The increasing use of low-cost lithium iron phosphate cathodes in low-end electric vehicles has sparked interest in Prussian blue analogues (PBAs) for lithium-ion batteries. A major challenge with iron hexacyanoferrate (FeHCFe), particularly in lithium-ion systems, is its slow kinetics in organic electrolytes and valence state inactivation in aqueous ones. We have addressed these issues by developing a polymeric cathode electrolyte interphase (CEI) layer through a ring-opening reaction of ethylene carbonate triggered by OH radicals from structural water.
View Article and Find Full Text PDFChem Commun (Camb)
October 2023
We investigate silicon oxycarbide nanotubes that incorporate Si, SiC, and silicon oxycarbide phases, which exhibit near zero-strain volume expansion, leading to reduced electrolyte decomposition. The composite effectively accommodates the formation of -LiSi, as validated by TEM analyses and electrochemical tests, thereby proposing a promising solution for Li-ion battery anodes.
View Article and Find Full Text PDFElectrochemical carbon-capture technologies, with renewable electricity as the energy input, are promising for carbon management but still suffer from low capture rates, oxygen sensitivity or system complexity. Here we demonstrate a continuous electrochemical carbon-capture design by coupling oxygen/water (O/HO) redox couple with a modular solid-electrolyte reactor. By performing oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) redox electrolysis, our device can efficiently absorb dilute carbon dioxide (CO) molecules at the high-alkaline cathode-membrane interface to form carbonate ions, followed by a neutralization process through the proton flux from the anode to continuously output a high-purity (>99%) CO stream from the middle solid-electrolyte layer.
View Article and Find Full Text PDFOver the past decade, lithium metal has been considered the most attractive anode material for high-energy-density batteries. However, its practical application has been hindered by its high reactivity with organic electrolytes and uncontrolled dendritic growth, resulting in poor Coulombic efficiency and cycle life. In this paper, we propose a design strategy for interface engineering using a conversion-type reaction of metal fluorides to evolve a LiF passivation layer and Li-M alloy.
View Article and Find Full Text PDFUnderstanding the local cation order in the crystal structure and its correlation with electrochemical performances has advanced the development of high-energy Mn-rich cathode materials for Li-ion batteries, notably Li- and Mn-rich layered cathodes (LMR, e.g., Li Ni Mn Co O ) that are considered as nanocomposite layered materials with C2/m Li MnO -type medium-range order (MRO).
View Article and Find Full Text PDFAbundant availability of seawater grants economic and resource-rich benefits to water electrolysis technology requiring high-purity water if undesired reactions such as chlorine evolution reaction (CER) competitive to oxygen evolution reaction (OER) are suppressed. Inspired by a conceptual computational work suggesting that OER is kinetically improved via a double activation within 7 Å-gap nanochannels, RuO catalysts are realized to have nanoscopic channels at 7, 11, and 14 Å gap in average (d ), and preferential activity improvement of OER over CER in seawater by using nanochanneled RuO is demonstrated. When the channels are developed to have 7 Å gap, the OER current is maximized with the overpotential required for triggering OER minimized.
View Article and Find Full Text PDFLithium metal batteries (LMBs) will be a breakthrough in automotive applications, but they require the development of next-generation solid-state electrolytes (SSEs) to stabilize the anode interface. Polymer-in-ceramic PEO/TiO nanocomposite SSEs show outstanding properties, allowing unprecedented LMBs durability and self-healing capabilities. However, the mechanism underlying the inhibition/delay of dendrite growth is not well understood.
View Article and Find Full Text PDFThe wet-chemical processability of sulfide solid electrolytes (SEs) provides intriguing opportunities for all-solid-state batteries. Thus far, sulfide SEs are wet-prepared either from solid precursors suspended in solvents (suspension synthesis) or from homogeneous solutions using SEs (solution process) with restricted composition spaces. Here, a universal solution synthesis method for preparing sulfide SEs from precursors, not only Li S, P S , LiCl, and Na S, but also metal sulfides (e.
View Article and Find Full Text PDFACS Appl Mater Interfaces
February 2022
The practical use of silicon anodes is interfered by the following key factors: volume expansion, slow kinetics, and low electrical and ionic conductivities. Many studies have focused on surface engineering from the particle to electrode level to achieve stability and energy density. Herein, simple nitrogen gas plasma is introduced as a surface treatment method for silicon-based electrodes to avoid the problems of material synthesis-based functionalizations (e.
View Article and Find Full Text PDFThe rational design of bifunctional electrocatalyst through simple synthesis with high activity remains a challenging task. Herein, Na/Al codoped Li-excess Li-Ru-Ni-O layered electrodes are demonstrated with defects/dislocations as an efficient bifunctional electrocatalyst toward lithium-ion battery (LIB) and oxygen evolution reaction (OER). Toward LIB cathode, specific capacity of 173 mAh g (0.
View Article and Find Full Text PDFSurface coating on alloy anodes renders an effective remedy to tolerate internal stress and alleviate the side reaction with electrolytes for long-lasting reversible lithium redox reactions in lithium-ion batteries. However, the role of surface coating on the interparticle connections of alloy anodes remains not fully understood. Herein, we exploit real-time lithiation and mechanic measurement of SnO nanoparticles via TEM with different coating layers, including conducting polymer polypyrrole and metal oxide MnO.
View Article and Find Full Text PDFThe application of transition metal fluorides as energy-dense cathode materials for lithium ion batteries has been hindered by inadequate understanding of their electrochemical capabilities and limitations. Here, we present an ideal system for mechanistic study through the colloidal synthesis of single-crystalline, monodisperse iron(II) fluoride nanorods. Near theoretical capacity (570 mA h g) and extraordinary cycling stability (>90% capacity retention after 50 cycles at C/20) is achieved solely through the use of an ionic liquid electrolyte (1 m LiFSI/PyrFSI), which forms a stable solid electrolyte interphase and prevents the fusing of particles.
View Article and Find Full Text PDFVolumetric energy density is considered a primary factor in developing high-energy batteries. Despite its significance, less efforts have been devoted to its improvement. Silicon-based materials have emerged as next-generation anodes for lithium-ion batteries due to their high specific capacity.
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