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dc.contributor.authorWu, Tongwei
dc.contributor.authorMelander, Marko M.
dc.contributor.authorHonkala, Karoliina
dc.date.accessioned2022-02-08T12:21:02Z
dc.date.available2022-02-08T12:21:02Z
dc.date.issued2022
dc.identifier.citationWu, T., Melander, M. M., & Honkala, K. (2022). Coadsorption of NRR and HER Intermediates Determines the Performance of Ru-N4 toward Electrocatalytic N2 Reduction. <i>ACS Catalysis</i>, <i>12</i>(4), 2505-2512. <a href="https://doi.org/10.1021/acscatal.1c05820" target="_blank">https://doi.org/10.1021/acscatal.1c05820</a>
dc.identifier.otherCONVID_104133239
dc.identifier.urihttps://jyx.jyu.fi/handle/123456789/79690
dc.description.abstractElectrochemical N2 reduction (NRR) to ammonia is seriously limited by the competing hydrogen evolution reaction (HER), but atomic-scale factors controlling HER/NRR competition are unknown. Herein we unveil the mechanism, thermodynamics, and kinetics determining the HER/NRR efficiency on the state-of-the-art NRR electrocatalyst, Ru-N4, using grand canonical ensemble density functional theory (GCE-DFT). We show that NRR/HER intermediates coadsorb on the catalyst where NRR intermediates suppress HER and selectivity is determined by the initial step forming *NNH or *H. Our results provide crucial insight into the complex NRR/HER competition, show the necessity of using GCE-DFT calculations, and suggest ways to improve NRR selectivity.en
dc.format.mimetypeapplication/pdf
dc.language.isoeng
dc.publisherAmerican Chemical Society (ACS)
dc.relation.ispartofseriesACS Catalysis
dc.rightsCC BY 4.0
dc.subject.otherhydrogen evolution reaction
dc.subject.otherelectrochemical N2 reduction
dc.subject.othergrand canonical ensemble density functional theory
dc.titleCoadsorption of NRR and HER Intermediates Determines the Performance of Ru-N4 toward Electrocatalytic N2 Reduction
dc.typearticle
dc.identifier.urnURN:NBN:fi:jyu-202202081442
dc.contributor.laitosKemian laitosfi
dc.contributor.laitosDepartment of Chemistryen
dc.contributor.oppiaineNanoscience Centerfi
dc.contributor.oppiaineResurssiviisausyhteisöfi
dc.contributor.oppiaineFysikaalinen kemiafi
dc.contributor.oppiaineNanoscience Centeren
dc.contributor.oppiaineSchool of Resource Wisdomen
dc.contributor.oppiainePhysical Chemistryen
dc.type.urihttp://purl.org/eprint/type/JournalArticle
dc.description.reviewstatuspeerReviewed
dc.format.pagerange2505-2512
dc.relation.issn2155-5435
dc.relation.numberinseries4
dc.relation.volume12
dc.type.versionpublishedVersion
dc.rights.copyright© 2022 The Authors. Published by American Chemical Society
dc.rights.accesslevelopenAccessfi
dc.relation.grantnumber317739
dc.relation.grantnumber338228
dc.subject.ysosähkökemia
dc.subject.ysovety
dc.subject.ysoelektrolyysi
dc.subject.ysokatalyysi
dc.subject.ysokatalyytit
dc.subject.ysohapetus-pelkistysreaktio
dc.format.contentfulltext
jyx.subject.urihttp://www.yso.fi/onto/yso/p8093
jyx.subject.urihttp://www.yso.fi/onto/yso/p16151
jyx.subject.urihttp://www.yso.fi/onto/yso/p8095
jyx.subject.urihttp://www.yso.fi/onto/yso/p8704
jyx.subject.urihttp://www.yso.fi/onto/yso/p15480
jyx.subject.urihttp://www.yso.fi/onto/yso/p28877
dc.rights.urlhttps://creativecommons.org/licenses/by/4.0/
dc.relation.doi10.1021/acscatal.1c05820
dc.relation.funderSuomen Akatemiafi
dc.relation.funderSuomen Akatemiafi
dc.relation.funderAcademy of Finlanden
dc.relation.funderAcademy of Finlanden
jyx.fundingprogramAkatemiahanke, SAfi
jyx.fundingprogramAkatemiatutkijan tehtävä, SAfi
jyx.fundingprogramAcademy Project, AoFen
jyx.fundingprogramResearch post as Academy Research Fellow, AoFen
jyx.fundinginformationT.W. acknowledges the support by the National Natural Science Foundation of China (No. 11874005), the China National Postdoctoral Program for Innovative Talents (No. BX2021053), China Postdoctoral Science Foundation (No.2021M700680) and China Scholarship Council (No. 201906070128). T.W. also acknowledges the support of the Shang Hai Tong Ji Gao Ting Yao Environment Science and Technology Development Foundation. M.M.M. and K.H. gratefully acknowledge support by the Academy of Finland (grant numbers 317739 and 338228), and the Jane and Aatos Erkko Foundation (funding to the LACOR project).


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