Solving the surface (electro-)chemical instability and the fading behavior of high voltage cathode materials cycled above 4.3 V vs Li/Li remains a major challenge for the next generation of high energy density Li-ion batteries. Here, we present a facile, environmentally friendly, cost effective and scalable method to address this problem by uniformly fluorinating the surface of cathode materials with a mild fluorinating agent (CHF) using a gas flow-type reactor.
View Article and Find Full Text PDFMaintaining the electrochemically and mechanically stable solid electrolyte interphase (SEI) is of highest importance for the performance of high-capacity anode materials such as silicon (Si). Applying flexible Li-ion permeable coatings to the electrode surface using molecular layer deposition (MLD) offers a strategy to improve the properties of the SEI and greatly contributes to an increase in the cycle life and capacity retention of Si electrodes. In this study, the long-term cycling of Si electrodes with an MLD alucone coating is investigated in the context of more stable SEI formation.
View Article and Find Full Text PDFSensors that can accurately assess oxygen (O) concentrations in real time are crucial for a wide range of applications spanning personal health monitoring, environmental protection, and industrial process development. Here a high-performance chemiresistive sensor that allows for the rapid detection of O at room temperature under visible light illumination is described. Inspired by the operating principles of dye-sensitized solar cells, the chemiresistor is based on a single-walled carbon nanotube-titania hybrid (SWCNT-TiO) bearing a molecular Re-based photosensitizer [(bpy)(CO)ReBr] (bpy = 4,4'-[P(O)(OH)]-2,2'-bipyridine).
View Article and Find Full Text PDFAngew Chem Int Ed Engl
November 2024
Broadening the scope of functionalities that can be covalently bound to single-walled carbon nanotubes (SWCNTs) is crucial for enhancing the versatility of this promising nanomaterial class in applied settings. Here we report the covalent linkage of triphenylphosphine oxide [PhP(O)] to SWCNTs, a hitherto overlooked surface functionality. We detail the synthesis and structural characterization of a new family of phosphine oxide-functionalized diaryliodonium salts that can facilitate direct PhP(O) transfer and afford novel SWCNTs with tunable PhP(O) content (SWCNT-P).
View Article and Find Full Text PDFCo-based catalysts are promising candidates to replace Ir/Ru-based oxides for oxygen evolution reaction (OER) catalysis in an acidic environment. However, both the reaction mechanism and the active species under acidic conditions remain unclear. In this study, by combining surface-sensitive soft X-ray absorption spectroscopy characterization with electrochemical analysis, we discover that the acidic OER activity of Co-based catalysts are determined by their surface oxidation/spin state.
View Article and Find Full Text PDFWe addressed the poor interfacial stability of the Li metal anode in Li-S batteries through molecular regulation of electrolytes using arylthiol additives with various numbers of anchoring sites. The dual functional tetrathiol additive markedly enhanced the Li anode interfacial stability, controlled the sulfur redox kinetics and suppressed side reactions towards polysulfides, thus leading to an improved capacity retention of 70% after 500 cycles at 1 C.
View Article and Find Full Text PDFSustainable water oxidation requires low-cost, stable, and efficient redox couples, photosensitizers, and catalysts. Here, we introduce the self-assembly of metal-atom-free organic-based semiconductive structures on the surface of carbon supports. The resulting TTF/TTF@carbon junction (TTF = tetrathiafulvalene) acts as an all-in-one highly stable redox-shuttle/photosensitizer/molecular-catalyst triad for the visible-light-driven water oxidation reaction (WOR) at neutral pH, eliminating the need for metallic or organometallic catalysts and sacrificial electron acceptors.
View Article and Find Full Text PDFSodium chromium hexacyanoferrate (NaCrHCF) is obtained here using a facile co-precipitation method at room temperature. The powder was investigated in terms of potential use as a cathode material for aqueous sodium-ion batteries under neutral conditions. The highest achieved discharge capacity of NaCrHCF was around ∼64 mA h g-1 at C/3 current rate.
View Article and Find Full Text PDFIn this paper we would like to show a new approach to an explanation of the nature of the discharge-charge curve of Na/Na(+)/NaxCoO2-y batteries, which can justify the existence of the step-like characteristics. This is still an open problem, which until now had no proper description in the literature. On the basis of comprehensive experimental studies of physicochemical properties of NaxCoO2-y cathode material (XRD, electrical conductivity, thermoelectric power, electronic specific heat) supported by calculations performed using the DFT method with accounting for chemical disorder, it has been shown that the observed step-like character of the discharge curve reflects the variation of the chemical potential of electrons (Fermi level) in the density of states of NaxCoO2-y, which is anomalously perturbed by the presence of the oxygen vacancy defects and sodium ordering.
View Article and Find Full Text PDF