{"status":"ok","message-type":"work","message-version":"1.0.0","message":{"indexed":{"date-parts":[[2026,8,7]],"date-time":"2026-08-07T14:23:38Z","timestamp":1786112618470,"version":"build-2736575974"},"reference-count":54,"publisher":"American Chemical Society (ACS)","issue":"30","license":[{"start":{"date-parts":[[2026,7,20]],"date-time":"2026-07-20T00:00:00Z","timestamp":1784505600000},"content-version":"stm-asf","delay-in-days":0,"URL":"https:\/\/doi.org\/10.15223\/policy-029"},{"start":{"date-parts":[[2026,7,20]],"date-time":"2026-07-20T00:00:00Z","timestamp":1784505600000},"content-version":"stm-asf","delay-in-days":0,"URL":"https:\/\/doi.org\/10.15223\/policy-037"},{"start":{"date-parts":[[2026,7,20]],"date-time":"2026-07-20T00:00:00Z","timestamp":1784505600000},"content-version":"stm-asf","delay-in-days":0,"URL":"https:\/\/doi.org\/10.15223\/policy-045"}],"funder":[{"DOI":"10.13039\/501100018617","name":"Liaoning Revitalization Talents Program","doi-asserted-by":"publisher","award":["XLYC2203179"],"award-info":[{"award-number":["XLYC2203179"]}],"id":[{"id":"10.13039\/501100018617","id-type":"DOI","asserted-by":"publisher"}]},{"DOI":"10.13039\/501100001809","name":"National Natural Science Foundation of China (NSFC)","doi-asserted-by":"crossref","award":["22288101"],"award-info":[{"award-number":["22288101"]}],"id":[{"id":"10.13039\/501100001809","id-type":"DOI","asserted-by":"crossref"}]},{"DOI":"10.13039\/501100001809","name":"National Natural Science Foundation of China (NSFC)","doi-asserted-by":"crossref","award":["22302195"],"award-info":[{"award-number":["22302195"]}],"id":[{"id":"10.13039\/501100001809","id-type":"DOI","asserted-by":"crossref"}]},{"DOI":"10.13039\/501100001809","name":"National Natural Science Foundation of China (NSFC)","doi-asserted-by":"crossref","award":["22372156"],"award-info":[{"award-number":["22372156"]}],"id":[{"id":"10.13039\/501100001809","id-type":"DOI","asserted-by":"crossref"}]},{"DOI":"10.13039\/501100001809","name":"National Natural Science Foundation of China (NSFC)","doi-asserted-by":"crossref","award":["22502197"],"award-info":[{"award-number":["22502197"]}],"id":[{"id":"10.13039\/501100001809","id-type":"DOI","asserted-by":"crossref"}]}],"content-domain":{"domain":[],"crossmark-restriction":false},"short-container-title":[],"published-print":{"date-parts":[[2026,8,5]]},"abstract":"<jats:title>Abstract<\/jats:title>\n                  <jats:p>SAPO-34 is the benchmark catalyst for the methanol-to-olefins (MTO) process, yet its catalytic lifetime remains limited, attracting increasing attention from both academia and industry. Here, we identify a previously unrecognized origin of SAPO-34 deactivation: stacking disorder, which is a type of structural defect difficult to detect by conventional PXRD, particularly in nanosized crystals. By combining advanced three-dimensional electron diffraction (3D ED), integrated differential phase-contrast scanning transmission electron microscopy (iDPC-STEM), and electron ptychography based on four-dimensional (4D) STEM data, we uncover atomic-level hidden stacking disorders in SAPO-34 synthesized using the conventional tetraethylammonium (TEA+) as the organic structure directing agent (OSDA). These disorders promote the formation of smaller aei cages, thereby accelerating catalyst deactivation. Guided by these structural insights, we identify a larger OSDA, N,N,N-trimethyladamantan-1-aminium (TMAda+), that suppresses aei-cage formation and yields stacking-disorder-free SAPO-34 with a markedly extended MTO lifetime. Furthermore, to circumvent the high cost of TMAda+, we develop a series of low-cost amine OSDAs that reproduce its structure-directing behavior, yielding SAPO-34 catalysts free of stacking disorder and with MTO performance comparable to that of TMAda+-directed catalyst, as confirmed by 3D ED and iDPC-STEM characterization. Among these catalysts, SAPO-34 directed by N,N-dimethylcyclohexylamine shows the highest catalytic durability. This work establishes a structural design strategy for producing stacking-disorder-free SAPO-34 with substantially enhanced MTO stability.<\/jats:p>","DOI":"10.1021\/jacs.6c09745","type":"journal-article","created":{"date-parts":[[2026,7,20]],"date-time":"2026-07-20T21:25:54Z","timestamp":1784582754000},"page":"32595-32603","source":"Crossref","is-referenced-by-count":0,"title":["Revealing\nand Controlling Atomic-Scale Stacking Disorder\nin SAPO-34 for Enhanced MTO Performance"],"prefix":"10.1021","volume":"148","author":[{"given":"Xiaona","family":"Liu","sequence":"first","affiliation":[{"name":"Dalian Institute of Chemical Physics, Chinese Academy of Sciences , , , ,","place":["Dalian, Liaoning, China, 116023"]},{"name":"University of Chinese Academy of Sciences , ,","place":["Beijing, China, 100049"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shitai","family":"Li","sequence":"additional","affiliation":[{"name":"Dalian Institute of Chemical Physics, Chinese Academy of Sciences , , , ,","place":["Dalian, Liaoning, China, 116023"]},{"name":"University of Chinese Academy of Sciences , ,","place":["Beijing, China, 100049"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chao","family":"Ma","sequence":"additional","affiliation":[{"name":"Dalian Institute of Chemical Physics, Chinese Academy of Sciences , , , ,","place":["Dalian, Liaoning, China, 116023"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yuanhao","family":"Li","sequence":"additional","affiliation":[{"name":"Dalian Institute of Chemical Physics, Chinese Academy of Sciences , , , ,","place":["Dalian, Liaoning, China, 116023"]},{"name":"University of Chinese Academy of Sciences , ,","place":["Beijing, China, 100049"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ke","family":"Long","sequence":"additional","affiliation":[{"name":"Dalian Institute of Chemical Physics, Chinese Academy of Sciences , , , ,","place":["Dalian, Liaoning, China, 116023"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chenyang","family":"Nie","sequence":"additional","affiliation":[{"name":"Dalian Institute of Chemical Physics, Chinese Academy of Sciences , , , ,","place":["Dalian, Liaoning, China, 116023"]},{"name":"University of Chinese Academy of Sciences , ,","place":["Beijing, China, 100049"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Nana","family":"Yan","sequence":"additional","affiliation":[{"name":"Dalian Institute of Chemical Physics, Chinese Academy of Sciences , , , ,","place":["Dalian, Liaoning, China, 116023"]},{"name":"University of Chinese Academy of Sciences , ,","place":["Beijing, China, 100049"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-5392-3915","authenticated-orcid":true,"given":"Peng","family":"Guo","sequence":"additional","affiliation":[{"name":"Dalian Institute of Chemical Physics, Chinese Academy of Sciences , , , ,","place":["Dalian, Liaoning, China, 116023"]},{"name":"University of Chinese Academy of Sciences , ,","place":["Beijing, China, 100049"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7999-2940","authenticated-orcid":true,"given":"Zhongmin","family":"Liu","sequence":"additional","affiliation":[{"name":"Dalian Institute of Chemical Physics, Chinese Academy of Sciences , , , ,","place":["Dalian, Liaoning, China, 116023"]},{"name":"University of Chinese Academy of Sciences , ,","place":["Beijing, China, 100049"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,7,20]]},"reference":[{"issue":"3","key":"2026080511140282100_cit1","doi-asserted-by":"publisher","first-page":"1922","DOI":"10.1021\/acscatal.5b00007","article-title":"Methanol to Olefins (MTO): From Fundamentals\nto Commercialization","volume":"5","author":"Tian","year":"2015","journal-title":"ACS Catal."},{"issue":"14","key":"2026080511140282100_cit2","doi-asserted-by":"publisher","first-page":"11585","DOI":"10.1021\/jacs.4c12145","article-title":"Methanol to\nOlefins (MTO): Understanding and Regulating Dynamic Complex Catalysis","volume":"147","author":"Lin","year":"2025","journal-title":"J. Am. Chem. Soc."},{"issue":"50","key":"2026080511140282100_cit3","doi-asserted-by":"publisher","first-page":"1902181","DOI":"10.1002\/adma.201902181","article-title":"Recent Progress in\nMethanol-to-Olefins (MTO) Catalysts","volume":"31","author":"Yang","year":"2019","journal-title":"Adv. Mater."},{"issue":"9","key":"2026080511140282100_cit4","doi-asserted-by":"publisher","first-page":"nwad120","DOI":"10.1093\/nsr\/nwad120","article-title":"Cavity-Controlled\nMethanol Conversion over Zeolite Catalysts","volume":"10","author":"Zhang","year":"2023","journal-title":"Natl. Sci. Rev."},{"key":"2026080511140282100_cit5","unstructured":"Database of Zeolite Structure. http:\/\/www.iza-structure.org\/databases\/."},{"issue":"20","key":"2026080511140282100_cit6","doi-asserted-by":"publisher","first-page":"7569","DOI":"10.1039\/C6CY01461E","article-title":"A Low-Temperature\nApproach to Synthesize Low-Silica SAPO-34 Nanocrystals and Their Application\nin the Methanol-to-Olefins (MTO) Reaction","volume":"6","author":"Gao","year":"2016","journal-title":"Catal.\nSci. Technol."},{"issue":"36","key":"2026080511140282100_cit7","doi-asserted-by":"publisher","first-page":"4805","DOI":"10.1039\/D4CC01017E","article-title":"A Rapid and Eco-Friendly\nApproach for the Synthesis of Low-Silica SAPO-34 with Excellent MTO\nCatalytic Performance","volume":"60","author":"Zou","year":"2024","journal-title":"Chem. Commun."},{"issue":"46","key":"2026080511140282100_cit8","doi-asserted-by":"publisher","first-page":"21408","DOI":"10.1021\/jacs.2c10495","article-title":"Directional\nConstruction of Active Naphthalenic Species within SAPO-34 Crystals\ntoward More Efficient Methanol-to-Olefin Conversion","volume":"144","author":"Wang","year":"2022","journal-title":"J. Am. Chem. Soc."},{"key":"2026080511140282100_cit9","doi-asserted-by":"publisher","first-page":"219","DOI":"10.1016\/j.cattod.2013.04.031","article-title":"Effect of Silicon Content\non the Catalytic Behavior of Chabazite Type Silicoaluminophosphate\nin the Transformation of Methanol to Short Chain Olefins","volume":"213","author":"A\u0301lvaro-Mun\u0303oz","year":"2013","journal-title":"Catal. 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Res."},{"key":"2026080511140282100_cit12","doi-asserted-by":"publisher","first-page":"425","DOI":"10.1016\/j.jcat.2021.01.012","article-title":"Silicon Redistribution,\nAcid Site Loss and the Formation of a Core\u2013Shell Texture upon\nSteaming SAPO-34 and Their Impact on Catalytic Performance in the\nMethanol-to-Olefins (MTO) Reaction","volume":"395","author":"Minova","year":"2021","journal-title":"J. Catal."},{"issue":"1\u20132","key":"2026080511140282100_cit13","doi-asserted-by":"publisher","first-page":"193","DOI":"10.1016\/j.apcata.2009.04.044","article-title":"Size Control\nof SAPO-34 Crystals and Their Catalyst\nLifetime in the Methanol-to-Olefin Reaction","volume":"362","author":"Nishiyama","year":"2009","journal-title":"Appl. Catal., A"},{"issue":"39","key":"2026080511140282100_cit14","doi-asserted-by":"publisher","first-page":"19783","DOI":"10.1039\/C5TA04642D","article-title":"Synthesis\nof Tri-Level Hierarchical SAPO-34 Zeolite with Intracrystalline Micro\u2013Meso\u2013Macroporosity\nShowing Superior MTO Performance","volume":"3","author":"Sun","year":"2015","journal-title":"J. Mater.\nChem. A"},{"issue":"4","key":"2026080511140282100_cit15","doi-asserted-by":"publisher","first-page":"542","DOI":"10.1093\/nsr\/nwx103","article-title":"The State-of-the-Art\nSynthetic Strategies for SAPO-34\nZeolite Catalysts in Methanol-to-Olefin Conversion","volume":"5","author":"Sun","year":"2018","journal-title":"Natl. Sci. Rev."},{"key":"2026080511140282100_cit16","doi-asserted-by":"publisher","first-page":"55","DOI":"10.1016\/j.micromeso.2018.01.002","article-title":"Probing Locations of Organic Structure-Directing Agents (OSDAs) and\nHost-Guest Interactions in CHA -Type SAPO-34\/44","volume":"264","author":"Yan","year":"2018","journal-title":"Microporous Mesoporous Mater."},{"issue":"5","key":"2026080511140282100_cit17","doi-asserted-by":"publisher","first-page":"4236","DOI":"10.1039\/C5NJ02351C","article-title":"SAPO-34 Templated by\nDipropylamine and Diisopropylamine: Synthesis and Catalytic Performance\nin the Methanol to Olefin (MTO) Reaction","volume":"40","author":"Fan","year":"2016","journal-title":"New\nJ. Chem."},{"key":"2026080511140282100_cit18","doi-asserted-by":"publisher","first-page":"2003046","DOI":"10.3866\/PKU.WHXB202003046","article-title":"Acid Properties of SAPO-34 Molecular\nSieves with Different Si Contents Templated by Various Organic Structure-Directing\nAgents","volume":"38","author":"Wang","year":"2020","journal-title":"Acta Phys.-Chim. Sin."},{"issue":"12","key":"2026080511140282100_cit19","doi-asserted-by":"publisher","first-page":"4205","DOI":"10.1021\/cm504284x","article-title":"Nanoporous Intergrowths:\nHow Crystal Growth Dictates Phase Composition and Hierarchical Structure\nin the CHA\/AEI System","volume":"27","author":"Smith","year":"2015","journal-title":"Chem. Mater."},{"issue":"4","key":"2026080511140282100_cit20","doi-asserted-by":"publisher","first-page":"588","DOI":"10.1021\/cs400007v","article-title":"Mechanisms of the Deactivation\nof SAPO-34 Materials with Different Crystal Sizes Applied as MTO Catalysts","volume":"3","author":"Dai","year":"2013","journal-title":"ACS Catal."},{"issue":"8","key":"2026080511140282100_cit21","doi-asserted-by":"publisher","first-page":"7373","DOI":"10.1021\/acscatal.9b02487","article-title":"Methanol to Olefins\nReaction Route Based on Methylcyclopentadienes as Critical Intermediates","volume":"9","author":"Zhang","year":"2019","journal-title":"ACS Catal."},{"key":"2026080511140282100_cit22","doi-asserted-by":"publisher","first-page":"8","DOI":"10.1016\/j.jcat.2013.01.024","article-title":"Insights into the Reaction\nMechanism\nof Methanol-to-Olefins Conversion in HSAPO-34 from First Principles:\nAre Olefins Themselves the Dominating Hydrocarbon Pool Species?","volume":"301","author":"Wang","year":"2013","journal-title":"J. Catal."},{"issue":"7","key":"2026080511140282100_cit23","doi-asserted-by":"publisher","first-page":"1879","DOI":"10.1016\/S1872-2067(21)63990-6","article-title":"An Integrated Approach\nto the Key Parameters in Methanol-to-Olefins Reaction Catalyzed by\nMFI\/MEL Zeolite Materials","volume":"43","author":"Liu","year":"2022","journal-title":"Chin. J. Catal."},{"key":"2026080511140282100_cit24","doi-asserted-by":"publisher","first-page":"112201","DOI":"10.1016\/j.micromeso.2022.112201","article-title":"Sustainable\nSynthesis of AEI\/CHA Intergrowth Zeolites for Methanol-to-Olefins\nConversion","volume":"344","author":"Li","year":"2022","journal-title":"Microporous Mesoporous Mater."},{"issue":"1","key":"2026080511140282100_cit25","doi-asserted-by":"publisher","first-page":"2212","DOI":"10.1038\/s41467-021-22438-z","article-title":"Resolving Atomic SAPO-34\/18\nIntergrowth Architectures for Methanol Conversion by Identifying Light\nAtoms and Bonds","volume":"12","author":"Shen","year":"2021","journal-title":"Nat. Commun."},{"issue":"107","key":"2026080511140282100_cit26","doi-asserted-by":"publisher","first-page":"104985","DOI":"10.1039\/C6RA23048B","article-title":"Influence of Template\nContent on\nSelective Synthesis of SAPO-18, SAPO-18\/34 Intergrowth and SAPO-34\nMolecular Sieves Used for Methanol-to-Olefins Process","volume":"6","author":"Wang","year":"2016","journal-title":"RSC Adv."},{"key":"2026080511140282100_cit27","doi-asserted-by":"publisher","first-page":"151101","DOI":"10.1016\/j.cej.2024.151101","article-title":"Synergic Regulation\nof Crystalline Phase, Composition and Morphology of SAPO-34 via Metal\nAssistance and in Situ Etching Strategy","volume":"489","author":"Zhang","year":"2024","journal-title":"Chem.\nEng. J."},{"key":"2026080511140282100_cit28","doi-asserted-by":"publisher","first-page":"177716","DOI":"10.1016\/j.cej.2026.177716","article-title":"Triethylamine-Directed\nSynthesis of Pure-CHA Hierarchical\nSAPO-34 via Seed\/HF Coupling for Efficient Methanol-to-Olefin Catalysis","volume":"541","author":"Chen","year":"2026","journal-title":"Chem. Eng. J."},{"key":"2026080511140282100_cit29","doi-asserted-by":"publisher","first-page":"1","DOI":"10.1016\/j.apcata.2015.06.027","article-title":"CHA\/AEI Intergrowth\nMaterials as Catalysts for the\nMethanol-to-Olefins Process","volume":"505","author":"Smith","year":"2015","journal-title":"Appl. Catal., A"},{"issue":"22","key":"2026080511140282100_cit30","doi-asserted-by":"publisher","first-page":"23097","DOI":"10.1021\/jacs.6c05033","article-title":"Unraveling Zeolite Heterogeneity\nand Its Impact on Catalysis","volume":"148","author":"Xu","year":"2026","journal-title":"J. Am. Chem. 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Mater."},{"issue":"15","key":"2026080511140282100_cit36","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202217004","article-title":"ECNU-13: A High-Silica\nZeolite with Three-Dimensional and High-Connectivity Multi-Pore Structures\nfor Selective Alkene Cracking","volume":"62","author":"Peng","year":"2023","journal-title":"Angew. Chem.,\nInt. Ed."},{"issue":"6576","key":"2026080511140282100_cit37","doi-asserted-by":"publisher","first-page":"62","DOI":"10.1126\/science.abg3793","article-title":"Single-Walled Zeolitic\nNanotubes","volume":"375","author":"Korde","year":"2022","journal-title":"Science"},{"issue":"10","key":"2026080511140282100_cit38","doi-asserted-by":"publisher","first-page":"11089","DOI":"10.1021\/jacs.5c22724","article-title":"Artificial Intelligence Predicted\nOSDAs Enable Direct Synthesis of Interlayer-Expanded Zeolites","volume":"148","author":"Wang","year":"2026","journal-title":"J. Am. Chem. 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Soc."},{"issue":"15","key":"2026080511140282100_cit41","doi-asserted-by":"publisher","first-page":"10257","DOI":"10.1021\/jacs.4c01393","article-title":"Unraveling a Stable 16-Ring Aluminophosphate\nDNL-11 through Three-Dimensional Electron Diffraction for Atmospheric\nWater Harvesting","volume":"146","author":"Nie","year":"2024","journal-title":"J. Am. Chem. Soc."},{"issue":"4","key":"2026080511140282100_cit42","doi-asserted-by":"publisher","first-page":"100237","DOI":"10.1016\/j.cjsc.2024.100237","article-title":"Application\nof Three-Dimensional\nElectron Diffraction in Structure Determination of Zeolites","volume":"43","author":"Li","year":"2024","journal-title":"Chin. J. Struct. Chem."},{"issue":"4","key":"2026080511140282100_cit43","doi-asserted-by":"publisher","first-page":"1206","DOI":"10.1039\/D0SC05731B","article-title":"Three-Dimensional Electron Diffraction\nfor Porous Crystalline Materials: Structural Determination and Beyond","volume":"12","author":"Huang","year":"2021","journal-title":"Chem. Sci."},{"issue":"4","key":"2026080511140282100_cit44","doi-asserted-by":"publisher","first-page":"100235","DOI":"10.1016\/j.cjsc.2024.100235","article-title":"DNL-16: A New Zeolitic Layered Silicate Unraveled by\nThree-Dimensional Electron Diffraction","volume":"43","author":"Ma","year":"2024","journal-title":"Chin.\nJ. Struct. Chem."},{"issue":"43","key":"2026080511140282100_cit45","doi-asserted-by":"publisher","first-page":"13475","DOI":"10.1002\/anie.201707452","article-title":"CIT-9: A Fault-Free\nGmelinite Zeolite","volume":"56","author":"Dusselier","year":"2017","journal-title":"Angew. Chem., Int. Ed."},{"issue":"28","key":"2026080511140282100_cit46","doi-asserted-by":"publisher","first-page":"10519","DOI":"10.1021\/ja4043615","article-title":"SSZ-52 a Zeolite with\nan 18-Layer Aluminosilicate Framework Structure\nRelated to That of the DeNOx Catalyst Cu-SSZ-13","volume":"135","author":"Xie","year":"2013","journal-title":"J. Am. Chem. Soc."},{"key":"2026080511140282100_cit47","doi-asserted-by":"publisher","first-page":"157750","DOI":"10.1016\/j.cej.2024.157750","article-title":"Enhancing Hydrothermal\nStability of NH3-SCR Reaction over Cu-SSZ-52 Catalyst by Increasing\nSi\/Al Ratio","volume":"502","author":"Jiang","year":"2024","journal-title":"Chem. Eng. 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