{"status":"ok","message-type":"work","message-version":"1.0.0","message":{"indexed":{"date-parts":[[2026,9,28]],"date-time":"2026-09-28T13:00:22Z","timestamp":1790600422759,"version":"4.1.0"},"reference-count":75,"publisher":"American Chemical Society (ACS)","issue":"9","license":[{"start":{"date-parts":[[2026,8,31]],"date-time":"2026-08-31T00:00:00Z","timestamp":1788134400000},"content-version":"vor","delay-in-days":0,"URL":"https:\/\/creativecommons.org\/licenses\/by\/4.0\/"}],"funder":[{"DOI":"10.13039\/100006151","name":"Basic Energy Sciences","doi-asserted-by":"publisher","award":["DE-SC0022053"],"award-info":[{"award-number":["DE-SC0022053"]}],"id":[{"id":"10.13039\/100006151","id-type":"DOI","asserted-by":"publisher"}]},{"DOI":"10.13039\/100000001","name":"National Science Foundation","doi-asserted-by":"publisher","id":[{"id":"10.13039\/100000001","id-type":"DOI","asserted-by":"publisher"}]}],"content-domain":{"domain":[],"crossmark-restriction":false},"short-container-title":[],"published-print":{"date-parts":[[2026,9,28]]},"abstract":"<jats:title>Abstract<\/jats:title>\n                  <jats:p>Hydrogen spillover occurs when H2 adsorbs on an active metal and is then transferred to a reducible metal oxide. While spillover is involved in many catalytic reactions, fundamental studies of spillover have been limited by the paucity of experimental methods available to study it. Here, we develop an experimental temperature-programmed reduction (TPR) protocol to rapidly compare spillover from different metals (Pt, Pd, Au ) onto P25 titania, using MnOx reduction probe reaction. X-ray photoelectron and UV\u2013visible spectroscopies indicated reduction to MnO in the presence and absence of active metals, and quantitative H2 consumption measurements were consistent across all samples. Observed MnOx reduction temperatures, which decrease by shifting as much as 150 \u00b0C, depend strongly on the metal loading and confirm H2 activation occurs at metal sites. Adding only 300 ppm Au caused the Kissinger apparent activation energy to decrease from 55 to &amp;lt;10 kJ\/mol. Comparisons across metals and loadings indicate that MnOx reduction is limited by H2 activation only at very low metal loadings and temperatures. Gold induces the largest shift in MnOx reduction, indicating that it is the most competent spillover metal under these conditions. At moderately higher loadings (\u22651 site\/100 nm2), Pt and Au become equivalent, signaling that MnOx reduction is no longer limited by H2 activation at higher metal loadings. Palladium is moderately slower, consistent with the generation of a PdHx phase at low temperature. At higher active site loadings, MnOx reduction depends primarily on the surface concentration of spillover H, providing a simple and useful approach for comparing catalysts.<\/jats:p>","DOI":"10.1021\/jacsau.6c00822","type":"journal-article","created":{"date-parts":[[2026,9,3]],"date-time":"2026-09-03T04:29:53Z","timestamp":1788409793000},"page":"5179-5189","source":"Crossref","is-referenced-by-count":1,"title":["Hydrogen Spillover\nfrom Pt, Pd, and Au Evaluated with\nMnO\n                    <i>x<\/i>\n                    Temperature-Programmed Reduction"],"prefix":"10.1021","volume":"6","author":[{"ORCID":"https:\/\/orcid.org\/0009-0002-8085-7719","authenticated-orcid":true,"given":"Mohammad","family":"Hamidizirasefi","sequence":"first","affiliation":[{"name":"The Pennsylvania State University , , , ,","place":["University Park, Pennsylvania, United States, 16802"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Audrey M.","family":"Battiste","sequence":"additional","affiliation":[{"name":"The Pennsylvania State University , , , ,","place":["University Park, Pennsylvania, United States, 16802"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Angela","family":"Pathickal Abraham","sequence":"additional","affiliation":[{"name":"The Pennsylvania State University , , , ,","place":["University Park, Pennsylvania, United States, 16802"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0003-3337-2388","authenticated-orcid":true,"given":"Andersen P.","family":"Dimon","sequence":"additional","affiliation":[{"name":"The Pennsylvania State University , , , ,","place":["University Park, Pennsylvania, United States, 16802"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8621-0361","authenticated-orcid":true,"given":"Bert D.","family":"Chandler","sequence":"additional","affiliation":[{"name":"The Pennsylvania State University , , , ,","place":["University Park, Pennsylvania, United States, 16802"]},{"name":"The Pennsylvania State University , , , ,","place":["University Park, Pennsylvania, United States, 16802"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,8,31]]},"reference":[{"issue":"2","key":"2026092808091423000_cit1","doi-asserted-by":"publisher","first-page":"411","DOI":"10.1021\/j100784a503","article-title":"Particle to\nParticle Migration of Hydrogen Atoms on Platinum\u2500Alumina Catalysts\nfrom Particle to Neighboring Particles","volume":"68","author":"Khoobiar","year":"1964","journal-title":"J. Phys.\nChem. A"},{"issue":"10","key":"2026092808091423000_cit2","doi-asserted-by":"publisher","first-page":"2753","DOI":"10.1021\/j100792a700","article-title":"Journal of Discussion of Robell,\nA. J.: Surface Diffusion of Hydrogen on Carbon","volume":"68","author":"Van Nordstrand","year":"1964","journal-title":"J. Phys. Chem. A"},{"issue":"1_4","key":"2026092808091423000_cit3","doi-asserted-by":"publisher","first-page":"171","DOI":"10.1524\/zpch.1969.64.1_4.171","article-title":"Adlineation, Portholes and Spillover","volume":"64","author":"Boudart","year":"1969","journal-title":"Z. Phys. Chem."},{"issue":"5785","key":"2026092808091423000_cit4","doi-asserted-by":"publisher","first-page":"332","DOI":"10.1126\/science.1128383","article-title":"Chemoselective Hydrogenation of Nitro\nCompounds with Supported Gold\nCatalysts","volume":"313","author":"Corma","year":"2006","journal-title":"Science"},{"issue":"16","key":"2026092808091423000_cit5","doi-asserted-by":"publisher","first-page":"20474","DOI":"10.1021\/acsami.3c00456","article-title":"Hydrogen Spillover-Accelerated\nSelective Hydrogenation on WO3 with ppm-Level Pd","volume":"15","author":"Sun","year":"2023","journal-title":"ACS Appl. Mater. Interfaces"},{"issue":"13","key":"2026092808091423000_cit6","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202422585","article-title":"Intensifying Interfacial\nReverse Hydrogen Spillover for Boosted Electrocatalytic Nitrate Reduction\nto Ammonia","volume":"64","author":"Ouyang","year":"2025","journal-title":"Angew. Chem., Int. Ed."},{"issue":"19","key":"2026092808091423000_cit7","doi-asserted-by":"publisher","DOI":"10.1002\/anie.9657522","article-title":"Harnessing Support-Dependent\nHydrogen Spillover for Ni-Based CO2 Hydrogenation","volume":"65","author":"Shun","year":"2026","journal-title":"Angew. Chem."},{"issue":"7","key":"2026092808091423000_cit8","doi-asserted-by":"publisher","first-page":"6203","DOI":"10.1021\/acscatal.7b04469","article-title":"Low-Temperature CO2Methanation over CeO2-Supported\nRu Single Atoms, Nanoclusters, and Nanoparticles Competitively Tuned\nby Strong Metal\u2013Support Interactions and H-Spillover Effect","volume":"8","author":"Guo","year":"2018","journal-title":"ACS Catal."},{"key":"2026092808091423000_cit9","doi-asserted-by":"publisher","DOI":"10.1016\/j.apcatb.2021.120590","article-title":"Improving methanol selectivity in\nCO2 hydrogenation by tuning the distance of Cu on catalyst","volume":"298","author":"Cui","year":"2021","journal-title":"Appl. Catal., B"},{"issue":"11","key":"2026092808091423000_cit10","doi-asserted-by":"publisher","first-page":"1062","DOI":"10.1038\/s41929-023-01040-0","article-title":"Generation\nof oxide surface patches promoting H-spillover in Ru\/(TiOx)MnO catalysts\nenables CO2 reduction to CO","volume":"6","author":"Kang","year":"2023","journal-title":"Nat. Catal."},{"issue":"11","key":"2026092808091423000_cit11","doi-asserted-by":"publisher","first-page":"3579","DOI":"10.1007\/s40843-024-3011-6","article-title":"Pt single atoms in oxygen vacancies\nboost reverse water-gas shift reaction by enhancing hydrogen spillover","volume":"67","author":"Kang","year":"2024","journal-title":"Sci. China Mater."},{"key":"2026092808091423000_cit12","doi-asserted-by":"publisher","first-page":"27","DOI":"10.1016\/j.cattod.2015.12.019","article-title":"v. Hydrogen spillover\nin the Fischer\u2013Tropsch synthesis: An analysis of gold as a\npromoter for cobalt\u2013alumina catalysts","volume":"275","author":"Nabaho","year":"2016","journal-title":"Catal. Today"},{"issue":"18","key":"2026092808091423000_cit13","doi-asserted-by":"publisher","first-page":"11857","DOI":"10.1021\/acscatal.3c03230","article-title":"Effect of Hydrogen\nSpillover on the Ru\/TiO2-Catalyzed Guaiacol Hydrodeoxygenation: Rutile\nvs Anatase TiO2","volume":"13","author":"Kim","year":"2023","journal-title":"ACS Catal."},{"issue":"40","key":"2026092808091423000_cit14","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202208237","article-title":"Hydrogen Spillover\nand Its Relation to Hydrogenation: Observations on Structurally Defined\nSingle-Atom Sites**","volume":"61","author":"Hu\u0308lsey","year":"2022","journal-title":"Angew. Chem., Int. Ed."},{"issue":"6660","key":"2026092808091423000_cit15","doi-asserted-by":"publisher","first-page":"886","DOI":"10.1126\/science.adi3416","article-title":"Tandem propane dehydrogenation and surface oxidation catalysts for\nselective propylene synthesis","volume":"381","author":"Wang","year":"2023","journal-title":"Science"},{"issue":"5","key":"2026092808091423000_cit16","doi-asserted-by":"publisher","first-page":"3159","DOI":"10.1021\/acscatal.0c05567","article-title":"Spillover in Heterogeneous Catalysis: New Insights\nand Opportunities","volume":"11","author":"Xiong","year":"2021","journal-title":"ACS Catal."},{"issue":"6","key":"2026092808091423000_cit17","doi-asserted-by":"publisher","first-page":"1161","DOI":"10.1016\/j.gee.2022.01.013","article-title":"Magic of hydrogen spillover: Understanding\nand application","volume":"7","author":"Shen","year":"2022","journal-title":"Green Energy Environ."},{"key":"2026092808091423000_cit18","doi-asserted-by":"publisher","DOI":"10.1016\/j.cej.2023.144691","article-title":"Hydrogen spillover\nas a promising strategy for boosting heterogeneous catalysis and hydrogen\nstorage","volume":"471","author":"Li","year":"2023","journal-title":"Chem. Eng. J."},{"issue":"2","key":"2026092808091423000_cit19","doi-asserted-by":"publisher","first-page":"268","DOI":"10.1039\/b807957a","article-title":"New sorbents for\nhydrogen storage by hydrogen spillover\u2500a\nreview","volume":"1","author":"Wang","year":"2008","journal-title":"Energy Environ. Sci."},{"issue":"27","key":"2026092808091423000_cit20","doi-asserted-by":"publisher","first-page":"14274","DOI":"10.1021\/jp212274y","article-title":"Hydrogen Spillover\nto Nonreducible\nSupports","volume":"116","author":"Prins","year":"2012","journal-title":"J. Phys. Chem. C"},{"issue":"5","key":"2026092808091423000_cit21","doi-asserted-by":"publisher","first-page":"2714","DOI":"10.1021\/cr200346z","article-title":"Hydrogen Spillover.\nFacts and Fiction","volume":"112","author":"Prins","year":"2012","journal-title":"Chem. 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Soc."},{"key":"2026092808091423000_cit25","doi-asserted-by":"publisher","DOI":"10.1038\/s41467-018-06100-9","article-title":"Identification of active sites on\nsupported metal catalysts with carbon nanotube hydrogen highways","volume":"9","author":"Briggs","year":"2018","journal-title":"Nat. Commun."},{"issue":"8","key":"2026092808091423000_cit26","doi-asserted-by":"publisher","first-page":"2299","DOI":"10.1021\/jacsau.3c00330","article-title":"How Pt Influences\nH2 Reactions on High Surface-Area Pt\/CeO2 Powder Catalyst Surfaces","volume":"3","author":"Lee","year":"2023","journal-title":"JACS Au"},{"issue":"22","key":"2026092808091423000_cit27","doi-asserted-by":"publisher","first-page":"7285","DOI":"10.1021\/acs.jpclett.9b02670","article-title":"Direct Probing\nof Oxygen Loss from the Surface Lattice of Correlated Oxides during\nHydrogen Spillover","volume":"10","author":"Yoon","year":"2019","journal-title":"J. Phys. Chem. Lett."},{"issue":"2","key":"2026092808091423000_cit28","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202414388","article-title":"Does H2 Temperature-Programmed\nReduction Always Probe\nSolid-State Redox Chemistry? The Case of Pt\/CeO2","volume":"64","author":"Lee","year":"2025","journal-title":"Angew. Chem., Int. Ed."},{"issue":"5","key":"2026092808091423000_cit29","doi-asserted-by":"publisher","first-page":"2831","DOI":"10.1039\/D5CS00680E","article-title":"From molecular\nhydrogen to reactive hydrogen: activation pathways and species variation\nin thermal catalytic heterogeneous hydrogenation","volume":"55","author":"Chen","year":"2026","journal-title":"Chem. Soc. Rev."},{"issue":"8","key":"2026092808091423000_cit30","doi-asserted-by":"publisher","first-page":"6472","DOI":"10.1021\/jacs.4c13711","article-title":"Operando Unveiling of Hydrogen Spillover Mechanisms\non Tungsten Oxide Surfaces","volume":"147","author":"Li","year":"2025","journal-title":"J. Am. Chem. Soc."},{"issue":"24","key":"2026092808091423000_cit31","doi-asserted-by":"publisher","first-page":"15194","DOI":"10.1021\/acscatal.1c04419","article-title":"Hydrogen Adsorption\nat the Au\/TiO2 Interface: Quantitative Determination and Spectroscopic\nSignature of the Reactive Interface Hydroxyl Groups at the Active\nSite","volume":"11","author":"Mahdavi-Shakib","year":"2021","journal-title":"ACS Catal."},{"issue":"6","key":"2026092808091423000_cit32","doi-asserted-by":"publisher","first-page":"895","DOI":"10.1021\/acs.accounts.3c00762","article-title":"Hydrogen Spillover Phenomenon at\nthe Interface of Metal-Supported Electrocatalysts for Hydrogen Evolution","volume":"57","author":"Li","year":"2024","journal-title":"Acc. Chem. Res."},{"issue":"12","key":"2026092808091423000_cit33","doi-asserted-by":"publisher","first-page":"5760","DOI":"10.1021\/jacs.9b13729","article-title":"Water Poisons\nH2 Activation at the Au\u2013TiO2 Interface by Slowing Proton and\nElectron Transfer between Au and Titania","volume":"142","author":"Kumar","year":"2020","journal-title":"J.\nAm. Chem. Soc."},{"issue":"8","key":"2026092808091423000_cit34","doi-asserted-by":"publisher","first-page":"710","DOI":"10.1038\/s41929-023-00996-3","article-title":"The role\nof surface hydroxyls in the entropy-driven adsorption and spillover\nof H2 on Au\/TiO2 catalysts","volume":"6","author":"Mahdavi-Shakib","year":"2023","journal-title":"Nat. Catal."},{"issue":"30","key":"2026092808091423000_cit35","doi-asserted-by":"publisher","first-page":"43926","DOI":"10.1021\/acsami.5c10678","article-title":"Insight into Interparticle Hydrogen\nSpillover Driven by Remote Metal Oxides","volume":"17","author":"Mori","year":"2025","journal-title":"ACS\nAppl. Mater. Interfaces"},{"issue":"33","key":"2026092808091423000_cit36","doi-asserted-by":"publisher","first-page":"29908","DOI":"10.1021\/jacs.5c06813","article-title":"Surface\nEntropy Mediated Hydrogen Spillover on Au\/TiO2: Influences of Strongly\nAdsorbed Water on H2 Adsorption Thermodynamics","volume":"147","author":"Yun","year":"2025","journal-title":"J. Am. Chem. Soc."},{"issue":"44","key":"2026092808091423000_cit37","doi-asserted-by":"publisher","first-page":"30091","DOI":"10.1021\/jacs.4c07539","article-title":"Upside-Down Adsorption:\nThe Counterintuitive Influences of Surface Entropy and Surface Hydroxyl\nDensity on Hydrogen Spillover","volume":"146","author":"Hart","year":"2024","journal-title":"J. Am. Chem.\nSoc."},{"issue":"45","key":"2026092808091423000_cit38","doi-asserted-by":"publisher","first-page":"28525","DOI":"10.1039\/D4CP03093A","article-title":"Effects of\noxide platforms on the dynamics and reduction characteristics of hydrogen\nspillover","volume":"26","author":"Shun","year":"2024","journal-title":"Phys. Chem. Chem. Phys."},{"issue":"27","key":"2026092808091423000_cit39","doi-asserted-by":"publisher","first-page":"8137","DOI":"10.1039\/D2SC00871H","article-title":"Revealing\nhydrogen spillover pathways in reducible metal oxides","volume":"13","author":"Shun","year":"2022","journal-title":"Chem. Sci."},{"issue":"41","key":"2026092808091423000_cit40","doi-asserted-by":"publisher","first-page":"17589","DOI":"10.1021\/acs.jpcc.2c05478","article-title":"Hydrogen\nInteraction with Oxide Supports in the Presence\nand Absence of Platinum","volume":"126","author":"Beck","year":"2022","journal-title":"J. Phys. Chem. 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Rev."},{"issue":"2","key":"2026092808091423000_cit43","doi-asserted-by":"publisher","first-page":"171","DOI":"10.1016\/S0040-6031(97)00258-X","article-title":"Thermochemistry of\nmanganese oxides in reactive gas atmospheres: Probing redox compositions\nin the decomposition course MnO2 \u2192 MnO","volume":"303","author":"Zaki","year":"1997","journal-title":"Thermochim. Acta"},{"key":"2026092808091423000_cit44","doi-asserted-by":"publisher","first-page":"475","DOI":"10.1016\/j.apsusc.2015.12.159","article-title":"XPS determination\nof Mn oxidation states in Mn (hydr)oxides","volume":"366","author":"Ilton","year":"2016","journal-title":"Appl.\nSurf. Sci."},{"key":"2026092808091423000_cit45","doi-asserted-by":"publisher","DOI":"10.1016\/j.apsusc.2021.149693","article-title":"Structural, optical and magnetic properties of \u03b1- and \u03b2-MnO2\nnanorods","volume":"557","author":"Gangwar","year":"2021","journal-title":"Appl. Surf. Sci."},{"issue":"1","key":"2026092808091423000_cit46","doi-asserted-by":"publisher","DOI":"10.1038\/s41598-025-95769-2","article-title":"Modification of photocatalytic activity\nand antibacterial\nproperties of Mn2O3 by Zn ions doping","volume":"15","author":"Nasr","year":"2025","journal-title":"Sci.\nRep."},{"key":"2026092808091423000_cit47","doi-asserted-by":"publisher","first-page":"265","DOI":"10.1016\/j.jmst.2023.05.059","article-title":"Tunning the bandgap of MnO2 homojunction by building\nactive high-index\nfacet to achieve rapid electron transfer for enhanced photocatalytic\nsterilization","volume":"168","author":"Zhang","year":"2024","journal-title":"J. Mater. Sci. Technol."},{"issue":"6","key":"2026092808091423000_cit48","doi-asserted-by":"publisher","first-page":"3786","DOI":"10.1021\/acs.jctc.0c00134","article-title":"Band Gap in\nMagnetic Insulators from a Charge Transition Level Approach","volume":"16","author":"Cipriano","year":"2020","journal-title":"J. Chem. Theory Comput."},{"issue":"18","key":"2026092808091423000_cit49","doi-asserted-by":"publisher","first-page":"9876","DOI":"10.1021\/jp300590d","article-title":"Band Gap Engineering\nof MnO via ZnO Alloying: A Potential\nNew Visible-Light Photocatalyst","volume":"116","author":"Kanan","year":"2012","journal-title":"J. Phys. Chem.\nC"},{"issue":"48","key":"2026092808091423000_cit50","doi-asserted-by":"publisher","first-page":"16469","DOI":"10.1021\/jacs.8b04991","article-title":"H2 Oxidation over Supported Au Nanoparticle Catalysts:\nEvidence for Heterolytic H2 Activation at the Metal\u2013Support\nInterface","volume":"140","author":"Whittaker","year":"2018","journal-title":"J. Am. Chem. Soc."},{"issue":"24","key":"2026092808091423000_cit51","doi-asserted-by":"publisher","first-page":"15194","DOI":"10.1021\/acscatal.1c04419","article-title":"Hydrogen Adsorption\nat the Au\/TiO2 Interface: Quantitative Determination and Spectroscopic\nSignature of the Reactive Interface Hydroxyl Groups at the Active\nSite","volume":"11","author":"Mahdavi-Shakib","year":"2021","journal-title":"ACS Catal."},{"issue":"14","key":"2026092808091423000_cit52","doi-asserted-by":"publisher","first-page":"7735","DOI":"10.1002\/anie.202013359","article-title":"Kinetics of H2 Adsorption\nat the\nMetal\u2013Support Interface of Au\/TiO2 Catalysts Probed by Broad\nBackground IR Absorbance","volume":"60","author":"Mahdavi-Shakib","year":"2021","journal-title":"Angew. Chem., Int.\nEd."},{"issue":"11","key":"2026092808091423000_cit53","doi-asserted-by":"publisher","first-page":"1702","DOI":"10.1021\/ac60131a045","article-title":"Reaction\nKinetics in Differential Thermal Analysis","volume":"29","author":"Kissinger","year":"1957","journal-title":"Anal.\nChem."},{"key":"2026092808091423000_cit54","doi-asserted-by":"publisher","first-page":"1","DOI":"10.1016\/j.tca.2012.04.008","article-title":"Homer Kissinger and the Kissinger equation","volume":"540","author":"Blaine","year":"2012","journal-title":"Thermochim. Acta"},{"issue":"7","key":"2026092808091423000_cit55","doi-asserted-by":"publisher","first-page":"1591","DOI":"10.1016\/0009-2509(80)80052-2","article-title":"Modelling of the reduction of manganese oxides with\nhydrogen","volume":"35","author":"De Bruijn","year":"1980","journal-title":"Chem. Eng. 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