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Tassadit Ouaneche, Lorenzo Stievano, Laure Monconduit, Claude Guéry, Moulay Tahar Sougrati, and Nadir Recham
Wiley
AbstractSodium‐ion batteries continue to rise in the energy storage landscape, their increasing adoption being driven by factors such as cost‐effectiveness and sustainability. As a consequence, there is a growing emphasis on the development of new electrode materials. Among these, olivine phosphates emerge as a promising family of cathode materials. However, viable synthesis routes are still lacking. In this study, cathode materials of olivine NaMn1‐xFexPO4 (x=0.34 and 1) were prepared by directly sodiating Mn1‐xFexPO4 through a solid‐state process at 300 °C. X‐ray diffraction, Mössbauer spectroscopy and electrochemical measurements were employed to study their structural and electrochemical features. NaMn0.66Fe0.34PO4 exhibits two pseudo‐plateaus profile with an average potential of ~3.2 V vs. Na+/Na0 with a reversible capacity reaching 75 mAh/g at C/20 via a monophasic (de)intercalation mechanism. In parallel, the intermediate composition Na0.5Mn0.66Fe0.34PO4 could be prepared via the solid‐state reaction of NaMn0.66Fe0.34PO4 and Mn0.66Fe0.34PO4. Such a solvent‐free sodiation process not only provides a simplified preparation of NMFP, but also offers easy scalability compared to the more laborious electrochemical sodiation route, making it an interesting prospect for future industrialization. Finally, this research confirms that the olivine NMFP is indeed an attractive candidate as a cathode material for SIBs.
Yu-Ping Ku, Kavita Kumar, Andreas Hutzler, Carina Götz, Michael Vorochta, Moulay Tahar Sougrati, Vicent Lloret, Konrad Ehelebe, Karl J. J. Mayrhofer, Simon Thiele,et al.
American Chemical Society (ACS)
C. Mir, D. Giaume, M. Morcrette, M. T. Sougrati, G. Wallez, M. Courty, M. Chakir, and P. Barboux
Royal Society of Chemistry (RSC)
We studied the electrochemical lithium intercalation in LiOHFeS. After a first irreversible reaction the resulting new material reversibly cycles one lithium atom involving the Fe3+/Fe2+ redox couple: Li2FeOS ↔ Li+ + e− + LiFeOS.
Tassadit Ouaneche, Lorenzo Stievano, Laure Monconduit, Claude Guéry, Moulay Tahar Sougrati, and Nadir Recham
Elsevier BV
Joshua Vauloup, Cécile Bouilhac, Moulay Tahar Sougrati, Lorenzo Stievano, Nicolas Coppey, Andrea Zitolo, Laure Monconduit, and Patrick Lacroix-Desmazes
Elsevier BV
Zinan Wang, Kaiqi Nie, Moulay Tahar Sougrati, Chang Wang, Zhiqi Liu, Jiaou Wang, Rile Ge, Qiong Zheng, and Junhu Wang
Elsevier BV
Zinan Wang, Moulay Tahar Sougrati, Qiong Zheng, Rile Ge, and Junhu Wang
American Chemical Society (ACS)
Prussian blue analogues receive tremendous attention owing to their spacious three-dimensional skeleton, high theoretical specific capacity, facile synthesis procedure, and high cost-effectiveness as among the most promising candidates for cathode materials in sodium-ion batteries (SIBs). Nonetheless, the practical specific capacity, especially under high current, is particularly frail due to the sluggish ion diffusion. In this study, the strategy of Ni substitution and formation of water-coordinated Fe is applied to lower the crystal field energy and elevate the active low-spin (LS) Fe content, which leads to a capacitive sodium storage mechanism, resulting in a substantial specific capacity under high current density. The delivered specific capacity of PW-325@2NiFe-55 is 95 mAh g-1 at 50 C, which is 72.5% capacity retention of the one at 0.5 C. Also, it maintains 80.2% of its initial specific capacity after 500 cycles at 5 C. Furthermore, a hypothesis of a joint diffusion-controlled and capacitive mechanism for high-spin (HS) Fe and a mere capacitive mechanism for LS Fe is put forward and verified through potentiastatic tests, operando 57Fe Mössbauer spectroscopy, and ex situ XRD, which provides a new horizon to enhance the electrochemical performance for SIBs.
Camilla Tacconis, Sunita Dey, Carson D. McLaughlin, M. Sougrati, Christopher A O'Keefe, Iuliia Mikulska, C. P. Grey and Siân E Dutton
Jason S. Bates, Jesse J. Martinez, Melissa N. Hall, Abdulhadi A. Al-Omari, Eamonn Murphy, Yachao Zeng, Fang Luo, Mathias Primbs, Davide Menga, Nicolas Bibent,et al.
American Chemical Society (ACS)
Mononuclear Fe ions ligated by nitrogen (FeNx) dispersed on nitrogen-doped carbon (Fe-N-C) serve as active centers for electrocatalytic O2 reduction and thermocatalytic aerobic oxidations. Despite their promise as replacements for precious metals in a variety of practical applications, such as fuel cells, the discovery of new Fe-N-C catalysts has relied primarily on empirical approaches. In this context, the development of quantitative structure-reactivity relationships and benchmarking of catalysts prepared by different synthetic routes and by different laboratories would be facilitated by the broader adoption of methods to quantify atomically dispersed FeNx active centers. In this study, we develop a kinetic probe reaction method that uses the aerobic oxidation of a model hydroquinone substrate to quantify the density of FeNx centers in Fe-N-C catalysts. The kinetic method is compared with low-temperature Mössbauer spectroscopy, CO pulse chemisorption, and electrochemical reductive stripping of NO derived from NO2- on a suite of Fe-N-C catalysts prepared by diverse routes and featuring either the exclusive presence of Fe as FeNx sites or the coexistence of aggregated Fe species in addition to FeNx. The FeNx site densities derived from the kinetic method correlate well with those obtained from CO pulse chemisorption and Mössbauer spectroscopy. The broad survey of Fe-N-C materials also reveals the presence of outliers and challenges associated with each site quantification approach. The kinetic method developed here does not require pretreatments that may alter active-site distributions or specialized equipment beyond reaction vessels and standard analytical instrumentation.
Geunsu Bae, Minho M. Kim, Man Ho Han, Junsic Cho, Dong Hyun Kim, Moulay-Tahar Sougrati, Jinjong Kim, Kug-Seung Lee, Sang Hoon Joo, William A. Goddard,et al.
Springer Science and Business Media LLC
Tassadit Ouaneche, Matthieu Courty, Lorenzo Stievano, Laure Monconduit, Claude Guéry, Moulay T. Sougrati, and Nadir Recham
Elsevier BV
Carlos Berlanga, Moulay Tahar Sougrati, Antonio J. Fernández-Ropero, Neyrouz Baaboura, Nicholas E. Drewett, Juan M. Lopez del Amo, Gene Nolis, Jose S. Garitaonandia, Marine Reynaud, Lorenzo Stievano,et al.
Royal Society of Chemistry (RSC)
Through a combination of multimodal operando, as well as and ex situ, and in situ techniques: Unravelling the intrinsic factors underlying the electrochemical activation of maricite-NaFePO4.
Aaron Roy, Leonardo Girardi, Dario Mosconi, Moulay Tahar Sougrati, Deborah Jones, Stefano Agnoli, and Frédéric Jaouen
Elsevier BV
Atin Pramanik, Alexis G. Manche, Megan T. Smeaton, Moulay‐Tahar Sougrati, Philip Lightfoot, and Anthony Robert Armstrong
Wiley
AbstractThe iron‐based polyanionic fluoro‐oxalate material, KFe(C2O4)F (KFCF), has been synthesized by hydrothermal methods. This compound shows promising reversible lithium and sodium insertion properties as a cathode material. The material delivered a first‐cycle discharge capacity of 120 mAh g−1 at ∼3.3 V (Li+/Li) and 97.4 mAh g−1 at ∼3.0 V (Na+/Na) in LIB and NIB, respectively. Stable cycling performance was observed in both cases. The involvement of reversible Fe2+/Fe3+ redox was confirmed by ex‐situ Mössbauer spectroscopy supported by first‐principles calculations. This study reveals promising performance from a mixed oxalate‐fluoride based polyanionic material thereby opening up further possibilities for materials discovery in the design of new electrode materials.
Fang Luo, Aaron Roy, Moulay Tahar Sougrati, Anastassiya Khan, David A. Cullen, Xingli Wang, Mathias Primbs, Andrea Zitolo, Frédéric Jaouen, and Peter Strasser
American Chemical Society (ACS)
While improved activity was recently reported for bimetallic iron-metal-nitrogen-carbon (FeMNC) catalysts for the oxygen reduction reaction (ORR) in acid medium, the nature of active sites and interactions between the two metals are poorly understood. Here, FeSnNC and FeCoNC catalysts were structurally and catalytically compared to their parent FeNC and SnNC catalysts. While CO cryo-chemisorption revealed a twice lower site density of M-Nx sites for FeSnNC and FeCoNC relative to FeNC and SnNC, the mass activity of both bimetallic catalysts is 50-100% higher than that of FeNC due to a larger turnover frequency in the bimetallic catalysts. Electron microscopy and X-ray absorption spectroscopy identified the coexistence of Fe-Nx and Sn-Nx or Co-Nx sites, while no evidence was found for binuclear Fe-M-Nx sites. 57Fe Mössbauer spectroscopy revealed that the bimetallic catalysts feature a higher D1/D2 ratio of the spectral signatures assigned to two distinct Fe-Nx sites, relative to the FeNC parent catalyst. Thus, the addition of the secondary metal favored the formation of D1 sites, associated with the higher turnover frequency.
Zinan Wang, Moulay Tahar Sougrati, Yawen He, Phuong Nam Le Pham, Wei Xu, Antonella Iadecola, Rile Ge, Wenhui Zhou, Qiong Zheng, Xianfeng Li,et al.
Elsevier BV
Diana I. Pchelina, Vera D. Sedykh, Nataliya I. Chistyakova, Vyacheslav S. Rusakov, Yulia A. Alekhina, Alexey N. Tselebrovskiy, Bernard Fraisse, Lorenzo Stievano, and Moulay Tahar Sougrati
Elsevier BV
Atin Pramanik, Alexis G. Manche, Moulay Tahar Sougrati, Alan V. Chadwick, Philip Lightfoot, and A. Robert Armstrong
American Chemical Society (ACS)
Benedikt Klobes, Manuel Angst, Daniela Fenske, Chinmay M. Konnur, Abdelfattah Mahmoud, and Moulay Tahar Sougrati
Elsevier BV
Jérôme Bodart, Nicolas Eshraghi, Moulay Tahar Sougrati, Frédéric Boschini, Pierre-Emmanuel Lippens, Bénédicte Vertruyen, and Abdelfattah Mahmoud
Elsevier BV
Hongxin Ge, Nicolas Bibent, Keyla Teixeira Santos, Kavita Kumar, Julien Jaxel, Moulay-Tahar Sougrati, Andrea Zitolo, Marc Dupont, Frédéric Lecoeur, Michel Mermoux,et al.
American Chemical Society (ACS)
Phuong Nam Le Pham, Romain Wernert, Maëlle Cahu, Moulay Tahar Sougrati, Giuliana Aquilanti, Patrik Johansson, Laure Monconduit, and Lorenzo Stievano
Royal Society of Chemistry (RSC)
A comprehensive evaluation of a Mn–Fe-based Prussian Blue Analogue suited as positive electrode material for K-ion batteries is made by complementary ex situ and operando characterization techniques – showing fundamental promises and limitations.
Fang Luo, Aaron Roy, Luca Silvioli, David A. Cullen, Andrea Zitolo, Moulay Tahar Sougrati, Ismail Can Oguz, Tzonka Mineva, Detre Teschner, Stephan Wagner,et al.
Springer Science and Business Media LLC
Fabien Eveillard, Quentin Loiseleux, Régis Porhiel, Malika El-Ghozzi, Pierre Bonnet, Moulay Tahar Sougrati, Diane Delbegue, and Katia Guerin
Elsevier BV
Thomas Marchandier, Sathiya Mariyappan, Maria A. Kirsanova, Artem M. Abakumov, Gwenaëlle Rousse, Dominique Foix, Moulay‐Tahar Sougrati, Marie Liesse Doublet, and Jean‐Marie Tarascon
Wiley