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The active metals employed in catalysts are predominantly presented as zero-dimensional nanoparticles, which limits their capacity to fully exploit atoms and electrons, resulting in unsatisfactory activity. Herein, we present triangular Ru nanosheet that features a two-dimensional structure characterized by a hexagonal close-packed atomic arrangement. The thickness of the Ru nanosheet is further tailored down to angstrom level, yielding Ru metallene. In contrast to Ru nanoparticles or regular nanosheet, our studies demonstrate that the unique geometric configuration of Ru metallene substantially stabilizes metallic Ru0 active sites enriched with abundant 4d electrons. Therefore, atomically thin Ru metallene delivers a high NH3 synthesis rate of 70.7 mmol gcat\u20131 h\u20131 at 400 \u00b0C and 1 MPa, surpassing Ru nanoparticles or nanosheets. This synthetic approach is broadly applicable to other transition metals (e.g., Fe and Mo). This work provides a new route for angstrom-level geometric engineering for NH3 synthesis catalysts.<\/jats:p>","DOI":"10.1021\/jacs.6c12661","type":"journal-article","created":{"date-parts":[[2026,8,22]],"date-time":"2026-08-22T09:57:50Z","timestamp":1787392670000},"page":"37330-37341","source":"Crossref","is-referenced-by-count":1,"title":["Geometry-Dependent\nElectronic Structure for Enhanced\nAmmonia Synthesis: From Nanoparticle to Nanosheet and Metallene"],"prefix":"10.1021","volume":"148","author":[{"given":"Yangyu","family":"Zhang","sequence":"first","affiliation":[{"name":"Fuzhou University , , ,","place":["Fuzhou, China, 350002"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7143-2658","authenticated-orcid":true,"given":"Mingbin","family":"Gao","sequence":"additional","affiliation":[{"name":"Xiamen University , , ,","place":["Xiamen, China, 361005"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jiaxin","family":"Li","sequence":"additional","affiliation":[{"name":"Fuzhou University , , ,","place":["Fuzhou, China, 350002"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-9233-4133","authenticated-orcid":true,"given":"Yanliang","family":"Zhou","sequence":"additional","affiliation":[{"name":"Fuzhou University , , ,","place":["Fuzhou, China, 350002"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Lirong","family":"Zheng","sequence":"additional","affiliation":[{"name":"Chinese Academy of Sciences , , ,","place":["Beijing, China, 100049"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4597-2359","authenticated-orcid":true,"given":"Xiuyun","family":"Wang","sequence":"additional","affiliation":[{"name":"Fuzhou University , , ,","place":["Fuzhou, China, 350002"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-0081-0367","authenticated-orcid":true,"given":"Lilong","family":"Jiang","sequence":"additional","affiliation":[{"name":"Fuzhou University , , ,","place":["Fuzhou, China, 350002"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,8,21]]},"reference":[{"issue":"6689","key":"2026090312092625900_cit1","doi-asserted-by":"publisher","first-page":"1357","DOI":"10.1126\/science.adn0558","article-title":"Spin-Mediated Promotion of Co Catalysts\nfor Ammonia Synthesis","volume":"383","author":"Zhang","year":"2024","journal-title":"Science"},{"issue":"3","key":"2026090312092625900_cit2","doi-asserted-by":"publisher","first-page":"248","DOI":"10.1038\/s41929-025-01302-z","article-title":"Electron and\nProton Storage on Separate Ru and BaO Domains Mediated by Conductive\nLow-Work-Function Carbon to Accelerate Ammonia Synthesis","volume":"8","author":"Baik","year":"2025","journal-title":"Nat. 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B"},{"key":"2026090312092625900_cit22","doi-asserted-by":"publisher","DOI":"10.1016\/j.jre.2025.09.030","article-title":"Thermal Stability of Ru-based Catalysts\nfor Soot Oxidation: Strong Metal-Support Interactions and Reaction\nScenarios","author":"Zheng","year":"2025","journal-title":"J. Rare Earths"},{"issue":"16","key":"2026090312092625900_cit23","doi-asserted-by":"publisher","first-page":"6107","DOI":"10.1021\/ja311848e","article-title":"CO Chemisorption and\nDissociation at High Coverages during CO Hydrogenation on Ru Catalysts","volume":"135","author":"Loveless","year":"2013","journal-title":"J. Am. Chem. Soc."},{"key":"2026090312092625900_cit24","doi-asserted-by":"publisher","first-page":"248","DOI":"10.1016\/j.cej.2018.09.166","article-title":"Does Shaping\nCatalysts Modify Active Phase Sites? A Comprehensive In Situ FTIR Spectroscopic Study on the Performance of a Model Ru\/Al2O3 Catalyst for the CO Methanation","volume":"357","author":"Bobadilla","year":"2019","journal-title":"Chem. Eng. J."},{"issue":"3","key":"2026090312092625900_cit25","doi-asserted-by":"publisher","first-page":"222","DOI":"10.1016\/S0169-4332(03)00146-6","article-title":"XPS, FTIR\nand TPR characterization of Ru\/Al2O3 catalysts","volume":"210","author":"Mazzieri","year":"2003","journal-title":"Appl. Surf. Sci."},{"issue":"39","key":"2026090312092625900_cit26","doi-asserted-by":"publisher","first-page":"15786","DOI":"10.1021\/ja207409q","article-title":"Understanding the Electronic\nStructure of 4d Metal Complexes: From Molecular Spinors to L-Edge\nSpectra of a di-Ru Catalyst","volume":"133","author":"Alperovich","year":"2011","journal-title":"J. Am. Chem. Soc."},{"issue":"12","key":"2026090312092625900_cit27","doi-asserted-by":"publisher","first-page":"8725","DOI":"10.1063\/1.461208","article-title":"Ru L-edge X-ray Absorption Studies\nof the Formation of Ru\u2013Cu Bimetallic Aggregates on Cu(100)","volume":"95","author":"Sham","year":"1991","journal-title":"J. Chem. Phys."},{"issue":"12","key":"2026090312092625900_cit28","doi-asserted-by":"publisher","first-page":"3970","DOI":"10.1021\/jacs.6b00124","article-title":"Water Durable Electride Y5Si3: Electronic Structure and Catalytic Activity for Ammonia\nSynthesis","volume":"138","author":"Lu","year":"2016","journal-title":"J. Am. Chem. Soc."},{"issue":"1","key":"2026090312092625900_cit29","doi-asserted-by":"publisher","first-page":"3958","DOI":"10.1038\/s41467-022-31660-2","article-title":"Subnanometric\nRu Clusters\nwith Upshifted D Band Center Improve performance for alkaline hydrogen\nevolution reaction","volume":"13","author":"Hu","year":"2022","journal-title":"Nat. Commun."},{"issue":"11","key":"2026090312092625900_cit30","doi-asserted-by":"publisher","first-page":"2410313","DOI":"10.1002\/advs.202410313","article-title":"Ammonia Synthesis\nOver an Iron Catalyst with an Inverse Structure","volume":"12","author":"Hattori","year":"2025","journal-title":"Adv. Sci."},{"issue":"51","key":"2026090312092625900_cit31","doi-asserted-by":"publisher","first-page":"16655","DOI":"10.1021\/jacs.6b08697","article-title":"Increased Back-Bonding Explains Step-Edge\nReactivity and Particle Size Effect for CO Activation on Ru Nanoparticles","volume":"138","author":"Foppa","year":"2016","journal-title":"J. Am. Chem. 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China Chem."},{"issue":"13","key":"2026090312092625900_cit35","doi-asserted-by":"publisher","first-page":"2415978","DOI":"10.1002\/adma.202415978","article-title":"2D Metastable-Phase\nHafnium Oxide Triggers Hydrogen Spillover for Boosting Hydrogen Production","volume":"37","author":"Wang","year":"2025","journal-title":"Adv. Mater."},{"issue":"19","key":"2026090312092625900_cit36","doi-asserted-by":"publisher","first-page":"3060","DOI":"10.1021\/acs.accounts.5c00501","article-title":"Unlocking Hydrogen\nSpillover: Dynamic Behavior and Advanced Applications","volume":"58","author":"Shun","year":"2025","journal-title":"Acc. Chem. 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Sci."},{"issue":"22","key":"2026090312092625900_cit42","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202404258","article-title":"Regulated Dual Defects\nof Bridging Organic and Terminal Inorganic Ligands in Iron-based Metal-Organic\nFramework Nodes for Efficient Photocatalytic Ammonia Synthesis","volume":"63","author":"Wang","year":"2024","journal-title":"Angew. Chem., Int. Ed."}],"container-title":["Journal of the American\nChemical Society"],"original-title":[],"language":"en","link":[{"URL":"https:\/\/pubs.acs.org\/doi\/pdf\/10.1021\/jacs.6c12661","content-type":"application\/pdf","content-version":"vor","intended-application":"unspecified"},{"URL":"https:\/\/pubs.acs.org\/jacsat\/article-pdf\/148\/34\/37330\/66981764\/jacs.6c12661.pdf","content-type":"application\/pdf","content-version":"vor","intended-application":"syndication"},{"URL":"https:\/\/pubs.acs.org\/jacsat\/article-pdf\/148\/34\/37330\/66981764\/jacs.6c12661.pdf","content-type":"unspecified","content-version":"vor","intended-application":"similarity-checking"}],"deposited":{"date-parts":[[2026,9,3]],"date-time":"2026-09-03T16:19:57Z","timestamp":1788452397000},"score":1,"resource":{"primary":{"URL":"https:\/\/pubs.acs.org\/jacsat\/article\/148\/34\/37330\/5285159\/Geometry-Dependent-Electronic-Structure-for"}},"subtitle":[],"short-title":[],"issued":{"date-parts":[[2026,8,21]]},"references-count":42,"journal-issue":{"issue":"34","published-online":{"date-parts":[[2026,8,21]]},"published-print":{"date-parts":[[2026,9,2]]}},"URL":"https:\/\/doi.org\/10.1021\/jacs.6c12661","relation":{},"ISSN":["0002-7863","1520-5126"],"issn-type":[{"value":"0002-7863","type":"print"},{"value":"1520-5126","type":"electronic"}],"subject":[],"published":{"date-parts":[[2026,8,21]]}}}