{"status":"ok","message-type":"work","message-version":"1.0.0","message":{"indexed":{"date-parts":[[2026,9,16]],"date-time":"2026-09-16T10:52:13Z","timestamp":1789555933643,"version":"build-2803163510"},"reference-count":76,"publisher":"American Association for the Advancement of Science (AAAS)","issue":"8","content-domain":{"domain":["www.science.org"],"crossmark-restriction":true},"short-container-title":["Sci. Adv."],"published-print":{"date-parts":[[2025,2,21]]},"abstract":"<jats:p>Compared to methanol, dimethyl ether (DME) is a more ideal and attractive raw material for industrial applications. Typically, the industrially zeolite-catalyzed methanol dehydration to DME occurs at temperatures above 423 kelvin. Improving catalytic reactivity and reducing energy consumption are urgently needed but remain challenging. Here, we report an unexplored associative strategy to realize DME formation at room temperature and the generation of olefins even at 413 kelvin, which is achieved by coinjecting basic acetone to manipulate the local chemical microenvironment of the methanol reactant inside the H-ZSM-5 zeolite. The crucial role of acetone in accelerating methanol direct dehydration to DME is highlighted as the obvious destabilization effect for the adsorbed methanol cluster with strong hydrogen bonds and the subsequent traction of water during DME formation. These findings offer more insights into the rational design of reaction systems by manipulating the local surroundings to regulate catalytic performances and should represent a large step forward in methanol conversion technology.<\/jats:p>","DOI":"10.1126\/sciadv.ads4018","type":"journal-article","created":{"date-parts":[[2025,2,19]],"date-time":"2025-02-19T18:59:36Z","timestamp":1739991576000},"update-policy":"https:\/\/doi.org\/10.34133\/aaas_crossmark","source":"Crossref","is-referenced-by-count":12,"title":["Microenvironment perturbations driving methanol low-temperature conversion over zeolite"],"prefix":"10.1126","volume":"11","author":[{"ORCID":"https:\/\/orcid.org\/0009-0006-5897-4141","authenticated-orcid":true,"given":"Fengqing","family":"Liu","sequence":"first","affiliation":[{"name":"State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics, National Center for Magnetic Resonance in Wuhan, Wuhan Institute of Physics and Mathematics, Innovation Academy for Precision Measurement Science and Technology, Chinese Academy of Sciences, Wuhan 430071, P. R. China."},{"name":"University of Chinese Academy of Sciences, Beijing 100049, P. R. China."}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9224-3111","authenticated-orcid":true,"given":"Xianfeng","family":"Yi","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics, National Center for Magnetic Resonance in Wuhan, Wuhan Institute of Physics and Mathematics, Innovation Academy for Precision Measurement Science and Technology, Chinese Academy of Sciences, Wuhan 430071, P. R. China."}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Tangkang","family":"Liu","sequence":"additional","affiliation":[{"name":"Interdisciplinary Institute of NMR and Molecular Sciences, Hubei Province for Coal Conversion and New Carbon Materials, School of Chemistry and Chemical Engineering, Wuhan University of Science and Technology, Wuhan 430081, P. R. China."}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8955-9497","authenticated-orcid":true,"given":"Wei","family":"Chen","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics, National Center for Magnetic Resonance in Wuhan, Wuhan Institute of Physics and Mathematics, Innovation Academy for Precision Measurement Science and Technology, Chinese Academy of Sciences, Wuhan 430071, P. R. China."}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0298-7286","authenticated-orcid":true,"given":"Jiabao","family":"Yang","sequence":"additional","affiliation":[{"name":"Key Laboratory of Petrochemical Catalytic Science and Technology, Liaoning Petrochemical University, Fushun 113001, P. R. China."}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-0131-8729","authenticated-orcid":true,"given":"Yao","family":"Xiao","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics, National Center for Magnetic Resonance in Wuhan, Wuhan Institute of Physics and Mathematics, Innovation Academy for Precision Measurement Science and Technology, Chinese Academy of Sciences, Wuhan 430071, P. R. China."}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-6494-5562","authenticated-orcid":true,"given":"Yucai","family":"Qin","sequence":"additional","affiliation":[{"name":"Key Laboratory of Petrochemical Catalytic Science and Technology, Liaoning Petrochemical University, Fushun 113001, P. R. China."}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Lijuan","family":"Song","sequence":"additional","affiliation":[{"name":"Key Laboratory of Petrochemical Catalytic Science and Technology, Liaoning Petrochemical University, Fushun 113001, P. R. China."}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7115-6510","authenticated-orcid":true,"given":"Anmin","family":"Zheng","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics, National Center for Magnetic Resonance in Wuhan, Wuhan Institute of Physics and Mathematics, Innovation Academy for Precision Measurement Science and Technology, Chinese Academy of Sciences, Wuhan 430071, P. R. China."},{"name":"Interdisciplinary Institute of NMR and Molecular Sciences, Hubei Province for Coal Conversion and New Carbon Materials, School of Chemistry and Chemical Engineering, Wuhan University of Science and Technology, Wuhan 430081, P. R. China."}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"221","reference":[{"key":"e_1_3_2_2_2","doi-asserted-by":"publisher","DOI":"10.1002\/anie.200503898"},{"key":"e_1_3_2_3_2","doi-asserted-by":"publisher","DOI":"10.1021\/acs.chemrev.2c00076"},{"key":"e_1_3_2_4_2","doi-asserted-by":"publisher","DOI":"10.1021\/acs.accounts.3c00187"},{"key":"e_1_3_2_5_2","doi-asserted-by":"publisher","DOI":"10.1021\/ar020006o"},{"key":"e_1_3_2_6_2","doi-asserted-by":"crossref","unstructured":"E. Zhan Z. Xiong W. Shen \u201cZeolite-catalyzed carbonylation of dimethyl ether\u201d in The Chemical Transformations of C1 Compounds (Wiley 2022) pp. 763\u2013791.","DOI":"10.1002\/9783527831883.ch17"},{"key":"e_1_3_2_7_2","doi-asserted-by":"publisher","DOI":"10.1126\/science.1219831"},{"key":"e_1_3_2_8_2","doi-asserted-by":"publisher","DOI":"10.1073\/pnas.2103840119"},{"key":"e_1_3_2_9_2","doi-asserted-by":"publisher","DOI":"10.1016\/j.apcatb.2017.05.085"},{"key":"e_1_3_2_10_2","doi-asserted-by":"crossref","unstructured":"K. Faungnawakij K. J. Suriye \u201cChapter 4\u2014Current catalytic processes with hybrid materials and composites for heterogeneous catalysis\u201d in New Future Developments in Catalysis (Elsevier 2013) pp. 79\u2013104.","DOI":"10.1016\/B978-0-444-53876-5.00004-0"},{"key":"e_1_3_2_11_2","doi-asserted-by":"publisher","DOI":"10.1021\/cs500967j"},{"key":"e_1_3_2_12_2","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201807113"},{"key":"e_1_3_2_13_2","doi-asserted-by":"publisher","DOI":"10.1021\/acscatal.1c04451"},{"key":"e_1_3_2_14_2","doi-asserted-by":"publisher","DOI":"10.1039\/D0CS01003K"},{"key":"e_1_3_2_15_2","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201204995"},{"key":"e_1_3_2_16_2","doi-asserted-by":"publisher","DOI":"10.1038\/352225a0"},{"key":"e_1_3_2_17_2","doi-asserted-by":"publisher","DOI":"10.1021\/cr00035a006"},{"key":"e_1_3_2_18_2","doi-asserted-by":"publisher","DOI":"10.1021\/ja0304244"},{"key":"e_1_3_2_19_2","doi-asserted-by":"publisher","DOI":"10.1038\/s41578-021-00347-3"},{"key":"e_1_3_2_20_2","doi-asserted-by":"publisher","DOI":"10.1021\/ja00251a004"},{"key":"e_1_3_2_21_2","doi-asserted-by":"publisher","DOI":"10.1093\/nsr\/nwac151"},{"key":"e_1_3_2_22_2","doi-asserted-by":"crossref","unstructured":"S. Xu Y. Zhi J. Han W. Zhang X. Wu T. Sun Y. Wei Z. Liu \u201cChapter two\u2014Advances in catalysis for methanol-to-olefins conversion\u201d in Advances in Catalysis C. Song Ed. (Academic Press 2017) vol. 61 pp. 37\u2013122.","DOI":"10.1016\/bs.acat.2017.10.002"},{"key":"e_1_3_2_23_2","doi-asserted-by":"publisher","DOI":"10.1126\/science.adg2491"},{"key":"e_1_3_2_24_2","doi-asserted-by":"publisher","DOI":"10.1126\/science.abo0356"},{"key":"e_1_3_2_25_2","doi-asserted-by":"publisher","DOI":"10.1038\/s41929-023-00945-0"},{"key":"e_1_3_2_26_2","doi-asserted-by":"publisher","DOI":"10.1093\/nsr\/nwx103"},{"key":"e_1_3_2_27_2","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202000269"},{"key":"e_1_3_2_28_2","doi-asserted-by":"publisher","DOI":"10.1021\/acs.chemrev.0c00016"},{"key":"e_1_3_2_29_2","doi-asserted-by":"publisher","DOI":"10.1038\/s41578-020-00250-3"},{"key":"e_1_3_2_30_2","doi-asserted-by":"publisher","DOI":"10.1038\/s41563-020-0753-1"},{"key":"e_1_3_2_31_2","doi-asserted-by":"publisher","DOI":"10.1039\/C9CC06334J"},{"key":"e_1_3_2_32_2","doi-asserted-by":"publisher","DOI":"10.1126\/science.abh3418"},{"key":"e_1_3_2_33_2","doi-asserted-by":"publisher","DOI":"10.1038\/39843"},{"key":"e_1_3_2_34_2","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202007790"},{"key":"e_1_3_2_35_2","doi-asserted-by":"publisher","DOI":"10.1021\/acscatal.7b00782"},{"key":"e_1_3_2_36_2","doi-asserted-by":"publisher","DOI":"10.1021\/acscatal.0c01454"},{"key":"e_1_3_2_37_2","doi-asserted-by":"publisher","DOI":"10.1021\/cr00007a010"},{"key":"e_1_3_2_38_2","doi-asserted-by":"publisher","DOI":"10.1038\/s41596-020-0385-6"},{"key":"e_1_3_2_39_2","doi-asserted-by":"publisher","DOI":"10.1016\/j.chempr.2021.05.023"},{"key":"e_1_3_2_40_2","doi-asserted-by":"publisher","DOI":"10.1021\/ar700210f"},{"key":"e_1_3_2_41_2","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201406823"},{"key":"e_1_3_2_42_2","doi-asserted-by":"publisher","DOI":"10.1063\/1.556018"},{"key":"e_1_3_2_43_2","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.7b10940"},{"key":"e_1_3_2_44_2","doi-asserted-by":"publisher","DOI":"10.1021\/ja954323k"},{"key":"e_1_3_2_45_2","doi-asserted-by":"publisher","DOI":"10.1038\/s41929-017-0002-4"},{"key":"e_1_3_2_46_2","doi-asserted-by":"publisher","DOI":"10.1021\/cr990132e"},{"key":"e_1_3_2_47_2","doi-asserted-by":"publisher","DOI":"10.1021\/acscatal.5b02367"},{"key":"e_1_3_2_48_2","doi-asserted-by":"publisher","DOI":"10.1126\/science.adf8042"},{"key":"e_1_3_2_49_2","doi-asserted-by":"publisher","DOI":"10.1038\/s41929-021-00618-w"},{"key":"e_1_3_2_50_2","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202006065"},{"key":"e_1_3_2_51_2","doi-asserted-by":"publisher","DOI":"10.1038\/s41929-020-00533-6"},{"key":"e_1_3_2_52_2","doi-asserted-by":"publisher","DOI":"10.1039\/D1CS00966D"},{"key":"e_1_3_2_53_2","doi-asserted-by":"publisher","DOI":"10.1021\/acs.chemrev.2c00896"},{"key":"e_1_3_2_54_2","doi-asserted-by":"publisher","DOI":"10.1021\/cs300722w"},{"key":"e_1_3_2_55_2","doi-asserted-by":"publisher","DOI":"10.1038\/371683a0"},{"key":"e_1_3_2_56_2","doi-asserted-by":"publisher","DOI":"10.1021\/ja056908c"},{"key":"e_1_3_2_57_2","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201410637"},{"key":"e_1_3_2_58_2","doi-asserted-by":"publisher","DOI":"10.1002\/jcc.23266"},{"key":"e_1_3_2_59_2","doi-asserted-by":"publisher","DOI":"10.1021\/ct400687b"},{"key":"e_1_3_2_60_2","doi-asserted-by":"publisher","DOI":"10.1016\/j.jcat.2016.12.011"},{"key":"e_1_3_2_61_2","doi-asserted-by":"publisher","DOI":"10.1016\/j.jcat.2018.01.032"},{"key":"e_1_3_2_62_2","doi-asserted-by":"publisher","DOI":"10.1038\/s41929-022-00906-z"},{"key":"e_1_3_2_63_2","doi-asserted-by":"publisher","DOI":"10.1039\/C5CS00029G"},{"key":"e_1_3_2_64_2","doi-asserted-by":"publisher","DOI":"10.1021\/acscatal.0c01501"},{"key":"e_1_3_2_65_2","first-page":"462","article-title":"Observation of spin exchange by two-dimensional fourier transform 13C cross polarization-magic-angle spinning","volume":"47","author":"Szeverenyi N. M.","year":"1982","unstructured":"N. M. Szeverenyi, M. J. Sullivan, G. E. Maciel, Observation of spin exchange by two-dimensional fourier transform 13C cross polarization-magic-angle spinning. J. Magn. Reson. 47, 462\u2013475 (1982).","journal-title":"J. Magn. Reson."},{"key":"e_1_3_2_66_2","unstructured":"R. R. Ernst G. Bodenhausen A. Wokaun. Principles of Nuclear Magnetic Resonance in One and Two Dimensions (Clarendon Press 1987)."},{"key":"e_1_3_2_67_2","unstructured":"Structure commission of the international zeolite association. http:\/\/www.iza-structure.org\/."},{"key":"e_1_3_2_68_2","doi-asserted-by":"publisher","DOI":"10.1039\/b810189b"},{"key":"e_1_3_2_69_2","doi-asserted-by":"publisher","DOI":"10.1016\/j.jcat.2012.05.015"},{"key":"e_1_3_2_70_2","unstructured":"M. J. Frisch G. W. Trucks H. B. Schlegel G. E. Scuseria M. A. Robb J. R. Cheeseman G. Scalmani V. Barone B. Mennucci G. A. Petersson H. Nakatsuji X. Li M. Caricato A. Marenich J. Bloino B. G. Janesko R. Gomperts B. Mennucci H. P. Hratchian J. V. Ortiz A. F. Izmaylov J. L. Sonnenberg D. Williams-Young F. Ding F. Lipparini F. Egidi J. Goings B. Peng A. Petrone T. Henderson D. Ranasinghe V. G. Zakrzewski J. Gao N. Rega G. Zheng W. Liang M. Hada M. Ehara K. Toyota R. Fukuda J. Hasegawa M. Ishida T. Nakajima Y. Honda O. Kitao H. Nakai T. Vreven K. Throssell J. A. Montgomery Jr. J. E. Peralta F. Ogliaro M. Bearpark J. J. Heyd E. Brothers K. N. Kudin V. N. Staroverov T. Keith R. Kobayashi J. Normand K. Raghavachari A. Rendell J. C. Burant S. S. Iyengar J. Tomasi M. Cossi J. M. Millam M. Klene C. Adamo R. Cammi J. W. Ochterski R. L. Martin K. Morokuma O. Farkas J. B. Foresman and D. J. Fox Gaussian 09 Revision B.01 (Gaussian Inc. 2010)."},{"key":"e_1_3_2_71_2","doi-asserted-by":"publisher","DOI":"10.1002\/jcc.22885"},{"key":"e_1_3_2_72_2","doi-asserted-by":"publisher","DOI":"10.1002\/wcms.1159"},{"key":"e_1_3_2_73_2","doi-asserted-by":"publisher","DOI":"10.1038\/s41592-019-0506-8"},{"key":"e_1_3_2_74_2","doi-asserted-by":"publisher","DOI":"10.1103\/PhysRevLett.80.890"},{"key":"e_1_3_2_75_2","doi-asserted-by":"publisher","DOI":"10.1063\/1.3382344"},{"key":"e_1_3_2_76_2","doi-asserted-by":"publisher","DOI":"10.1103\/PhysRevB.54.1703"},{"key":"e_1_3_2_77_2","doi-asserted-by":"publisher","DOI":"10.1002\/wcms.31"}],"container-title":["Science Advances"],"original-title":[],"language":"en","link":[{"URL":"https:\/\/www.science.org\/doi\/pdf\/10.1126\/sciadv.ads4018","content-type":"unspecified","content-version":"vor","intended-application":"similarity-checking"}],"deposited":{"date-parts":[[2025,4,17]],"date-time":"2025-04-17T10:31:41Z","timestamp":1744885901000},"score":1,"resource":{"primary":{"URL":"https:\/\/www.science.org\/doi\/10.1126\/sciadv.ads4018"}},"subtitle":[],"short-title":[],"issued":{"date-parts":[[2025,2,21]]},"references-count":76,"journal-issue":{"issue":"8","published-print":{"date-parts":[[2025,2,21]]}},"alternative-id":["10.1126\/sciadv.ads4018"],"URL":"https:\/\/doi.org\/10.1126\/sciadv.ads4018","relation":{},"ISSN":["2375-2548"],"issn-type":[{"value":"2375-2548","type":"electronic"}],"subject":[],"published":{"date-parts":[[2025,2,21]]},"assertion":[{"value":"2024-08-12","order":0,"name":"received","label":"Received","group":{"name":"publication_history","label":"Publication History"}},{"value":"2025-01-17","order":2,"name":"accepted","label":"Accepted","group":{"name":"publication_history","label":"Publication History"}},{"value":"2025-02-19","order":3,"name":"published","label":"Published","group":{"name":"publication_history","label":"Publication History"}}],"article-number":"eads4018"}}