首页|氨三乙酸配位辅助原位合成Ni@B-HZSM-5对苯和甲醇烷基化反应的影响

氨三乙酸配位辅助原位合成Ni@B-HZSM-5对苯和甲醇烷基化反应的影响

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利用氨三乙酸离子(NTA3-)与Ni2+的配位作用在强碱溶液中原位合成了负载B-Ni的HZSM-5分子筛(Ni@B-HZSM-5).采用X射线衍射(XRD)、扫描电子显微镜(SEM)、透射电子显微镜(TEM)、X射线荧光光谱(XRF)、低温N2吸附-脱附、吡啶红外光谱(Py-IR)、NH3程序升温脱附(NH3-TPD)和H2程序升温还原(H2-TPR)等手段对Ni@B-HZSM-5催化剂进行了表征,采用固定床反应器评价其苯和甲醇烷基化反应性能,并与浸渍法负载的Ni/HZSM-5分子筛催化剂进行了对比.结果表明:原位合成的Ni@B-HZSM-5催化剂中B和Ni分布均匀,具有丰富的弱酸和适宜的加氢能力,甲醇加氢形成甲烷的副反应在一定程度上被抑制;在温度460 ℃、H2压力0.4 MPa、n(苯)∶n(甲醇)=1.2∶1和质量空速2 h-1条件下,4%Ni@B2-HZSM-5催化苯和甲醇烷基化反应,苯转化率可达46.4%,甲苯和二甲苯总选择性达到95.9%,其中C8芳烃选择性为35.1%,C8芳烃中乙苯摩尔分数为6.1%;并表现出优异的稳定性,比浸渍法Ni/HZSM-5分子筛催化剂性能更佳.
Effect of In-Situ Synthesis of Ni@B-HZSM-5 by Nitrilotriacetic Acid Coordination Assistance on Alkylation of Benzene With Methanol
In this work,nitrilotriacetic acid ion(NTA3-)was used to coordinate with Ni2+in strong alkaline solution for the in-situ synthesis of B-Ni-supported ZSM-5 zeolite(Ni@B-HZSM-5).The catalyst was characterized by means of X-ray diffraction(XRD),scanning electron microscopy(SEM),transmission electron microscopy(TEM),X-ray fluorescence spectroscopy(XRF),N2 adsorption-desorption,pyridine adsorption IR spectra(Py-IR),NH3 temperature programmed desorption(NH3-TPD)and H2 temperature programmed reduction(H2-TPR).Moreover,the alkylation of benzene with methanol was evaluated in a fixed-bed reactor,and was compared to that of Ni/HZSM-5 zeolite prepared using impregnation method.The results indicate that the Ni@B-HZSM-5 catalyst prepared by in-situ synthesis exhibits uniform distribution of B and Ni,abundant weak acid and suitable hydrogenation capability,and the side reaction of methanol hydrogenation to methane is inhibited to some extent.Under the temperature of 460 ℃,H2 pressure of 0.4 MPa,n(benzene)∶n(methanol)of 1.2∶1 and MHSV of 2 h 1,4%Ni@B2-HZSM-5 has good catalytic activity in alkylation of benzene with methanol,the benzene conversion can reach up to 46.4%,the total selectivity for toluene and xylene is 95.9%,the selectivity of C8 aromatics is 35.1%,and the molar fraction of ethylbenzene in C8 aromatics is 6.1%,exhibiting excellent stability,which has better catalytic performance than Ni/HZSM-5 zeolite prepared using impregnation method.

Ni@B-HZSM-5in-situ synthesisbenzenemethanolalkylation

蔡润、代小平、王琦、冯博、曹轶华、霍猛、黄星亮

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中国石油大学(北京)化学工程与环境学院重质油国家重点实验室,北京 102249

Ni@B-HZSM-5 原位合成 甲醇 烷基化

国家自然科学基金项目国家自然科学基金项目

2157628822278425

2024

石油学报(石油加工)
中国石油学会

石油学报(石油加工)

CSTPCD北大核心
影响因子:0.764
ISSN:1001-8719
年,卷(期):2024.40(1)
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