Iridium (Ir) is the most active and durable anode catalyst for the oxygen evolution reaction (OER) for proton exchange membrane water electrolyzers (PEMWEs). However, their large-scale applications are hindered by high costs and scarcity of Ir. Lowering Ir loadings below 1.
View Article and Find Full Text PDFAn environmental-friendly and sustainable carbon-based host is one of the most competitive strategies for achieving high loading and practicality of Li-S batteries. However, the polysulfide conversion reaction kinetics is still limited by the nonuniform or monofunctional catalyst configuration in the carbon host. In this work, we propose a catalysis mode based on "relay-type" co-operation by adjacent dual-metal single atoms for high-rate and durable Li-S batteries.
View Article and Find Full Text PDFJ Am Chem Soc
November 2023
Ammonia is of great importance in fertilizer production and chemical synthesis. It can also potentially serve as a carbon-free energy carrier for a future hydrogen economy. Motivated by a worldwide effort to lower carbon emissions, ammonia synthesis by lithium-mediated electrochemical nitrogen reduction (LiNR) has been considered as a promising alternative to the Haber-Bosch process.
View Article and Find Full Text PDFAnode-free lithium (Li) batteries are attractive owing to their high energy density. However, Li loss by forming solid-electrolyte interphase (SEI) during cell activation leads to a ≈25% capacity decrease, and the capacity constantly fades upon cycling due to the side reactions on the copper (Cu) current collector. This paper reports high-initial-efficiency, long-cycle-life, and long-calendar-life anode-free Li batteries by using an organic Li salt monolayer bonded on Cu.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
July 2023
Anode-free lithium (Li) metal batteries are desirable candidates in pursuit of high-energy-density batteries. However, their poor cycling performances originated from the unsatisfactory reversibility of Li plating/stripping remains a grand challenge. Here we show a facile and scalable approach to produce high-performing anode-free Li metal batteries using a bioinspired and ultrathin (250 nm) interphase layer comprised of triethylamine germanate.
View Article and Find Full Text PDFThe rising demand for energy density of cathodes means the need to raise the voltage or capacity of cathodes. Transition metal (TM) doping has been employed to enhance the electrochemical properties in multiple aspects. The redox voltage of doped cathodes usually falls in between the voltage of undoped layered cathodes.
View Article and Find Full Text PDFLithium metal is a very promising anode material for achieving high energy density for next generation battery systems due to its low redox potential and high theoretical specific capacity of 3860 mA h g. However, dendrite formation and low coulombic efficiency during cycling greatly hindered its practical applications. The formation of a stable solid electrolyte interphase (SEI) on the lithium metal anode (LMA) holds the key to resolving these problems.
View Article and Find Full Text PDFElectrochemical oxygen reduction could proceed via either 4e-pathway toward maximum chemical-to-electric energy conversion or 2e-pathway toward onsite HO production. Bulk Pt catalysts are known as the best monometallic materials catalyzing O-to-HO conversion, however, controversies on the reduction product selectivity are noted for atomic dispersed Pt catalysts. Here, we prepare a series of carbon supported Pt single atom catalyst with varied neighboring dopants and Pt site densities to investigate the local coordination environment effect on branching oxygen reduction pathway.
View Article and Find Full Text PDFOrganic electrode materials have been considered as promising candidates for the next generation rechargeable battery systems due to their high theoretical capacity, versatility, and environmentally friendly nature. Among them, organosulfur compounds have been receiving more attention in conjunction with the development of lithium-sulfur batteries. Usually, organosulfide electrodes can deliver a relatively high theoretical capacity based on reversible breakage and formation of disulfide (S-S) bonds.
View Article and Find Full Text PDFThe increasing demand for energy storage is calling for improvements in cathode performance. In traditional layered cathodes, the higher energy of the metal 3d over the O 2p orbital results in one-band cationic redox; capacity solely from cations cannot meet the needs for higher energy density. Emerging anionic redox chemistry is promising to access higher capacity.
View Article and Find Full Text PDFAnionic redox is an effective way to boost the energy density of layer-structured metal-oxide cathodes for rechargeable batteries. However, inherent rigid nature of the TMO (TM: transition metals) subunits in the layered materials makes it hardly tolerate the inner strains induced by lattice glide, especially at high voltage. Herein, P2-Na Mg [Mn Co Mg □ ]O (□: TM vacancy) is designed that contains vacancies in TM sites, and Mg ions in both TM and sodium sites.
View Article and Find Full Text PDFSulfurized polyacrylonitrile (SPAN) is a promising high-capacity cathode material. In this work, we use spatially resolved X-ray absorption spectroscopy combined with X-ray fluorescence (XRF) microscopy, X-ray photoelectron spectroscopy, and scanning electron microscopy to examine the structural transformation of SPAN and the critical role of a robust cathode-electrolyte interface (CEI) on the electrode. LiS species forms during the cycling of SPAN.
View Article and Find Full Text PDFA novel electrolyte system with an excellent low-temperature performance for lithium-ion batteries (LIBs) has been developed and studied. It was discovered for the first time, in this work, that when isoxazole (IZ) was used as the main solvent, the ionic conductivity of the electrolyte for LIBs is more than doubled in a temperature range between -20 and 20 °C compared to the baseline electrolyte using ethylene carbonate-ethyl methyl carbonate as solvents. To solve the problem of solvent co-intercalation into the graphite anode and/or electrolyte decomposition, the lithium difluoro(oxalato)borate (LiDFOB) salt and fluoroethylene carbonate (FEC) additive were used to form a stable solid electrolyte interphase on the surface of the graphite anode.
View Article and Find Full Text PDFHigh-nickel content cathode materials offer high energy density. However, the structural and surface instability may cause poor capacity retention and thermal stability of them. To circumvent this problem, nickel concentration-gradient materials have been developed to enhance high-nickel content cathode materials' thermal and cycling stability.
View Article and Find Full Text PDFP3-Na0.65Mn0.5Al0.
View Article and Find Full Text PDFA comprehensive understanding of the solid-electrolyte interphase (SEI) composition is crucial to developing high-energy batteries based on lithium metal anodes. A particularly contentious issue concerns the presence of LiH in the SEI. Here we report on the use of synchrotron-based X-ray diffraction and pair distribution function analysis to identify and differentiate two elusive components, LiH and LiF, in the SEI of lithium metal anodes.
View Article and Find Full Text PDFLiNiMnCoO (NMC) is an important class of high-energy-density cathode materials. The possibility of changing both and in the chemical formula provides numerous materials with diverse electrochemical and structural properties. It is highly desirable to have guidance on correlating NMC structural and electrochemical properties with their chemical composition for material designing and screening.
View Article and Find Full Text PDFHigh-energy-density batteries with a LiCoO (LCO) cathode are of significant importance to the energy-storage market, especially for portable electronics. However, their development is greatly limited by the inferior performance under high voltages and challenging temperatures. Here, highly stable lithium (Li) metal batteries with LCO cathode, through the design of in situ formed, stable electrode/electrolyte interphases on both the Li anode and the LCO cathode, with an advanced electrolyte, are reported.
View Article and Find Full Text PDFThe use of anion redox reactions is gaining interest for increasing rechargeable capacities in alkaline ion batteries. Although anion redox coupling of S and (S) through dimerization of S-S in sulfides have been studied and reported, an anion redox process through electron hole formation has not been investigated to the best of our knowledge. Here, we report an O3-NaCrTiS cathode that delivers a high reversible capacity of ~186 mAh g (0.
View Article and Find Full Text PDFA Prussian blue LiFeFe(CN) thin-film cathode is fabricated by a nonvacuum coating technology without post-annealing process. The thin film of the solid electrolyte lithium phosphorus oxynitride (LiPON) is deposited onto the cathode by using radio-frequency magnetron sputtering. Then, the lithium metal anode is deposited on the LiPON film by the thermal evaporation method to fabricate the all-solid-state LiFeFe(CN)/LiPON/Li battery with a thickness of 16 μm and a size of ∼10 cm.
View Article and Find Full Text PDFLiNiCoAlO (NCA) has been proven to be a good cathode material for lithium-ion batteries (LIBs), especially in electric vehicle applications. However, further elevating energy density of NCA is very challenging. Increasing the charging voltage of NCA is an effective method, but its structural instability remains a problem.
View Article and Find Full Text PDFThe increasing demands of energy storage require the significant improvement of current Li-ion battery electrode materials and the development of advanced electrode materials. Thus, it is necessary to gain an in-depth understanding of the reaction processes, degradation mechanism, and thermal decomposition mechanisms under realistic operation conditions. This understanding can be obtained by in situ/operando characterization techniques, which provide information on the structure evolution, redox mechanism, solid-electrolyte interphase (SEI) formation, side reactions, and Li-ion transport properties under operating conditions.
View Article and Find Full Text PDFMost P2-type layered oxides suffer from multiple voltage plateaus, due to Na/vacancy-order superstructures caused by strong interplay between Na-Na electrostatic interactions and charge ordering in the transition metal layers. Here, Mg ions are successfully introduced into Na sites in addition to the conventional transition metal sites in P2-type Na[MnNi]O as new cathode materials for sodium-ion batteries. Mg ions in the Na layer serve as "pillars" to stabilize the layered structure, especially for high-voltage charging, meanwhile Mg ions in the transition metal layer can destroy charge ordering.
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