
浏览全部资源
扫码关注微信
1.华东理工大学 化工学院 大型工业反应器工程教育部工程研究中心 化学工程联合国家重点实验室,上海 200237
2.煤液化气化及高效低碳利用全国重点实验室,上海 200237
3.宁波工程学院 材料化学学院,浙江 宁波 315200
余江峰(1999—),硕士研究生,研究方向为低碳化工,E-mail:yujiangfeng0615@163.com。
钱炜鑫(1983—),博士,副教授,研究方向为低碳化工,E-mail:wxqian@ecust.edu.cn。
收稿:2025-03-04,
修回:2025-04-15,
纸质出版:2026-01-25
移动端阅览
余江峰,张海涛,马宏方等.Zn-Ag双金属改性丝光沸石催化剂在二甲醚羰基化反应中的性能研究[J].低碳化学与化工,2026,51(1):54-62.
YU Jiangfeng,ZHANG Haitao,MA Hongfang,et al.Study on performance of Zn-Ag bimetallic modified mordenite catalyst in dimethyl ether carbonylation reaction[J].Low-Carbon Chemistry and Chemical Engineering,2026,51(1):54-62.
余江峰,张海涛,马宏方等.Zn-Ag双金属改性丝光沸石催化剂在二甲醚羰基化反应中的性能研究[J].低碳化学与化工,2026,51(1):54-62. DOI: 10.12434/j.issn.2097-2547.20250082.
YU Jiangfeng,ZHANG Haitao,MA Hongfang,et al.Study on performance of Zn-Ag bimetallic modified mordenite catalyst in dimethyl ether carbonylation reaction[J].Low-Carbon Chemistry and Chemical Engineering,2026,51(1):54-62. DOI: 10.12434/j.issn.2097-2547.20250082.
针对二甲醚(DME)羰基化反应中丝光沸石(MOR)催化剂易失活问题,采用离子交换法引入Zn和Ag双金属对MOR进行改性,旨在优化其酸性位点分布及孔道结构以提升催化性能。通过水热合成法制备了系列催化剂,结合XRD、ICP-AES、SEM、NH
3
-TPD和Py-IR等表征手段分析了其物化性质,并在固定床反应器中评价了其催化活性。结果表明,引入Ag后,催化剂八元环孔道的Brønsted酸量和酸强度明显增大;引入Zn后,十二元环孔道的Lewis酸量增大,可协同促进CO吸附及反应动力学。在200 ℃、1.0 MPa及空速2400 mL/(g·h)条件下,1Ag/2Zn-MOR催化性能最优。在该催化剂作用下反应3 h时,DME转化率达98%;反应25 h后,DME转化率仍保持90%且乙酸甲酯选择性始终大于99%。Zn-Ag双金属改性通过调控催化剂酸位分布与孔结构,可有效提升催化活性与稳定性,为DME羰基化高效催化剂的开发提供了理论依据。
In response to the problem of easy deactivation of mordenite (MOR) catalyst in the dimethyl ether (DME) carbonylation reaction
the ion-exchange method was adopted to introduce Zn and Ag bimetals for the modification of MOR to optimize the distribution of acidic sites and the pore structure so as to enhance the catalytic performance. A series of catalysts were prepared by hydrothermal synthesis method
and their physicochemical properties were analyzed by characterization techniques
such as XRD
ICP-AES
SEM
NH
3
-TPD and Py-IR. The catalytic activity was evaluated in a fixed bed reactor. The results show that after the introduction of Ag
both the amount and strength of Brønsted acid in eight-membered ring channels of the catalyst increase significantly. After the introduction of Zn
the amount of Lewis acid in the twelve-membered ring channels increases
which synergistically promotes the adsorption of CO and the reaction k
inetics. Under the conditions of 200 ℃
1.0 MPa and space velocity of 2400 mL/(g·h)
the 1Ag/2Zn-MOR catalyst demonstrates the optimal catalytic performance. After reaction for 3 h with the catalyst
the conversion rate of DME reaches 98%. Even after reaction for 25 h
the DME conversion rate still remains 90%
and the selectivity of methyl acetate is always greater than 99%. The modification with Zn-Ag bimetals can effectively enhance the catalytic activity and stability by regulating the distribution of acid sites and the pore structure of the catalyst
which provides a theoretical foundation for the development of highly efficient catalysts for DME carbonylation.
吴伟杰 , 王勃 , 李逸欣 , 等 . 新能源开发潜力及现货市场影响研究 [J ] . 东北电力技术 , 2025 , 46 ( 2 ): 23 - 27 .
WU W J , WANG B , LI Y X , et al . Research on the potential of new energy development and its impact on the spot market [J ] . Northeast Electric Power Technology , 2025 , 46 ( 2 ): 23 - 27 .
REN X F , WANG Y R , LIU A M , et al . Current progress and performance improvement of Pt/C catalysts for fuel cells [J ] . Journal of Materials Chemistry A , 2020 , 8 ( 46 ): 24284 - 24306 .
何顺 . 合成气经甲醇和乙酸中间体接力催化直接制乙醇的研究 [D ] . 厦门 : 厦门大学 , 2022 .
HE S . Studies on direct transformation of syngas to ethanol via methanol and acetic acid intermediates by relay catalysis [D ] . Xiamen : Xiamen University , 2022 .
白丽军 , 王明义 , 丁传敏 , 等 . 合成气制乙醇的研究进展 [J ] . 现代化工 , 2021 , 41 ( 12 ): 27 - 31+37 .
BAI L J , WANG M Y , DING C M , et al . Research progress on syngas to ethanol process [J ] . Modern Chemical Industry , 2021 , 41 ( 12 ): 27 - 31+37 .
刘以银 . 氢型丝光沸石改性及其二甲醚羰基化和乙酸甲酯加氢性能研究 [D ] . 广州 : 华南理工大学 , 2021 .
LIU Y Y . Study on modification of hydrogen mordenite and its dimethyl ether carbonylation and methyl acetate hydrogenation performance [D ] . Guangzhou : South China University of Technology , 2021 .
LUSARDI M , CHEN T T , KALE M , et al . Carbonylation of dimethyl ether to methyl acetate over SSZ-13 [J ] . ACS Catalysis , 2019 , 10 ( 1 ): 842 - 851 .
LU P , YU W J , WANG K , et al . Acid-modified mordenite for enhancing methyl acetate production from dimethyl ether carbonylation [J ] . Fuel , 2024 , 376 : 132714 .
KIPNIS M A , VOLNINA E A . Methyl acetate synthesis by dimethyl ether carbonylation in the presence of zeolites: A review [J ] . Kinetics and Catalysis , 2022 , 63 ( 2 ): 129 - 140 .
DONG C C , LIU Y D , XIA Y M , et al . Size effect on diffusion and catalytic performance of mordenite in dimethyl ether carbonylation [J ] . Catalysts , 2023 , 13 ( 7 ): 1049 .
WANG Y , LIU X Q , LIU J , et al . Carbon quantum dot implanted graphite carbon nitride nanotubes: Excellent charge separation and enhanced photocatalytic hydrogen evolution [J ] . Angewandte Chemie International Edition , 2018 , 57 ( 20 ): 5867 - 5873 .
ZHOU Y F , YU M C , LIANG H J , et al . Novel dual-effective Z-scheme heterojunction with g -C 3 N 4 , Ti 3 C 2 MXene and black phosphorus for improving visible light-induced degradation of ciprofloxacin [J ] . Applied Catalysis B: Environmental , 2021 , 291 : 120105 .
YANG H , HE D Y , ZHANG T T , et al . Magnetic carbon nanotubes/red phosphorus/graphitic carbon nitride heterojunction for highly efficient visible-light photocatalytic water disinfection [J ] . Chemical Engineering Journal , 2023 , 466 : 143309 .
ZHANG X , LI Y P , QIU S B , et al . Synthesis of methyl acetate by dimethyl ether carbonylation over Cu/HMOR: Effect of catalyst preparation method [J ] . Chinese Journal of Chemical Physics , 2013 , 26 ( 1 ): 77 - 82 .
WANG S R , GUO W W , ZHU L J , et al . Methyl acetate synthesis from dimethyl ether carbonylation over mordenite modified by cation exchange [J ] . The Journal of Physical Chemistry C , 2015 , 119 ( 1 ): 524 - 533 .
WANG S R , GUO W W , ZHU L J , et al . Methyl acetate synthesis from dimethyl ether carbonylation over mordenite modified by cation exchange [J ] . The Journal of Physical Chemistry C , 2015 , 119 ( 1 ): 524 - 533 .
LU Q J , QIAN W X , MA H F , et al . Silver-modified nano mordenite for carbonylation of dimethyl ether [J ] . Catalysts , 2021 , 11 ( 2 ): 197 .
赵鹏 . 丝光沸石的合成与改性及其二甲醚羰基化反应性能 [D ] . 上海 : 华东理工大学 , 2020 .
ZHAO P . Synthesis and modification mordenite and its performance of dimethyl ether carbonylation [D ] . Shanghai : East China University of Science and Technology , 2020 .
WEBSTER C E , COTTONE A , DRAGO R S . Multiple equilibrium analysis description of adsorption on Na-mordenite and H-mordenite [J ] . Journal of the American Chemical Society , 1999 , 121 ( 51 ): 12127 - 12139 .
SHENG H B , MA H F , QIAN W X , et al . Platinum-copper bimetallic-modified nanoprism mordenite for carbonylation of dimethyl ether [J ] . Energy & Fuels , 2019 , 33 ( 10 ): 10159 - 10166 .
LI Y , HUANG S Y , CHENG Z Z , et al . Promoting the activity of Ce-incorporated MOR in dimethyl ether carbonylation through tailoring the distribution of Brønsted acids [J ] . Applied Catalysis B: Environmental , 2019 , 256 : 117777 .
HE T , LIU X C , XU S T , et al . Role of 12-ring channels of mordenite in DME carbonylation investigated by solid-state NMR [J ] . The Journal of Physical Chemistry C , 2016 , 120 ( 39 ): 22526 - 22531 .
HUANG S Y , WANG Y , WANG Z Z , et al . Cu-doped zeolites for catalytic oxidative carbonylation: The role of Brønsted acids [J ] . Applied Catalysis A: General , 2012 , 417/418 : 236 - 242 .
ZHAO P , QIAN W X , MA H F , et al . Effect of Zr incorporation on mordenite catalyzed dimethyl ether carbonylation [J ] . Catalysis Letters , 2021 , 151 : 940 - 954 .
CHU Y Y , LO A Y , WANG C , et al . Origin of high selectivity of dimethyl ether carbonylation in the 8-membered ring channel of mordenite zeolite [J ] . The Journal of Physical Chemistry C , 2019 , 123 ( 25 ): 15503 - 15512 .
PRIYA S S , BHANUCHANDER P , KUMAR V P , et al . Platinum supported on H-mordenite: A highly efficient catalyst for selective hydrogenolysis of glycerol to 1,3-propanediol [J ] . ACS Sustainable Chemistry & Engineering , 2016 , 4 ( 3 ): 1212 - 1222 .
WANG M X , HUANG S Y , LV J , et al . Modifying the acidity of H-MOR and its catalytic carbonylation of dimethyl ether [J ] . Chinese Journal of Catalysis , 2016 , 37 ( 9 ): 1530 - 1537 .
0
浏览量
0
下载量
0
CNKI被引量
关联资源
相关文章
相关作者
相关机构
蜀公网安备51012202001533