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Defective Ru-doped α-MnO2 nanorods enabling efficient hydrazine oxidation for energy-saving hydrogen production via proton exchange membranes at near-neutral pH

2023-08-15Journal article Restricted access
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dc.contributor.authorYu, Zhipeng
dc.contributor.authorSi, Chaowei
dc.contributor.authorSabaté, Ferran
dc.contributor.authorLaGrow, Alec P.
dc.contributor.authorTai, Zhixin
dc.contributor.authorDiaconescu, Vlad Martin
dc.contributor.authorSimonelli, Laura
dc.contributor.authorMeng, Lijian
dc.contributor.authorSabater, Maria J.
dc.contributor.authorLi, Bo
dc.contributor.authorLiu, Lifeng
dc.date.accessioned2023-09-13T14:03:42Z
dc.date.embargo2031
dc.date.issued2023-08-15
dc.description.abstractProton exchange membrane water electrolysis (PEMWE) showes substantial advantages over the conventional alkaline water electrolysis (AWE) for power-to-hydrogen (PtH) conversion, given the faster response and wider dynamic current range of the PEMWE technology. However, PEMWE is currently still expensive due partly to the high voltage needed to operate at high current densities and inevitable usage of precious iridium/rutheniumbased catalysts to expedite the slow kinetics of the oxygen evolution reaction (OER) and to ensure sufficient durability under strongly acidic conditions. Herein, we report that ruthenium doped α-manganese oxide (Ru/ α-MnO2) nanorods show outstanding electrocatalytic performance toward the hydrazine (N2H4) oxidation reaction (HzOR) in near-neutral media (weak alkaline and weak acid), which can be used to replace the energydemanding OER for PEMWE. The as-prepared Ru/α-MnO2 is found to comprise abundant defects. When used to catalyze HzOR in the acid-hydrazine electrolyte (0.05 M H2SO4 + 0.5 M N2H4), it can deliver an anodic current density of 10 mA cm􀀀 2 at a potential as low as 0.166 V vs. reversible hydrogen electrode (RHE). Moreover, Ru/ α-MnO2 exhibits remarkable corrosion/oxidation resistance and remains electrochemically stable during HzOR for at least 1000 h. Theoretical calculations and experimental studies prove that Ru doping elongates the Mn–O bond and produces abundant cationic defects, which induces charge delocalization and significantly lowers material’s electrical resistance and overpotential, resulting in excellent HzOR catalytic activity and stability. The introduction of N2H4 significantly reduces the energy demand for hydrogen production, so that PEMWE can be accomplished under remarkably low voltages of 0.254 V at 10 mA cm􀀀 2 and 0.935 V at 100 mA cm􀀀 2 for a long term without notable degradation. This work opens a new avenue toward energy-saving PEMWE with earthabundant OER catalysts.pt_PT
dc.description.sponsorshipL. Liu acknowledges the start-up grant of the Songshan Lake Materials Laboratory (Grant No. Y2D1051Z311) and financial support from the Ministry of Science & Technology of China (Grant No. 22J4021Z311). B. Li is supported by Natural Science Foundation of Liao Ning Province (2021-MS-004) and ShenYang Normal University (BS202208). Z. P. Yu is financially supported by the China Scholarship Council (Grant No. 201806150015). Additionally, this work was also partially supported by the National Innovation Agency of Portugal through the Mobilizador project (Baterias 2030, Grant No. POCI-01-0247-FEDER-046109).pt_PT
dc.description.versioninfo:eu-repo/semantics/publishedVersionpt_PT
dc.identifier.doi10.1016/j.cej.2023.144050pt_PT
dc.identifier.urihttp://hdl.handle.net/10400.22/23529
dc.language.isoengpt_PT
dc.peerreviewedyespt_PT
dc.publisherElsevierpt_PT
dc.relationPOCI-01-0247-FEDER-046109pt_PT
dc.relation.publisherversionhttps://www.sciencedirect.com/science/article/pii/S138589472302781X?via%3Dihubpt_PT
dc.rights.urihttp://creativecommons.org/licenses/by-nc-nd/4.0/pt_PT
dc.subjectCationic defectpt_PT
dc.subjectRu dopingpt_PT
dc.subjectPEM water electrolysispt_PT
dc.subjectHydrazine oxidation reactionpt_PT
dc.subjectElectrocatalysispt_PT
dc.titleDefective Ru-doped α-MnO2 nanorods enabling efficient hydrazine oxidation for energy-saving hydrogen production via proton exchange membranes at near-neutral pHpt_PT
dc.typejournal article
dspace.entity.typePublication
oaire.citation.startPage144050pt_PT
oaire.citation.titleChemical Engineering Journalpt_PT
oaire.citation.volume470pt_PT
person.familyNameMeng
person.givenNameLijian
person.identifier236430
person.identifier.ciencia-idC31B-0091-BD12
person.identifier.orcid0000-0001-6071-3502
person.identifier.scopus-author-id7202236050
rcaap.rightsclosedAccesspt_PT
rcaap.typearticlept_PT
relation.isAuthorOfPublicationcb02ae05-0786-47ff-b480-2fde7ef93e0d
relation.isAuthorOfPublication.latestForDiscoverycb02ae05-0786-47ff-b480-2fde7ef93e0d

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