Proc Natl Acad Sci U S A
January 2025
High degree of fluorination for ether electrolytes has resulted in improved cycling stability of lithium metal batteries due to stable solid electrolyte interphase (SEI) formation and good oxidative stability. However, the sluggish ion transport and environmental concerns of high fluorination degree drive the need to develop less fluorinated structures. Here, we depart from the traditional ether backbone and introduce bis(2-fluoroethoxy)methane (F2DEM), featuring monofluorination of the acetal backbone.
View Article and Find Full Text PDFLithium metal batteries (LMB) have high energy densities and are crucial for clean energy solutions. The characterization of the lithium metal interphase is fundamentally and practically important but technically challenging. Taking advantage of synchrotron X-ray, which has the unique capability of analyzing crystalline/amorphous phases quantitatively with statistical significance, we study the composition and dynamics of the LMB interphase for a newly developed important LMB electrolyte that is based on fluorinated ether.
View Article and Find Full Text PDFWastewater treatment produces a large amount of sludge, where the minimizing of the disposed sludge is essential for environmental protection. The co-combustion of sludge with coal is a preferable method for sewage sludge disposal from the economic and environmental perspective. The co-combustion of sludge has been widely used in the industry with the advantages of large processing capacity.
View Article and Find Full Text PDFIntrinsically stretchable electronics with skin-like mechanical properties have been identified as a promising platform for emerging applications ranging from continuous physiological monitoring to real-time analysis of health conditions, to closed-loop delivery of autonomous medical treatment. However, current technologies could only reach electrical performance at amorphous-silicon level (that is, charge-carrier mobility of about 1 cm V s), low integration scale (for example, 54 transistors per circuit) and limited functionalities. Here we report high-density, intrinsically stretchable transistors and integrated circuits with high driving ability, high operation speed and large-scale integration.
View Article and Find Full Text PDFAll-solid-state batteries (ASSBs) working at room and mild temperature have demonstrated inspiring performances over recent years. However, the kinetic attributes of the interface applicable to the subzero temperatures are still unidentified, restricting the low-temperature interface design and operation. Herein, a host of cathode interfaces are constructed and investigated to unlock the critical interface features required for cryogenic temperatures.
View Article and Find Full Text PDFSilicon is regarded as the most promising candidate due to its ultrahigh theoretical energy density (4200 mAh g). However, the large volume expansion of silicon nanoparticles would result in the destruction of electrodes and a shortened cycle lifetime. Here, inspired by the natural structure of bamboo, the silicon anode with vascular bundle-like structure is proposed to improve the electrochemical performance for the first time.
View Article and Find Full Text PDFThe composition of the solid electrolyte interphase (SEI) plays an important role in controlling Li-electrolyte reactions, but the underlying cause of SEI composition differences between electrolytes remains unclear. Many studies correlate SEI composition with the bulk solvation of Li ions in the electrolyte, but this correlation does not fully capture the interfacial phenomenon of SEI formation. Here, we provide a direct connection between SEI composition and Li-ion solvation by forming SEIs using polar substrates that modify interfacial solvation structures.
View Article and Find Full Text PDFLithium-sulfur (Li-S) batteries with high energy density and low cost are promising for next-generation energy storage. However, their cycling stability is plagued by the high solubility of lithium polysulfide (LiPS) intermediates, causing fast capacity decay and severe self-discharge. Exploring electrolytes with low LiPS solubility has shown promising results toward addressing these challenges.
View Article and Find Full Text PDFStretchable polymer semiconductors (PSCs) are essential for soft stretchable electronics. However, their environmental stability remains a longstanding concern. Here we report a surface-tethered stretchable molecular protecting layer to realize stretchable polymer electronics that are stable in direct contact with physiological fluids, containing water, ions and biofluids.
View Article and Find Full Text PDFImproving Coulombic efficiency (CE) is key to the adoption of high energy density lithium metal batteries. Liquid electrolyte engineering has emerged as a promising strategy for improving the CE of lithium metal batteries, but its complexity renders the performance prediction and design of electrolytes challenging. Here, we develop machine learning (ML) models that assist and accelerate the design of high-performance electrolytes.
View Article and Find Full Text PDFInorganic-rich solid-electrolyte interphases (SEIs) on Li metal anodes improve the electrochemical performance of Li metal batteries (LMBs). Therefore, a fundamental understanding of the roles played by essential inorganic compounds in SEIs is critical to realizing and developing high-performance LMBs. Among the prevalent SEI inorganic compounds observed for Li metal anodes, LiN is often found in the SEIs of high-performance LMBs.
View Article and Find Full Text PDFSilicon is expected to become the ideal anode material for the next generation of high energy density lithium battery because of its high theoretical capacity (4200 mAh g ). However, for silicon electrodes, the initial coulombic efficiency (ICE) is low and the volume of the electrode changes by over 300% after lithiation. The capacity of the silicon electrode decreases rapidly during cycling, hindering the practical application.
View Article and Find Full Text PDFFast-charging is considered as one of the most desired features needed for lithium-ion batteries to accelerate the mainstream adoption of electric vehicles. However, current battery charging protocols mainly consist of conservative rate steps to avoid potential hazardous lithium plating and its associated parasitic reactions. A highly sensitive onboard detection method could enable battery fast-charging without reaching the lithium plating regime.
View Article and Find Full Text PDFThe electrodeposition of low surface area lithium is critical to successful adoption of lithium metal batteries. Here, we discover the dependence of lithium metal morphology on electrical resistance of substrates, enabling us to design an alternative strategy for controlling lithium morphology and improving electrochemical performance. By modifying the current collector with atomic layer deposited conductive (ZnO, SnO) and resistive (AlO) nanofilms, we show that conductive films promote the formation of high surface area lithium deposits, whereas highly resistive films promote the formation of lithium clusters of low surface area.
View Article and Find Full Text PDFNext-generation light-emitting displays on skin should be soft, stretchable and bright. Previously reported stretchable light-emitting devices were mostly based on inorganic nanomaterials, such as light-emitting capacitors, quantum dots or perovskites. They either require high operating voltage or have limited stretchability and brightness, resolution or robustness under strain.
View Article and Find Full Text PDFDesigning a stable solid-electrolyte interphase on a Li anode is imperative to developing reliable Li metal batteries. Herein, we report a suspension electrolyte design that modifies the Li solvation environment in liquid electrolytes and creates inorganic-rich solid-electrolyte interphases on Li. LiO nanoparticles suspended in liquid electrolytes were investigated as a proof of concept.
View Article and Find Full Text PDFAlthough liquid-solid interfaces are foundational in broad areas of science, characterizing this delicate interface remains inherently difficult because of shortcomings in existing tools to access liquid and solid phases simultaneously at the nanoscale. This leads to substantial gaps in our understanding of the structure and chemistry of key interfaces in battery systems. We adopt and modify a thin film vitrification method to preserve the sensitive yet critical interfaces in batteries at native liquid electrolyte environments to enable cryo–electron microscopy and spectroscopy.
View Article and Find Full Text PDFShape memory polymers are promising materials in many emerging applications due to their large extensibility and excellent shape recovery. However, practical application of these polymers is limited by their poor energy densities (up to ∼1 MJ/m). Here, we report an approach to achieve a high energy density, one-way shape memory polymer based on the formation of strain-induced supramolecular nanostructures.
View Article and Find Full Text PDF1,2-Dimethoxyethane (DME) is a common electrolyte solvent for lithium metal batteries. Various DME-based electrolyte designs have improved long-term cyclability of high-voltage full cells. However, insufficient Coulombic efficiency at the Li anode and poor high-voltage stability remain a challenge for DME electrolytes.
View Article and Find Full Text PDFNext-generation wearable electronics require enhanced mechanical robustness and device complexity. Besides previously reported softness and stretchability, desired merits for practical use include elasticity, solvent resistance, facile patternability and high charge carrier mobility. Here, we show a molecular design concept that simultaneously achieves all these targeted properties in both polymeric semiconductors and dielectrics, without compromising electrical performance.
View Article and Find Full Text PDFPolymeric electronic materials have enabled soft and stretchable electronics. However, the lack of a universal micro/nanofabrication method for skin-like and elastic circuits results in low device density and limited parallel signal recording and processing ability relative to silicon-based devices. We present a monolithic optical microlithographic process that directly micropatterns a set of elastic electronic materials by sequential ultraviolet light-triggered solubility modulation.
View Article and Find Full Text PDFThe electrolyte plays a critical role in lithium-ion batteries, as it impacts almost every facet of a battery's performance. However, our understanding of the electrolyte, especially solvation of Li, lags behind its significance. In this work, we introduce a potentiometric technique to probe the relative solvation energy of Li in battery electrolytes.
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