{"status":"ok","message-type":"work","message-version":"1.0.0","message":{"indexed":{"date-parts":[[2026,10,23]],"date-time":"2026-10-23T19:47:31Z","timestamp":1792784851441,"version":"4.5.0"},"reference-count":35,"publisher":"American Chemical Society (ACS)","issue":"41","license":[{"start":{"date-parts":[[2026,10,8]],"date-time":"2026-10-08T00:00:00Z","timestamp":1791417600000},"content-version":"stm-asf","delay-in-days":0,"URL":"https:\/\/doi.org\/10.15223\/policy-029"},{"start":{"date-parts":[[2026,10,8]],"date-time":"2026-10-08T00:00:00Z","timestamp":1791417600000},"content-version":"stm-asf","delay-in-days":0,"URL":"https:\/\/doi.org\/10.15223\/policy-037"},{"start":{"date-parts":[[2026,10,8]],"date-time":"2026-10-08T00:00:00Z","timestamp":1791417600000},"content-version":"stm-asf","delay-in-days":0,"URL":"https:\/\/doi.org\/10.15223\/policy-045"}],"funder":[{"DOI":"10.13039\/501100012226","name":"Fundamental Research Funds for the Central Universities","doi-asserted-by":"publisher","award":["20720220011"],"award-info":[{"award-number":["20720220011"]}],"id":[{"id":"10.13039\/501100012226","id-type":"DOI","asserted-by":"publisher"}]},{"name":"National Key Basic Research Program of China","award":["2021YFA1500600"],"award-info":[{"award-number":["2021YFA1500600"]}]},{"name":"Strategic Priority Research Program of the Chinese Academy of Sciences","award":["XDB0600300"],"award-info":[{"award-number":["XDB0600300"]}],"id":[{"id":"https:\/\/ror.org\/034t30j35","id-type":"ROR","asserted-by":"crossref"}]},{"name":"New Cornerstone Science Foundation","award":["XPLORER PRIZE"],"award-info":[{"award-number":["XPLORER PRIZE"]}]},{"name":"CAS Project for Young Scientists in Basic Research","award":["YSBR-004"],"award-info":[{"award-number":["YSBR-004"]}]},{"name":"National Natural Science Foundation of China (NSFC)","award":["22325205"],"award-info":[{"award-number":["22325205"]}],"id":[{"id":"https:\/\/ror.org\/01h0zpd94","id-type":"ROR","asserted-by":"crossref"}]},{"name":"National Natural Science Foundation of China (NSFC)","award":["22688202"],"award-info":[{"award-number":["22688202"]}],"id":[{"id":"https:\/\/ror.org\/01h0zpd94","id-type":"ROR","asserted-by":"crossref"}]},{"name":"Open Research Fund of Suzhou Laboratory","award":["SZLAB-1608-2025-TS038"],"award-info":[{"award-number":["SZLAB-1608-2025-TS038"]}]}],"content-domain":{"domain":[],"crossmark-restriction":false},"short-container-title":[],"published-print":{"date-parts":[[2026,10,21]]},"abstract":"<jats:title>Abstract<\/jats:title>\n                  <jats:p>Constructing bifunctional catalysts with synergistic interfaces is a promising strategy to overcome the sluggish kinetics of the hydrogen evolution reaction (HER) in alkaline media, where interfacial proton transfer plays a critical role in the reaction kinetics. However, how bifunctional interfaces regulate the interfacial environment governing proton transfer remains poorly understood, particularly at the nanoscale. Here, using well-defined Pt\/Ni and Pt\/NiO model systems, we integrate spatially resolved scanning electrochemical microscopy, hydration force measurements, and ab initio molecular dynamics simulations across multiple length scales to establish a correlation among local HER kinetics, interfacial electrostatics, and hydration structure. Specifically, the Pt\/NiO-derived interface exhibits a lower potential of zero charge (PZC) that is closer to the HER operating potential together with a more interconnected interfacial hydrogen-bond network. In contrast, the Pt\/Ni-derived interface exhibits a higher PZC and a less-interconnected hydration structure. These results identify interfacial electrostatics and hydration organization within the electric double layer (EDL) as important factors governing the enhanced HER kinetics at bifunctional interfaces.<\/jats:p>","DOI":"10.1021\/jacs.6c12095","type":"journal-article","created":{"date-parts":[[2026,10,9]],"date-time":"2026-10-09T01:01:53Z","timestamp":1791507713000},"page":"44431-44439","source":"Crossref","is-referenced-by-count":0,"title":["Electric Double Layer\nOrganization of Proton-Transfer\nPathways Regulates Alkaline Hydrogen Evolution"],"prefix":"10.1021","volume":"148","author":[{"given":"Yuran","family":"Li","sequence":"first","affiliation":[{"name":"Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian National Laboratory for Clean Energy , , ,","place":["Dalian, China, 116023"]},{"name":"University of Chinese Academy of Sciences , ,","place":["Beijing, China, 100049"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Peimeng","family":"Qiu","sequence":"additional","affiliation":[{"name":"Wuhan University , , ,","place":["Wuhan, China, 430072"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhongrui","family":"Min","sequence":"additional","affiliation":[{"name":"Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian National Laboratory for Clean Energy , , ,","place":["Dalian, China, 116023"]},{"name":"University of Chinese Academy of Sciences , ,","place":["Beijing, China, 100049"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0000-4080-6592","authenticated-orcid":true,"given":"Fusai","family":"Sun","sequence":"additional","affiliation":[{"name":"Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian National Laboratory for Clean Energy , , ,","place":["Dalian, China, 116023"]},{"name":"University of Chinese Academy of Sciences , ,","place":["Beijing, China, 100049"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0003-9433-5521","authenticated-orcid":true,"given":"Ziyuan","family":"Wang","sequence":"additional","affiliation":[{"name":"Queens College , , , ,","place":["Flushing, New York, United States, 11367"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0001-0911-3111","authenticated-orcid":true,"given":"Junhao","family":"Cui","sequence":"additional","affiliation":[{"name":"Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian National Laboratory for Clean Energy , , ,","place":["Dalian, China, 116023"]},{"name":"University of Chinese Academy of Sciences , ,","place":["Beijing, China, 100049"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0006-3066-2250","authenticated-orcid":true,"given":"Chenwei","family":"Ni","sequence":"additional","affiliation":[{"name":"Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian National Laboratory for Clean Energy , , ,","place":["Dalian, China, 116023"]},{"name":"University of Chinese Academy of Sciences , ,","place":["Beijing, China, 100049"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-9301-7850","authenticated-orcid":true,"given":"Can","family":"Li","sequence":"additional","affiliation":[{"name":"Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian National Laboratory for Clean Energy , , ,","place":["Dalian, China, 116023"]},{"name":"University of Chinese Academy of Sciences , ,","place":["Beijing, China, 100049"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-6231-4521","authenticated-orcid":true,"given":"Xiuli","family":"Wang","sequence":"additional","affiliation":[{"name":"Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian National Laboratory for Clean Energy , , ,","place":["Dalian, China, 116023"]},{"name":"University of Chinese Academy of Sciences , ,","place":["Beijing, China, 100049"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9604-8778","authenticated-orcid":true,"given":"Tong","family":"Sun","sequence":"additional","affiliation":[{"name":"University of Science and Technology Beijing , , ,","place":["Beijing, China, 100083"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shengli","family":"Chen","sequence":"additional","affiliation":[{"name":"Wuhan University , , ,","place":["Wuhan, China, 430072"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-9828-6988","authenticated-orcid":true,"given":"Fengtao","family":"Fan","sequence":"additional","affiliation":[{"name":"Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian National Laboratory for Clean Energy , , ,","place":["Dalian, China, 116023"]},{"name":"University of Chinese Academy of Sciences , ,","place":["Beijing, China, 100049"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,10,8]]},"reference":[{"issue":"7","key":"2026102111080311700_cit1","doi-asserted-by":"publisher","first-page":"2255","DOI":"10.1039\/C4EE00440J","article-title":"New Insights into the Electrochemical\nHydrogen Oxidation and Evolution Reaction Mechanism","volume":"7","author":"Durst","year":"2014","journal-title":"Energy Environ. Sci."},{"issue":"6321","key":"2026102111080311700_cit2","doi-asserted-by":"publisher","DOI":"10.1126\/science.aad4998","article-title":"Combining Theory and Experiment in\nElectrocatalysis: Insights into Materials Design","volume":"355","author":"Seh","year":"2017","journal-title":"Science"},{"issue":"20","key":"2026102111080311700_cit3","doi-asserted-by":"publisher","first-page":"10253","DOI":"10.1039\/D4CS00370E","article-title":"Insights into the pH\nEffect on Hydrogen Electrocatalysis","volume":"53","author":"Cui","year":"2024","journal-title":"Chem. Soc.\nRev."},{"issue":"3","key":"2026102111080311700_cit4","doi-asserted-by":"publisher","first-page":"J23","DOI":"10.1149\/1.1856988","article-title":"Trends in the Exchange Current for\nHydrogen Evolution","volume":"152","author":"N\u00f8rskov","year":"2005","journal-title":"J. Electrochem. Soc."},{"key":"2026102111080311700_cit5","doi-asserted-by":"publisher","first-page":"1053","DOI":"10.1039\/tf9585401053","article-title":"The Rate of\nElectrolytic Hydrogen Evolution and the Heat of Adsorption of Hydrogen","volume":"54","author":"Parsons","year":"1958","journal-title":"Trans. Faraday Soc."},{"issue":"1","key":"2026102111080311700_cit6","doi-asserted-by":"publisher","first-page":"5848","DOI":"10.1038\/ncomms6848","article-title":"Correlating Hydrogen Oxidation and Evolution Activity on Platinum\nat Different pH with Measured Hydrogen Binding Energy","volume":"6","author":"Sheng","year":"2015","journal-title":"Nat. Commun."},{"issue":"4","key":"2026102111080311700_cit7","doi-asserted-by":"publisher","first-page":"17031","DOI":"10.1038\/nenergy.2017.31","article-title":"Interfacial Water\nReorganization\nas a pH-Dependent Descriptor of the Hydrogen Evolution Rate on Platinum\nElectrodes","volume":"2","author":"Ledezma-Yanez","year":"2017","journal-title":"Nat. Energy"},{"issue":"6060","key":"2026102111080311700_cit8","doi-asserted-by":"publisher","first-page":"1256","DOI":"10.1126\/science.1211934","article-title":"Enhancing Hydrogen\nEvolution Activity in Water Splitting by Tailoring Li+ -Ni(OH)2 -Pt Interfaces","volume":"334","author":"Subbaraman","year":"2011","journal-title":"Science"},{"issue":"6","key":"2026102111080311700_cit9","doi-asserted-by":"publisher","first-page":"550","DOI":"10.1038\/nmat3313","article-title":"Trends in Activity for the Water Electrolyser Reactions\non 3d M(Ni,Co,Fe,Mn) Hydr(Oxy)Oxide Catalysts","volume":"11","author":"Subbaraman","year":"2012","journal-title":"Nat. Mater."},{"issue":"10","key":"2026102111080311700_cit10","doi-asserted-by":"publisher","first-page":"900","DOI":"10.1038\/s41929-022-00846-8","article-title":"Hydrogen Bond Network\nConnectivity in the Electric\nDouble Layer Dominates the Kinetic pH Effect in Hydrogen Electrocatalysis\non Pt","volume":"5","author":"Li","year":"2022","journal-title":"Nat. Catal."},{"issue":"8","key":"2026102111080311700_cit11","doi-asserted-by":"publisher","first-page":"859","DOI":"10.1038\/s41560-023-01302-y","article-title":"Understanding Hydrogen\nElectrocatalysis by Probing the Hydrogen-Bond Network of Water at\nthe Electrified Pt\u2013Solution Interface","volume":"8","author":"Sun","year":"2023","journal-title":"Nat. Energy"},{"issue":"8","key":"2026102111080311700_cit12","doi-asserted-by":"publisher","first-page":"1022","DOI":"10.1038\/s41563-023-01584-3","article-title":"Amorphous Nickel Hydroxide\nShell Tailors Local Chemical\nEnvironment on Platinum Surface for Alkaline Hydrogen Evolution Reaction","volume":"22","author":"Wan","year":"2023","journal-title":"Nat. Mater."},{"issue":"31","key":"2026102111080311700_cit13","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202508239","article-title":"Anomalous pH-Dependence\nof Ru for Hydrogen Electrochemistry","volume":"64","author":"Fang","year":"2025","journal-title":"Angew.\nChem., Int. Ed."},{"issue":"14","key":"2026102111080311700_cit14","doi-asserted-by":"publisher","first-page":"9623","DOI":"10.1021\/jacs.3c12934","article-title":"Platinum Surface\nWater Orientation Dictates Hydrogen Evolution Reaction Kinetics in\nAlkaline Media","volume":"146","author":"Shah","year":"2024","journal-title":"J. Am. Chem. Soc."},{"issue":"1","key":"2026102111080311700_cit15","doi-asserted-by":"publisher","first-page":"7834","DOI":"10.1038\/s41467-024-52131-w","article-title":"Effect of Ion-Specific Water Structures\nat Metal Surfaces on Hydrogen Production","volume":"15","author":"Tian","year":"2024","journal-title":"Nat.\nCommun."},{"issue":"17","key":"2026102111080311700_cit16","doi-asserted-by":"publisher","first-page":"14122","DOI":"10.1021\/jacs.4c14511","article-title":"Electric-Double-Layer\nMechanism of Surface Oxophilicity in Regulating the Alkaline Hydrogen\nElectrocatalytic Kinetics","volume":"147","author":"Jiang","year":"2025","journal-title":"J. Am. Chem. Soc."},{"issue":"10","key":"2026102111080311700_cit17","doi-asserted-by":"publisher","first-page":"986","DOI":"10.1038\/s41929-025-01421-7","article-title":"Electrolyte\nEffects in Proton-Electron Transfer Reactions\nand Implications for Renewable Fuels and Chemicals Synthesis","volume":"8","author":"Sebastia\u0301n-Pascual","year":"2025","journal-title":"Nat. Catal."},{"issue":"6","key":"2026102111080311700_cit18","doi-asserted-by":"publisher","first-page":"678","DOI":"10.1038\/s41929-024-01156-x","article-title":"Edge Sites Dominate\nthe Hydrogen Evolution Reaction on Platinum Nanocatalysts","volume":"7","author":"Huang","year":"2024","journal-title":"Nat. Catal."},{"issue":"7857","key":"2026102111080311700_cit19","doi-asserted-by":"publisher","first-page":"67","DOI":"10.1038\/s41586-021-03454-x","article-title":"Correlative\nOperando\nMicroscopy of Oxygen Evolution Electrocatalysts","volume":"593","author":"Mefford","year":"2021","journal-title":"Nature"},{"issue":"35","key":"2026102111080311700_cit20","doi-asserted-by":"publisher","first-page":"31722","DOI":"10.1021\/jacs.5c08371","article-title":"In Situ Identification of Dynamic Active Sites in the Electrocatalytic\nNitrate Reduction Reaction","volume":"147","author":"Zhao","year":"2025","journal-title":"J. Am. Chem. Soc."},{"issue":"32","key":"2026102111080311700_cit21","doi-asserted-by":"publisher","first-page":"11561","DOI":"10.1039\/D2NR01807A","article-title":"Tailored Synthesis\nof Molecularly Thin Platinum Nanosheets Using Designed 2D Surfactant\nSolids","volume":"14","author":"Yamamoto","year":"2022","journal-title":"Nanoscale"},{"issue":"11","key":"2026102111080311700_cit22","doi-asserted-by":"publisher","first-page":"11522","DOI":"10.1021\/nn5057673","article-title":"Surface-Energy-Assisted\nPerfect Transfer of Centimeter-Scale Monolayer and Few-Layer MoS2 Films onto Arbitrary Substrates","volume":"8","author":"Gurarslan","year":"2014","journal-title":"ACS\nNano"},{"key":"2026102111080311700_cit23","doi-asserted-by":"publisher","first-page":"1","DOI":"10.1016\/j.jpowsour.2019.04.073","article-title":"Composition- and Shape-Controlled\nSynthesis of the PtNi Alloy Nanotubes\nwith Enhanced Activity and Durability toward Oxygen Reduction Reaction","volume":"429","author":"Fan","year":"2019","journal-title":"J. Power Sources"},{"issue":"27","key":"2026102111080311700_cit24","doi-asserted-by":"publisher","first-page":"17844","DOI":"10.1039\/C5CP02490K","article-title":"Electron Transfer\nKinetics on Natural Crystals of MoS2 and Graphite","volume":"17","author":"Velicky\u0301","year":"2015","journal-title":"Phys. Chem. Chem. Phys."},{"issue":"5","key":"2026102111080311700_cit25","doi-asserted-by":"publisher","first-page":"5209","DOI":"10.1021\/acs.chemrev.1c00176","article-title":"Contact Electrification at the Liquid\u2013Solid\nInterface","volume":"122","author":"Lin","year":"2022","journal-title":"Chem. Rev."},{"issue":"15","key":"2026102111080311700_cit26","doi-asserted-by":"publisher","first-page":"4211","DOI":"10.1002\/anie.201612183","article-title":"Hydrophobic\nWater Probed Experimentally at the Gold Electrode\/Aqueous Interface","volume":"56","author":"Tong","year":"2017","journal-title":"Angew. Chem., Int. Ed."},{"key":"2026102111080311700_cit27","unstructured":"Su, S.\n          \n          Atomic Force Microscopy\nResolved Semiconductor-Electrolyte Interface for Photocatalytic Water\nSplitting, Ph.D. Dissertation, University\nof Twente, 2023."},{"issue":"33","key":"2026102111080311700_cit28","doi-asserted-by":"publisher","first-page":"29977","DOI":"10.1021\/jacs.5c07325","article-title":"Tuning the Hydrogen Evolution Reaction\nActivity and Mechanism on Pt via Nano-Confinement of Interfacial Water","volume":"147","author":"Tao","year":"2025","journal-title":"J. Am. Chem. Soc."},{"issue":"3","key":"2026102111080311700_cit29","doi-asserted-by":"publisher","first-page":"2859","DOI":"10.1021\/acs.analchem.9b05502","article-title":"Mapping the Potential of Zero Charge\nand Electrocatalytic Activity of Metal\u2013Electrolyte Interface\nvia a Grain-by-Grain Approach","volume":"92","author":"Wang","year":"2020","journal-title":"Anal. Chem."},{"issue":"43","key":"2026102111080311700_cit30","doi-asserted-by":"publisher","first-page":"39181","DOI":"10.1021\/jacs.5c09493","article-title":"Manipulating Interfacial\nCharge Distribution\nfor Water Reduction","volume":"147","author":"Wu","year":"2025","journal-title":"J. Am. Chem. Soc."},{"issue":"1","key":"2026102111080311700_cit31","doi-asserted-by":"publisher","first-page":"1844","DOI":"10.1038\/s41467-025-56966-9","article-title":"Kinetic Cation\nEffect in Alkaline Hydrogen Electrocatalysis and Double Layer Proton\nTransfer","volume":"16","author":"Li","year":"2025","journal-title":"Nat. Commun."},{"key":"2026102111080311700_cit32","doi-asserted-by":"publisher","first-page":"36","DOI":"10.1016\/j.jelechem.2014.03.030","article-title":"Potential of Zero Charge\nof Glassy\nCarbon at Elevated Temperatures","volume":"724","author":"Zebardast","year":"2014","journal-title":"J. Electroanal.\nChem."},{"issue":"25","key":"2026102111080311700_cit33","doi-asserted-by":"publisher","first-page":"21672","DOI":"10.1021\/jacs.5c03433","article-title":"Cation-Driven Modulation\nof Interfacial Solvation Structures for Enhanced Alkaline Hydrogen\nOxidation Kinetics","volume":"147","author":"Men","year":"2025","journal-title":"J. Am. Chem. Soc."},{"issue":"24","key":"2026102111080311700_cit34","doi-asserted-by":"publisher","first-page":"246103","DOI":"10.1103\/PhysRevLett.90.246103","article-title":"Resolution of an\nAncient Surface Science Anomaly: Work Function Change Induced by N\nAdsorption on W {100}","volume":"90","author":"Michaelides","year":"2003","journal-title":"Phys. Rev. Lett."},{"issue":"15","key":"2026102111080311700_cit35","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202422062","article-title":"Platinum-Nickel Oxide Cluster-Cluster\nHeterostructure Enabling Fast\nHydrogen Evolution for Anion Exchange Membrane Water Electrolyzers","volume":"137","author":"Zheng","year":"2025","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.6c12095","content-type":"application\/pdf","content-version":"vor","intended-application":"unspecified"},{"URL":"https:\/\/pubs.acs.org\/jacsat\/article-pdf\/doi\/10.1021\/jacs.6c12095\/68794927\/jacs.6c12095.pdf","content-type":"application\/pdf","content-version":"vor","intended-application":"syndication"},{"URL":"https:\/\/pubs.acs.org\/jacsat\/article-pdf\/doi\/10.1021\/jacs.6c12095\/68794927\/jacs.6c12095.pdf","content-type":"unspecified","content-version":"vor","intended-application":"similarity-checking"}],"deposited":{"date-parts":[[2026,10,21]],"date-time":"2026-10-21T15:31:53Z","timestamp":1792596713000},"score":1,"resource":{"primary":{"URL":"https:\/\/pubs.acs.org\/jacsat\/article\/148\/41\/44431\/5447454\/Electric-Double-Layer-Organization-of-Proton"}},"subtitle":[],"short-title":[],"issued":{"date-parts":[[2026,10,8]]},"references-count":35,"journal-issue":{"issue":"41","published-online":{"date-parts":[[2026,10,8]]},"published-print":{"date-parts":[[2026,10,21]]}},"URL":"https:\/\/doi.org\/10.1021\/jacs.6c12095","relation":{},"ISSN":["0002-7863","1520-5126"],"issn-type":[{"value":"0002-7863","type":"print"},{"value":"1520-5126","type":"electronic"}],"subject":[],"published":{"date-parts":[[2026,10,8]]}}}