{"status":"ok","message-type":"work","message-version":"1.0.0","message":{"indexed":{"date-parts":[[2026,10,16]],"date-time":"2026-10-16T22:42:55Z","timestamp":1792190575543,"version":"4.4.0"},"reference-count":37,"publisher":"American Chemical Society (ACS)","issue":"31","license":[{"start":{"date-parts":[[2026,7,31]],"date-time":"2026-07-31T00:00:00Z","timestamp":1785456000000},"content-version":"stm-asf","delay-in-days":0,"URL":"https:\/\/doi.org\/10.15223\/policy-029"},{"start":{"date-parts":[[2026,7,31]],"date-time":"2026-07-31T00:00:00Z","timestamp":1785456000000},"content-version":"stm-asf","delay-in-days":0,"URL":"https:\/\/doi.org\/10.15223\/policy-037"},{"start":{"date-parts":[[2026,7,31]],"date-time":"2026-07-31T00:00:00Z","timestamp":1785456000000},"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":["XLYC2202003"],"award-info":[{"award-number":["XLYC2202003"]}],"id":[{"id":"10.13039\/501100018617","id-type":"DOI","asserted-by":"publisher"}]},{"DOI":"10.13039\/501100009965","name":"Dalian Science and Technology Bureau","doi-asserted-by":"publisher","award":["2025RG01"],"award-info":[{"award-number":["2025RG01"]}],"id":[{"id":"10.13039\/501100009965","id-type":"DOI","asserted-by":"publisher"}]},{"DOI":"10.13039\/501100012226","name":"Fundamental Research Funds for the Central Universities","doi-asserted-by":"publisher","award":["DUT23LAB612"],"award-info":[{"award-number":["DUT23LAB612"]}],"id":[{"id":"10.13039\/501100012226","id-type":"DOI","asserted-by":"publisher"}]},{"DOI":"10.13039\/501100012226","name":"Fundamental Research Funds for the Central Universities","doi-asserted-by":"publisher","award":["DUT25Z2708"],"award-info":[{"award-number":["DUT25Z2708"]}],"id":[{"id":"10.13039\/501100012226","id-type":"DOI","asserted-by":"publisher"}]},{"DOI":"10.13039\/501100001809","name":"National Natural Science Foundation of China","doi-asserted-by":"publisher","award":["U24B20198"],"award-info":[{"award-number":["U24B20198"]}],"id":[{"id":"10.13039\/501100001809","id-type":"DOI","asserted-by":"publisher"}]}],"content-domain":{"domain":[],"crossmark-restriction":false},"short-container-title":[],"published-print":{"date-parts":[[2026,8,12]]},"abstract":"<jats:title>Abstract<\/jats:title>\n                  <jats:p>The electrocatalytic nitrite reduction reaction (eNO2\u2013RR) presents an extraordinary surge in clean yet green ammonia (NH3) synthesis due to mild operation and its promising compatibility with renewable energy sources. Nevertheless, the sluggish NO2\u2013 reaction kinetics and the competing hydrogen evolution reaction (HER) remain challenging for efficient NO2\u2013-to-NH3 electrosynthesis. Herein, we reveal a strong dependence of H2O structure on KCl concentration in the electrolyte and decouple the KCl-induced water disordering mechanism for efficient NH3 electrosynthesis. This disrupts the hydrogen-bond network of H2O and increases the proportion of K+-H2O species, thereby transforming an ordered proton-hopping network into a disordered environment. This ordering-to-disordering transition increases the activation entropy and lowers the activation enthalpy, leading to a reduction in the apparent free energy and enabling a 2.9-fold enhancement in NH3 production compared to the conventional electrolyte. The KCl\u2013water electrolyte exhibits an exceptional NH3 yield rate of 111.3 mg cm\u20132 h\u20131, a Faradaic efficiency of 99.6% at \u22120.5 V vs RHE, and stable operation for over 1000 h at 1 A cm\u20132. Multiscale theoretical simulations further confirm that the K+ ions suppress the HER by elevating the water dissociation barrier from 0.1 to 0.7 eV, while the Cl\u2013 ions lower the *NO-to-*NOH hydrogenation barrier, thereby promoting the eNO2\u2013RR kinetics. Moreover, the proposed KCl-induced H2O disordering mechanism for efficient eNO2\u2013RR is universal, delivering consistent performance gains across various catalysts.<\/jats:p>","DOI":"10.1021\/jacs.6c09584","type":"journal-article","created":{"date-parts":[[2026,8,4]],"date-time":"2026-08-04T14:04:25Z","timestamp":1785852265000},"page":"33598-33606","source":"Crossref","is-referenced-by-count":1,"title":["Mechanistic\nInsights into KCl-Induced Water Disordering\nfor Efficient Ammonia Electrosynthesis"],"prefix":"10.1021","volume":"148","author":[{"given":"Bingzhi","family":"Qian","sequence":"first","affiliation":[{"name":"Dalian University of Technology , , ,","place":["Dalian, China, 116024"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-3359-1970","authenticated-orcid":true,"given":"Chang","family":"Yu","sequence":"additional","affiliation":[{"name":"Dalian University of Technology , , ,","place":["Dalian, China, 116024"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yingbin","family":"Liu","sequence":"additional","affiliation":[{"name":"Dalian University of Technology , , ,","place":["Dalian, China, 116024"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Rulong","family":"Ma","sequence":"additional","affiliation":[{"name":"Dalian University of Technology , , ,","place":["Dalian, China, 116024"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhen","family":"Cai","sequence":"additional","affiliation":[{"name":"Dalian University of Technology , , ,","place":["Dalian, China, 116024"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Feng","family":"He","sequence":"additional","affiliation":[{"name":"Dalian University of Technology , , ,","place":["Dalian, China, 116024"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jieshan","family":"Qiu","sequence":"additional","affiliation":[{"name":"Beijing University of Chemical Technology , , ,","place":["Beijing, China, 100029"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,7,31]]},"reference":[{"issue":"7753","key":"2026081210082228800_cit1","doi-asserted-by":"publisher","first-page":"536","DOI":"10.1038\/s41586-019-1134-2","article-title":"Molybdenum-Catalysed\nAmmonia Production with Samarium Diiodide and Alcohols or Water","volume":"568","author":"Ashida","year":"2019","journal-title":"Nature"},{"issue":"5386","key":"2026081210082228800_cit2","doi-asserted-by":"publisher","first-page":"98","DOI":"10.1126\/science.282.5386.98","article-title":"Ammonia Synthesis\nat Atmospheric Pressure","volume":"282","author":"Marnellos","year":"1998","journal-title":"Science"},{"issue":"8010","key":"2026081210082228800_cit3","doi-asserted-by":"publisher","first-page":"92","DOI":"10.1038\/s41586-024-07276-5","article-title":"Long-Term\nContinuous Ammonia Electrosynthesis","volume":"629","author":"Li","year":"2024","journal-title":"Nature"},{"issue":"38","key":"2026081210082228800_cit4","doi-asserted-by":"publisher","first-page":"20711","DOI":"10.1002\/anie.202107858","article-title":"Schottky Barrier-Induced\nSurface Electric Field Boosts Universal Reduction of NOx\u2013 in Water to Ammonia","volume":"60","author":"Gao","year":"2021","journal-title":"Angew.\nChem., Int. Ed."},{"issue":"19","key":"2026081210082228800_cit5","doi-asserted-by":"publisher","first-page":"8849","DOI":"10.1039\/D5EE01513H","article-title":"A Hybrid Plasma-Electro-Membrane\nTriple Intensified System over PdNPs\/Fe\u2013N\u2013C\nfor Ammonium Fertilizer Synthesis","volume":"18","author":"Wang","year":"2025","journal-title":"Energy Environ.\nSci."},{"issue":"38","key":"2026081210082228800_cit6","doi-asserted-by":"publisher","DOI":"10.1002\/aenm.202202105","article-title":"Efficient Ammonia Production Beginning from Enhanced Air Activation","volume":"12","author":"Meng","year":"2022","journal-title":"Adv. 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Soc."},{"issue":"51","key":"2026081210082228800_cit23","doi-asserted-by":"publisher","first-page":"35305","DOI":"10.1021\/jacs.4c12858","article-title":"Controlling\nthe\nReaction Pathways of Mixed NOxHy Reactants in\nPlasma-Electrochemical Ammonia Synthesis","volume":"146","author":"Ge","year":"2024","journal-title":"J.\nAm. Chem. Soc."},{"issue":"5","key":"2026081210082228800_cit24","doi-asserted-by":"publisher","first-page":"402","DOI":"10.1038\/s41929-023-00951-2","article-title":"Ultralow Overpotential\nNitrate Reduction to Ammonia via a Three-Step\nRelay Mechanism","volume":"6","author":"Han","year":"2023","journal-title":"Nat. Catal."},{"issue":"26","key":"2026081210082228800_cit25","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202303327","article-title":"Enhancing\nElectrochemical Nitrate\nReduction to Ammonia over Cu Nanosheets via Facet Tandem Catalysis","volume":"62","author":"Fu","year":"2023","journal-title":"Angew. Chem., Int. Ed."},{"issue":"1","key":"2026081210082228800_cit26","doi-asserted-by":"publisher","DOI":"10.1038\/s41467-023-44469-4","article-title":"Spin Polarized\nFe1\u2013Ti Pairs for Highly Efficient Electroreduction\nNitrate to Ammonia","volume":"15","author":"Dai","year":"2024","journal-title":"Nat. Commun."},{"issue":"40","key":"2026081210082228800_cit27","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202410517","article-title":"Highly Stable\nPerovskite Oxides for\nElectrocatalytic Acidic NOx\u2013 Reduction\nStreamlining Ammonia Synthesis from Air","volume":"63","author":"Guo","year":"2024","journal-title":"Angew.\nChem., Int. Ed."},{"issue":"7","key":"2026081210082228800_cit28","doi-asserted-by":"publisher","first-page":"2991","DOI":"10.1039\/D3EE01301D","article-title":"Laser-Controlled Tandem Catalytic Sites of CuNi Alloys\nwith Ampere-Level Electrocatalytic Nitrate-to-Ammonia Reduction Activities\nfor Zn\u2013Nitrate Batteries","volume":"16","author":"Yu","year":"2023","journal-title":"Energy Environ.\nSci."},{"issue":"7","key":"2026081210082228800_cit29","doi-asserted-by":"publisher","first-page":"759","DOI":"10.1038\/s41565-022-01121-4","article-title":"Efficient Conversion of Low-Concentration\nNitrate Sources into Ammonia on a Ru-Dispersed Cu Nanowire Electrocatalyst","volume":"17","author":"Chen","year":"2022","journal-title":"Nat. Nanotechnol."},{"issue":"8","key":"2026081210082228800_cit30","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202417696","article-title":"Interfacial Water Regulation\nfor Nitrate Electroreduction to Ammonia\nat Ultralow Overpotentials","volume":"37","author":"Wan","year":"2025","journal-title":"Adv. Mater."},{"issue":"5160","key":"2026081210082228800_cit31","doi-asserted-by":"publisher","first-page":"826","DOI":"10.1126\/science.264.5160.826","article-title":"Surface\nVibrational Spectroscopic\nStudies of Hydrogen Bonding and Hydrophobicity","volume":"264","author":"Du","year":"1994","journal-title":"Science"},{"issue":"6470","key":"2026081210082228800_cit32","doi-asserted-by":"publisher","first-page":"444","DOI":"10.1038\/368444a0","article-title":"Voltage-Dependent\nOrdering of Water Molecules at an Electrode\u2013Electrolyte Interface","volume":"368","author":"Toney","year":"1994","journal-title":"Nature"},{"key":"2026081210082228800_cit33","doi-asserted-by":"publisher","first-page":"90","DOI":"10.1016\/j.cplett.2013.03.065","article-title":"Local Statistical\nInterpretation for Water Structure","volume":"568\u2013569","author":"Sun","year":"2013","journal-title":"Chem. Phys.\nLett."},{"issue":"14","key":"2026081210082228800_cit34","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202500167","article-title":"In-tandem\nElectrochemical Reduction of Nitrate to Ammonia on Ultrathin-Sheet-Assembled\nIron-Nickel Alloy Nanoflowers","volume":"64","author":"Chandra Majhi","year":"2025","journal-title":"Angew. Chem.,\nInt. Ed."},{"issue":"25","key":"2026081210082228800_cit35","doi-asserted-by":"publisher","first-page":"21432","DOI":"10.1021\/jacs.5c00400","article-title":"Selective Mass Accumulation at the Metal\u2013Polymer\nBridging Interface for Efficient Nitrate Electroreduction to Ammonia\nand Zn-Nitrate Batteries","volume":"147","author":"Chao","year":"2025","journal-title":"J. Am. Chem. Soc."},{"issue":"4","key":"2026081210082228800_cit36","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202523740","article-title":"Co1Zn Single-Atom Alloy Boosts Active Hydrogen Spillover\nfor Highly Efficient Electrosynthesis of Ammonia Over 2 A cm\u20132 Current Density","volume":"65","author":"Chen","year":"2026","journal-title":"Angew. Chem., Int. Ed."},{"key":"2026081210082228800_cit37","doi-asserted-by":"publisher","first-page":"1032","DOI":"10.1038\/s41929-024-01200-w","article-title":"Electrochemical\nNitrate Reduction to Ammonia with Cation Shuttling in a Solid Electrolyte\nReactor","volume":"7","author":"Chen","year":"2024","journal-title":"Nat. Catal."}],"container-title":["Journal of the American\nChemical Society"],"original-title":[],"language":"en","link":[{"URL":"https:\/\/pubs.acs.org\/doi\/pdf\/10.1021\/jacs.6c09584","content-type":"application\/pdf","content-version":"vor","intended-application":"unspecified"},{"URL":"https:\/\/pubs.acs.org\/jacsat\/article-pdf\/148\/31\/33598\/66351207\/jacs.6c09584.pdf","content-type":"application\/pdf","content-version":"vor","intended-application":"syndication"},{"URL":"https:\/\/pubs.acs.org\/jacsat\/article-pdf\/148\/31\/33598\/66351207\/jacs.6c09584.pdf","content-type":"unspecified","content-version":"vor","intended-application":"similarity-checking"}],"deposited":{"date-parts":[[2026,8,12]],"date-time":"2026-08-12T14:23:16Z","timestamp":1786544596000},"score":1,"resource":{"primary":{"URL":"https:\/\/pubs.acs.org\/jacsat\/article\/148\/31\/33598\/5238097\/Mechanistic-Insights-into-KCl-Induced-Water"}},"subtitle":[],"short-title":[],"issued":{"date-parts":[[2026,7,31]]},"references-count":37,"journal-issue":{"issue":"31","published-online":{"date-parts":[[2026,7,31]]},"published-print":{"date-parts":[[2026,8,12]]}},"URL":"https:\/\/doi.org\/10.1021\/jacs.6c09584","relation":{},"ISSN":["0002-7863","1520-5126"],"issn-type":[{"value":"0002-7863","type":"print"},{"value":"1520-5126","type":"electronic"}],"subject":[],"published":{"date-parts":[[2026,7,31]]}}}