Yolk-Shell MnSe/ZnSe Heterostructures with Selenium Vacancies Encapsulated in Carbontubes for High-Efficiency Sodium/Potassium Storage.

The pursuit of high-performance batteries has propelled the investigation into advanced materials and design methodologies. Herein, the yolk-shell MnSe/ZnSe heterojunction encapsulated in hollow carbontubes (MnSe/ZnSe@HCTs) is prepared as a prospective electrode material for sodium/potassium batteries. The band structure in the heterojunction is methodically adjusted and regulated by intentionally utilizing Mn with unpaired electrons in the 3d orbital. The ZnSe shell confer effectively mitigates volumetric expansion challenges inherent in ions insertion/extraction processes and 1D carbontubular conductive substrate avert the aggregation of MnSe/ZnSe nanoparticles. Concurrently, the heterojunctions implantation induces sublattice distortion and charge redistribution, enriching active sites and regulating band structure. The selenium vacancies within these heterojunctions contribute to the provision of abundant active sites, thereby promoting efficient ions insertion/extraction. In sodium-ion batteries (SIBs), MnSe/ZnSe@HCTs present a superior capacity of 475 mA hg-1 at 0.1 A g-1 and sustains a capacity of 408.5 mAh g-1 even after 1000 cycles. In potassium-ion batteries (KIBs), MnSe/ZnSe@HCTs deliver a higher specific capacity of 422 mAh g-1 at a current density of 0.1 A g-1 and maintain a high coulombic efficiency of 99% after 1000 cycles. The yolk-shell structured MnSe/ZnSe heterojunction demonstrates excellent electrode properties for high-performance sodium/potassium batteries, holding significant promise for future energy storage applications.

Electrodeposition of Ni/Cu Bimetallic Conductive Metal-Organic Frameworks Electrocatalysts with Boosted Oxygen Reduction Activity for Zinc-Air Batteries.

Zinc-air batteries employing non-Pt cathodes hold significant promise for advancing cathodic oxygen reduction reaction (ORR). However, poor intrinsic electrical conductivity and aggregation tendency hinder the application of metal-organic frameworks (MOFs) as active ORR cathodes. Conductive MOFs possess various atomically dispersed metal centers and well-aligned inherent topologies, eliminating the additional carbonization processes for achieving high conductivity. Here, a novel room-temperature electrochemical cathodic electrodeposition method is introduced for fabricating uniform and continuous layered 2D bimetallic conductive MOF films cathodes without polymeric binders, employing the organic ligand 2,3,6,7,10,11-hexaiminotriphenylene (HITP) and varying the Ni/Cu ratio. The influence of metal centers on modulating the ORR performance is investigated by density functional theory (DFT), demonstrating the performance of bimetallic conductive MOFs can be effectively tuned by the unpaired 3d electrons and the Jahn-Teller effect in the doped Cu. The resulting bimetallic Ni2.1Cu0.9(HITP)2 exhibits superior ORR performance, boasting a high onset potential of 0.93 V. Moreover, the assembled aqueous zinc-air battery demonstrates high specific capacity of 706.2 mA h g-1, and exceptional long-term charge/discharge stability exceeding 1250 cycles.

Solvent Induced Activation Reaction of MoS2 Nanosheets within Nitrogen/Sulfur-Codoped Carbon Network Boosting Sodium Ion Storage.

MoS2 , as a classical 2D material, becomes a capable anode candidate for sodium-ion batteries. However, MoS2 presents a disparate electrochemical performance in the ether-based and ester-based electrolyte with unclear mechanism. Herein, tiny MoS2 nanosheets embedded in nitrogen/sulfur-codoped carbon (MoS2 @NSC) networks are designed and fabricated through an uncomplicated solvothermal method. Thanks to the ether-based electrolyte, the MoS2 @NSC shows a unique capacity growth in the original stage of cycling. But in the ester-based electrolyte, MoS2 @NSC shows a usual capacity decay. The increasing capacity puts down to the gradual transformation from MoS2 to MoS3 with the structure reconstruction. Based on the above mechanism, MoS2 @NSC demonstrates an excellent recyclability and the specific capacity keeps around 286 mAh g-1 at 5 A g-1 after 5000 cycles with an ultralow capacity fading rate of only 0.0034% per cycle. In addition, a MoS2 @NSC‖Na3 V2 (PO4 )3 full cell with ether-based electrolyte is assembled and demonstrates a capacity of 71 mAh g-1 , suggesting the potential application of MoS2 @NSC. Here the electrochemical conversion mechanism of MoS2 is revealed in the ether-based electrolyte and significance of the electrolyte design on the promoting Na ion storage behavior is highlighted.

Exploring The Synergistic Effect Of CoSeP/CoP Interface Catalyst For Efficient Urea Electrolysis.

Electrocatalytic oxidation of urea (UOR) is a potential energy-saving hydrogen production technology that can replace oxygen evolution reaction (OER). Therefore, CoSeP/CoP interface catalyst is synthesized on nickel foam using hydrothermal, solvothermal, and in situ template methods. The strong interaction of tailored CoSeP/CoP interface promotes the hydrogen production performance of electrolytic urea. During the hydrogen evolution reaction (HER), the overpotential can reach 33.7 mV at 10 mA cm-2 . The cell voltage can reach 1.36 V at 10 mA cm-2 in the overall urea electrolytic process. Notably, the overall urine electrolysis performance of the catalyst in the human urine medium can reach 1.40 V at 10 mA cm-2 and can exhibit durable cycle stability at 100 mA cm-2 . Density functional theory (DFT) proves that the CoSeP/CoP interface catalyst can better adsorb and stabilize reaction intermediates CO* and NH* on its surface through a strong synergistic effect, thus enhancing the catalytic activity.

Ultrathin-Walled Bi2 S3 Nanoroll/MXene Composite toward High Capacity and Fast Lithium Storage.

It is extremely important to develop a high energy density power source with rapid charge-discharge rate to meet people's growing needs. Hence, the development of advanced electrode materials is the top priority. Herein, a simple yet elaborate vacuum-assisted room-temperature phase transfer method is reported to transform MXene nanosheets from water into organic solution. Subsequently, an in-situ growth strategy is employed to deposit ultrathin-walled bismuth sulfide (Bi2 S3 ) nanorolls on MXene surface to prepare Bi2 S3 /MXene composite as an efficient and high-performance anode material for lithium-ion batteries. Attributed to the unique nanoroll-like structure and the strong synergistic effect, the Bi2 S3 /MXene-10 composite can deliver the high discharge capacities of 849 and 541 mAh g-1 at 0.1 and 5 A g-1 , respectively. The Bi2 S3 /MXene-10 electrode can deliver a high specific capacity of 541 mAh g-1 even after 600 cycles at a large current density of 1 A g-1 , proving the superb cycling stability of the Bi2 S3 /MXene-10 composite. Additionally, the simple vacuum-assisted room-temperature phase transfer strategy can enlighten researchers to expand the potential application of MXene. Furthermore, the formation mechanism of Bi2 S3 nanorolls is also proposed, which may open a new avenue to design and fabricate other nanoroll-like structures.

High-Energy-Density Aqueous Magnesium-Ion Battery Based on a Carbon-Coated FeVO4 Anode and a Mg-OMS-1 Cathode.

Porous FeVO4 is prepared by hydrothermal method and further modified by coating with carbon to obtain FeVO4 /C with a hierarchical pore structure. FeVO4 /C is used as an anodic electrode in aqueous rechargeable magnesium-ion batteries. The FeVO4 /C material not only has improved electrical conductivity as a result of the carbon coating layer, but also has an increased specific surface area as a result of the hierarchical pore structure, which is beneficial for magnesium-ion insertion/deinsertion. Therefore, an aqueous rechargeable magnesium-ion full battery is successfully constructed with FeVO4 /C as the anode, Mg-OMS-1 (OMS=octahedral molecular sieves) as the cathode, and 1.0 mol L-1 MgSO4 as the electrolyte. The discharge capacity of the Mg-OMS-1//FeVO4 /C aqueous battery is 58.9 mAh g-1 at a current density of 100 mA g-1 ; this value is obtained by calculating the total mass of two electrodes and the capacity retention rate of this device is 97.7 % after 100 cycles, with almost 100 % coulombic efficiency, which indicates that the system has a good electrochemical reversibility. Additionally, this system can achieve a high energy density of 70.4 Wh kg-1 , which provides powerful evidence that an aqueous magnesium-ion battery is possible.

Synthesis of Hierarchically Porous Sandwich-Like Carbon Materials for High-Performance Supercapacitors.

For the first time, hierarchically porous carbon materials with a sandwich-like structure are synthesized through a facile and efficient tri-template approach. The hierarchically porous microstructures consist of abundant macropores and numerous micropores embedded into the crosslinked mesoporous walls. As a result, the obtained carbon material with a unique sandwich-like structure has a relatively high specific surface (1235 m2 g-1 ), large pore volume (1.30 cm3 g-1 ), and appropriate pore size distribution. These merits lead to a comparably high specific capacitance of 274.8 F g-1 at 0.2 A g-1 and satisfying rate performance (87.7 % retention from 1 to 20 A g-1 ). More importantly, the symmetric supercapacitor with two identical as-prepared carbon samples shows a superior energy density of 18.47 Wh kg-1 at a power density of 179.9 W kg-1 . The asymmetric supercapacitor based on as-obtained carbon sample and its composite with manganese dioxide (MnO2 ) can reach up to an energy density of 25.93 Wh kg-1 at a power density of 199.9 W kg-1 . Therefore, these unique carbon material open a promising prospect for future development and utilization in the field of energy storage.

Enhanced sodium-storage performances of crumpled MXene nanosheets via alkali treatment-induced active ammonium ions.

Ti3C2Tx MXene demonstrates excellent potential as an anode material for sodium-ion capacitors. However, the narrow interlayer spacing and self-stacking phenomenon limit its applicability. In this study, we demonstrate an easy two-step method involving freezing and crumpling of MXene nanosheets to improve their Na-ion storage via the addition of ammonium ions (referred to as FCM nanosheets). Flat MXene particles aggregate and undergo folding in an alkaline solution. Ammonium ions can penetrate the gaps between MXene nanosheets, expanding interlayer spaces and inducing the formation of folds. Compared to MXene nanosheets, FCM nanosheets exhibit improved ion transfer kinetics and additional high capacity owing to the intercalated ammonium ions. The manufactured FCM anode exhibits remarkable electrochemical properties, including a high specific capacity of 313 mAhg-1 and stability over 15,000 cycles.

Dual carbon engineering enabling 1T/2H MoS2 with ultrastable potassium ion storage performance.

Potassium-ion batteries (PIBs) as a promising and low-cost battery technology offer the advantage of utilizing abundant and cost-effective K-salt sources. However, the effective adoption of PIBs necessitates the identification of suitable electrode materials. The 1T phase of MoS2 exhibits enhanced electronic conductivity and greater interlayer spacing compared to the 2H phase, leading to a capable potassium ion storage ability. Herein, we fabricated dual carbon engineered 1T/2H MoS2via a secure and straightforward ammonia-assisted hydrothermal method. The 1T/2H MoS2@rGO@C structure demonstrated an expanded interlayer spacing (9.3 Å). Additionally, the sandwich-like structural design not only enhanced material conductivity but also effectively curbed the agglomeration of nanosheets. Remarkably, 1T/2H MoS2@rGO@C exhibited impressive potassium storage ability, delivering capacities of 351.0 mA h g-1 at 100 mA g-1 and 233.8 mA h g-1 at 1000 mA g-1 following 100 and 1000 cycles, respectively. Moreover, the construction of a K-ion full cell was successfully achieved, utilizing perylene tetracarboxylic dianhydride (PTCDA) as the cathode, and manifesting a capacity of 294.3 mA h g-1 at 100 mA g-1 after 160 cycles. This underscores the substantial potential of employing the 1T/2H MoS2@rGO@C electrode material for PIBs.

Regulating nitrogen/sulfur terminals on 3D porous Ti3C2 MXene with enhanced reaction kinetics toward high-performance alkali metal ion storage.

In this paper, we have developed a simple and efficient sulfur-amine chemistry strategy to prepare a three-dimensional (3D) porous Ti3C2Tx composite with large amounts of N and S terminal groups. The well-designed 3D macroporous architecture presents enlarged interlayer spacing, large specific surface area, and unique porous structure, which successfully solves the re-stacking issue of MXene during storage and electrode fabrication. It is the amount of concentrated hydrochloric acid added to the S-EDA (ethylenediamine)/MXene colloidal suspension that is critical to the formation of 3D morphology. In addition, N and S terminals on MXene could improve the adsorption ability of K+. Owing to the synergistic effect of the structure design and terminal modification, the N, S codoped three-dimensional porous Ti3C2Tx (3D-NSPM) material shows a high surface capacitive contribution and rapid diffusion kinetics for K+ and Na+. As a result, the as-prepared 3D-NSPM delivers high reversible capacity (237 and 273 mAh g-1 at 0.1 A g-1 for PIBs and SIBs, respectively), superb cycling stability (84.9% capacity retention after 10,000 cycles at 1 A g-1 in PIBs and 74.0% capacity retention after 2200 cycles at 1 A g-1 in SIBs), and excellent rate capability (111 and 196 mAh g-1 at 5 A g-1 for PIBs and SIBs, respectively), which are superior to other MXene-based anodes for PIBs and SIBs. Moreover, the described strategy provides a new insight for constructing the 3D porous structure from 2D building blocks beyond MXene.

Nanoconfinement of ultra-small Bi2Te3 nanocrystals on reduced graphene oxide: a pathway to high-performance sodium-ion battery anodes.

Bismuth telluride (Bi2Te3) nanomaterials have attracted considerable attention owing to their intriguing physicochemical properties and wide-ranging potential applications arising from their distinctive layered structure and nanoscale size effects. However, synthesizing sub-100 nm ultra-small Bi2Te3 nanocrystals remains a formidable challenge. To date, there has been little investigation on the performance of these ultra-small Bi2Te3 nanocrystals in sodium-ion batteries (SIBs). This study presents a general strategy for synthesizing ultra-small Bi2Te3 nanocrystals on reduced graphene oxide (Bi2Te3/rGO) through a nanoconfinement approach. First-principles calculations and electrochemical kinetic studies confirm that the ultra-small Bi2Te3/rGO composite material can effectively mitigate volumetric expansion, preserve electrode integrity, and enhance electron transfer, Na-ion adsorption, and diffusion capacity. As a result, the Bi2Te3/rGO electrode demonstrates a remarkable initial specific capacity of 521 mA h g-1 at 0.1 A g-1, showcasing outstanding rate behaviour and long-lasting cycle life exceeding 800 cycles at 1 A g-1 while preserving exceptional rate properties. The function of the battery is indicated by ex situ TEM and XPS findings, which propose a conventional dual mechanism involving conversion and alloying. This work paves the way for rapid advancements in Bi2Te3-based SIB anodes while contributing to our understanding of sodium ion storage mechanisms.

Iron-doping and facet engineering of NiSe octahedron for synergistically enhanced triiodide reduction activity in photovoltaics.

Reasonable design of cost-effective counter electrode (CE) catalysts for triiodide (I3-) reduction reaction (IRR) by simultaneously combining heteroatom doping and facet engineering is highly desired in iodine-based dye-sensitized solar cells (DSSCs), but really challenging. Herein, the density function theory (DFT) calculations were first conducted to demonstrate that the Fe-doped NiSe (111) showed an appropriate adsorption energy for I3-, increased number of metal active sites, reinforced charge-transfer ability, and strong interaction between 3d states of metal sites and 5p state of I1 atoms in I3-, compared to NiSe (111). Based on this finding, the well-defined Fe-NiSe octahedron with exposed (111) plane (marked as Fe-NiSe (111)) and NiSe octahedron with the same exposed plane (named as NiSe (111)) are controllably synthesized. When the as-prepared Fe-NiSe (111) and NiSe (111) worked as CE catalysts, Fe-NiSe (111) exhibits improved electrochemical performance with higher power conversion efficiency (PCE) than NiSe (111), providing new opportunity to replace precious Pt for DSSCs.

Synergistic enhancement of oxygen vacancy enrichment and morphology regulation in CeO2-NiCo2O4 heterostructure catalysts for high-performance cathodes in direct borohydride-hydrogen peroxide fuel cells.

Hydrogen peroxide (H2O2) emerges as a viable oxidant for fuel cells, necessitating the development of an efficient and cost-effective electrocatalyst for the hydrogen peroxide reduction reaction (HPRR). In this study, we synthesized a self-supporting, highly active HPRR electrocatalyst comprising two morphologically distinct components: CeO2-NiCo2O4 nanowires and CeO2-NiCo2O4 metal organic framework derivatives, via a two-step hydrothermal process followed by air calcination. X-ray diffraction and transmission electron microscopy analysis confirmed the presence of CeO2 and NiCo2O4, revealing the amalgamated interface between them. CeO2 exhibits multifunctionality in regulating the surface electronic configuration of NiCo2O4, fostering synergistic connections, and introducing oxygen deficiencies to enhance the catalytic efficacy in HPRR. Electrochemical measurements demonstrate a reduction current density of 789.9 mA·cm-2 at -0.8 V vs. Ag/AgCl. The assembly of direct borohydride-hydrogen peroxide fuel cell (DBHPFC) exhibits a peak power density of 45.2 mW·cm-2, demonstrating durable stability over a continuous operation period of 120 h. This investigation providing evidence that the fabrication of heterostructured catalysts based on CeO2 for HPRR is a viable approach for the development of high-efficiency electrocatalysts in fuel cell technology.

A graphene-like hollow sphere anode for lithium-ion batteries.

We report a flash Joule heating method for the rapid preparation of graphene-like materials. The L-GHS exhibited a uniform diameter of 200 nm and an ideal specific surface area of 670 m2 g-1. Meanwhile, the specific capacity of L-GHS remained at 942 mA h g-1 after 600 cycles (1 A g-1), which shows excellent electrochemical performance.

A High-Rate and Long-Life Aqueous Rechargeable Mg-Ion Battery Based on an Organic Anode Integrating Diimide and Triazine.

Aqueous Mg-ion batteries (MIBs) lack reliable anode materials. This study concerns the design and synthesis of a new anode material - a π-conjugate of 3D-poly(3,4,9,10-perylenetracarboxylic diimide-1,3,5-triazine-2,4,6-triamine) [3D-P(PDI-T)] - for aqueous MIBs. The increased aromatic structure inhibits solubility in aqueous electrolytes, enhancing its structural stability. The 3D-P(PDI-T) anode exhibits several notable characteristics, including an extremely high rate capacity of 358 mAh g-1 at 0.05 A g-1 , A 3D-P(PDI-T)‖Mg2 MnO4 full cell exhibits a reversible capacity of 148 mAh g-1 and a long cycle life of 5000 cycles at 0.5 A g-1 . The charge storage mechanism reveals a synergistic interaction of Mg2+ and H+ cations with C-N/C=O groups. The assembled 3D-P(PDI-T)‖Mg2 MnO4 full cell exhibits a capacity retention of around 95 % after 5000 cycles at 0.5 A g-1 . This 3D-P(PDI-T) anode sustained its framework structure during the charge-discharge cycling of Mg-ion batteries. The reported results provide a strong basis for a cutting-edge molecular engineering technique to afford improved organic materials that facilitate efficient charge-storage behavior of aqueous Mg-ion batteries.

A Potential Polycarbonyl Polyimide as Anode Material for Lithium-Ion Batteries.

Organic polymers have been considered reliable candidates for lithium storage due to their high capacity and lack of volume expansion. Compared with other organic polymers, polyimide has become a very promising electrode material for lithium-ion batteries (LIBs) because of its easy synthesis, customizable structure and structural stability. A large number of studies have confirmed that the benzene ring structure of polyimide has strong lithium storage capacity as an anode material. Hence, we designed and synthesized polyimide organic polymer (PBPAQ) for the first time. The unique spherical flower structure of this material enhances the interaction between the electrode material and the electrolyte by increasing the contact area. The PBPAQ anode has a specific discharge capacity of 738 mAh g-1 after 100 cycles at 0.1 A g-1 . The excellent lithium storage performance of this material laid a foundation for the research of the anode of LIBs in the future.

Hierarchical CoNiO2 Microflowers Assembled by Mesoporous Nanosheets as Efficient Electrocatalysts for Hydrogen Evolution Reaction.

In order to alleviate the energy crisis and propel a low-carbon economy, hydrogen (H2) plays an important role as a renewable cleaning resource. To break the hydrogen evolution reaction (HER) bottleneck, we need high-efficiency electrocatalysts. Based on the synergistic effect between bimetallic oxides, hierarchical mesoporous CoNiO2 nanosheets can be fabricated. Combining physical representations with electrochemical measurements, the resultant CoNiO2 catalysts present the hierarchical microflowers morphology assembled by mesoporous nanosheets. The ultrathin two-dimensional nanosheets and porous surface characteristics provide the vast channels for electrolyte injection, thus endowing CoNiO2 the outstanding HER performance. The excellent performance with a fewer onset potential of 94 mV, a smaller overpotential at 10 mA cm-2, a lower Tafel slope of 109 mV dec-1 and better stability after 1000 cycles makes CoNiO2 better than that of metallic Co and metallic Ni.

Boosting Magnesium Ion Storage Behavior via Heteroelement Doping in a Porous Tunnel Framework Cathode for Aqueous Mg-Ion Batteries.

To relieve the overwhelming pressure on fossil energy, aqueous magnesium ion batteries attracted tremendous attention owing to their low cost and high safety. However, the cathode materials are apt to occur lattice distortion because of the electrostatic interaction between magnesium ions and crystal. The 2×2 manganese octahedral molecular sieve with potassium ions and water located in the tunnels (K-OMS-2), utilized as a cathode material for chargeable magnesium ions batteries, is exposed to irreversible Mg2+ intercalation/deintercalation due to lattice distortion, which heavily damages the electrochemical properties and declines the capacity. Herein, we carry out an ion doping strategy to overcome the above issues, leading to an enhanced Mg Mg2+ storage behavior. The Nb or V cation is successfully doped into K-OMS-2 by a facile reflux method under room temperature. The specific surface area is enlarged by the addition of cations, which promise a large electrode-electrolyte contact area. The Nb and V doped K-OMS-2 present a capacity of 252.6 and 265.9 mAh/g at 20 mA/g, respectively. This work demonstrates an ion doping approach toward exploiting the stable and high-capacity Mg-ion battery cathode and provides potential cathode materials for a large-scale aqueous Mg-ion-based energy storage system.

Surface engineering of core-shell MoS2@N-doped carbon spheres as stable and ultra-long lifetime anode for sodium-ion batteries.

MoS2 is regarded as a hopeful anode candidate for sodium-ion batteries (SIBs) due to their various merits such as high specific capacity, abundant raw material reserves and low cost. However, their practical application is impeded by unsatisfied cycling ability due to the intense mechanical stress and unstable solid electrolyte interphase (SEI) during Na+ insertion/extraction process. Herein, spherical MoS2@polydopamine derived highly conductive N-doped carbon (NC) shell composites (MoS2@NC) are designed and synthesized to promote the cycling stability. The internal MoS2 core is optimized and restructured from the original micron-sized block to the ultra-fine nanosheets during initial 100-200 cycles, which not only improves the utilization of electrode materials but also shortens the ion transport distance. The outer flexible NC shell effectively maintains the original spherical structure of the overall electrode material and prevents the occurrence of large-scale agglomeration, which is conducive to form a stable SEI layer. Therefore, the core-shell MoS2@NC electrode presents a remarkable cyclic stability and a capable rate performance. Under a high rate of 20 A g-1, the high capacity of 428 mAh g-1 can be acquired after over ultra-long 10,000 cycles without obvious capacity loss. Moreover, the MoS2@NC‖Na3V2(PO4)3 full-cell assembled by employing commercial Na3V2(PO4)3 cathode can achieve a high capacity retention of 91.4% after 250 cycles at 0.4 A g-1. This work reveals the promising prospect of MoS2-based materials as anode of SIBs, and also has some inspirations on the structural design for conversion-type electrode materials.

Microwave-ultra-fast recovery of valuable metals from spent lithium-ion batteries by deep eutectic solvents.

The large-scale use of electric vehicles produced massive discarded lithium-ion batteries, containing many recyclable valuable metals and toxic and harmful substances. Biodegradable and recyclable deep eutectic solvent (DES) is considered a green recycling technology for spent LIBs. Herein, we proposed a microwave-enhanced approach to shorten the leaching time in the urea/lactic acid: choline chloride: ethylene glycol DES system. The dipole moments induced by urea or lactic acid on LiCoO2 surface increased over two orders of magnitude under the high electric field. Because of this, over 90 % of Li and Co can be fast leached at 4 min and 160 W in the urea/lactic acid: choline chloride: ethylene glycol DES system. Meanwhile, we established two models to explain the leaching mechanism of metal ions from their leaching kinetics and micro-level behavior, and named them dot-etching and layer-peeling processes, respectively. By further analyzing, we found that the dot-etching can be attributed to the synergistic effect of reduction and coordination, which caused the surface of leaching residues porous. The layer-peeling process depends on neutralization, and the leaching residues had a smooth surface in this process. This work highlights the effect of microwave-enhanced strategy and DES surface chemistry on spent electrode materials recovery.