Proc Natl Acad Sci U S A
October 2024
Lithium (Li) metal has been recognized as a promising anode to advance the energy density of current Li-based batteries. However, the growth of the solid-electrolyte interphase (SEI) layer and dendritic Li microstructure pose significant challenges for the long-term operation of Li metal batteries (LMBs). Herein, we propose the utilization of a suspension electrolyte with dispersed magnetically responsive nanosheets whose orientation can be manipulated by an external magnetic field during cell operation for realizing in situ regeneration in LMBs.
View Article and Find Full Text PDFElectronic systems and devices operating at significant power levels demand sophisticated solutions for heat dissipation. Although materials with high thermal conductivity hold promise for exceptional thermal transport across nano- and microscale interfaces under ideal conditions, their performance often falls short by several orders of magnitude in the complex thermal interfaces typical of real-world applications. This study introduces mechanochemistry-mediated colloidal liquid metals composed of Galinstan and aluminium nitride to bridge the practice-theory disparity.
View Article and Find Full Text PDFElectrocatalytic CO reduction is garnering significant interest due to its potential applications in mitigating CO and producing fuel. However, the scaling up of related catalysis is still hindered by several challenges, including the cost of the catalytic materials, low selectivity, small current densities to maintain desirable selectivity. In this study, Fluorine (F) atoms were introduced into an N-doped carbon-supported single nickel (Ni) atom catalyst via facile polymer-assisted pyrolysis.
View Article and Find Full Text PDFAs one of the most promising electrochemical energy storage systems, aqueous batteries are attracting great interest due to their advantages of high safety, high sustainability, and low costs when compared with commercial lithium-ion batteries, showing great promise for grid-scale energy storage. This invited tutorial review aims to provide universal design principles to address the critical challenges at the electrode-electrolyte interfaces faced by various multivalent aqueous battery systems. Specifically, deposition regulation, ion flux homogenization, and solvation chemistry modulation are proposed as the key principles to tune the inter-component interactions in aqueous batteries, with corresponding interfacial design strategies and their underlying working mechanisms illustrated.
View Article and Find Full Text PDFHabitual daytime napping is a common behavioral and lifestyle practice in particular countries and is often considered part of a normal daily routine. However, recent evidence suggests that the health effects of habitual daytime napping are controversial. We systematically searched PubMed, Web of Science, Embase, and Cochrane Library databases from inception to March 9, 2024, to synthesize cohort studies of napping and health outcome risk.
View Article and Find Full Text PDFSolid inorganics, known for kinetically inhibiting polymer crystallization and enhancing ionic conductivity, have attracted significant attention in solid polymer electrolytes. However, current composite polymer electrolytes (CPEs) are still facing challenges in Li metal batteries, falling short of inhibiting severe dendritic growth and resulting in very limited cycling life. This study introduces GaInSn (Galinstan) liquid metal (LM) as an active liquid alternative to conventional passive solid fillers, aiming at realizing self-healing protection against dendrite problems.
View Article and Find Full Text PDFAtmospheric water harvesting (AWH) is recognized as a crucial strategy to address the global challenge of water scarcity by tapping into the vast reserves of atmospheric moisture for potable water supply. Within this domain, sorbents lie in the core of AWH technologies as they possess broad adaptability across a wide spectrum of humidity levels, underpinned by the cyclic sorption and desorption processes of sorbents, necessitating a multi-scale viewpoint regarding the rational material and chemical selection and design. This Invited Review delves into the essential sorption mechanisms observed across various classes of sorbent systems, emphasizing the water-sorbent interactions and the progression of water networks.
View Article and Find Full Text PDFIn pursuit of higher energy density in lithium-ion batteries, silicon (Si) has been recognized as a promising candidate to replace commercial graphite due to its high theoretical capacity. However, the pulverization issue of Si microparticles during lithiation/delithiation results in electrical contact loss and increased side reactions, significantly limiting its practical applications. Herein, we propose to utilize liquid metal (LM) particles as the bridging agent, which assemble conductive MXene (TiCT) sheets via coordination chemistry, forming cage-like structures encapsulating mSi particles as self-healing high-energy anodes.
View Article and Find Full Text PDFLithium-ion batteries with fast-charging/discharging properties are urgently needed for the mass adoption of electric vehicles. Here, we show that fast charging/discharging, long-term stable and high energy charge-storage properties can be realized in an artificial electrode made from a mixed electronic/ionic conductor material (Fe/LiM, where M = O, F, S, N) enabled by a space charge principle. Particularly, the Fe/LiO electrode is able to be charged/discharged to 126 mAh g in 6 s at a high current density of up to 50 A g, and it also shows stable cycling performance for 30,000 cycles at a current density of 10 A g, with a mass-loading of ~2.
View Article and Find Full Text PDFProc Natl Acad Sci U S A
April 2024
Electrochromic (EC) displays with electronically regulating the transmittance of solar radiation offer the opportunity to increase the energy efficiency of the building and electronic products and improve the comfort and lifestyle of people. Despite the unique merit and vast application potential of EC technologies, long-awaited EC windows and related visual content displays have not been fully commercialized due to unsatisfactory production cost, durability, color, and complex fabrication processes. Here we develop a unique EC strategy and system based on the natural host and guest interactions to address the above issues.
View Article and Find Full Text PDFBistable electrochromic (EC) materials and systems offer significant potential for building decarbonization through their optical modulation and energy efficiency. However, challenges such as limited design strategies and bottlenecks in cost, fabrication, and color have hindered the full commercialization of energy-saving EC windows and displays, with few materials achieving true bistability. Herein, a novel strategy for designing bistable electrochromic materials is proposed by leveraging supramolecular interactions.
View Article and Find Full Text PDFThe electrochemical nitrate reduction reaction (NORR) holds promise for converting nitrogenous pollutants to valuable ammonia products. However, conventional electrocatalysis faces challenges in effectively driving the complex eight-electron and nine-proton transfer process of the NORR while also competing with the hydrogen evolution reaction. In this study, we present the thermally enhanced electrocatalysis of nitrate-to-ammonia conversion over nickel-modified copper oxide single-atom alloy oxide nanowires.
View Article and Find Full Text PDFRational manipulation and assembly of discrete colloidal particles into architected superstructures have enabled several applications in materials science and nanotechnology. Optical manipulation techniques, typically operated in fluid media, facilitate the precise arrangement of colloidal particles into superstructures by using focused laser beams. However, as the optical energy is turned off, the inherent Brownian motion of the particles in fluid media impedes the retention and reconfiguration of such superstructures.
View Article and Find Full Text PDFBatteries utilizing a sodium (Na) metal anode with a liquid electrolyte are promising for affordable large-scale energy storage. However, a deep understanding of the intrinsic degradation mechanisms is limited by challenges in accessing the buried interfaces. Here, cryogenic electron microscopy of intact electrode:separator:electrode stacks is performed and degradation and failure of symmetric Na||Na coin cells occurs through the infiltration of Na metal through the pores of the separator rather than by mechanical puncturing by dendrites is revealed.
View Article and Find Full Text PDFAll-solid-state lithium batteries (ASSLBs) face critical challenges of low cathode loading and poor rate performances, which handicaps their energy/power densities. The widely-accepted aim of high ionic conductivity and low interfacial resistance seems insufficient to overcome these challenges. Here, it is revealed that an efficient ion percolating network in the cathode exerts a more critical influence on the electrochemical performance of ASSLBs.
View Article and Find Full Text PDFProc Natl Acad Sci U S A
February 2024
Transition metals and related compounds are known to exhibit high catalytic activities in various electrochemical reactions thanks to their intriguing electronic structures. What is lesser known is their unique role in storing and transferring electrons in battery electrodes which undergo additional solid-state conversion reactions and exhibit substantially large extra capacities. Here, a full dynamic picture depicting the generation and evolution of electrochemical interfaces in the presence of metallic nanoparticles is revealed in a model CoCO/Li battery via an in situ magnetometry technique.
View Article and Find Full Text PDFTo meet the growing demands in both energy and power densities of lithium ion batteries, electrode structures must be capable of facile electron and ion transport while minimizing the content of electrochemically inactive components. Herein, binder-free LiFePO (LFP) cathodes are fabricated with a multidimensional conductive architecture that allows for fast-charging capability, reaching a specific capacity of 94 mAh g at 4 C. Such multidimensional networks consist of active material particles wrapped by 1D single-walled carbon nanotubes (CNTs) and bound together using 2D MXene (TiCT) nanosheets.
View Article and Find Full Text PDFEmerging organic contaminants in water matrices have challenged ecosystems and human health safety. Persulfate-based advanced oxidation processes (PS-AOPs) have attracted much attention as they address potential water purification challenges. However, overcoming the mass transfer constraint and the catalyst's inherent site agglomeration in the heterogeneous system remains urgent.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
February 2024
Polyaniline (PANI), with merits of high electronic conductivity and capacity, is a promising material for zinc (Zn)-ion batteries. However, its redox window in Zn batteries is often limited, mainly due to the oxidative degradation at high potentials-in which imine groups can be attacked by water molecules. Here, we introduce phytic acid, a kind of supermolecule acid radical ion, as a dopant and electrolyte additive.
View Article and Find Full Text PDFProc Natl Acad Sci U S A
November 2023
Interfacial catalysis occurs ubiquitously in electrochemical systems, such as batteries, fuel cells, and photocatalytic devices. Frequently, in such a system, the electrode material evolves dynamically at different operating voltages, and this electrochemically driven transformation usually dictates the catalytic reactivity of the material and ultimately the electrochemical performance of the device. Despite the importance of the process, comprehension of the underlying structural and compositional evolutions of the electrode material with direct visualization and quantification is still a significant challenge.
View Article and Find Full Text PDFAqueous Zn metal batteries are promising candidates for large-scale energy storage due to their intrinsic advantages. However, Zn tends to deposit irregularly and forms dendrites driven by the uneven space electric field distribution near the Zn-electrolyte interphase. Herein it is demonstrated that trace addition of Co single atom anchored carbon (denoted as CoSA/C) in the electrolyte regulates the microspace electric field at the Zn-electrolyte interphase and unifies Zn deposition.
View Article and Find Full Text PDFProc Natl Acad Sci U S A
September 2023
Water scarcity is a pressing global issue, requiring innovative solutions such as atmospheric water harvesting (AWH), which captures moisture from the air to provide potable water to many water-stressed areas. Thermoresponsive hydrogels, a class of temperature-sensitive polymers, demonstrate potential for AWH as matrices for hygroscopic components like salts predominantly due to their relatively energy-efficient desorption properties compared to other sorbents. However, challenges such as limited swelling capacity due to the salting-out effect and difficulty in more complete water release hinder the effectiveness of conventional hydrogel sorbents.
View Article and Find Full Text PDFOver the past few years, lithium-ion batteries have been extensively adopted in electric transportation. Meanwhile, the energy density of lithium-ion battery packs has been significantly improved, thanks to the development of materials science and packing technology. Despite recent progress in electric vehicle cruise ranges, the increase in battery charging rates remains a pivotal problem in electrodes with commercial-level mass loadings.
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