Entropy-driven Hydrated Eutectic Electrolytes with Diverse Solvation Configurations for All-Temperature Zn-Ion Batteries.

Batteries always encounter uncontrollable failure or performance decay under extreme temperature environments, which is largely limited by the properties of electrolytes. Herein, an entropy-driven hydrated eutectic electrolyte (HEE) with diverse solvation configurations is proposed to expand the operating temperature range of Zn-ion batteries. The HEE possesses over 40 types of Zn2+ solvation structure with uniform distribution, contributing to its much higher solvation configurational entropy compared to the conventional aqueous counterpart (only 6 types). These effectively promotes its anti-freezing ability under ultralow temperatures, with a high ionic conductivity of 0.42 mS cm-1 even at a low temperature of -40 °C. Moreover, the entropy-driven property can simultaneously enhance the thermal stability under a high temperature over +140 °C. Therefore, the HEE can enable full cells stably working over a wide temperature range of -40~+80 °C, performing over 1500 cycles with 100% capacity retention at -40 °C and 1000 cycles with ~72% capacity retention at +80 °C. This inspiring concept of entropy-driven electrolyte with quantized solvation configurational entropy value has charming potential for designing future special batteries with excellent adaptability towards extreme temperature environments.

Self-Powered Agricultural Product Preservation and Wireless Monitoring Based on Dual-Functional Triboelectric Nanogenerator.

The global annual vegetable and fruit waste accounts for more than one-fifth of food waste, mainly due to deterioration. In addition, agricultural product spoilage can produce foodborne illnesses and threaten public health. Eco-friendly preservation technologies for extending the shelf life of agricultural products are of great significance to socio-economic development. Here, we report a dual-functional TENG (DF-TENG) that can simultaneously prolong the storage period of vegetables and realize wireless storage condition monitoring by harvesting the rotational energy. Under the illumination of the self-powered high-voltage electric field, the deterioration of vegetables can be effectively slowed down. It can not only decrease the respiration rate and weight loss of pakchoi but also increase the chlorophyll levels (∼33.1%) and superoxide dismutase activity (∼11.1%) after preservation for 4 days. Meanwhile, by harvesting the rotational energy, the DF-TENG can be used to drive wireless sensors for monitoring the storage conditions and location information of vegetables during transportation in real time. This work provides a new direction for self-powered systems in cost-effective and eco-friendly agricultural product preservation, which may have far-reaching significance to the construction of a sustainable society for reducing food waste.

All-Round Ionic Liquids for Shuttle-Free Zinc-Iodine Battery.

The practical implementation of aqueous zinc-iodine batteries (ZIBs) is hindered by the rampant Zn dendrites growth, parasite corrosion, and polyiodide shuttling. In this work, ionic liquid EMIM[OAc] is employed as an all-round solution to mitigate challenges on both the Zn anode and the iodine cathode side. First, the EMIM+ embedded lean-water inner Helmholtz plane (IHP) and inert solvation sheath modulated by OAc- effectively repels H2 O molecules away from the Zn anode surface. The preferential adsorption of EMIM+ on Zn metal facilitates uniform Zn nucleation via a steric hindrance effect. Second, EMIM+ can reduce the polyiodide shuttling by hindering the iodine dissolution and forming an EMIM+ -I3 - dominated phase. These effects holistically enhance the cycle life, which is manifested by both Zn || Zn symmetric cells and Zn-I2 full cells. ZIBs with EAc deliver a capacity decay rate of merely 0.01 ‰ per cycle after over 18,000 cycles at 4 A g-1 , and lower self-discharge and better calendar life than the ZIBs without ionic liquid EAc additive.

Janus interface enables reversible Zn-ion battery by regulating interfacial water structure and crystal-orientation.

To tackle the shortcomings of traditional battery systems, there has been much focus on aqueous Zn-ion batteries due to various advantages. However, they still suffer from poor stability of Zn anodes. Here, a methionine additive with unique Janus properties is proposed to regulate the behavior of the interface between Zn anodes and the electrolyte environment. Systematic characterizations as well as calculations elucidate that the Janus additive is adsorbed on the Zn anode via zincophilic -NH2, changing the structure of the electric double layer and breaking the hydrogen bonding network among H2O molecules through hydrophobic S-CH3. At the same time, it can induce preferential formation of Zn(101) with high reversibility. The above two functions contribute to the dendrite inhibiting ability of Zn anodes. As validated, fabricated Zn//Zn symmetric cells achieve stable cycles of 4500 h, 1165 h, and 318 h at 1, 5 and 10 mA cm-2/mA h cm-2, respectively. Furthermore, Zn//Cu asymmetric cells with an average coulombic efficiency of 98.9% for 2200 stable cycles can be realized. Finally, Zn//MnO2 full cells exhibit 79.9% capacity retention with an ultra-high coulombic efficiency of 99.9% for 1000 cycles, much better than that of the pure Zn(ClO4)2 system, indicating the great potential of this useful strategy in aqueous batteries.

A host potassiophilicity strategy for unprecedentedly stable and safe K metal batteries.

Creating high-performance host materials for potassium (K) metal anodes remains a significant challenge due to the complex preparation process and poor K reversibility. In our work, we developed a potassiophilicity strategy using an oxygen-modified carbon cloth (O-CC) network as a host for K metal anodes. The O-CC network exhibited superior potassiophilic ability, and this improvement was also observed in other carbon hosts using the same process. The oxygen-induced epoxy group in the carbon network regulates interface electrons and enables strong binding of K adatoms through orbital hybridization, resulting in fewer side reactions with the electrolyte and promoting K-ion desolvation and uniform deposition. These factors result in unprecedented stability of the carbon network host, with a long lifespan of over 5500 hours at 0.5 mA cm-2/0.5 mA h cm-2 and 3500 h at 1 mA cm-2/0.5 mA h cm-2 in symmetric cells for K metal anodes, surpassing the cycle life of all previously reported K metal anodes. Furthermore, a high average coulombic efficiency of over 99.3% is demonstrated in O-CC//K cells during 210 cycles. The O-CC also exhibited a stable electrochemical performance, with a capacity retention of 73.3% in full cells coupled with a perylene-3,4,9,10-tetracarboxylic dianhydride cathode. We believe that this new strategy holds great promise for metal anodes in battery applications.

Electrolyte and Interphase Engineering of Aqueous Batteries Beyond "Water-in-Salt" Strategy.

Aqueous batteries are promising alternatives to non-aqueous lithium-ion batteries due to their safety, environmental impact, and cost-effectiveness. However, their energy density is limited by the narrow electrochemical stability window (ESW) of water. The "Water-in-salts" (WIS) strategy is an effective method to broaden the ESW by reducing the "free water" in the electrolyte, but the drawbacks (high cost, high viscosity, poor low-temperature performance, etc.) also compromise these inherent superiorities. In this review, electrolyte and interphase engineering of aqueous batteries to overcome the drawbacks of the WIS strategy are summarized, including the developments of electrolytes, electrode-electrolyte interphases, and electrodes. First, the main challenges of aqueous batteries and the problems of the WIS strategy are comprehensively introduced. Second, the electrochemical functions of various electrolyte components (e.g., additives and solvents) are summarized and compared. Gel electrolytes are also investigated as a special form of electrolyte. Third, the formation and modification of the electrolyte-induced interphase on the electrode are discussed. Specifically, the modification and contribution of electrode materials toward improving the WIS strategy are also introduced. Finally, the challenges of aqueous batteries and the prospects of electrolyte and interphase engineering beyond the WIS strategy are outlined for the practical applications of aqueous batteries.

Boosting photodetection performance of Cs2AgBiBr6 through A-site Rb substitution and interfacial engineering.

Bismuth-based double perovskite Cs2AgBiBr6 shows promise as a photodetection material. However, its detection performance and application are limited by high-exciton binding energy and poor carrier mobility. In this study, we address these limitations by delicately designing a solution-based method for incorporating A-site Rubidium (Rb) substitution into Cs2AgBiBr6 double perovskite films. The introduction of Rb resulted in a significant decrease in trap defect density and an improvement in film quality. The trap-filled limit voltage (VTFL) of pure and Rb-doped CABB film is determined to be 1.71 V and 0.48 V, respectively. Subsequently, by introducing an ultrathin atomic-layer-deposited (ALD) TiO2 films, the fabricated CABB photodetectors exhibit significantly improved photoresponse performance. The response speed and -3dB bandwidth are boosted from ∼93 ms to ∼350 µs and broadened from 1.4 kHz to 17 kHz, respectively. Density Functional Theory (DFT) calculations indicate Rb-substitution shortens the bond length and weaken exciton binding energy. Furthermore, we demonstrate a wireless near ultraviolet (UV) light communication system using CABB photodetectors as light receivers. Our findings provide an efficient approach to utilize A-site cation substitution as a tuning parameter for photodetection in high-exciton binding energy perovskite materials, thereby extending the potential applications of other functional perovskites.

Thiamethoxam adsorption by ZnCl2 modified cow manure biochar: Mechanism and quantitative prediction.

The overuse of thiamethoxam (THM) has threatened the survival of living organisms and it is necessary to find an environmentally friendly material to remove THM frequently detected in water. Biochar prepared from cow manure modified with ZnCl2 (Zn-CBC) was used to remove THM. Compared to the unmodified cow manure biochar (CBC), the removal ratio of THM by Zn-CBC was enhanced 35 times. In the mechanistic analysis, SEM and BET showed that Zn-CBC had a good pore structure and its specific surface area (166.502 m2 g-1) increased to 17 times that of CBC, indicating that Zn-CBC had good pore adsorption properties. The adsorption kinetic and isotherm implied that the main mechanism was chemisorption including π-π interaction and H-bonding. Furthermore, the stable graphitized structure of Zn-CBC allowed for efficient adsorption and reusability. In addition, this study constructed an intelligent prediction model using batch experiment data, and the high R2 (0.978) and low RMSE (0.057) implied that the model could accurately and quantitatively predict the adsorption efficiency. This paper provides a novel perspective to simultaneously remove the neonicotinoid insecticides and realize the resource utilization of cow manure.

Triboelectric nanogenerators as self-powered sensors for biometric authentication.

As a prerequisite for ensuring the safety and stability of people's daily lives, security monitoring has become increasingly important in the current rapid development of the economy. Intelligent sensing technology with lower power consumption will promote the upgradation of electronic devices and expand new application requirements. In this review, the recent progress in triboelectric nanogenerators (TENGs) as self-powered intelligent sensors for monitoring different kinds of biometric characteristics is summarized, including sliding behavior, handwriting behavior, keystroke dynamics, gait characteristics, and voice characteristics. Additionally, the applications of self-powered systems based on TENGs in individual electronics authentication and home security are comprehensively summarized. Finally, the remaining challenges and open opportunities are also discussed.

Perovskite-based color camera inspired by human visual cells.

There are two primary types of photoreceptor cells in the human eye: cone cells and rod cells that enable color vision and night vision, respectively. Herein, inspired by the function of human visual cells, we develop a high-resolution perovskite-based color camera using a set of narrowband red, green, blue, and broadband white perovskite photodetectors as imaging sensors. The narrowband red, green, and blue perovskite photodetectors with color perceptions mimic long-, medium-, and short-wavelength cones cells to achieve color imaging ability. Also, the broadband white perovskite photodetector with better detectivity mimics rod cells to improve weak-light imaging ability. Our perovskite-based camera, combined with predesigned pattern illumination and image reconstruction technology, is demonstrated with high-resolution color images (up to 256 × 256 pixels) in diffuse mode. This is far beyond previously reported advanced perovskite array image sensors that only work in monochrome transmission mode. This work shows a new approach to bio-inspired cameras and their great potential to strongly mimic the ability of the natural eye.

Tailoring water structure with high-tetrahedral-entropy for antifreezing electrolytes and energy storage at -80 °C.

One of unsolved puzzles about water lies in how ion-water interplay affects its freezing point. Here, we report the direct link between tetrahedral entropy and the freezing behavior of water in Zn2+-based electrolytes by analyzing experimental spectra and molecular simulation results. A higher tetrahedral entropy leads to lower freezing point, and the freezing temperature is directly related to the entropy value. By tailoring the entropy of water using different anions, we develop an ultralow temperature aqueous polyaniline| |Zn battery that exhibits a high capacity (74.17 mAh g-1) at 1 A g-1 and -80 °C with ~85% capacity retention after 1200 cycles due to the high electrolyte ionic conductivity (1.12 mS cm-1). Moreover, an improved cycling life is achieved with ~100% capacity retention after 5000 cycles at -70 °C. The fabricated battery delivers appreciably enhanced performance in terms of frost resistance and stability. This work serves to provide guidance for the design of ultralow temperature aqueous batteries by precisely tuning the water structure within electrolytes.

Pt-Quantum-Dot-Modified Sulfur-Doped NiFe Layered Double Hydroxide for High-Current-Density Alkaline Water Splitting at Industrial Temperature.

Suitable electrocatalysts for industrial water splitting can veritably promote practical hydrogen applications. Rational surface design is exceptionally significant for electrocatalysts to bridge the gap between fundamental science and industrial expectation in water splitting. Here, Pt-quantum-dot-modified sulfur-doped NiFe layered double hydroxides (Pt@S-NiFe LDHs) are designed with eximious catalytic activity toward hydrogen evolution reaction (HER) under industrial condition. Benefiting from enhanced binding energy, mass transfer, and hydrogen release, Pt@S-NiFe LDHs exhibit outstanding activity in HER at high current densities. Notably, it obtains an impressively low overpotential of 71 mV and long-term stability of 200 h at 100 mA cm-2 , exceeding commercial 40% Pt/C and most reported Pt-based electrocatalysts. Its mass activity is 2.7 times higher than that of 40% Pt/C with an overpotential of 100 mV. Furthermore, at industrial temperature (65 °C), the electrolyzer based on Pt@S-NiFe LDH needs just 1.62 V to reach the current density of 100 mA cm-2 , superior to that of the commercial one of 40% Pt/C//IrO2 . This work provides rational ideas to develop electrocatalysts with exceptional performance for industrial high-temperature water splitting at high current densities.

Bifunctional Alloy/Solid-Electrolyte Interphase Layer for Enhanced Potassium Metal Batteries Via Prepassivation.

Potassium (K) metal batteries have attracted great attention owing to their low price, widespread distribution, and comparable energy density. However, the arbitrary dendrite growth and side reactions of K metal are attributed to high environmental sensitivity, which is the Achilles' heel of its commercial development. Interface engineering between the current collector and K metal can tailor the surface properties for K-ion flux accommodation, dendrite growth inhibition, parasitic reaction suppression, etc. We have designed bifunctional layers via prepassivation, which can be recognized as an O/F-rich Sn-K alloy and a preformed solid-electrolyte interphase (SEI) layer. This Sn-K alloy with high substrate-related binding energy and Fermi level demonstrates strong potassiophilicity to homogeneously guide K metal deposition. Simultaneously, the preformed SEI layer can effectually eliminate side reactions initially, which is beneficial for the spatially and temporally KF-rich SEI layer on K metal. K metal deposition and protection can be implemented by the bifunctional layers, delivering great performance with a low nucleation overpotential of 0.066 V, a high average Coulombic efficiency of 99.1%, and durable stability of more than 900 h (1 mA cm-2, 1 mAh cm-2). Furthermore, the high-voltage platform, energy, and power densities of K metal batteries can be realized with a conventional Prussian blue analogue cathode. This work provides a paradigm to passivate fragile interfaces for alkali metal anodes.

Self-Healing of Prussian Blue Analogues with Electrochemically Driven Morphological Rejuvenation.

Maintaining the morphology of electrode materials with high invertibility contributes to the prolonged cyclic stability of battery systems. However, the majority of electrode materials tend to degrade during the charge-discharge process owing to the inevitable increase in entropy. Herein, a self-healing strategy is designed to promote morphology rejuvenation in Prussian blue analogue (PBA) cathodes by cobalt doping. Experimental characterization and theoretical calculations demonstrate that a trace amount of cobalt can decelerate the crystallization process and restore the cracked areas to ensure perfect cubic structures of PBA cathodes. The electric field controls the kinetic dynamics, rather than the conventional thermodynamics, to realize the "electrochemically driven dissolution-recrystallization process" for the periodic self-healing phenomenon. The properties of electron transportation and ion diffusion in bulk PBA are also improved by the doping strategy, thus boosting the cyclability with 4000 cycles in a diluent electrolyte. This discovery provides a new paradigm for the construction of self-healing electrodes for cathodes.

Anion-Trap Engineering toward Remarkable Crystallographic Reorientation and Efficient Cation Migration of Zn Ion Batteries.

Zn batteries are considered as potential candidates in future power sources, however suffer problems of rampant dendrite/by-product on Zn anodes, torpid Zn2+ transfer/diffusion and poor energy density. Inspired by the host-guest interaction chemistry, an anion-trap agent ß-cyclodextrin (ß-CD) is introduced into the Zn(ClO4 )2 electrolyte to induce dominant Zn (002) deposition and improve Zn2+ migration behaviors. The anion ClO4 - is revealed to be trapped inside the cavity of ß-CD, impairing barriers for Zn2+ migration and significantly elevating the Zn2+ transference number to 0.878. Meanwhile, the ß-CD@ClO4 - complex shows the function in preferential growth of the Zn (002), blocking the approach of dendrite growth. Above combined functions lead to substantial enhancement in long-term stability and cell capacity, as proved by 10 times longer life of Zn||Zn symmetric cells and 57 % capacity increasement of Zn-MnO2 full cells (at 0.1 A g-1 ) compared with that of pure Zn(ClO4 )2 electrolyte.

Perovskite Wide-Angle Field-Of-View Camera.

Researchers have attempted to create wide-angle field-of-view (FOV) cameras inspired by the structure of the eyes of animals, including fisheye and compound eye cameras. However, realizing wide-angle FOV cameras simultaneously exhibiting low distortion and high spatial resolution remains a significant challenge. In this study, a novel wide-angle FOV camera is developed by combining a single large-area flexible perovskite photodetector (FP-PD) using computational technology. With this camera, the proposed single-photodetector imaging technique can obtain high-spatial-resolution images using only a single detector, and the large-area FP-PD can be bent further to collect light from a wide-angle FOV. The proposed camera demonstrates remarkable features of an extraordinarily tunable wide FOV (greater than 150°), high spatial resolution of 256 × 256 pixels, and low distortion. It is believed that the proposed compatible and extensible camera prototype will promote the development of high-performance versatile FOV cameras.

Chaotropic Polymer Additive with Ion Transport Tunnel Enable Dendrite-Free Zinc Battery.

Zn batteries are considered the new-generation candidate for large-scale energy storage systems, taking both safety and environmental problems into account. They are still restricted by unexpected dendrite/byproducts occurring on the Zn anodes. We hereby screen a powerful polymer type additive, hyaluronic acid (HA), to regulate the typical ZnSO4 electrolyte for obtaining dendrite-free Zn ion batteries. The intrinsically chaotropic property of the HA molecule can efficiently destruct the original hydrogen-bonds from H2O-H2O, thus restricting the common parasitic reactions derived from the large amount of active water molecules. Simultaneously, the abundant functional groups along the long chain from HA additives can construct an effective tunnel for transferring Zn2+ smoothly, enabling an obviously improved Zn ion transference number of 0.62. Owning to the above intriguing mechanism for regulating the solvation structure of electrolyte systems, the HA additives can greatly increase the cycling life of Zn-Zn symmetric cells to 2200 and 800 h under the conditions of 1 mA cm-2/1 mAh cm-2 and 5 mA cm-2/5 mAh cm-2, respectively. Modified performance for both Zn-Ti and Zn-MnO2 can all be realized by this valid additive, elucidating it can be potentially utilized in large-scale Zn based aqueous energy storage devices.

New enhancement mechanism of an ether-based electrolyte in cobalt sulfide-containing potassium-ion batteries.

The performance of potassium (K)-ion batteries (KIBs) is not only dependent on electrode materials but also highly related to the electrolyte. In this work, we obtained a cobalt sulfide (CoS)-containing hybrid by the hydrothermal method and subsequent thermal treatment for K-ion storage. After ether-based electrolyte matching, the CoS-containing hybrid achieves a specific capacity of 229 mA h g-1 at 1 A g-1 after 300 cycles, and presents enhanced performance in the ether-based electrolyte. According to our measurement and calculation, the CoS-containing hybrid in the ether-based electrolyte promotes the formation of a highly anionic coordination solvated structure, which contributes to the enhancement of the stability of the electrolyte for K-ion storage. In addition, the strong coordination of anions also facilitates the rapid separation of the solvent during the potassiation process, which is also in favor of the decrease of the side reaction of the CoS@RGO hybrid for KIBs. We believe that our work will provide a new perspective on electrolyte engineering to boost the electrode material performance for K-ion storage.

Design of reduced graphene oxide coating carbon sub-microspheres hierarchical nanostructure for ultra-stable potassium storage performance.

The development of high-performance carbon-based anode materials is still a significant challenge for K-ion storage. In our work, we designed reduced graphene oxide coating carbon sub-microspheres hierarchical nanostructure (CS@RGO) hierarchical nanostructure via a simple freeze-drying and subsequent pyrolysis as anode for K-ion batteries (KIBs), which presented an excellent electrochemical performance for K-ion storage, with a reversible specific capacity of 295 mAh g-1 after 100 cycles at 100 mAh g-1. Even at a high current density of 1 A g-1, our CS@RGO still achieves ultra-stable K-ion storage of 200 mAh g-1 at 1 A g-1 after 5000 cycles almost without capacity fade. According to the galvanostatic intermittent titration technique result, the CS@RGO hybrid receives a high average diffusion coefficient of 7.35 × 10-8 cm2 s-1, contributing to the rapid penetration of K-ion, which facilitates the enhancement of electrochemical performance for KIBs. Besides, we also use Raman spectra to investigate the electrochemical behavior of our CS@RGO hybrid for K-ion storage and confirm the reaction process. We believe that our work will offer the opportunity to enable ultra-stable carbon-based materials by the structure design in the K-ion battery field.

Achieving dual-color imaging by dual-band perovskite photodetectors coupled with algorithms.

Dual-color or multispectral imaging based on conventional optical imaging techniques is suffering from the bottleneck of complex manufacturing and time consumption caused by multiple imaging. Herein, we develop a dual-color computational imaging system combining a vertically stacked dual-channel dual-band perovskite photodetectors (PDs) and the advanced Fourier imaging algorithm. Significantly, our imaging system bypasses the complex fabrication process of high-density dual-band PD arrays and is enabled to capture two high-resolution spectral images at the same time. Based on the experiments and simulations, we confirm that the spectral overlap of dual-band PDs will cause detrimental effect for color identification, and optimizing the bandwidth spectrum is beneficial for achieving much better spectral imaging. Moreover, we have further improved the imaging quality by increasing the sampling rate and suppressing current fluctuations. We suggest that these results provide important interesting insights for the development of advanced imaging systems, including IR imaging, THz imaging, multispectral/hyperspectral imaging, etc.