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Time-resolved spectroscopy uncovers deprotonation-induced reconstruction in oxygen-evolution NiFe-based (oxy)hydroxides.
Nat Commun
January 2025
National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, PR China.
Transition-metal layered double hydroxides are widely utilized as electrocatalysts for the oxygen evolution reaction (OER), undergoing dynamic transformation into active oxyhydroxides during electrochemical operation. Nonetheless, our understanding of the non-equilibrium structural changes that occur during this process remains limited. In this study, utilizing in situ energy-dispersive X-ray absorption spectroscopy and machine learning analysis, we reveal the occurrence of deprotonation and elucidate the role of incorporated iron in facilitating the transition from nickel-iron layered double hydroxide (NiFe LDH) into its active oxyhydroxide.
View Article and Find Full Text PDFOperando Studies Redirect Spatiotemporal Restructuration of Model Coordinated Oxides in Electrochemical Oxidation.
Adv Mater
December 2024
WA School of Mines: Minerals, Energy and Chemical Engineering, Curtin University, Perth, WA, 6102, Australia.
Article Synopsis
- Tetrahedral, pyramidal, and octahedral metal-oxygen coordinated ligands are key to metal-oxide structures, with their behavior during electrochemical oxidation being critical yet underexplored.
- A study links oxygen-evolving performance to structural properties of model oxides, finding that pyramidal structures are more vulnerable to hydroxide (OH) attacks, leading to transformation into active amorphous CoOOH.
- The research proposes an ion-tuning strategy to improve both activity and stability in metal oxides, addressing the challenge of balancing performance and structural durability in electrochemical applications.
Crystallographic Dimensionality Determines the Electrochemical Reaction Mechanism in Alkali Transition-Metal Chlorides.
J Am Chem Soc
November 2024
Department of Chemistry, Boston College, Chestnut Hill, Massachusetts 02467, United States.
Intense research efforts on transition metal chalcogenides (oxides and sulfides), pnictides (nitrides and phosphides), and fluorides have demonstrated the complex, intertwined effects of structural and chemical changes on their electrochemical response leading to intercalation, conversion, or displacement reactions when reacting with lithium. Prior efforts largely left halides unexplored due to their heightened solubility in classical liquid electrolytes. In this work, we employ superconcentrated electrolytes to demonstrate the composition- and structure-dependent electrochemical reactivity of AMCl compounds (A = Li or Na and M = Cr, Mn, Fe, and Co).
View Article and Find Full Text PDFBuckling cluster-based H-bonded icosahedral capsules and their propagation to a robust zeolite-like supramolecular framework.
Nat Commun
October 2024
Key Laboratory of Colloid and Interface Chemistry, Ministry of Education, School of Chemistry and Chemical Engineering, State Key Laboratory of Crystal Materials, Shandong University, Jinan, PR China.
Hydrogen-bonded assembly of multiple components into well-defined icosahedral capsules akin to virus capsids has been elusive. In parallel, constructing robust zeolitic-like cluster-based supramolecular frameworks (CSFs) without any coordination covalent bonding linkages remains challenging. Herein, we report a cluster-based pseudoicosahedral H-bonded capsule Cu, which is buckled by the self-organization of judiciously designed constituent copper clusters and anions.
View Article and Find Full Text PDFOrganic phosphates (OP) are important nutrient components for living cells in natural environments, where they readily interact with ubiquitous iron phases such as hydrous ferric oxide, ferrihydrite (FHY). FHY partakes in many key bio(geo)chemical reactions including iron-mediated carbon storage in soils, or iron-storage in living organisms. However, it is still unknown how OP affects the formation, structure and properties of FHY.
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