Toxic metal pollution is one of the environmental problems that seriously affect water resources and ecosystems. Antimony, recognized for its teratogenic and carcinogenic properties, poses significant health risks due to its widespread presence in natural water sources. In this study, cobalt-doped manganese oxide bimetallic composites were designed as an efficient adsorbent for the antimony removal from water. The adsorbent exhibits robust performance over a range of pH values, achieves a significant adsorption capacity of 591.1 mg/g, and exhibits adsorption equilibrium within 25 min. The effectiveness of the adsorption is attributed to the interaction between metal-O bonds and antimony, as well as the hydrogen bonding. In line with the concept of sustainable development, waste adsorbents are used as negative electrodes for SbO2--based aqueous alkaline batteries. It exhibits a high reversible specific capacity of 122.8 mAh.g(-1). This research not only sheds light on innovative approaches to antimony removal but also opens up avenues for the sustainable reuse of waste materials, in line with the principles of sustainable development.

Ion exchange is a promising synthetic method for alleviating severe cation mixing in traditional layered oxide materials for lithium-ion batteries, leading to enhanced structural stability. However, the underlying mechanisms of ion exchange are still not fully understood. Such a fundamental study of the ion-exchange mechanism is needed for achieving the controllable synthesis of layered oxides with a stable structure. Herein, we thoroughly unearth the underlying mechanism that triggers the ion exchange of Ni-rich materials in aqueous solutions by examining time-resolved structural evolution combined with theoretical calculations. Our results reveal that the reaction pathway of ion exchange can be divided into two steps: protonation and lithiation. The proton is the key to achieving charge balance in the ion exchange process, as revealed by X-ray adsorption spectroscopy and inductive coupled plasma analysis. In addition, the intermediate product shows high lattice distortion during ion exchange, but it ends up with a most stable product with high lattice energy. Such apparent discrepancies in lattice energy between materials before and after ion exchange emphasize the importance of synthetic design in structural stability. This work provides new insights into the ion-exchange synthesis of Ni-rich oxide materials, which advances the development of cathode materials for high-performance lithium-ion batteries.

An organic cathode material for zinc-ion batteries shows a reliable proton transport mechanism. It uses a pyrazine ring as the energy storage unit and H+ as the shuttle ion, enabling high functionality utilization with rapid redox kinetics.

Lithium sulfide (Li2S) is the critical raw material used for the synthesis of sulfide solid-state electrolytes, but its high cost and pollution restrict the commercialization of sulfide solid-state electrolytes and sulfide-based all-solid-state batteries. A new green and cost-effective method for the synthesis of high-quality Li2S is designed and proposed in this work. The method of reducing Li2SO4 with H2 circumvents the disadvantages of many side reactions, complicated purification processes, impure products and emission of greenhouse gases (CO and CO2) associated with traditional carbothermal reduction methods, and high-purity Li2S (H-Li2S) is obtained. Subsequently, H-Li5.6PS4.6Cl1.4 solid electrolyte was synthesized and compared with the C-Li5.6PS4.6Cl1.4 electrolyte synthesized from commercial Li2S (C-Li2S). The ionic conductivity (8.06 mS cm-1) and chemical/electrochemical stability as cathode/anode material were better than those of C-Li5.6PS4.6Cl1.4. Besides, the rate performance and long cycling stability of an all-solid-state lithium battery NCM//Li5.6PS4.6Cl1.4//Li-In assembled with H-Li5.6PS4.6Cl1.4 are better than those of batteries assembled with C-Li5.6PS4.6Cl1.4. It can maintain a discharge capacity of 133.23 mA h g-1 after 300 cycles at 1C (95% of the initial discharge capacity), and has a high discharge capacity of 127.9 mA h g-1 at 3C. The high electrochemical performance of the all-solid-state battery confirms the superiority of high-purity H-Li2S and the advantages of the hydrogen reduction method. A new low-cost method for the synthesis of high-quality Li2S is designed and applied to sulfide solid electrolyte and all-solid-state battery.

Anionic redox activity can trigger structural instability in Li‐rich Mn‐based cathodes. Lattice oxygen activity can be tuned through liquid acid‐induced spinel phases and oxygen vacancies. However, the liquid‐acid‐modified surface is still attacked by the electrolyte. Besides, the underlying mechanism of spinel phase suppression of lattice oxygen activity is controversial. Here, a solid acid strategy for modification is proposed and the underlying mechanism is investigated in detail. Unique solid acid can in situ generate an interface protection layer and remarkably stabilize the structure. Theoretical calculations and experimental characterizations reveal that the spinel phase suppresses the irreversible loss of lattice oxygen by decreasing the O 2p non‐bonding energy level and enriching electrons at the layered/spinel phase interface. The inert layer on the surface prevents highly active O n− from being attacked by electrolytes. The obtained material exhibits significantly reduced irreversible lattice oxygen release and improved electrochemical performance. After 300 cycles, a slow capacity fading of 0.177 mAh g −1 per cycle and suppressed voltage fading are achieved. This study reveals the regulation method and mechanism for the anion activity of oxide cathodes in next‐generation Li‐ion batteries.

The efficient and high-quality production for hydrogen through water electrolysis at high current densities is crucial for commercial utilization. However, the performance of existing hydrogen evolution reaction (HER) electrocatalysts is far from satisfactory. In this regard, we proposed a method to prepare Rh-Ni(OH)(2) catalyst based on Nickel foam (NF). The hydrolysis galvanic replacement of nickel boride with RhCl3 led to produce a lattice contraction in Ni(OH)(2) due to the rigid pressure generated, resulting in outstanding HER performance at high current densities. It achieves an industrial current density of 500 mA cm(-2) with an overpotential of 130 mV. Furthermore, at the industrially prefer temperature of 80 degrees C, only 67 mV overpotential is required. The catalyst also demonstrated exceptional stability, maintaining excellent performance even after a stability test of 100 days with a current density of 200 mA cm(-2). Through Density-functional theory (DFT) calculations, Rh series reduced the hydrogen adsorption free energy.

Aqueous Zn-metal batteries open up promising prospects for large-scale energy storage due to the advantages of ample components, cost-effectiveness, and safety features. However, the notorious dendritic development and unavoidable hydrogen evolution reaction of Zn have grown to be one of the main barriers inhibiting its further commercialization. Despite substantial studies, the mechanism of nucleation and deposition of Zn2+ ions on zinc layer surfaces remains elusive. Here, inspired by additive, the SnCl2 additive is introduced to initiate the in-situ formation of the ZnS-rich solid electrolyte interphase (SEI) layer on the Zn anode, which creates a protective "shielding effect" that hinders direct contact between water and the zinc surface, suppressing the random growth of Zn dendrites in the whole process. The mechanism of Zn nucleation was revealed by employing high-resolution transmission electron microscopy, consecutive electron diffraction coupled with finite element method (FEM) simulations. Moreover, spontaneously formed 3D architecture consists of micorsized hemispherical Sn particles not only suppresses the Zn dendrite growth by reducing the local current density, but also enables the lateral growth of Zn crystals by increasing the average surface energy. Such an electrolyte enables a long cycle life of over 2000 h in the Zn||Zn cell. Importantly, the assembled Zn||MnVO full cells with SnCl2 electrolyte also delivers substantial capacity (171.1mA h g-1 at 1 A h g-1), presenting a promising application. These discoveries not only deepen the comprehension of fundamental scientific knowledge regarding the microscopic reaction mechanism of the Zn anode but also offer significant insights for optimizing performance.

Lithium sulfide (Li2S) is a key raw material for synthesizing sulfide solid electrolytes (SSEs), which has been considered as one of the most promising solid electrolytes for all-solid-state lithium batteries (ASSLBs). However, the high cost of Li2S limits the development of SSEs. Herein, a novel approach for the preparation of Li2S through carbothermal reduction of lithium sulfate (Li2SO4) is designed and optimized. Two novel strategies for purifying rough Li2S materials are proposed in this work. A low raw material cost of $148 kg-1 and a high yield of 88.50 % are achieved. Subsequently, Li6PS5Cl and Li9.54Si1.74P1.44S11.7Cl0.3 solid electrolytes are synthesized with the selfmade Li2S and the corresponding electrochemical performances are evaluated. In NCMA|Li6PS5Cl|Li/In system, a high discharge capacity of 135 mAh g- 1 is maintained after 500 cycles at 1C. In NCMA|Li9.54Si1.74P1.44S11.7Cl0.3| Li/In system, a high discharge capacity of 132 mAh g- 1 is maintained after 350 cycles at 1C. The high capacity and long cycle life demonstrate the effectiveness of Li2S preparation and purification strategy proposed in this work.

High-capacity Li-rich Mn-based oxides (LRMOs) show great potential for enhancing the energy density of all-solid-state lithium batteries (ASSLBs). However, the intrinsically low electronic/ionic conductivity of LRMOs and bulk structural degradation lead to an inferior electrochemical performance. Herein, a single-crystal Li1.2Ni0.13Mn0.54Co0.13O2 (SC- LRMO) cathode is developed to address the challenges associated with charge-transport limitations and mechanical degradation of conventional polycrystalline (PC)-LRMO in ASSLBs. The results indicate that composite cathodes using small SC-LRMO achieve excellent electrochemical performance. Specifically, SC-LRMO not only delivers a high specific capacity of 316 mAh g(-1) at 0.05C but also exhibits a capacity retention of 86% after 300 cycles at 1C, outperforming the PC-LRMO (243 mAh g(-1), 84%). Comprehensive characterization reveals that the small single-crystal microstructure of SC-LRMO facilitates electrochemical reaction and mitigates detrimental mechanical degradation. Overall, this work expedites the practical application of LRMO cathodes in high-energy-density ASSLBs through dedicated morphology design.

Sulfide-based superionic conductors present great promise to achieve high energy density and safety for all-solid-state sodium batteries (ASSSBs). However, the poor electrolyte/electrode interface compatibility and humid air stability seriously hinder their deployment in ASSSBs. Herein, a series of high-performance Na3-square Sb1-4x(SnWCaTi)xS4 sulfide-based solid electrolytes (SSEs) are reported by coupling the vacancy effect with configurational entropy, which displays an excellent interface stability against sodium metal and an extraordinary tolerance toward the moist atmosphere, even for water. The optimized electrolyte effectively inhibits the detrimental mixed ion-electron conducting interphase formation, achieving the ultra-stable operation of Na-Na symmetric cell up to 1000 h. Furthermore, the Na+ diffusion kinetics is obviously enhanced by increasing the Na sites local anisotropy and Na vacancies. Eventually, the assembled TiS2//Na5Sn ASSSBs deliver a remarkable reversible capacity of 211.6 mAh g-1 at 0.5C with a long-term cycling performance of 450 cycles at room temperature. More importantly, it achieves a steady running up to 100 cycles at 1C even if this electrolyte is placed in the air with a dew temperature of 13.8 degrees C for 30 min, the highest values in the state-of-the-art sulfide-based ASSSBs. The well-designed SSEs open a new avenue for realizing the advanced and powerful ASSSBs. In this work, a humid air stability sulfide-based solid electrolyte for all-solid-state sodium batteries (ASSSBs) with excellent electrochemical performance is synthesized by coupling the vacancy effect with the configurational entropy strategy. The assembled TiS2//Na5Sn ASSSBs deliver remarkable long-term cycling performance and achieve a stable operation under different exposure time in a humid atmosphere with a dew temperature of 13.8 degrees C. image

Sodium-ion batteries (SIBs) are anticipated to be a potentially more cost-effective alternative to lithium-ion batteries (LIBs) for large-scale energy storage. Carbon materials are practical anodes, but the traditional production of hard carbon for SIBs often requires high temperatures exceeding 1300 degrees C. Aiming for a more economical approach, this work presents a carbon material synthesized through the low-temperature carbonization of 2,3-diaminophenazine and terephthalic acid IPB-C (600). Despite its low specific surface area, this carbon material demonstrates exceptional capacity and cycling stability because of its interlayer warping feature. It delivers a specific capacity of 370 mAh g(-1) at 300 mA g(-1) and maintains 77.98 % capacity retention after 1500 cycles. This research highlights the potential for producing high-capacity carbon negative electrode materials with cost-effective bulk chemicals for SIBs.

Sulfide solid electrolytes have attracted wide attention due to their high ionic conductivity. Li6PS5Cl is one of the most promising electrolytes for all-solid-state lithium batteries with high-energy-density. It is reported that the disordered arrangement of Cl- in the aragonite structure has a significant effect on the conductivity of Li6PS5Cl. In this work, the disorder of anion sites is modestly regulated by adjusting the ratio of S and Cl in Li6-xPS5-xCl1+x electrolyte. In addition, to verify the commonality of this strategy, Li5.6PS4.6Cl1.4 is prepared using self-made Li2S, and similar results are obtained. On this basis, the density of Li5.6PS4.6Cl1.4 electrolyte sheet is improved by hot-pressing, which can successfully inhibit the growth of lithium dendrites. As expected, the ionic conductivity of the sulfide electrolyte and the electrochemical performance of the ASSLBs are greatly improved. A highest ionic conductivity of 8.2 x 10(-3) S cm(-1) of Li5.6PS4.6Cl1.4 is obtained at room temperature. A high capacity retention of 99.99 % is maintained for NCM811 @Li2O//Li5.6PS4.6Cl1.4//Li-In system after 400 cycles at 1 C with ultra-high cathode loading of 35.6 mg cm(-2). Besides, the cost of sulfide electrolytes can be reduced as the decreased usage of Li2S. This work proposes a novel synthesis method of low-cost and high-performance Li6-xPS5-xCl1+x electrolytes.

Developing a highly efficient catalyst for the oxygen evolution reaction (OER) is of great significance for its application in electrocatalytic water splitting. Herein, a solid-solid transformation strategy has been developed to construct sulfur-doped Ni0.5Co0.5Fe2O4 spinel porous single-crystal nanosheet arrays on nickel foam (S-NCFO/NF). The single-crystalline nanosheet self-assembled nanostructures can provide fast charge transfer channels. With the effect of S-doping, a distorted/incomplete octahedral structure nanosheet can be formed. The unique porous S-NCFO nanosheets can provide a large number of active sites and sufficiently contact the electrolyte to adsorb OH- and desorb O-2. By virtue of the porous single-crystal nanosheet, sulfur-doped spinel structure, and the unique self-assembled nanosheet configurations, the S-NCFO/NF electrode exhibits enhanced OER performance with low overpotentials at 100 mA cm(-2) of 300 mV in 1 M KOH and 317 mV in 1 M KOH + 0.5 M NaCl. The synthesis strategy provides insight for the preparation and application of self-assembled nanostructures in electrocatalytic seawater splitting.

V5S8 has received extensive attention in the field of sodium-ion batteries (SIBs) due to its two-dimensional (2D) layered structure, and weak van der Waals forces between V-S accelerate the transport of sodium ions. However, the long-term cycling of V5S8 still suffers from volume expansion and low conductivity. Herein, a hollow nanotube V5S8@C (H-V5S8@C) with improved conductivity was synthesized by a solvothermal method to alleviate cracking caused by volume expansion. Benefiting from the large specific surface area of the hollow nanotube structure and uniform carbon coating, H-V5S8@C exhibits a more active site and enhanced conductivity. Meanwhile, the heterojunction formed by a few residual MoS2 and the outer layer of V5S8 stabilizes the structure and reduces the ion migration barrier with fast Na+ transport. Specifically, the H-V5S8@C anode provides an enhanced rate performance of 270.1 mAh g-1 at 15 A g-1 and high cycling stability of 291.7 mAh g-1 with a retention rate of 90.98% after 300 cycles at 5 A g-1. This work provides a feasible approach for the structural design of 2D layered materials, which can promote the practical application of fast-charging sodium-ion batteries.

Constructing an environmentally friendly and efficient electrocatalyst holds important and profound significance for energy-efficient hydrogen production. Replacing the oxygen evolution reaction with a lower potential urea oxidation reaction (UOR) may save energy in water electrolysis to produce hydrogen. The UOR is characterized by its high energy barrier, which results in slow reaction kinetics. In this study, we introduced Ba(OH)2 into Ni(OH)2 to form uniform nanosheets. Due to the introduction of Ba2+, the lattice expansion of Ni(OH)2 was triggered, leading to significant improvement in UOR activity. The catalyst achieved a current density of 100 mA cm-2 at only 1.316 V and exhibited remarkable stability over time. Density functional theory (DFT) calculations demonstrate that the Ba-Ni(OH)2 site significantly reduces the energy barrier for urea adsorption, intermediate steps, and desorption. This work provides a novel and environmentally friendly strategy for constructing energy-efficient and highly efficient catalysts through the doping of alkaline earth metals.

Lithium metal is the most promising anode for next-generation batteries due to its highest theoretical capacity and lowest electrochemical potential. However, its dendritic growth hinders its practical use due to the consequent poor reversibility, potential short-circuit, and safety concerns. Suppressing lithium dendrite is difficult since dendritic growth is thermodynamically and kinetically favorable. Herein, we guide lithium to uniformly deposit along the opposite direction to normal by a nanolayer Au coating on a commercial polypropylene separator. It prevents lithium dendrites from piercing the separator, instead of inhibiting dendrites growth only. Au is lithiophilic, and lithium is calculated to be more attracted to Au and is confirmed to uniformly deposit on Au at the separator side rather than on the current collector side. Furthermore, Au also regulates the morphology of deposited lithium from a mossy state to a bulky state. In this work, the symmetric cell with the designed structure achieves excellent electrochemical performances of a long-life cycle over 2,000 h at 1 C for 1 mA h cm-2. Pairing with LiFePO4 cathode as a full cell, lithium metal anode with Au-modified polypropylene separator exhibits extraordinary performance with a high Coulombic efficiency of 99.23% over 800 cycles at 1 C.

LiCoO 2 plays a key role in energy storage devices due to its high energy density. And the volumetric energy density of LiCoO 2 cathode can be significantly improved by increasing the charging cut‐off voltage to 4.6 V. However, the increase in resistance at the LiCoO 2 interface, and the damage to the LiCoO 2 from the outside to the inside by the HF generated that caused by the decomposition of the organic electrolyte and LiPF 6 under 4.6 V conditions are not conducive to structural stability during cycling. Here, it is shown that the decomposition of electrolyte and LiPF 6 is effectively mitigated by inhibiting the interfacial catalytic activity of LiCoO 2 using an atomically thin layer of MXenes as a interlayer. Density functional theory results suggest that the decomposition energy of LiPF 6 is 1.13 and 3.21 eV at the interface of LiCoO 2 and MXenes, respectively. Time of Flight Secondary Ion Mass Spectrometry results further indicate that the decomposition products of the organic electrolyte and LiPF 6 have a thinner thickness at the interface of MXenes (5 nm) than LiCoO 2 (10 nm). This study provides a new and universal strategy for stabilizing the cathode interface to support the development of high energy density lithium‐ion batteries.

In this paper, we combine NTGK with flow and heat transfer model to perform numerical calculations on battery and cold plate to investigate thermal characteristics of li-ion batteries cooled by liquid and performance of cold plate during entire discharge process. A battery heat generation model is created using Kriging method after impacts of ambient temperature, SOC, and discharge rate are examined. Additionally, a new sort of cold plate is suggested based on constructal-theory, which performs better than conventional cold plate. Constructal cold plate reduces time needed for battery average temperature and maximum temperature differential to 25 °C and 5 °C by 15.25 % and 10.58 % for TimeT and TimeΔT, respectively, and pressure drop Δp by 22.89 % when compared to straight channel cold plate. Cooling effect of constructal cold plate is marginally inferior to that of serpentine cold plate, but flow resistance is greatly decreased, and pressure drop is only about one-tenth that of serpentine cold plate. Performance of constructal cold plate was examined using orthogonal optimization to determine effects of width of inlet and outlet and length of major channels. TimeT, TimeΔT, and Δp are decreased by 11 %, 14.69 %, and 15.22 % after optimization, and comprehensive performance is nearly doubled with improved performance.

Antimony-based materials are rapidly developing towards industrialization, making it crucial to control potential toxicity and address sustainable antimony management. A strategy has been proposed to remove antimony from wastewater and sustainably convert the resulting antimony-enriched waste adsorbent into electrode materials. Herein, the porphyrin ligand-based zirconium metal-organic framework (PCN-222) was constructed for antimony adsorption. The antimony is initially adsorbed onto the Zr cluster nodes, spreads along the skeleton through hydrogen bonds, and finally terminates at the N-coordination fixed sites in the porphyrin ligand. Afterwards adsorption, the antimony-enriched waste adsorbent is converted to Sb nanoparticles embedded in N-doped porous carbon composite by one-step carbothermal reduction. The composite is applied into SbO2--based aqueous alkaline battery, which displays a high specific capacity with 122.5 mAh/g at 1 A/g and good cycling stability. The work provides valuable insights into the treatment of contaminated water and the management of antimony resources.

Li-rich Mn-based [xLi2MnO3 center dot(1-x)LiMO2] (LR) cathodes are low cost and have high energy density, indicating high commercialization potential. However, the low initial coulombic efficiency, poor rate performance, and inferior cycling durability of LR cathodes confer difficulty in such commercialization. Herein, we proposed the use of a few-layer MXene (Ti3C2) to improve electrochemical performance. We found that the few-layer MXene can improve the conductivity and provide additional capacity at low voltage (2.25 V), thereby greatly increasing the initial coulombic efficiency, rate, and cycle performance. The additional capacity may have originated from an interface space-charge storage with capacitive properties, that is, the storage and transport of ions and electrons at the interface of Ti3C2 and LR particles. The modified sample exhibited an initial coulombic efficiency of 94.3 % and 158 mAh g-1 at 5C. Even after 300 cycles at 5C, it retained 87.3 % of its capacity. This novel strategy can serve as a reference for the modification of other electrode materials and can also expand the application of MXene in the field of batteries.