC03023,2021AAC03063)。

摘　　要：采用一步法制备了掺杂不同物质的量分数氧化镧(La_(2)O_(3))的双孔镍基催化剂,将其用于甲烷干重整反应。结合N_(2)物理吸/脱附、X射线衍射(XRD)、H_(2)程序升温还原(H2-TPR)、程序升温加氢(TPH)、热重(TG)和激光拉曼光谱(Raman)等表征方法对催化剂性质的分析,探讨了La_(2)O_(3)掺杂量对催化剂活性、稳定性及抗积炭性能的影响。结果表明,少量La_(2)O_(3)掺杂的催化剂能保持较好的双孔结构,且催化性能显著提升。80 h活性评价期间,催化剂M100-OM-8%Ni/La_(3)-Al的催化活性保持在较高水平且反应物转化率下降均不超过1%,同时催化剂积炭量仅为3.11%;而过量La_(2)O_(3)的引入破坏了催化剂的孔结构,催化剂稳定性显著降低。Ni-based catalysts with bimodal porous structure doped with different La_(2)O_(3) molar contents were prepared by onestep method for dry reforming of methane reaction.A series of characterization have carried out to analyze the activity,stability and anti-coking properties of catalysts,such as N_(2) physical adsorption/desorption,X-ray diffraction(XRD),H_(2)-temperature programmed reduction(H_(2)-TPR),temperature-programmed hydrogenation(TPH),thermal analysis(TG),laser Raman spectroscopy(Raman)and so on.The results show that the doped catalyst with a small amount of La_(2)O_(3) maintains a good bimodal porous structure and the catalytic performance is significantly improved.During the 80 h activity evaluation period,the catalytic activity of the catalyst M100-OM-8%Ni/La_(3)-Al remains at a high level and the conversion rate of the reactants do not decrease by more than 1%.At the same time,the carbon deposition of this catalyst is only 3.11%.However,the introduction of excessive La_(2)O_(3) destroys the pore structure of the catalyst,and the stability of the catalyst is significantly reduced.

关 键 词：氧化镧 甲烷干重整 双孔镍基催化剂 抗积炭性能 掺杂改性 

分 类 号：TQ426[化学工程]