Catalytic Activity of Defect-Engineered Transition Me tal Dichalcogenides Mapped with Atomic-Scale Precision by Electrochemical Scanning Tunneling Microscopy

dc.contributorAalto-yliopistofi
dc.contributorAalto Universityen
dc.contributor.authorLunardon, Marcoen_US
dc.contributor.authorKosmala, Tomaszen_US
dc.contributor.authorGhorbani-Asl, Mahdien_US
dc.contributor.authorKrasheninnikov, Arkady V.en_US
dc.contributor.authorKolekar, Sadhuen_US
dc.contributor.authorDurante, Christianen_US
dc.contributor.authorBatzill, Matthiasen_US
dc.contributor.authorAgnoli, Stefanoen_US
dc.contributor.authorGranozzi, Gaetanoen_US
dc.contributor.departmentDepartment of Applied Physicsen
dc.contributor.groupauthorSoft Matter and Wettingen
dc.contributor.organizationUniversity of Padovaen_US
dc.contributor.organizationHelmholtz-Zentrum Dresden-Rossendorf EVen_US
dc.contributor.organizationUniversity of South Floridaen_US
dc.date.accessioned2023-02-20T05:14:01Z
dc.date.available2023-02-20T05:14:01Z
dc.date.issued2023-01-16en_US
dc.descriptionFunding Information: This work has been partially supported by the MIUR (PRIN 2017: Multi-e, 20179337R7) and the Cariparo Foundation (project Synergy, Progetti di Eccellenza 2018). M.B. acknowledges support from the U.S. National Science Foundation under award 2140038. The National Science Centre, Poland, is acknowledged for funding (grant no. 2021/43/D/ST3/02873). The University of Padova is acknowledged for support through the grant P-Disc 2022 (MUSYCA). The “Excellence Initiative – Research University” program is acknowledged for support. Publisher Copyright: © 2023 The Authors. Published by American Chemical Society.
dc.description.abstractUnraveling structure-activity relationships is a key objective of catalysis. Unfortunately, the intrinsic complexity and structural heterogeneity of materials stand in the way of this goal, mainly because the activity measurements are area-averaged and therefore contain information coming from different surface sites. This limitation can be surpassed by the analysis of the noise in the current of electrochemical scanning tunneling microscopy (EC-STM). Herein, we apply this strategy to investigate the catalytic activity toward the hydrogen evolution reaction of monolayer films of MoSe2. Thanks to atomically resolved potentiodynamic experiments, we can evaluate individually the catalytic activity of the MoSe2 basal plane, selenium vacancies, and different point defects produced by the intersections of metallic twin boundaries. The activity trend deduced by EC-STM is independently confirmed by density functional theory calculations, which also indicate that, on the metallic twin boundary crossings, the hydrogen adsorption energy is almost thermoneutral. The micro- and macroscopic measurements are combined to extract the turnover frequency of different sites, obtaining for the most active ones a value of 30 s-1 at −136 mV vs RHE.en
dc.description.versionPeer revieweden
dc.format.extent9
dc.format.extent972-980
dc.format.mimetypeapplication/pdfen_US
dc.identifier.citationLunardon, M, Kosmala, T, Ghorbani-Asl, M, Krasheninnikov, A V, Kolekar, S, Durante, C, Batzill, M, Agnoli, S & Granozzi, G 2023, ' Catalytic Activity of Defect-Engineered Transition Me tal Dichalcogenides Mapped with Atomic-Scale Precision by Electrochemical Scanning Tunneling Microscopy ', ACS Energy Letters, vol. 8, no. 2, pp. 972-980 . https://doi.org/10.1021/acsenergylett.2c02599en
dc.identifier.doi10.1021/acsenergylett.2c02599en_US
dc.identifier.issn2380-8195
dc.identifier.otherPURE UUID: a6840c50-6449-4007-8f64-1bd35a715701en_US
dc.identifier.otherPURE ITEMURL: https://research.aalto.fi/en/publications/a6840c50-6449-4007-8f64-1bd35a715701en_US
dc.identifier.otherPURE LINK: http://www.scopus.com/inward/record.url?scp=85146553098&partnerID=8YFLogxKen_US
dc.identifier.otherPURE FILEURL: https://research.aalto.fi/files/100313247/Catalytic_Activity_of_Defect_Engineered_Transition_Me_tal_Dichalcogenides_Mapped_with_Atomic_Scale_Precision_by_Electrochemical_Scanning_Tunneling_Microscopy.pdfen_US
dc.identifier.urihttps://aaltodoc.aalto.fi/handle/123456789/119791
dc.identifier.urnURN:NBN:fi:aalto-202302202138
dc.language.isoenen
dc.publisherAMERICAN CHEMICAL SOCIETY
dc.relation.ispartofseriesACS Energy Lettersen
dc.relation.ispartofseriesVolume 8, issue 2en
dc.rightsopenAccessen
dc.titleCatalytic Activity of Defect-Engineered Transition Me tal Dichalcogenides Mapped with Atomic-Scale Precision by Electrochemical Scanning Tunneling Microscopyen
dc.typeA1 Alkuperäisartikkeli tieteellisessä aikakauslehdessäfi
dc.type.versionpublishedVersion
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