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Nevertheless, a precise understanding of the multistep reaction network and the nature of the active sites remains elusive. We herein report a strategically designed series of model catalysts with systematically varied Mg\/Si ratios\u2500SiO2, 0.5MgO\u2013SiO2, 4MgO\u2013SiO2, and MgO\u2500enabling the unambiguous identification of active site structures. Through comprehensive characterization and kinetic evaluation using distinct feedstocks (ethanol, acetaldehyde, their mixtures, and crotyl alcohol), we decouple the complex reaction pathway and establish quantitative structure\u2013activity relationships for each key step: dehydrogenation, aldol condensation, and dehydration. The 4MgO\u2013SiO2 catalyst, comprising amorphous Mg2SiO4, possesses the highest density of basic sites and delivers the superior activity for ethanol dehydrogenation to acetaldehyde (0.087 \u03bcmol\u00b7g\u20131\u00b7s\u20131). In marked contrast, the 0.5MgO\u2013SiO2 catalyst, characterized by unique Si(OMg)(OH)(OSi)2 and Si(OMg)(OSi)3 structures, exhibits the highest concentration of acid sites. This specific acidic architecture drives exceptional performance in both acetaldehyde condensation to crotonaldehyde (0.865 \u03bcmol\u00b7g\u20131\u00b7s\u20131) and crotyl alcohol dehydration to 1,3-butadiene (7.355 \u03bcmol\u00b7g\u20131\u00b7s\u20131). Interestingly, even pure SiO2, with its distinct Si\u2013OH acid sites, shows notable dehydration activity (5.344 \u03bcmol\u00b7g\u20131\u00b7s\u20131), highlighting that both the acid site identity and density collectively govern dehydration activity. This work provides a novel mechanistic blueprint, demonstrating that ethanol-to-1,3-butadiene conversion follows a precise site-demand sequence: dehydrogenation is favored on strong bases, while condensation and dehydration are accelerated on tailored acid sites. These insights offer a clear strategy for the design of highly selective multifunctional catalysts for complex cascade reactions.<\/jats:p>","DOI":"10.1021\/acsomega.6c08013","type":"journal-article","created":{"date-parts":[[2026,8,12]],"date-time":"2026-08-12T17:02:12Z","timestamp":1786554132000},"page":"50602-50615","source":"Crossref","is-referenced-by-count":0,"title":["Insights into Active\nSites of Dehydrogenation\u2013Condensation\u2013Dehydration\nSteps in Ethanol-to-1,3-Butadiene Conversion over Tailored MgO\u2013SiO2 Catalysts"],"prefix":"10.1021","volume":"11","author":[{"given":"Zhefei","family":"Zhang","sequence":"first","affiliation":[{"name":"Beijing University of Chemical Technology , , ,","place":["Beijing, P. R. China, 100029"]},{"name":"The First Affiliated Hospital of Guangxi Medical University , , , ,","place":["Nanning, Guangxi Zhuang Autonomous, P. R. China, 530021"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8393-6589","authenticated-orcid":true,"given":"Qiangqiang","family":"Zhu","sequence":"additional","affiliation":[{"name":"Beijing University of Chemical Technology , , ,","place":["Beijing, P. R. China, 100029"]},{"name":"Sinopec Research Institute of Petroleum Processing , , ,","place":["Beijing, P. R. China, 100083"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5578-6747","authenticated-orcid":true,"given":"Bin","family":"Wang","sequence":"additional","affiliation":[{"name":"Beijing University of Chemical Technology , , ,","place":["Beijing, P. R. China, 100029"]},{"name":"Beijing Synthetic Bio-Manufacturing Technology Innovation Center , ,","place":["Beijing, P. R. China, 102209"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Honglin","family":"Ren","sequence":"additional","affiliation":[{"name":"Beijing Institute of Technology , , ,","place":["Beijing, P. R. China, 100081"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chunliang","family":"Shang","sequence":"additional","affiliation":[{"name":"Beijing Institute of Technology , , ,","place":["Beijing, P. R. China, 100081"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xinyi","family":"Tan","sequence":"additional","affiliation":[{"name":"Beijing Institute of Technology , , ,","place":["Beijing, P. R. China, 100081"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,8,12]]},"reference":[{"issue":"46","key":"2026083119150509000_cit1","doi-asserted-by":"publisher","first-page":"11980","DOI":"10.1002\/anie.201305058","article-title":"Shale Gas Revolution: An Opportunity\nfor the Production of Biobased Chemicals?","volume":"52","author":"Bruijnincx","year":"2013","journal-title":"Angew.\nChem., Int. 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Catal., B"},{"issue":"1","key":"2026083119150509000_cit5","doi-asserted-by":"publisher","first-page":"83","DOI":"10.3390\/catal14010083","article-title":"An Analysis\nof Fixed-Bed Catalytic\nReactors Performances for One-Stage Butadiene Synthesis from Ethanol","volume":"14","author":"Brosteanu","year":"2024","journal-title":"Catalysts"},{"issue":"4","key":"2026083119150509000_cit6","doi-asserted-by":"publisher","first-page":"363","DOI":"10.1038\/s41929-023-00945-0","article-title":"Origin of\nActive Sites on Silica\u2013Magnesia Catalysts and Control of Reactive\nEnvironment in the One-Step Ethanol-to-Butadiene Process","volume":"6","author":"Chung","year":"2023","journal-title":"Nat. Catal."},{"key":"2026083119150509000_cit7","doi-asserted-by":"publisher","DOI":"10.1016\/j.cattod.2024.115017","article-title":"Tuning Acid and\nBasic Features on\nMgxAlOy-SiO2 Impacted Ethanol Upgrading\nto 1,3-Butadiene","volume":"444","author":"Santos","year":"2025","journal-title":"Catal. 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Soc."},{"issue":"4","key":"2026083119150509000_cit23","doi-asserted-by":"publisher","first-page":"2760","DOI":"10.1021\/acscatal.8b00014","article-title":"Mechanistic\nInsights into One-Step Catalytic Conversion of Ethanol\nto Butadiene over Bifunctional Zn\u2013Y\/Beta Zeolite","volume":"8","author":"Yan","year":"2018","journal-title":"ACS Catal."},{"issue":"5","key":"2026083119150509000_cit24","doi-asserted-by":"publisher","first-page":"3703","DOI":"10.1021\/acscatal.7b00433","article-title":"Zeolite Structural\nConfinement Effects\nEnhance One-Pot Catalytic Conversion of Ethanol to Butadiene","volume":"7","author":"Dai","year":"2017","journal-title":"ACS Catal."},{"issue":"5","key":"2026083119150509000_cit25","doi-asserted-by":"publisher","first-page":"3333","DOI":"10.1021\/acscatal.2c06055","article-title":"Cascade Reaction\nof Ethanol to Butadiene over Ag-Promoted,\nSilica- or Zeolite-Supported Ta, Y, Pr, or La Oxide Catalysts","volume":"13","author":"Mamedov","year":"2023","journal-title":"ACS Catal."},{"issue":"17","key":"2026083119150509000_cit26","doi-asserted-by":"publisher","first-page":"7113","DOI":"10.1021\/acs.chemmater.3c01407","article-title":"Non-Hydrolytic\nSol\u2013Gel Routes to Bifunctional\nCu\u2013Ta\u2013SiO2 Catalysts for the Upgrading of\nEthanol to Butadiene","volume":"35","author":"Dochain","year":"2023","journal-title":"Chem. 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