Selective production of olefins from methanol over a heteroatomic SAPO-34 zeolite

被引:1
作者
Zhu, Zhaodong [1 ]
Fan, Mengtian [1 ]
He, Meng [1 ]
Ana, Bing [1 ]
Chen, Yinlin [1 ]
Xu, Shaojun [2 ]
Zhou, Tianze [1 ]
Sheveleva, Alena M. [1 ]
Kippax-Jones, Meredydd [1 ]
Shan, Lutong [1 ]
Cheng, Yongqiang [4 ]
Cavaye, Hamish [5 ]
Armstrong, Jeff [5 ]
Rudic, Svemir [5 ]
Parker, Stewart F. [5 ]
Thornley, William [6 ]
Tillotson, Evan [6 ]
Lindley, Matthew [6 ]
Tian, Shenglong [7 ]
Lee, Daniel [2 ]
Fu, Shiyu [8 ]
Frogleyi, Mark D. [9 ]
Tuna, Floriana [1 ,3 ]
Mcinnes, Eric J. L. [1 ,3 ]
Haigh, Sarah J. [6 ]
Yang, Sihai [1 ,10 ]
机构
[1] Univ Manchester, Dept Chem, Manchester M13 9PL, England
[2] Univ Manchester, Dept Chem, Manchester M13 9PL, England
[3] Univ Manchester, Photon Sci Inst, Manchester M13 9PL, England
[4] Oak Ridge Natl Lab, Chem & Engn Mat Div CEMD, Neutron Sci Directorate, Oak Ridge, TN 37831 USA
[5] STFC Rutherford Appleton Lab, ISIS Facil, Didcot OX11 0QX, England
[6] Univ Manchester, Dept Mat, Manchester M13 9PL, England
[7] Chinese Acad Sci, Dalian Inst Chem Phys, CAS Key Lab Sci & Technol Appl Catalysis, Dalian 116023, Peoples R China
[8] South China Univ Technol, State Key Lab Pulp & Paper Engn, Guangzhou 510641, Peoples R China
[9] Diamond Light Source, Harwell Sci Campus, Didcot OX11 0DE, England
[10] Peking Univ, Coll Chem & Mol Engn, Beijing Natl Lab Mol Sci, Beijing 100871, Peoples R China
基金
英国工程与自然科学研究理事会;
关键词
SAPO-34; Propylene; Inelastic neutron scattering; Trimethyloxonium; CARBON BOND FORMATION; MOLECULAR-SIEVES; DIMETHYL ETHER; CONVERSION; HYDROCARBONS; MTO; PERFORMANCE; MECHANISM; CATALYST; SURFACE;
D O I
10.1016/j.scib.2024.12.050
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
The methanol-to-olefins (MTO) process has the potential to bridge future gaps in the supply of sustainable lower olefins. Promoting the selectivity of propylene and ethylene and revealing the catalytic role of active sites are challenging goals in MTO reactions. Here, we report a novel heteroatomic silicoaluminophosphate (SAPO) zeolite, SAPO-34-Ta, which incorporates active tantalum(V) sites within the framework to afford an optimal distribution of acidity. SAPO-34-Ta exhibits a remarkable total selectivity of 85.8% for propylene and ethylene with a high selectivity of 54.9% for propylene on full conversion of methanol at 400 degrees C. In situ and operando synchrotron powder X-ray diffraction, diffuse reflectance infrared Fourier transform spectroscopy and inelastic neutron scattering, coupled with theoretical calculations, reveal trimethyloxonium as the key reaction intermediate, promoting the formation of first carbon-carbon bonds in olefins. The tacit cooperation between tantalum(V) and Br & oslash;nsted acid sites within SAPO-34 provides an efficient platform for selective production of lower olefins from methanol. (c) 2025 Science China Press. Published by Elsevier B.V. and Science China Press. All rights are reserved, including those for text and data mining, AI training, and similar technologies.
引用
收藏
页码:694 / 703
页数:10
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