Now showing 1 - 10 of 11
  • 2020Journal Article Research Paper
    [["dc.bibliographiccitation.artnumber","034009"],["dc.bibliographiccitation.issue","3"],["dc.bibliographiccitation.journal","Journal of Physics: Energy"],["dc.bibliographiccitation.volume","2"],["dc.contributor.affiliation","Villalobos, Javier;"],["dc.contributor.affiliation","Golnak, Ronny;"],["dc.contributor.affiliation","Xi, Lifei;"],["dc.contributor.affiliation","Schuck, Götz;"],["dc.contributor.affiliation","Risch, Marcel;"],["dc.contributor.author","Villalobos, Javier"],["dc.contributor.author","Golnak, Ronny"],["dc.contributor.author","Xi, Lifei"],["dc.contributor.author","Schuck, Götz"],["dc.contributor.author","Risch, Marcel"],["dc.date.accessioned","2021-04-14T08:24:16Z"],["dc.date.available","2021-04-14T08:24:16Z"],["dc.date.issued","2020"],["dc.date.updated","2022-02-09T13:18:45Z"],["dc.description.abstract","AbstractManganese oxides have received much attention over the years among the wide range of electrocatalysts for the oxygen evolution reaction (OER) due to their low toxicity, high abundance and rich redox chemistry. While many previous studies focused on the activity of these materials, a better understanding of the material transformations relating to activation or degradation is highly desirable, both from a scientific perspective and for applications. We electrodeposited Na-containing MnOx without long-range order from an alkaline solution to investigate these aspects by cyclic voltammetry, scanning electron microscopy and x-ray absorption spectroscopy at the Mn-K and Mn-L edges. The pristine film was assigned to a layered edge-sharing Mn3+/4+ oxide with Mn-O bond lengths of mainly 1.87 Å and some at 2.30 Å as well as Mn-Mn bond lengths of 2.87 Å based on fits to the extended x-ray fine structure. The decrease of the currents at voltages before the onset of the OER followed power laws with three different exponents depending on the number of cycles and the Tafel slope decreases from 186 ± 48 to 114 ± 18 mV dec−1 after 100 cycles, which we interpret in the context of surface coverage with unreacted intermediates. Post-mortem microscopy and bulk spectroscopy at the Mn-K edge showed no change of the microstructure, bulk local structure or bulk Mn valence. Yet, the surface region of MnOx oxidized toward Mn4+, which explains the reduction of the currents in agreement with literature. Surprisingly, we find that MnOx reactivates after 30 min at open-circuit (OC), where the currents and also the Tafel slope increase. Reactivation processes during OC are crucial because OC is unavoidable when coupling the electrocatalysts to intermittent power sources such as solar energy for sustainable energy production."],["dc.description.sponsorship","H2020 European Research Councilhttp://dx.doi.org/10.13039/100010663"],["dc.identifier.doi","10.1088/2515-7655/ab9fe2"],["dc.identifier.eissn","2515-7655"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/81226"],["dc.language.iso","en"],["dc.notes.intern","DOI Import GROB-399"],["dc.publisher","IOP Publishing"],["dc.relation.eissn","2515-7655"],["dc.relation.orgunit","Institut für Materialphysik"],["dc.rights.uri","http://creativecommons.org/licenses/by/4.0"],["dc.title","Reversible and irreversible processes during cyclic voltammetry of an electrodeposited manganese oxide as catalyst for the oxygen evolution reaction"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.subtype","original_ja"],["dspace.entity.type","Publication"]]
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  • 2017Journal Article Research Paper
    [["dc.bibliographiccitation.artnumber","154"],["dc.bibliographiccitation.issue","5"],["dc.bibliographiccitation.journal","Catalysts"],["dc.bibliographiccitation.volume","7"],["dc.contributor.author","Risch, Marcel"],["dc.date.accessioned","2018-10-17T06:48:28Z"],["dc.date.available","2018-10-17T06:48:28Z"],["dc.date.issued","2017"],["dc.description.abstract","Oxygen reduction is considered a key reaction for electrochemical energy conversion but slow kinetics hamper application in fuel cells and metal-air batteries. In this review, the prospect of perovskite oxides for the oxygen reduction reaction (ORR) in alkaline media is reviewed with respect to fundamental insight into activity and possible mechanisms. For gaining these insights, special emphasis is placed on highly crystalline perovskite films that have only recently become available for electrochemical interrogation. The prospects for applications are evaluated based on recent progress in the synthesis of perovskite nanoparticles. The review concludes with the current understanding of oxygen reduction on perovskite oxides and a perspective on opportunities for future fundamental and applied research."],["dc.description.sponsorship","Deutsche Forschungsgemeinschaft"],["dc.identifier.doi","10.3390/catal7050154"],["dc.identifier.purl","https://resolver.sub.uni-goettingen.de/purl?gs-1/14630"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/16066"],["dc.language.iso","en"],["dc.notes.intern","Merged from goescholar"],["dc.notes.status","final"],["dc.publisher","MDPI"],["dc.relation.eissn","2073-4344"],["dc.relation.orgunit","Fakultät für Physik"],["dc.relation.orgunit","Institut für Materialphysik"],["dc.rights","CC BY 4.0"],["dc.title","Perovskite Electrocatalysts for the Oxygen Reduction Reaction in Alkaline Media"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.subtype","original_ja"],["dc.type.version","published_version"],["dspace.entity.type","Publication"]]
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  • 2017Journal Article Research Paper
    [["dc.bibliographiccitation.firstpage","1700109"],["dc.bibliographiccitation.issue","12"],["dc.bibliographiccitation.journal","Advanced sustainable systems"],["dc.bibliographiccitation.volume","1"],["dc.contributor.author","Mierwaldt, Daniel"],["dc.contributor.author","Roddatis, Vladimir"],["dc.contributor.author","Risch, Marcel"],["dc.contributor.author","Scholz, Julius"],["dc.contributor.author","Geppert, Janis"],["dc.contributor.author","Abrishami, Majid Ebrahimizadeh"],["dc.contributor.author","Jooss, Christian"],["dc.date.accessioned","2020-12-10T14:06:44Z"],["dc.date.available","2020-12-10T14:06:44Z"],["dc.date.issued","2017"],["dc.identifier.doi","10.1002/adsu.201700109"],["dc.identifier.issn","2366-7486"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/70006"],["dc.language.iso","en"],["dc.notes.intern","DOI Import GROB-354"],["dc.relation","SFB 1073: Kontrolle von Energiewandlung auf atomaren Skalen"],["dc.relation","SFB 1073 | Topical Area C | C02 In situ hochauflösende Untersuchung des aktiven Zustands bei der photo- und elektrochemischen Wasserspaltung"],["dc.relation.orgunit","Institut für Materialphysik"],["dc.rights","CC BY-NC 4.0"],["dc.title","Environmental TEM Investigation of Electrochemical Stability of Perovskite and Ruddlesden-Popper Type Manganite Oxygen Evolution Catalysts"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.subtype","original_ja"],["dc.type.version","published_version"],["dspace.entity.type","Publication"]]
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  • 2017Journal Article Research Paper
    [["dc.bibliographiccitation.firstpage","4479"],["dc.bibliographiccitation.issue","22"],["dc.bibliographiccitation.journal","ChemSusChem"],["dc.bibliographiccitation.lastpage","4490"],["dc.bibliographiccitation.volume","10"],["dc.contributor.author","Köhler, Lennart"],["dc.contributor.author","Abrishami, Majid Ebrahimizadeh"],["dc.contributor.author","Roddatis, Vladimir"],["dc.contributor.author","Geppert, Janis"],["dc.contributor.author","Risch, Marcel"],["dc.date.accessioned","2018-10-17T06:32:18Z"],["dc.date.available","2018-10-17T06:32:18Z"],["dc.date.issued","2017"],["dc.description.abstract","Targeted improvement of the low efficiency of water oxidation during the oxygen evolution reaction (OER) is severely hindered by insufficient knowledge of the electrocatalytic mechanism on heterogeneous surfaces. We chose LiMn2 O4 as a model system for mechanistic investigations as it shares the cubane structure with the active site of photosystem II and the valence of Mn3.5+ with the dark-stable S1 state in the mechanism of natural photosynthesis. The investigated LiMn2 O4 nanoparticles are electrochemically stable in NaOH electrolytes and show respectable activity in any of the main metrics. At low overpotential, the key mechanistic parameters of Tafel slope, Nernst slope, and reaction order have constant values on the RHE scale of 62(1) mV dec-1 , 1(1) mV pH-1 , -0.04(2), respectively. These values are interpreted in the context of the well-studied mechanism of natural photosynthesis. The uncovered difference in the reaction sequence is important for the design of efficient bio-inspired electrocatalysts."],["dc.identifier.doi","10.1002/cssc.201701582"],["dc.identifier.pmid","28921902"],["dc.identifier.purl","https://resolver.sub.uni-goettingen.de/purl?gs-1/14992"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/16065"],["dc.language.iso","en"],["dc.notes.intern","Merged from goescholar"],["dc.notes.status","final"],["dc.relation","SFB 1073: Kontrolle von Energiewandlung auf atomaren Skalen"],["dc.relation","SFB 1073 | Topical Area C | C05 Kontrolle Elektronen-getriebener Chemie durch Interkalation"],["dc.relation","SFB 1073 | Topical Area Z | Z02 Hochauflösende Charakterisierung von Grenzflächen"],["dc.relation.eissn","1864-564X"],["dc.relation.orgunit","Fakultät für Physik"],["dc.relation.orgunit","Institut für Materialphysik"],["dc.rights","CC BY-NC 4.0"],["dc.rights.uri","http://creativecommons.org/licenses/by-nc/4.0"],["dc.title","Mechanistic Parameters of Electrocatalytic Water Oxidation on LiMn2 O4 in Comparison to Natural Photosynthesis"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.subtype","original_ja"],["dc.type.version","published_version"],["dspace.entity.type","Publication"]]
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  • 2019Journal Article Research Paper
    [["dc.bibliographiccitation.firstpage","1266"],["dc.bibliographiccitation.issue","4"],["dc.bibliographiccitation.journal","Journal of Synchrotron Radiation"],["dc.bibliographiccitation.lastpage","1271"],["dc.bibliographiccitation.volume","26"],["dc.contributor.author","Döring, Florian"],["dc.contributor.author","Risch, Marcel"],["dc.contributor.author","Rösner, Benedikt"],["dc.contributor.author","Beye, Martin"],["dc.contributor.author","Busse, Philipp"],["dc.contributor.author","Kubiček, Katharina"],["dc.contributor.author","Glaser, Leif"],["dc.contributor.author","Miedema, Piter S."],["dc.contributor.author","Soltau, Jakob"],["dc.contributor.author","Raiser, Dirk"],["dc.contributor.author","Guzenko, Vitaliy A."],["dc.contributor.author","Szabadics, Lukas"],["dc.contributor.author","Kochanneck, Leif"],["dc.contributor.author","Baumung, Max"],["dc.contributor.author","Buck, Jens"],["dc.contributor.author","Jooss, Christian"],["dc.contributor.author","Techert, Simone"],["dc.contributor.author","David, Christian"],["dc.date.accessioned","2020-12-10T18:25:59Z"],["dc.date.available","2020-12-10T18:25:59Z"],["dc.date.issued","2019"],["dc.description.abstract","X-ray absorption spectroscopy (XAS) is a powerful element-specific technique that allows the study of structural and chemical properties of matter. Often an indirect method is used to access the X-ray absorption (XA). This work demonstrates a new XAS implementation that is based on off-axis transmission Fresnel zone plates to obtain the XA spectrum of La0.6Sr0.4MnO3 by analysis of three emission lines simultaneously at the detector, namely the O 2p-1s, Mn 3s-2p and Mn 3d-2p transitions. This scheme allows the simultaneous measurement of an integrated total fluorescence yield and the partial fluorescence yields (PFY) of the Mn 3s-2p and Mn 3d-2p transitions when scanning the Mn L-edge. In addition to this, the reduction in O fluorescence provides another measure for absorption often referred to as the inverse partial fluorescence yield (IPFY). Among these different methods to measure XA, the Mn 3s PFY and IPFY deviate the least from the true XA spectra due to the negligible influence of selection rules on the decay channel. Other advantages of this new scheme are the potential to strongly increase the efficiency and throughput compared with similar measurements using conventional gratings and to increase the signal-to-noise of the XA spectra as compared with a photodiode. The ability to record undistorted bulk XA spectra at high flux is crucial for future in situ spectroscopy experiments on complex materials."],["dc.identifier.doi","10.1107/S1600577519003898"],["dc.identifier.issn","1600-5775"],["dc.identifier.pmid","31274453"],["dc.identifier.purl","https://resolver.sub.uni-goettingen.de/purl?gs-1/16305"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/75901"],["dc.language.iso","en"],["dc.notes.intern","DOI Import GROB-354"],["dc.relation","SFB 1073: Kontrolle von Energiewandlung auf atomaren Skalen"],["dc.relation","SFB 1073 | Topical Area C | C02 In situ hochauflösende Untersuchung des aktiven Zustands bei der photo- und elektrochemischen Wasserspaltung"],["dc.relation","SFB 1073 | Topical Area C | C05 Kontrolle Elektronen-getriebener Chemie durch Interkalation"],["dc.relation.eissn","1600-5775"],["dc.relation.issn","1600-5775"],["dc.relation.orgunit","Institut für Materialphysik"],["dc.relation.workinggroup","RG Techert (Structural Dynamics in Chemical Systems)"],["dc.title","A zone-plate-based two-color spectrometer for indirect X-ray absorption spectroscopy"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.subtype","original_ja"],["dspace.entity.type","Publication"]]
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  • 2019Journal Article Research Paper
    [["dc.bibliographiccitation.firstpage","2218"],["dc.bibliographiccitation.issue","9"],["dc.bibliographiccitation.journal","Sustainable Energy & Fuels"],["dc.bibliographiccitation.lastpage","2226"],["dc.bibliographiccitation.volume","3"],["dc.contributor.author","Baumung, Max"],["dc.contributor.author","Schönewald, Florian"],["dc.contributor.author","Erichsen, Torben"],["dc.contributor.author","Volkert, Cynthia A."],["dc.contributor.author","Risch, Marcel"],["dc.date.accessioned","2021-10-15T08:51:41Z"],["dc.date.available","2021-10-15T08:51:41Z"],["dc.date.issued","2019"],["dc.description.abstract","We investigate LiMn2O4 as a model catalyst for the oxygen evolution reaction (OER), because it shares the cubane structure with the active site of photosystem II. Specifically, we study the influence of different particle sizes of LiMn2O4 on the OER in a sodium hydroxide electrolyte. The product currents of manganese corrosion and oxygen evolution were obtained by rotating ring disk electrodes (RRDE). Physical characterization by various methods supports identical surface chemistry and microstructure of the pristine powders. We obtained similar oxygen current densities of 40(14) μA cmECSA−2 and 26(5) μA cmECSA−2 for micro- and nano-sized particles at 1.68 V vs. RHE. However, the total current densities differed drastically and while the micro-powder had a high disk current density of 205(2) μA cmECSA−2, its faradaic efficiency was only 25%. In contrast, the faradaic efficiency of the nanopowder was at least 75%. We hypothesize that a Mn redox process may occur in the bulk in parallel and possibly in combination with oxygen evolution on the surface based on the observed difference between the total and product current densities. Knowledge of the product currents is crucial for distinguishing the mechanisms of corrosion and catalysis and for designing better catalysts with high faradaic efficiency."],["dc.identifier.doi","10.1039/C8SE00551F"],["dc.identifier.purl","https://resolver.sub.uni-goettingen.de/purl?gs-1/16500"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/90942"],["dc.identifier.url","https://publications.goettingen-research-online.de/handle/2/62345"],["dc.language.iso","en"],["dc.relation","SFB 1073: Kontrolle von Energiewandlung auf atomaren Skalen"],["dc.relation","SFB 1073 | Topical Area C | C05 Kontrolle Elektronen-getriebener Chemie durch Interkalation"],["dc.relation.issn","2398-4902"],["dc.relation.orgunit","Institut für Materialphysik"],["dc.rights","CC BY 3.0"],["dc.title","Influence of particle size on the apparent electrocatalytic activity of LiMn2O4 for oxygen evolution"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.subtype","original_ja"],["dc.type.version","published_version"],["dspace.entity.type","Publication"]]
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  • 2020Journal Article Research Paper
    [["dc.bibliographiccitation.firstpage","032003"],["dc.bibliographiccitation.issue","3"],["dc.bibliographiccitation.journal","Journal of Physics: Energy"],["dc.bibliographiccitation.volume","2"],["dc.contributor.affiliation","Antipin, Denis;"],["dc.contributor.affiliation","Risch, Marcel;"],["dc.contributor.author","Antipin, Denis"],["dc.contributor.author","Risch, Marcel"],["dc.date.accessioned","2021-04-14T08:24:17Z"],["dc.date.available","2021-04-14T08:24:17Z"],["dc.date.issued","2020"],["dc.date.updated","2022-02-09T13:18:46Z"],["dc.description.abstract","AbstractThe oxygen evolution reaction (OER) is considered a key reaction for electrochemical energy conversion but slow kinetics hamper application in electrolyzers, metal-air batteries and other applications that rely on sustainable protons from water oxidation. In this review, the prospect of epitaxial perovskite oxides for the OER at room temperature in alkaline media is reviewed with respect to fundamental insight into systematic trends of the activity. First, we thoroughly define the perovskite structure and its parameter space. Then, the synthesis methods used to make electrocatalytic epitaxial perovskite oxide are surveyed, and we classify the different kinds of electrodes that can be assembled for electrocatalytic investigations. We discuss the semiconductor physics of epitaxial perovskite electrodes and their consequences for the interpretation of catalytic results. Prototypical mechanisms of the OER are introduced and comparatively discussed. OER investigations on epitaxial perovskite oxides are comprehensively surveyed and selected trends are graphically highlighted. The review concludes with a short perspective on opportunities for future electrocatalytic research on epitaxial perovskite oxide systems."],["dc.description.sponsorship","H2020 European Research Councilhttp://dx.doi.org/10.13039/100010663"],["dc.identifier.doi","10.1088/2515-7655/ab812f"],["dc.identifier.eissn","2515-7655"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/81227"],["dc.language.iso","en"],["dc.notes.intern","DOI Import GROB-399"],["dc.publisher","IOP Publishing"],["dc.relation.eissn","2515-7655"],["dc.relation.orgunit","Institut für Materialphysik"],["dc.rights.uri","http://creativecommons.org/licenses/by/4.0"],["dc.title","Trends of epitaxial perovskite oxide films catalyzing the oxygen evolution reaction in alkaline media"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.subtype","original_ja"],["dspace.entity.type","Publication"]]
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  • 2016Journal Article Research Paper
    [["dc.bibliographiccitation.artnumber","921"],["dc.bibliographiccitation.issue","11"],["dc.bibliographiccitation.journal","Materials"],["dc.bibliographiccitation.volume","9"],["dc.contributor.author","Abrishami, Majid Ebrahimizadeh"],["dc.contributor.author","Risch, Marcel"],["dc.contributor.author","Scholz, Julius"],["dc.contributor.author","Roddatis, Vladimir"],["dc.contributor.author","Osterthun, Norbert"],["dc.contributor.author","Jooss, Christian"],["dc.date.accessioned","2018-11-07T10:06:08Z"],["dc.date.available","2018-11-07T10:06:08Z"],["dc.date.issued","2016"],["dc.description.abstract","An improved understanding of the correlation between the electronic properties of Mn-O bonds, activity and stability of electro-catalysts for the oxygen evolution reaction (OER) is of great importance for an improved catalyst design. Here, an in-depth study of the relation between lattice structure, electronic properties and catalyst performance of the perovskite Ca1-xPrxMnO3 and the first-order RP-system Ca2-xPrxMnO4 at doping levels of x = 0, 0.25 and 0.5 is presented. Lattice structure is determined by X-ray powder diffraction and Rietveld refinement. X-ray absorption spectroscopy of Mn-L and O-K edges gives access to Mn valence and covalency of the Mn-O bond. Oxygen evolution activity and stability is measured by rotating ring disc electrode studies. We demonstrate that the highest activity and stability coincidences for systems with a Mn-valence state of +3.7, though also requiring that the covalency of the Mn-O bond has a relative minimum. This observation points to an oxygen evolution mechanism with high redox activity of Mn. Covalency should be large enough for facile electron transfer from adsorbed oxygen species to the MnO6 network; however, it should not be hampered by oxidation of the lattice oxygen, which might cause a crossover to material degradation. Since valence and covalency changes are not entirely independent, the introduction of the energy position of the e(g)(up arrow) pre-edge peak in the O-K spectra as a new descriptor for oxygen evolution is suggested, leading to a volcano-like representation of the OER activity."],["dc.identifier.doi","10.3390/ma9110921"],["dc.identifier.isi","000390114400007"],["dc.identifier.purl","https://resolver.sub.uni-goettingen.de/purl?gs-1/14105"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/39033"],["dc.notes.intern","Merged from goescholar"],["dc.notes.status","zu prüfen"],["dc.notes.submitter","Najko"],["dc.relation","SFB 1073: Kontrolle von Energiewandlung auf atomaren Skalen"],["dc.relation","SFB 1073 | Topical Area C | C02 In situ hochauflösende Untersuchung des aktiven Zustands bei der photo- und elektrochemischen Wasserspaltung"],["dc.relation.issn","1996-1944"],["dc.relation.orgunit","Fakultät für Physik"],["dc.relation.orgunit","Institut für Materialphysik"],["dc.rights","CC BY 4.0"],["dc.title","Oxygen Evolution at Manganite Perovskite Ruddlesden-Popper Type Particles: Trends of Activity on Structure, Valence and Covalence"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.peerReviewed","yes"],["dc.type.subtype","original_ja"],["dc.type.version","published_version"],["dspace.entity.type","Publication"]]
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  • 2019Journal Article Research Paper
    [["dc.bibliographiccitation.firstpage","1"],["dc.bibliographiccitation.issue","20"],["dc.bibliographiccitation.journal","ChemPhysChem"],["dc.bibliographiccitation.lastpage","9"],["dc.bibliographiccitation.volume","20"],["dc.contributor.author","Baumung, Max"],["dc.contributor.author","Kollenbach, Leon"],["dc.contributor.author","Xi, Lifei"],["dc.contributor.author","Risch, Marcel"],["dc.date.accessioned","2019-11-11T13:15:13Z"],["dc.date.accessioned","2021-10-11T11:33:49Z"],["dc.date.available","2019-11-11T13:15:13Z"],["dc.date.available","2021-10-11T11:33:49Z"],["dc.date.issued","2019"],["dc.description.abstract","Chemical and structural changes preceding electrocatalysis obfuscate the nature of the active state of electrocatalysts for the oxygen evolution reaction (OER), which calls for model systems to gain systematic insight. We investigated the effect of bulk oxidation on the overpotential of ink-casted LiMn2 O4 electrodes by a rotating ring-disk electrode (RRDE) setup and X-ray absorption spectroscopy (XAS) at the K shell core level of manganese ions (Mn-K edge). The cyclic voltammogram of the RRDE disk shows pronounced redox peaks in lithium hydroxide electrolytes with pH between 12 and 13.5, which we assign to bulk manganese redox based on XAS. The onset of the OER is pH-dependent on the scale of the reversible hydrogen electrode (RHE) with a Nernst slope of -40(4) mV/pH at -5 μA monitored at the RRDE ring. To connect this trend to catalyst changes, we develop a simple model for delithiation of LiMn2 O4 in LiOH electrolytes, which gives the same Nernst slope of delithiation as our experimental data, i. e., 116(25) mV/pH. From this data, we construct an ERHE -pH diagram that illustrates robustness of LiMn2 O4 against oxidation above pH 13.5 as also verified by XAS. We conclude that manganese oxidation is the origin of the increase of the OER overpotential at pH lower than 14 and also of the pH dependence on the RHE scale. Our work highlights that vulnerability to transition metal redox may lead to increased overpotentials, which is important for the design of stable electrocatalysts."],["dc.description.sponsorship","collaborative research center (CRC)"],["dc.description.sponsorship","HZB http://dx.doi.org/10.13039/100013110"],["dc.identifier.doi","10.1002/cphc.201900601"],["dc.identifier.eissn","1439-7641"],["dc.identifier.isbn","31359564"],["dc.identifier.issn","1439-4235"],["dc.identifier.purl","https://resolver.sub.uni-goettingen.de/purl?gs-1/16655"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/90626"],["dc.language.iso","en"],["dc.notes.intern","Migrated from goescholar"],["dc.relation","SFB 1073: Kontrolle von Energiewandlung auf atomaren Skalen"],["dc.relation","SFB 1073 | Topical Area C | C05 Kontrolle Elektronen-getriebener Chemie durch Interkalation"],["dc.relation.eissn","1439-7641"],["dc.relation.issn","1439-7641"],["dc.relation.issn","1439-4235"],["dc.relation.orgunit","Fakultät für Physik"],["dc.relation.orgunit","Institut für Materialphysik"],["dc.rights","CC BY 3.0"],["dc.rights.access","openAccess"],["dc.rights.uri","https://creativecommons.org/licenses/by/3.0/"],["dc.subject","X-ray absorption spectroscopy; aqueous battery; electrocatalysis; oxygen evolution reaction; pH dependence"],["dc.subject.ddc","530"],["dc.title","Undesired Bulk Oxidation of LiMn2O4 Increases Overpotential of Electrocatalytic Water Oxidation in Lithium Hydroxide Electrolytes"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.peerReviewed","yes"],["dc.type.subtype","original_ja"],["dc.type.version","published_version"],["dspace.entity.type","Publication"]]
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  • 2020Journal Article Research Paper
    [["dc.bibliographiccitation.issue","1"],["dc.bibliographiccitation.journal","Communications Materials"],["dc.bibliographiccitation.volume","1"],["dc.contributor.author","Lole, Gaurav"],["dc.contributor.author","Roddatis, Vladimir"],["dc.contributor.author","Ross, Ulrich"],["dc.contributor.author","Risch, Marcel"],["dc.contributor.author","Meyer, Tobias"],["dc.contributor.author","Rump, Lukas"],["dc.contributor.author","Geppert, Janis"],["dc.contributor.author","Wartner, Garlef"],["dc.contributor.author","Blöchl, Peter"],["dc.contributor.author","Jooss, Christian"],["dc.date.accessioned","2021-10-15T10:20:45Z"],["dc.date.available","2021-10-15T10:20:45Z"],["dc.date.issued","2020"],["dc.description.abstract","Real time in-situ microscopy imaging of surface structure and atom dynamics of heterogeneous catalysts is an important step for understanding reaction mechanisms. Here, using in-situ environmental transmission electron microscopy (ETEM), we directly visualize surface atom dynamics at manganite perovskite catalyst surfaces for oxygen evolution reaction (OER), which are ≥20 times faster in water than in other ambients. Comparing (001) surfaces of La0.6Sr0.4MnO3 and Pr0.67Ca0.33MnO3 with similar initial manganese valence state and OER activity, but very different OER stability, allows us to distinguish between reversible surface adatom dynamics and irreversible surface defect chemical reactions. We observe enhanced reversible manganese adatom dynamics due to partial solvation in adsorbed water for the highly active and stable La0.6Sr0.4MnO3 system, suggesting that aspects of homogeneous catalysis must be included for understanding the OER mechanism in heterogeneous catalysis."],["dc.identifier.doi","10.1038/s43246-020-00070-6"],["dc.identifier.uri","https://resolver.sub.uni-goettingen.de/purl?gro-2/90946"],["dc.language.iso","en"],["dc.relation","SFB 1073: Kontrolle von Energiewandlung auf atomaren Skalen"],["dc.relation","SFB 1073 | Topical Area B | B02 Photonen-getriebener Energietransfer über Grenzflächen zwischen Materialien mit starken Korrelationen"],["dc.relation","SFB 1073 | Topical Area C | C02 In situ hochauflösende Untersuchung des aktiven Zustands bei der photo- und elektrochemischen Wasserspaltung"],["dc.relation","SFB 1073 | Topical Area C | C03 Vom Elektronentransfer zur chemischen Energiespeicherung: ab-initio Untersuchungen korrelierter Prozesse"],["dc.relation.issn","2662-4443"],["dc.relation.orgunit","Institut für Materialphysik"],["dc.rights","CC BY 4.0"],["dc.title","Dynamic observation of manganese adatom mobility at perovskite oxide catalyst interfaces with water"],["dc.type","journal_article"],["dc.type.internalPublication","yes"],["dc.type.subtype","original_ja"],["dc.type.version","published_version"],["dspace.entity.type","Publication"]]
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