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Habitual 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. A total of 44 cohort studies with 1,864,274 subjects aged 20-86 years (mean age 56.4 years) were included. Overall, habitual napping increased the risk of several adverse health outcomes, including all-cause mortality, cardiovascular disease, metabolic disease, and cancer, and decreased the risk of cognitive impairment and sarcopenia. Individuals with a napping duration of 30 min or longer exhibited a higher risk of all-cause mortality, cardiovascular disease, and metabolic disease, whereas those with napping durations less than 30 min had no significant risks. No significant differences in napping and health risks were observed for napping frequency, percentage of nappers, sample size, sex, age, body mass index, follow-up years, or comorbidity status. These findings indicate that individuals with a long napping duration should consider shortening their daily nap duration to 30 min or less.
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As 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. In the end, we present a critical analysis on the remaining obstacles necessitated to overcome for the use of aqueous batteries under different practical conditions and provide future prospects towards further advancement of sustainable aqueous energy storage systems with high energy and long durability.
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Given the growing emphasis on energy efficiency, environmental sustainability, and agricultural demand, there's a pressing need for decentralized and scalable ammonia production. Converting nitrate ions electrochemically, which are commonly found in industrial wastewater and polluted groundwater, into ammonia offers a viable approach for both wastewater treatment and ammonia production yet limited by low producibility and scalability. Here we report a versatile and scalable solution-phase synthesis of high-entropy single-atom nanocages (HESA NCs) in which Fe and other five metals-Co, Cu, Zn, Cd, and In-are isolated via cyano-bridges and coordinated with C and N, respectively. Incorporating and isolating the five metals into the matrix of Fe resulted in Fe-C5 active sites with a minimized symmetry of lattice as well as facilitated water dissociation and thus hydrogenation process. As a result, the Fe-HESA NCs exhibited a high selectivity toward NH3 from the electrocatalytic reduction of nitrate with a Faradaic efficiency of 93.4% while maintaining a high yield rate of 81.4 mg h-1 mg-1.
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Solid 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 Ga62.5In21.5Sn16 (Galinstan) liquid metal (LM) as an active liquid alternative to conventional passive solid fillers, aiming at realizing self-healing protection against dendrite problems. Compared to solid inorganics, for example silica, LM droplets could more significantly reduce polymer crystallinity and enhance Li-ion conductivity due to their liquid nature, especially at temperatures below the polymer melting point. More importantly, LMs are unraveled as dynamic chemical traps, which are capable of blocking and consuming lithium dendrites upon contact via in situ alloying during battery operation and further inhibiting dendritic growth due to the lower deposition energy barrier of the formed Li-LM alloy. As a proof of concept, by strategically designing an asymmetric CPE with the active LM filling, a solid-state Li/LiFePO4 battery achieves promising full-cell functionality with notable rate performance and stable cycle life. This active filler-mediated self-healing approach could bring new insights into the battery design in versatile solid-state systems.
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Atmospheric 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. A special focus is placed on the insights derived from isotherm profiles, which elucidate sorbent structures and sorption dynamics. From these foundational principles, we derive material and chemical design guidelines and identify key tuning factors from a structural-functional perspective across multiple material systems, addressing their fundamental chemistries and unique attributes. The review further navigates through system-level design considerations to optimize water production efficiency. This review aims to equip researchers in the field of AWH with a thorough understanding of the water-sorbent interactions, material design principles, and system-level considerations essential for advancing this technology.
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Lithium-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/LixM, where M = O, F, S, N) enabled by a space charge principle. Particularly, the Fe/Li2O electrode is able to be charged/discharged to 126 mAh g-1 in 6 s at a high current density of up to 50 A g-1, and it also shows stable cycling performance for 30,000 cycles at a current density of 10 A g-1, with a mass-loading of ~2.5 mg cm-2 of the electrode materials. This study demonstrates the critical role of the space charge storage mechanism in advancing electrochemical energy storage and provides an unconventional perspective for designing high-performance anode materials for lithium-ion batteries.
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In 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 (Ti3C2Tx) sheets via coordination chemistry, forming cage-like structures encapsulating mSi particles as self-healing high-energy anodes. Due to the integration of robust Ti3C2Tx sheets and deformable LM particles as conductive buffering cages, simultaneously high-rate capability and cyclability can be realized. Post-mortem analysis revealed the cage structural integrity and the maintained electrical percolating network after cycling. This work introduces an effective approach to accommodate structural change via a resilient encapsulating cage and offers useful interface design considerations for versatile battery electrodes.
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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. A completely reusable and sustainable EC device has been fabricated with potential advantages of extremely low cost, ideal user-/environment friendly property, and excellent optical modulation, which is benefited from the extracted biomass EC materials and reusable transparent electrodes involved in the system. The as-prepared EC window and nonemissive transparent display also show comprehensively excellent properties: high transmittance change (>85%), broad spectra modulation covering Ultraviolet (UV), Visible (Vis) to Infrared (IR) ranges, high durability (no attenuation under UV radiation for more than 1.5 mo), low open voltage (0.9 V), excellent reusability (>1,200 cycles) of the device's key components and reversibility (>4,000 cycles) with a large transmittance change, and pleasant multicolor. It is anticipated that unconventional exploration and design principles of dynamic host-guest interactions can provide unique insight into different energy-saving and sustainable optoelectronic applications.
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Bistable 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. These interactions facilitate reversible color transitions, stabilize the colored structure, and enable spatial confinement to inhibit diffusion, thereby achieving bistable electrochromism. The mechanisms and materials underlying these unconventional electrochromic systems are substantiated through detailed characterization. This strategy enables the preparation of low-cost and sustainable transparent electrochromic displays with high performance. Notably, the display information remains clearly visible for more than 2 h without consuming energy. Involving biomass materials and removable device structures also enhances the sustainability and scalability of EC technology applications and development. These results demonstrate the crucial role of supramolecular chemistry in the development of cutting-edge materials for applications such as energy-saving smart windows.
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The electrochemical nitrate reduction reaction (NO3RR) 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 NO3RR 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. The catalyst demonstrates improved ammonia production performance with a Faradaic efficiency of approximately 80% and a yield rate of 9.7 mg h-1 cm-2 at +0.1 V versus a reversible hydrogen electrode at elevated cell temperatures. In addition, this thermally enhanced electrocatalysis system displays impressive stability, interference resistance, and favorable energy consumption and greenhouse gas emissions for the simulated industrial wastewater treatment. Complementary in situ analyses confirm that the significantly superior relay of active hydrogen species formed at Ni sites facilitates the thermal-field-coupled electrocatalysis of Cu surface-adsorbed *NOx hydrogenation. Theoretical calculations further support the thermodynamic and kinetic feasibility of the relay catalysis mechanism for the NO3RR over the Ni1Cu model catalyst. This study introduces a conceptual thermal-electrochemistry approach for the synergistic regulation of complex catalytic processes, highlighting the potential of multifield-coupled catalysis to advance sustainable-energy-powered chemical synthesis technologies.
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Rational 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. Overcoming this fundamental limitation, we present on-demand, three-dimensional (3D) optical manipulation of colloidal particles in a phase-change solid medium made of surfactant bilayers. Unlike liquid crystal media, the lack of fluid flow within the bilayer media enables the assembly and retention of colloids for diverse spatial configurations. By utilizing the optically controlled temperature-dependent interactions between the particles and their surrounding media, we experimentally exhibit the holonomic microscale control of diverse particles for repeatable, reconfigurable, and controlled colloidal arrangements in 3D. Finally, we demonstrate tunable light-matter interactions between the particles and 2D materials by successfully manipulating and retaining these particles at fixed distances from the 2D material layers. Our experimental results demonstrate that the particles can be retained for over 120 days without any change in their relative positions or degradation in the bilayers. With the capability of arranging particles in 3D configurations with long-term stability, our platform pushes the frontiers of optical manipulation for distinct applications such as metamaterial fabrication, information storage, and security.
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All-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. By constructing vertical alignment of Li0.35La0.55TiO3 nanowires (LLTO NWs) in solid-state cathode through magnetic manipulation, the ionic conductivity of the cathode increases twice compared with the cathode consisted of randomly distributed LLTO NWs. The all-solid-state LiFePO4/Li cells using poly(ethylene oxide) as the electrolyte is able to deliver high capacities of 151 mAh g-1 (2 C) and 100 mAh g-1 (5 C) at 60 °C, and a room-temperature capacity of 108 mAh g-1 can be achieved at a charging rate of 2 C. Furthermore, the cell can reach a high areal capacity of 3 mAh cm-2 even with a practical LFP loading of 20 mg cm-2. The universality of this strategy is also presented showing the demonstration in LiNi0.8Co0.1Mn0.1O2 cathodes. This work offers new pathways for designing ASSLBs with improved energy/power densities.
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Batteries 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. It is shown the interior structure of the cell (electrode:separator:electrode) must be preserved and deconstructing the cell into different layers for characterization results in artifacts. In intact cell stacks, minimal liquid is found between the electrodes and separator, leading to intimate electrode:separator interfaces. After electrochemical cycling, Na infiltrates into the pore free-volume, growing through the separator to create electrical shorts and degradation. The Na infiltration occurs at interfacial regions devoid of solid-electrolyte interphase (SEI), revealing SEI plays an important role in preventing Na from growing into the separator by being a physical barrier that the plated Na cannot penetrate. These results shed new light on the fundamental failure mechanisms in Na batteries and demonstrate the importance of preserving the cell structure and buried interfaces.
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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 CoCO3/Li battery via an in situ magnetometry technique. Beyond the conventional reduction to a Li2CO3/Co mixture under battery operation, further decomposition of Li2CO3 is realized by releasing interfacially stored electrons from its adjacent Co nanoparticles, whose subtle variation in the electronic structure during this charge transfer process has been monitored in real time. The findings in this work may not only inspire future development of advanced electrode materials for next-generation energy storage devices but also open up opportunities in achieving in situ monitoring of important electrocatalytic processes in many energy conversion and storage systems.
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Emerging 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. Herein, the abundant metal-anchored loading (≈6-8 g m-2) of alginate hydrogel membranes coupled with cross-flow mode as an efficient strategy for water purification applications is proposed. The organic flux of the confined hydrogel interfaces sharply enlarges with the reduction of the thickness of the boundary layer via the pressure field. The normalized property of the system displays a remarkable organic (sulfonamides) elimination rate of 4.87 × 104 mg min-1 mol-1. Furthermore, due to the fast reaction time (<1 min), cross-flow mode only reaches a meager energy cost (≈2.21 Wh m-3) under the pressure drive field. It is anticipated that this finding provides insight into the novel design with ultrafast organic removal performance and low techno-economic cost (i.e., energy operation cost, material, and reagent cost) for the field of water purification under various PS-AOPs challenging scenarios.
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To 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 LiFePO4 (LFP) cathodes are fabricated with a multidimensional conductive architecture that allows for fast-charging capability, reaching a specific capacity of 94 mAh g-1 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 (Ti3C2Tx) nanosheets. The CNTs form a porous coating layer and improve local electron transport across the LFP surface, while the Ti3C2Tx nanosheets provide simultaneously high electrode integrity and conductive pathways through the bulk of the electrode. This work highlights the ability of multidimensional conductive fillers to realize simultaneously superior electrochemical and mechanical properties, providing useful insights into future fast-charging electrode designs for scalable electrochemical systems.
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Aqueous 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. Through preferential adsorption of CoSA/C on the Zn surface, the atomically dispersed Co-N3 with strong charge polarization effect can redistribute the local space electric field and regulate ion flux. Moreover, the dynamic adsorption/desorption of CoSA/C upon plating/stripping offers sustainable long-term regulation. Therefore, Zn||Zn symmetric cells with CoSA/C electrolyte additive deliver stable cycling up to 1600 h (corresponding to a cumulative plated capacity of 8 Ah cm-2 ) at a high current density of 10 mA cm-2 , demonstrating the sustainable feature of microspace electric field regulation at high current density and capacity.
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Zn-MnO2 batteries have attracted extensive attention for grid-scale energy storage applications, however, the energy storage chemistry of MnO2 in mild acidic aqueous electrolytes remains elusive and controversial. Using α-MnO2 as a case study, we developed a methodology by coupling conventional coin batteries with customized beaker batteries to pinpoint the operating mechanism of Zn-MnO2 batteries. This approach visually simulates the operating state of batteries in different scenarios and allows for a comprehensive study of the operating mechanism of aqueous Zn-MnO2 batteries under mild acidic conditions. It is validated that the electrochemical performance can be modulated by controlling the addition of Mn2+ to the electrolyte. The method is utilized to systematically eliminate the possibility of Zn2+ and/or H+ intercalation/de-intercalation reactions, thereby confirming the dominance of the MnO2 /Mn2+ dissolution-deposition mechanism. By combining a series of phase and spectroscopic characterizations, the compositional, morphological and structural evolution of electrodes and electrolytes during battery cycling is probed, elucidating the intrinsic battery chemistry of MnO2 in mild acid electrolytes. Such a methodology developed can be extended to other energy storage systems, providing a universal approach to accurately identify the reaction mechanism of aqueous aluminum-ion batteries as well.
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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. In this work, we demonstrate a protocol for studying the dynamic evolution of the electrode material under electrochemical processes by integrating microscopic and spectroscopic analyses, operando magnetometry techniques, and density functional theory calculations. The presented methodology provides a real-time picture of the chemical, physical, and electronic structures of the material and its link to the electrochemical performance. Using Co(OH)2 as a prototype battery electrode and by monitoring the Co metal center under different applied voltages, we show that before a well-known catalytic reaction proceeds, an interfacial storage process occurs at the metallic Co nanoparticles/LiOH interface due to injection of spin-polarized electrons. Subsequently, the metallic Co nanoparticles act as catalytic activation centers and promote LiOH decomposition by transferring these interfacially residing electrons. Most intriguingly, at the LiOH decomposition potential, electronic structure of the metallic Co nanoparticles involving spin-polarized electrons transfer has been shown to exhibit a dynamic variation. This work illustrates a viable approach to access key information inside interfacial catalytic processes and provides useful insights in controlling complex interfaces for wide-ranging electrochemical systems.
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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. Various in/ex situ analyses and theoretical calculations prove that the steric hindrance effect can prevent electroactive sites from the attack by water molecules. Meanwhile, the redox reaction can be stabilized by an even distribution of electron cloud due to the conjugated structure of phenazine groups. Accordingly, the assembled Zn-PANI battery can allow stable and long-term charge-discharge reactions to occur at a potential as high as 2.0 V with a discharged plateau of 1.5 V, and it also shows high rate performance and stable long cycle life (75% capacity retention after 1000 cycles at 10 A g-1).