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    <title language="eng">Long-term corrosion studies of CrCoNi and CrMnFeCoNi in sulfuric acid</title>
    <abstract language="eng">This study investigates the long-term corrosion behavior of CrCoNi and CrMnFeCoNi MPEAs over 28 d in 1 M H2SO4. Corrosion progression and passive film evolution were analyzed using open circuit potential measurements, electrochemical impedance spectroscopy, X-ray photoelectron spectroscopy, and scanning electron microscopy. Unlike short-term polarization tests, where CrCoNi exhibited intergranular corrosion, long-term immersion resulted in a stable, Cr-rich passive oxide layer. In contrast, CrMnFeCoNi formed a porous mixed oxide layer, increasing its susceptibility to degradation and revealing a distinct corrosion mechanism. X-ray photoelectron spectroscopy tracking at weekly intervals showed that prolonged immersion led to the transformation of sulfide/sulfite species into a sulfate-containing surface film. This effect was only detectable in long-term corrosion studies. These findings provide new insights into the time-dependent degradation mechanisms of MPEAs and demonstrate that corrosion mechanisms differ significantly from short-term polarization tests. This highlights the need for long-term studies to properly assess material stability in practical applications.</abstract>
    <parentTitle language="eng">npj Materials Degradation</parentTitle>
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Corrosion progression and passive film evolution were analyzed using open circuit potential measurements, electrochemical impedance spectroscopy, X-ray photoelectron spectroscopy, and scanning electron microscopy. Unlike short-term polarization tests, where CrCoNi exhibited intergranular corrosion, long-term immersion resulted in a stable, Cr-rich passive oxide layer. In contrast, CrMnFeCoNi formed a porous mixed oxide layer, increasing its susceptibility to degradation and revealing a distinct corrosion mechanism. X-ray photoelectron spectroscopy tracking at weekly intervals showed that prolonged immersion led to the transformation of sulfide\/sulfite species into a sulfate-containing surface film. This effect was only detectable in long-term corrosion studies. These findings provide new insights into the time-dependent degradation mechanisms of MPEAs and demonstrate that corrosion mechanisms differ significantly from short-term polarization tests. 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Electrochim. Acta 48, 1093\u20131104 (2003).","journal-title":"Electrochim. Acta"},{"key":"637_CR61","doi-asserted-by":"crossref","first-page":"87","DOI":"10.1016\/0013-4686(96)00170-3","volume":"42","author":"M Keddam","year":"1997","unstructured":"Keddam, M., Kuntz, C., Takenouti, H., Schuster, D. &amp; Zuili, D. Exfoliation corrosion of aluminium alloys examined by electrode impedance. Electrochim. Acta 42, 87\u201397 (1997).","journal-title":"Electrochim. Acta"},{"key":"637_CR62","doi-asserted-by":"crossref","first-page":"1177","DOI":"10.1016\/S0010-938X(01)00145-7","volume":"44","author":"HY Ma","year":"2002","unstructured":"Ma, H. Y., Li, G. Q., Chen, S. C., Zhao, S. Y. &amp; Cheng, X. L. Impedance investigation of the anodic iron dissolution in perchloric acid solution. Corros. Sci. 44, 1177\u20131191 (2002).","journal-title":"Corros. Sci."},{"key":"637_CR63","doi-asserted-by":"crossref","first-page":"673","DOI":"10.1016\/S0010-938X(69)80098-3","volume":"9","author":"G Gilli","year":"1969","unstructured":"Gilli, G., Borea, P. &amp; Zucchi, F. &amp; Trabanel.G. Passivation of Ni caused by layers of salts in concentrated H2SO4. Corros. Sci. 9, 673 (1969). &amp;.","journal-title":"Corros. Sci."},{"key":"637_CR64","doi-asserted-by":"crossref","first-page":"927","DOI":"10.1016\/0013-4686(67)80093-8","volume":"12","author":"U Ebersbach","year":"1967","unstructured":"Ebersbach, U., Schwabe, K. &amp; Ritter, K. On the kinetics of the anodic passivation of iron, cobalt and nickel. Electrochim. Acta 12, 927\u2013938 (1967).","journal-title":"Electrochim. Acta"},{"key":"637_CR65","doi-asserted-by":"crossref","first-page":"3637","DOI":"10.1149\/1.1393952","volume":"147","author":"JR Kish","year":"2000","unstructured":"Kish, J. R., Ives, M. B. &amp; Rodda, J. R. Corrosion mechanism of nickel in hot, concentrated H2SO4. J. Electrochem. Soc. 147, 3637 (2000).","journal-title":"J. Electrochem. Soc."},{"key":"637_CR66","doi-asserted-by":"crossref","first-page":"3812","DOI":"10.1016\/j.corsci.2006.01.009","volume":"48","author":"Y Zhang","year":"2006","unstructured":"Zhang, Y., Macdonald, D. D., Urquidi-Macdonald, M., Engelhardt, G. R. &amp; Dooley, R. B. Passivity breakdown on AISI Type 403 stainless steel in chloride-containing borate buffer solution. Corros. Sci. 48, 3812\u20133823 (2006).","journal-title":"Corros. Sci."},{"key":"637_CR67","doi-asserted-by":"crossref","first-page":"421","DOI":"10.1016\/j.jelechem.2004.05.032","volume":"572","author":"DD Macdonald","year":"2004","unstructured":"Macdonald, D. D., Sun, A., Priyantha, N. &amp; Jayaweera, P. An electrochemical impedance study of alloy-22 in NaCl brine at elevated temperature: II. Reaction mechanism analysis. J. Electroanal. Chem. 572, 421\u2013431 (2004).","journal-title":"J. Electroanal. Chem."},{"key":"637_CR68","volume":"237","author":"MZ Chen","year":"2024","unstructured":"Chen, M. Z. et al. Insights into the passivity and electrochemistry of CoCrFeMnNi high entropy alloy fabricated by underwater laser direct metal deposition. Corros. Sci. 237, 112289 (2024).","journal-title":"Corros. Sci."},{"key":"637_CR69","doi-asserted-by":"crossref","first-page":"338","DOI":"10.1016\/j.actamat.2018.09.040","volume":"161","author":"G Laplanche","year":"2018","unstructured":"Laplanche, G. et al. Phase stability and kinetics of a \u03c3-phase precipitation in CrMnFeCoNi high-entropy alloys. Acta Mater. 161, 338\u2013351 (2018).","journal-title":"Acta Mater."},{"key":"637_CR70","doi-asserted-by":"crossref","first-page":"C563","DOI":"10.1149\/2.1061709jes","volume":"164","author":"YM Chen","year":"2017","unstructured":"Chen, Y. M., Rudawski, N. G., Lambers, E. &amp; Orazem, M. E. Application of impedance spectroscopy and surface analysis to obtain oxide film thickness. J. Electrochem. Soc. 164, C563\u2013C573 (2017).","journal-title":"J. Electrochem. Soc."}],"container-title":["npj Materials Degradation"],"original-title":[],"language":"en","link":[{"URL":"https:\/\/www.nature.com\/articles\/s41529-025-00637-z.pdf","content-type":"application\/pdf","content-version":"vor","intended-application":"text-mining"},{"URL":"https:\/\/www.nature.com\/articles\/s41529-025-00637-z","content-type":"text\/html","content-version":"vor","intended-application":"text-mining"},{"URL":"https:\/\/www.nature.com\/articles\/s41529-025-00637-z.pdf","content-type":"application\/pdf","content-version":"vor","intended-application":"similarity-checking"}],"deposited":{"date-parts":[[2025,7,13]],"date-time":"2025-07-13T10:14:31Z","timestamp":1752401671000},"score":1,"resource":{"primary":{"URL":"https:\/\/www.nature.com\/articles\/s41529-025-00637-z"}},"subtitle":[],"short-title":[],"issued":{"date-parts":[[2025,7,13]]},"references-count":70,"journal-issue":{"issue":"1","published-online":{"date-parts":[[2025,12]]}},"alternative-id":["637"],"URL":"https:\/\/doi.org\/10.1038\/s41529-025-00637-z","relation":{},"ISSN":["2397-2106"],"issn-type":[{"value":"2397-2106","type":"electronic"}],"subject":[],"published":{"date-parts":[[2025,7,13]]},"assertion":[{"value":"14 February 2025","order":1,"name":"received","label":"Received","group":{"name":"ArticleHistory","label":"Article History"}},{"value":"28 June 2025","order":2,"name":"accepted","label":"Accepted","group":{"name":"ArticleHistory","label":"Article History"}},{"value":"13 July 2025","order":3,"name":"first_online","label":"First Online","group":{"name":"ArticleHistory","label":"Article History"}},{"value":"The authors declare that they have no known competing financial interests or personal relationship that could have appeared to influence the work reported in this paper.","order":1,"name":"Ethics","group":{"name":"EthicsHeading","label":"Competing interests"}}],"article-number":"86"}}</enrichment>
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    <licence>Creative Commons - CC BY - Namensnennung 4.0 International</licence>
    <author>Annica Wetzel</author>
    <author>Ann-Kathrin Hans</author>
    <author>Marcus von der Au</author>
    <author>Izabella Brand</author>
    <author>Gunther Wittstock</author>
    <author>Özlem Özcan Sandikcioglu</author>
    <author>Julia Witt</author>
    <subject>
      <language>eng</language>
      <type>uncontrolled</type>
      <value>Long-term corrosion</value>
    </subject>
    <subject>
      <language>eng</language>
      <type>uncontrolled</type>
      <value>Multi-principal element alloys (MPEAs)</value>
    </subject>
    <subject>
      <language>eng</language>
      <type>uncontrolled</type>
      <value>X-ray photoelectron spectroscopy (XPS)</value>
    </subject>
    <collection role="ddc" number="620">Ingenieurwissenschaften und zugeordnete Tätigkeiten</collection>
    <collection role="institutes" number="">6 Materialchemie</collection>
    <collection role="institutes" number="">6.2 Material- und Oberflächentechnologien</collection>
    <collection role="themenfelder" number="">Material</collection>
    <collection role="themenfelder" number="">Degradationsmechanismen</collection>
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    <title language="eng">The comparison of the corrosion behavior of the CrCoNi medium entropy alloy and CrMnFeCoNi high entropy alloy</title>
    <abstract language="eng">This work presents the determination of the corrosion characteristics of CrCoNi (medium entropy alloy) and CrMnFeCoNi (high entropy alloy) in 0.1 M NaCl and 0.1 M H2SO4. The morphology and chemical composition of the oxide layers formed on CrCoNi and CrMnFeCoNi were comparatively analyzed by scanning Kelvin probe microscopy (SKPFM) and scanning electron microscopy (SEM) and supported with chemical analysis by means of inductively coupled plasma mass spectrometry (ICP-MS) and X-Ray photoelectron spectroscopy (XPS). The analysis of the 3p core level peaks showed that the oxide layer (native and after anodic passivation) on CrCoNi consisted mainly of Cr oxides, while the oxide layer on CrMnFeCoNi was primarily composed of a mixture of Cr and Fe oxides. In addition, XPS was utilized to assess the oxide layer thicknesses. These results were compared to the thicknesses obtained by means of electrochemical impedance spectroscopy (EIS), with both approaches yielding values up to about 4 nm depending on the electrolyte and the alloy. Cyclic polarization measurements indicated superior corrosion resistance of CrCoNi in both aqueous environments compared to CrMnFeCoNi, as well as to AISI 304 stainless steel.</abstract>
    <parentTitle language="eng">Applied Surface Science</parentTitle>
    <identifier type="doi">10.1016/j.apsusc.2022.154171</identifier>
    <identifier type="issn">0169-4332</identifier>
    <identifier type="urn">urn:nbn:de:kobv:b43-559902</identifier>
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    <enrichment key="date_peer_review">19.10.2022</enrichment>
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    <licence>Creative Commons - CC BY - Namensnennung 4.0 International</licence>
    <author>Annica Wetzel</author>
    <author>Marcus von der Au</author>
    <author>P. M. Dietrich</author>
    <author>Jörg Radnik</author>
    <author>Özlem Özcan Sandikcioglu</author>
    <author>Julia Witt</author>
    <subject>
      <language>eng</language>
      <type>uncontrolled</type>
      <value>Medium entropy alloy</value>
    </subject>
    <subject>
      <language>eng</language>
      <type>uncontrolled</type>
      <value>High entropy alloy</value>
    </subject>
    <subject>
      <language>eng</language>
      <type>uncontrolled</type>
      <value>SKPFM</value>
    </subject>
    <subject>
      <language>eng</language>
      <type>uncontrolled</type>
      <value>XPS</value>
    </subject>
    <subject>
      <language>eng</language>
      <type>uncontrolled</type>
      <value>Passivation</value>
    </subject>
    <subject>
      <language>eng</language>
      <type>uncontrolled</type>
      <value>Corrosion</value>
    </subject>
    <collection role="ddc" number="620">Ingenieurwissenschaften und zugeordnete Tätigkeiten</collection>
    <collection role="institutes" number="">1 Analytische Chemie; Referenzmaterialien</collection>
    <collection role="institutes" number="">1.1 Anorganische Spurenanalytik</collection>
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    <collection role="institutes" number="">6.1 Oberflächen- und Dünnschichtanalyse</collection>
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    <file>https://opus4.kobv.de/opus4-bam/files/55990/AppSurfSci_2022_Wetzel.pdf</file>
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    <publishedYear>2024</publishedYear>
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    <title language="eng">Transpassive Metal Dissolution vs. Oxygen Evolution Reaction: Implication for Alloy Stability and Electrocatalysis</title>
    <title language="deu">Transpassive Metallauflösung vs. Sauerstoffentwicklung:&#13;
Auswirkungen auf Legierungsstabilität und Elektrokatalyse</title>
    <abstract language="eng">Multi-principal element alloys (MPEAs) are gaining interest in corrosion and electrocatalysis research due to their electrochemical stability across a broad pH range and the design flexibility they offer. Using the equimolar CrCoNi alloy, we observe significant metal dissolution in a corrosive electrolyte (0.1 M NaCl, pH 2) concurrently with the oxygen evolution reaction (OER) in the transpassive region despite the absence of hysteresis in polarization curves or other obvious corrosion indicators. We present a characterization scheme to delineate the contribution of OER and alloy dissolution, using scanning electrochemical microscopy (SECM) for OER-onset detection, and quantitative chemical analysis with inductively coupled-mass spectrometry (ICP-MS) and ultraviolet visible light (UV-Vis) spectroscopy to elucidate metal dissolution processes. In-situ electrochemical atomic force microscopy (EC-AFM) revealed that the transpassive metal dissolution on CrCoNi is dominated by intergranular corrosion. These results have significant implications for the stability of MPEAs in corrosion systems, emphasizing the necessity of analytically determining metal ions released from MPEA electrodes into the electrolyte when evaluating Faradaic efficiencies of OER catalysts. The release of transition metal ions not only reduces the Faradaic efficiency of electrolyzers but may also cause poisoning and degradation of membranes in electrochemical reactors.</abstract>
    <abstract language="deu">Multi-Hauptelement-Legierungen (MPEAs) gewinnen in der Korrosions- und Elektrokatalyseforschung aufgrund ihrer elektrochemischen Stabilität über einen breiten pH-Bereich und der Vielfalt der möglichen chemischen Zusammensetzungen zunehmend an Interesse. In unseren Untersuchungen mit der äquimolaren CrCoNi-Legierung in einem sauren Elektrolyten (0.1 M NaCl, pH 2) beobachteten wir eine signifikante Metallauflösung, die mit der Sauerstoffentwicklungsreaktion (OER) im transpassiven Bereich einhergeht, obwohl in zyklischen Polarisationskurven keine Hysterese auftrat oder andere offensichtliche Korrosionsindikatoren vorlagen. In diesem Artikel wird ein Charakterisierungskonzept eingeführt, dass die Beiträge der OER und der Legierungsauflösung differenziert. Hierfür kommt die elektrochemische Rastermikroskopie (SECM) zum Nachweis des Beginns der OER und die quantitative chemische Analyse mit induktiv gekoppelter Massenspektrometrie (ICP-MS) und UV/Vis-Spektrometrie zur Aufklärung der Metallauflösungsprozesse zum Einsatz. Die elektrochemische In situ-Atomkraftmikroskopie (EC-AFM) zeigte, dass die intergranulare Korrosion der dominierende Mechanismus der transpassive Metallauflösung von CrCoNi ist. Diese Ergebnisse besitzen erhebliche Auswirkungen für die Beurteilung der Stabilität von MPEAs in Korrosionssystemen und der Stromausbeute von OER-Katalysatoren auf der Basis von MPEAs. Die Daten unterstreichen die Notwendigkeit der analytischen Bestimmung von Metallionen, die von MPEA-Elektroden freigesetzt werden. Die Freisetzung von Übergangsmetallionen verringert nicht nur die Stromausbeute von Elektrolyseuren, sondern kann zu einer Schädigung von Membranen in elektrochemischen Reaktoren führen.</abstract>
    <parentTitle language="eng">Angewandte Chemie International Edition</parentTitle>
    <identifier type="doi">10.1002/anie.202317058</identifier>
    <identifier type="urn">urn:nbn:de:kobv:b43-597045</identifier>
    <enrichment key="opus.source">publish</enrichment>
    <enrichment key="date_peer_review">20.03.2024</enrichment>
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    <licence>Creative Commons - CC BY - Namensnennung 4.0 International</licence>
    <author>Annica Wetzel</author>
    <author>Daniel Morell</author>
    <author>Marcus von der Au</author>
    <author>Gunther Wittstock</author>
    <author>Özlem Özcan Sandikcioglu</author>
    <author>Julia Witt</author>
    <subject>
      <language>eng</language>
      <type>uncontrolled</type>
      <value>Transpassive dissolution</value>
    </subject>
    <subject>
      <language>eng</language>
      <type>uncontrolled</type>
      <value>Corrosion</value>
    </subject>
    <subject>
      <language>eng</language>
      <type>uncontrolled</type>
      <value>Multi-prinicpal element alloys (MPEAs)</value>
    </subject>
    <subject>
      <language>eng</language>
      <type>uncontrolled</type>
      <value>Passivation</value>
    </subject>
    <collection role="ddc" number="620">Ingenieurwissenschaften und zugeordnete Tätigkeiten</collection>
    <collection role="institutes" number="">1 Analytische Chemie; Referenzmaterialien</collection>
    <collection role="institutes" number="">1.4 Non-Target-Analytik</collection>
    <collection role="institutes" number="">6 Materialchemie</collection>
    <collection role="institutes" number="">6.2 Material- und Oberflächentechnologien</collection>
    <collection role="themenfelder" number="">Material</collection>
    <collection role="themenfelder" number="">Degradationsmechanismen</collection>
    <collection role="literaturgattung" number="">Verlagsliteratur</collection>
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    <thesisPublisher>Bundesanstalt für Materialforschung und -prüfung (BAM)</thesisPublisher>
    <file>https://opus4.kobv.de/opus4-bam/files/59704/2024.Wetzel_et_al.AngewChemIntEd.e202317058_DE.pdf</file>
    <file>https://opus4.kobv.de/opus4-bam/files/59704/2024.Wetzel_et_al.AngewChemIntEd.e202317058.pdf</file>
  </doc>
  <doc>
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    <publishedYear>2024</publishedYear>
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    <pageLast>9</pageLast>
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    <title language="eng">Transpassive Behavior of Equimolar CrMnFeCoNi and CrCoNi Multi‐Principal Element Alloys in an Alkaline NaCl Electrolyte</title>
    <abstract language="eng">AbstractWe investigated the corrosion properties and transpassive behavior of CrMnFeCoNi and CrCoNi multi‐principal element alloys (MPEAs) in a 0.1 M NaCl electrolyte at pH 12. By using SECM‐based tip substrate voltammetry (TSV) in combination with the chemical analysis of the electrolyte, we were able to differentiate between anodic metal dissolution and oxygen evolution in the transpassive range. Our investigations have shown that CrCoNi has a significantly higher corrosion resistance compared to CrMnFeCoNi. In the studied alkaline environment, a transpassive oxide film is formed on the surface of CrCoNi during secondary passivation. This transpassive oxide film appears to play a significant role in oxygen evolution, as the increase in TSV currents at the microelectrode coincides with the corresponding current density plateau of the voltametric current trace. The formation of the transpassive oxide film was not observed in previous studies conducted in acidic environments. Moreover, the alkaline electrolyte induced a positive hysteresis and mild pitting corrosion, in addition to intergranular corrosion, which was the sole corrosion process observed at acidic pH levels. These findings enhance the understanding of the processes governing the transpassivity of CrMnFeCoNi and CrCoNi MPEAs in alkaline environments and have potential implications for the development of application‐tailored corrosion‐resistant MPEAs.</abstract>
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    <author>Annica Wetzel</author>
    <author>Daniel Morell</author>
    <author>Marcus von der Au</author>
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      <value>Oxygen evolution reaction</value>
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      <value>Transpassive region</value>
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