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In this study, within the defined orthogonal array of Taguchi design, the hydrothermal process parameters have been optimized for fabricating the smallest particle sized iron oxide (Fe2O3) particles. The finest particle size (210 nm) has been achieved when 0.02 M FeCl3 solution at pH 10 is hydrothermally treated for 90 min with an autoclave filling ratio of 100% (D3). Afterwards, to improve the physical properties of iron oxide particles, carbon black powder is added into the precursor solution as the seeding agent before the hydrothermal treatment. Structural and morphological analyses show that upon the existence of carbon in the precursor solution, C-supported Fe2O3 (D5) is fabricated. In the latter, carbon is present in graphitic form and no carbide formation is detected. Electrochemical test results verify that unlike to Fe2O3 (D3), C-supported Fe2O3 (D5) electrode performs lower charge transfer resistance and polarization leading to higher first coulombic efficiency, capacity retention, and improved rate performance, eventually. Thanks to the favorable characteristics of the latter, after 150 cycles, D5 performs 550, 390, and 333 mAh g(-1) discharge capacities under loads of 50 mA g(-1), 500 mA g(-1), and 1.5 A g(-1), respectively. Finally, to understand the contribution of capacitive and diffusion-controlled reactions to the total stored charge, an adopted sweep rate method has been used. The calculated voltammograms reveal that fabricating C-supported Fe2O3 particles led to improved rate performance because faradaic reactions that occur at the surface of the material prevail.

Lithium metal anodes are among the most promising candidates for further increasing the energy density of lithium ion batteries and all-solid-state batteries. A reduction of the anode thickness by using ultrathin lithium metal films is a crucial requirement to achieve a significant overall reduction of thickness on cell level. However, besides anode stabilization, realizing scalable technologies for an efficient production of thin lithium metal anodes is one of the most challenging obstacles for the success of various next-generation battery chemistries. In this publication we introduce a disruptive lithium melt deposition process for thin lithium metal coating on thin copper current collector foils. The wetting of molten lithium on the substrate can only be achieved through a lithiophilic interlayer. As a result fast and homogeneous lithium spreading on the substrate is enabled allowing roll-to-roll coating with liquid-deposition technologies as demonstrated in this contribution with a speed of several meters per minute and reaching 100 mm width. With this new process the anode thickness can be tuned in a wide range (1 - 30 µm). Evaluation in a prototype solid battery system shows high electrochemical lithium utilization and no detrimental effects compared to commercially available lithium reference foils.

The remaining useful life (RUL) prediction is critical for the safe and reliable operation of lithium-ion battery (LIB) systems, which characterizes the aging status of the battery and provides early warning for battery replacement. Most existing RUL prediction methods rely on empirical aging models, and the role of the battery mechanism is not considered in the subsequent algorithm settings. The accuracy and stability of data-driven algorithms are severely limited by battery aging data. A new electrochemical-model-based particle filter (PF) framework for LIB RUL prediction is proposed in this paper. Parameters of a simplified electrochemical model (SEM) are used as state variables of the PF algorithm and these parameters can be identified by applying specially designed current excitations to the battery. The SEM-based capacity simulation process is taken as the observation equation in the PF algorithm framework. Therefore, the mechanism of the battery is fully considered when making the RUL prediction. The proposed method is validated through cyclic aging experiment of a cylindrical LFP/graphite LIB of 45Ah. The accuracy of the method is compared with a data-driven-based PF framework for RUL prediction and shows better accuracy and stability, which provides a choice for achieving high-quality RUL prediction.

α1-LiVOPO_4, β-LiVOPO_4, and α-LiVOPO_4 are known as multiple lithium intercalation cathode materials. They were characterized by means of half-cell performance, operando X-ray diffraction (XRD), X-ray absorption spectroscopy (XAS), and differential scanning calorimetry (DSC). The operando XRD revealed differences in crystal structure evolution during charging/ discharging among the three crystal phases. Although the charge/discharge profiles and the crystal structure evolution behaviors were the same among the three crystal phases in the range of 3.5 - 4.5 V, the profiles and behaviors differed completely in the range of 1.0 - 3.5 V. The thermal stability of each phase of LiVOPO_4 is similar to that of LiFePO_4 in the fully charged state from the results of the DSC profiles.

Thermally reversible self-healing polymer (SHP) electrolyte membranes are obtained by Diels-Alder cycloaddition and electrolyte embedding. The SHP electrolytes membranes are found to display high ionic conductivity, suitable flexibility, remarkable mechanical properties and self-healing ability. The decomposition potential of the SHP electrolyte membrane is about 4.8 V (vs. Li/Li+) and it possesses excellent electrochemical stability, better than that of the commercial PE film which is only stable up to 4.5 V (vs. Li/Li+). TGA results show that the SHP electrolyte membrane is thermally stable up to 280 °C in a nitrogen atmosphere. When the SHP electrolyte membrane is used as a separator in a lithium-ion battery with an LCO-based cathode, the SHP membrane achieved excellent rate capability and stable cycling for over 100 cycles, and the specific discharge capacity could be almost fully recovered after self-healing. Furthermore, the electrolyte membrane exhibits excellent electrochemical performance, suggesting its potential for application in lithium-ion batteries as separator material.

In this work, a facile, wet chemical synthesis was utilized to achieve a series of lithium manganese oxide (LiMn2O4, (LMO) with 1-5%wt. graphene oxide (GO) composites. The average crystallite sizes estimated by the Rietveld method of LMO/GO nanocomposites were in the range of 18-27 nm. The electrochemical performance was studied using CR2013 coin-type cell batteries prepared from pristine LMO material and LMO modified with 5%wt. GO. Synthesized materials were tested as positive electrodes for Li-ion batteries in the voltage range between 3.0 and 4.3 V at room temperature. The specific discharge capacity after 100 cycles for LMO and LMO/5%wt. GO were 84 and 83 mAh g(-1), respectively. The LMO material modified with 5%wt. of graphene oxide flakes retained more than 91% of its initial specific capacity, as compared with the 86% of pristine LMO material. Web of Science 14 15 art. no. 4134

Carbon-coated Li4Ti5O12 (LTO) has been prepared using polyimide (PI) as a carbon source via the thermal imidization of polyamic acid (PAA) followed by a carbonization process. In this study, the PI with different structures based on pyromellitic dianhydride (PMDA), 4,4′-oxydianiline (ODA), and p-phenylenediamine (p-PDA) moieties have been synthesized. The effect of the PI structure on the electrochemical performance of the carbon-coated LTO has been investigated. The results indicate that the molecular arrangement of PI can be improved when the rigid p-PDA units are introduced into the PI backbone. The carbons derived from the p-PDA-based PI show a more regular graphite structure with fewer defects and higher conductivity. As a result, the carbon-coated LTO exhibits a better rate performance with a discharge capacity of 137.5 mAh/g at 20 C, which is almost 1.5 times larger than that of bare LTO (94.4 mAh/g).

We investigated the applicability of an ionic liquid electrolyte to a phosphorus‐doped Si (P‐doped Si) electrode to improve the performance and safety of the lithium‐ion battery. The electrode exhibited excellent cycling performance with a discharge capacity of 1000 mA h g-1 over 1400 cycles in the ionic liquid electrolyte, whereas the capacity decayed at the 170th cycle in the organic electrolyte. The lithiation/delithiation reaction of P‐doped Si occurred a localized region in the organic electrolyte, which generated a high stress and large strain. The strain accumulated under repeated charge‐discharge cycling, leading to severe electrode disintegration. In contrast, the reaction of P‐doped Si proceeded uniformly in the ionic liquid electrolyte, which suppressed the electrode disintegration. The P‐doped Si electrode also showed good rate performance in the ionic liquid electrolyte; a discharge capacity of 1000 mA h g-1 was retained at 10 C.

Compared to the liquid electrolyte, lithium solid-state electrolytes have obtained increasing attention for all-solid-state lithium ion battery on account of the safety requirement and higher energy density. However, many challenges remained in the solid-state electrolytes such as lower ionic conductivity, complex interface and unstable physical or electrochemical properties. One of the effective strategies is finding new type of lithium solid-state electrolytes with improved properties. The traditional trial and error methods acquire a lot of resources and time to verify the new solid-state electrolyte. Recently, some new lithium solid-state electrolytes were predicted through machine learning (ML), which has been proved to be an efficient and reliable method for screening new functional materials. This paper reviews the recent process of lithium solid-state electrolytes discovered based on ML algorithm. The selection and preprocessing of the datasets in ML technology are illustrated initially, and then the latest developments in screening lithium solid-state electrolytes through different ML algorithm are summarized and discussed in detail. Lastly, the stability of the candidate solid-state electrolyte and the challenges in discovering new lithium solid-state electrolytes through ML are highlighted.

Ammonium molybdate tetrahydrate ((NH4)6Mo7O24) (AMT) is commonly used as the precursor to synthesize Mo‑based oxides or sulfides for lithium ion batteries (LIBs). However, the electrochemical lithium storage ability of AMT itself is unclear so far. In the present work, AMT is directly examined as a promising anode material for Li‑ion batteries with good capacity and cycling stability. To further improve the electrochemical performance of AMT, AMT/polydopamine (PDA) composite was simply synthesized via recrystallization and freeze drying methods. Unlike with block shape for AMT, the as‑prepared AMT/PDA composite shows flake morphology. The initial discharge capacity of AMT/PDA is reached up to 1471 mAh g−1. It delivers a reversible discharge capacity of 702 mAh g−1 at a current density of 300 mA g−1, and a stable reversible capacity of 383.6 mA h g−1 is retained at a current density of 0.5 A g−1 after 400 cycles. Moreover, the lithium storage mechanism is fully investigated. The results of this work could potentially expand the application of AMT and Mo‑based anode for LIBs.

Highly stable lithium-ion battery cycling of niobium tungsten oxide (Nb16W5O55, NWO) is demonstrated in full cells with cathode materials LiNi0.6Mn0.2Co0.2O2 (NMC-622) and LiFePO4 (LFP). The cells show high rate performance and long-term stability under 5 C and 10 C cycling rates with a conventional carbonate electrolyte without any additives. The degradation of the cell performance is mainly attributed to the increased charge transfer resistance at the NMC side, consistent with the ex situ XRD and XPS analysis demonstrating the structural stability of NWO during cycling together with minimal electrolyte decomposition. Finally, we demonstrate the temperature-dependent performance of this full cell at 10, 25 and 60 ��C and confirm, using operando XRD, that the structural change of the NWO material during lithiation/de-lithiation at 60 ��C is very similar to its behaviour at 25 ��C, reversible and with a low volume change. With the merits of high rate performance and long cycle life, the combination of NWO and a commercial cathode represents a promising, safe battery for fast charge/discharge applications., This work was supported by EPSRC via the LIBATT grant (EP/M009521/1) and via an Impact Acceleration Account Follow-On grant (EP/R511675/1). The X-ray photoelectron (XPS) data collection was performed at the EPSRC National Facility for XPS (���HarwellXPS���), operated by Cardiff University and UCL, under Contract No. PR16195. We thank S. Shivareddy from CB2Tech Ltd. for advice on variable temperature cell operation. CPG and KJG are shareholders of a company that aims to commercialise fast charging anode materials.

We report a new process technique for electrode manufacturing for all solid-state batteries. Porous electrodes are manufactured by a tape casting process and subsequently infiltrated by a plastic crystal polymer electrolyte (PCPE). With a following isostatic lamination process, the PCPE was further integrated deeply into the porous electrode layer, forming a composite electrode. The PCPE comprises the plastic crystal succinonitrile (SN), lithium conductive salt LiTFSI and polyacrylonitrile (PAN) and exhibits suitable thermal, rheological (ƞ = 0.6 Pa s @ 80 °C 1 s−1) and electrochemical properties (σ &gt, 10−4 S/cm @ 45 °C). We detected a lowered porosity of infiltrated and laminated electrodes through Hg porosimetry, showing a reduction from 25.6% to 2.6% (NCM infiltrated to laminated) and 32.9% to 4.0% (LTO infiltrated to laminated). Infiltration of PCPE into the electrodes was further verified by FESEM images and EDS mapping of sulfur content of the conductive salt. Cycling tests of full cells with NCM and LTO electrodes with PCPE separator at 45 °C showed up to 165 mAh/g at 0.03C over 20 cycles, which is about 97% of the total usable LTO capacity with a coulomb efficiency of between 98 and 99%. Cycling tests at 0.1C showed a capacity of ~128 mAh/g after 40 cycles. The C-rate of 0.2C showed a mean capacity of 127 mAh/g. In summary, we could manufacture full cells using a plastic crystal polymer electrolyte suitable for NCM and LTO active material, which is easily to be integrated into porous electrodes and which is being able to be used in future cell concepts like bipolar stacked cells.

Li2ZnTi2.9Cr0.1O8 and Li2ZnTi3O8 were synthesized by the liquid phase method and then studied comparatively using X-ray diffraction (XRD), scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), galvanostatic charge–discharge testing, cyclic stability testing, rate performance testing, and electrochemical impedance spectroscopy (EIS). The results showed that Cr-doped Li2ZnTi3O8 exhibited much improved cycle performance and rate performance compared with Li2ZnTi3O8. Li2ZnTi2.9Cr0.1O8 exhibited a discharge ability of 156.7 and 107.5 mA h g−1 at current densities of 2 and 5 A g−1, respectively. In addition, even at a current density of 1 A g−1, a reversible capacity of 162.2 mA h g−1 was maintained after 200 cycles. The improved electrochemical properties of Li2ZnTi2.9Cr0.1O8 are due to its increased electrical conductivity.

The impacts on battery cell ageing from high current operation are investigated using commercial cells. This study utilised two tests&ndash, (i) to establish the maximum current limits before cell failure and (ii) applying this maximum current until cell failure. Testing was performed to determine how far cycling parameters could progress beyond the manufacturer&rsquo, s recommendations. Current fluxes were increased up to 100 C cycling conditions without the cell undergoing catastrophic failure. Charge and discharge current capabilities were possible at magnitudes of 1.38 and 4.4 times, respectively, more than that specified by the manufacturer&rsquo, s claims. The increased current was used for longer term cycling tests to 500 cycles and the resulting capacity loss and resistance increase was dominated by thermal fatigue of the electrodes. This work shows that there is a discrepancy between manufacturer-stated current limits and actual current limits of the cell, before the cell undergoes catastrophic failure. This presumably is based on manufacturer-defined performance and lifetime criteria, as well as prioritised safety factors. For certain applications, e.g., where high performance is needed, this gap may not be suitable, this paper shows how this gap could be narrowed for these applications using the testing described herein.

In order to improve the stability of high voltage electrolyte for 5 V-level LiNi0.5Mn1.5O4 cathode material, adiponitrile (ADN) with high oxidation stability was selected as the main solvent, meanwhile, 2% fluoroethylene carbonate (FEC) as the additive with good film forming effect was also used. And then, the effect of 2 mol L-1 LiBF4-GBL/ADN+2% FEC on the electrochemical performance of LiNi0.5Mn1.5O4 was explored at room temperature. The electrolyte system containing FEC can improve the cycle stability of the battery. At 1 C rate, the cycle capacity retention rate can reach 83% after 100 cycles, while the capacity retention rate of the electrolyte system without FEC and the ordinary commercial electrolyte system is only 77 and 68%, respectively. Besides, the rate performance of the battery with the addition of FEC also shows excellent performance, however, this kind of advantage is not obvious under the conditon of large rate. In addition, under the conditon of the synergistic effect between adiponitrile and fluoroethylene carbonate, the high-voltage electrolyte exhibits the good compatibility and lithium reversibility in the full cell with Li4Ti5O12 as the negative electrode.

The Li4Ti5O12/C composites were prepared by a hydrothermal method with in situ carbon addition. The influence of the morphology and content of various carbon materials (conductive carbon black, mesoporous carbon G_157M, and carbon replicas) on the electrochemical performance of the Li4Ti5O12/C composites was investigated. The obtained composites were characterized using X-ray diffraction, scanning electron microsopy, high-resolution transmission electron microscopy, thermogravimetric analysis, Raman spectroscopy, and N2 sorption-desorption isotherms. Morphology of the Li4Ti5O12/C composites depends on the carbon matrix used, while both morphology and the amount of carbon material have a great impact on the rate capability and cycling stability of the obtained composites. At low current densities, the Li4Ti5O12/C composite with 5 wt.% G_157M exhibits the highest discharge capacity, while at high charge-discharge rates, the Li4Ti5O12/carbon black composites show the best electrochemical performance. Thus, at ~0.1C, 5C, and 18C rates, the discharge capacities of the obtained Li4Ti5O12/C composites are 175, 120, and 70 mAh/g for G_157M, 165, 126, and 78 mAh/g for carbon replicas, and 173, 128, and 93 mAh/g for carbon black. After 100 cycles, their capacity retention is no less than 95%, suggesting their promising application perspective.

The development of new appropriate anode material with low cost is still main issue for sodium-ion batteries (SIBs) and lithium-ion batteries (LIBs). Here, Cr2P2O7 with an in-situ formed carbon layer has been fabricated through a facile solid-state method and its storage performance in SIBs and LIBs has been reported first. The Cr2P2O7@C delivers 238 mA h g&minus, 1 and 717 mA h g&minus, 1 at 0.05 A g&minus, 1 in SIBs and LIBs, respectively. A capacity of 194 mA h g&minus, 1 is achieved in SIBs after 300 cycles at 0.1 A g&minus, 1 with a high capacity retention of 92.4%. When tested in LIBs, 351 mA h g&minus, 1 is maintained after 600 cycles at 0.1 A g&minus, 1. The carbon coating layer improves the conductivity and reduces the side reaction during the electrochemical process, and hence improves the rate performance and enhances the cyclic stability.

Li2ZnTi3-xNbxO8 (x = 0, 0.05, 0.1) (LZTNO) materials are synthesized through ball milling assisted solid state synthesis and its structural, morphological and electrochemical investigations are carried out. All LZTNO samples exhibit a spinel type structure with space group P4332 and small amounts of anatase TiO2 are also found in doped samples. The structure and mechanism of electrochemical reaction of Li2ZnTi3O8 (LZTO) is not changed or disturbed significantly with the introduction of small amount of Nb+5 dopant. All samples show a uniform size distribution but Li2ZnTi2 · 95Nb0 · 05O8 (LZTNO-05) displays less agglomeration and more uniform size distribution. Also, the LZTNO-05 sample exhibit low charge transfer resistance and higher reversibility. Galvanostatic charge-discharge reveals highest discharge capacities of 223.9, 211, 173.7, 140, 83.7 mA h g−1 of LZTNO-05 at different C-rates 0.1C, 0.2C, 1C, 2C, and 5C, respectively. Pristine LZTO shows smaller discharge capacities of 197, 184, 146, 129.8 and 68.9 mA h g−1 at 0.1C, 0.2C, 1C, 2C and 5C rates, respectively. LZTNO-05 is prepared by a cost-effective route with excellent electrochemical properties making it more attractive as potential anode electrode for commercialization.

Kinetic Monte Carlo simulations are applied to simulate the insertion of lithium ions into graphite. The present results show how the kinetics of lithium ion intercalation in graphite rules the global process, leading to metastable phases. The relatively slow rate of the events of insertion (deinsertion) of lithium ions into (from) graphite is found to yield the intercalation structures proposed by Daumas and Hérold. These arrangements can be considered as frustrated, metastable structures, with a higher energy than that of the equilibrium state. Fil: Gavilán Arriazu, Edgardo Maximiliano. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Investigaciones en Físico-química de Córdoba. Universidad Nacional de Córdoba. Facultad de Ciencias Químicas. Instituto de Investigaciones en Físico-química de Córdoba; Argentina. Universidad Nacional de Santiago del Estero; Argentina Fil: Pinto, Oscar Alejandr. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro de Investigaciones y Transferencia de Santiago del Estero. Universidad Nacional de Santiago del Estero. Centro de Investigaciones y Transferencia de Santiago del Estero; Argentina Fil: López de Mishima, B. A.. Universidad Nacional de Santiago del Estero. Instituto de Bionanotecnología del Noa. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Tucumán. Instituto de Bionanotecnología del Noa; Argentina Fil: Barraco Diaz, Daniel Eugenio. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Física Enrique Gaviola. Universidad Nacional de Córdoba. Instituto de Física Enrique Gaviola; Argentina Fil: Oviedo, Oscar Alejandro. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Investigaciones en Físico-química de Córdoba. Universidad Nacional de Córdoba. Facultad de Ciencias Químicas. Instituto de Investigaciones en Físico-química de Córdoba; Argentina Fil: Leiva, Ezequiel Pedro M.. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Instituto de Investigaciones en Físico-química de Córdoba. Universidad Nacional de Córdoba. Facultad de Ciencias Químicas. Instituto de Investigaciones en Físico-química de Córdoba; Argentina

A facile, one-pot hydrothermal method was used to synthesize Nickel selenide (NiSe) nanoparticles decorated with reduced graphene oxide nanosheets (rGO), denoted as NiSe/rGO. The NiSe/rGO exhibits good electrochemical performance when tested as anodes for Na-ion batteries (SIBs) and Li-ion batteries (LIBs). An initial reversible capacity of 423 mA h g&minus, 1 is achieved for SIBs with excellent cyclability (378 mA h g&minus, 1 for 50th cycle at 0.05 A g&minus, 1). As anode for LIBs, it delivers a remarkable reversible specific capacity of 1125 mA h g&minus, 1 at 0.05 A g&minus, 1. The enhanced electrochemical performance of NiSe/rGO nanocomposites can be ascribed to the synergic effects between NiSe nanoparticles and rGO, which provide high conductivity and large specific surface area, indicating NiSe/rGO as very promising Na/Li storage materials.

The blending of different lithium insertion compounds has been proven to be a promising approach to design advanced electrodes for future lithium-ion batteries. Blending of certain lithium insertion compounds is done to combine the best properties of the individual active materials and to improve the energy or power density as well as cycling and storage durability. Furthermore, the blend can be tailored to meet specific requirements regarding costs, environmental issues and safety aspects. Herein, we report recent insights into the electrochemical behavior of blended lithium insertion cathodes. This review does not claim to summarize all recent literature, but rather is a critical overview of blended lithium insertion cathodes based on recent research findings. Latest thermodynamic studies enlighten certain mechanisms particularly occurring in blended insertion electrodes. Recent reports on active material combinations, including type-, mass ratio- and design-dependencies, reveal substantial improvements and synergetic effects regarding the electrochemical properties of the blended electrodes. Special experimental methods and setups are developed and applied to examine transport processes in blended insertion electrodes, revealing significant differences towards insertion electrodes containing a single type of active material. First approaches of modeling and simulation of blended insertion electrodes provide valuable information on the microscopic processes within the electrode and adequately reflect the experimental findings on the macro scale.

To develop high-performance anode materials of lithium ion batteries (LIBs) for practical high energy application, a grain boundaries enriched hierarchically mesoporous MnO/C microsphere composite has been fabricated by an in-situ carbonization process. The mesoporous MnO/C microsphere is constructed by abundant grains and grain boundaries that are uniformly embedded in a carbon matrix. Such unique nanoarchitecture exhibits high tap density and structural stability, and provides 3D continuous transport pathways for electrons and Li-ions, enabling high electrochemical stability and improved lithium storage kinetics. As a consequence, the mesoporous MnO/C electrode delivers ever-increasing specific capacity (1200 mAh g−1 after 100 cycles at 100 mA g−1) and excellent rate capability (588 mAh g−1 at 2 A g−1). Such superior lithium storage performance suggests that the hierarchically mesoporous MnO/C microsphere electrode should be one of the most promising anode materials for electric vehicle and grid energy storage application.

EJK would like to thank the Alistore ERI for the award of a studentship, ScotChem for an award of postgraduate and early career researcher exchanges (PECRE) and Christian Masquelier for his supervision at LRCS. The authors thank EPSRC Capital for Great Technologies Grant EP/L017008/1. The cycling performance of LiCoPO4 (LCP) as a high voltage positive electrode material in lithium‐ion batteries is enhanced by partial magnesium substitution for cobalt. Structural investigation of magnesium‐doped LCP using combined powder neutron and X‐ray diffraction reveals a decrease in anti‐site defects. In addition, the reduced unit cell volume variation during the charging process is observed by operando X‐ray diffraction measurements. Characterisation of the surface shows the presence of a Mg‐rich layer on the surface that might prevent detrimental reactions with the electrolyte. The combined beneficial effects of magnesium doping in LCP result in improved capacity retention. Postprint

Rapidly-growing demand for wearable and flexible devices is boosting the development of flexible lithium ion batteries (LIBs). The exploitation of flexible electrodes with high mechanical properties and superior electrochemical performances has been a key challenge for the rapid practical application of flexible LIBs. Herein, a flexible composite electrode was prepared from the mixed solutions of Li[Li0.2Ni0.13Co0.13Mn0.54]O2 (LLOs), carbon nanotubes(CNTs), and nanofibrillated celluloses (NFCs) via a vacuum filtration method. The resulting LLOs/CNTs/NFCs electrode delivered an initial discharge capacity of 253 mAh g-1 at 0.1 C in the voltage range from 2.0 to 4.6 V, and retained a reversible capacity of 178 mAh g-1 with 83% capacity retention after 100 cycles at 1 C. The LLOs/CNTs/NFCs electrode exhibited excellent flexibility along with repeated bending in the bending test. The LLOs/CNTs/NFCs electrode after bending test remained a discharge capacity of 149 mAh g-1 after 100 cycles at 1 C, and the corresponding capacity retentions was 76%. The excellent electrochemical performance and high flexibility can be ascribed to the framework formed by CNTs with high conductivity and NFCs with good mechanical properties. The results imply that the as-fabricated electrode can be a promising candidate for the flexible LIBs.

LiNi0.5Mn1.5O4 (LNMO) is a potential cathode material for lithium-ion batteries with outstanding energy density and high voltage plateau (>4.7 V). However, the interfacial side reaction between LNMO and the liquid electrolyte seriously causes capacity fading during cycling at the high voltage. Here, p-toluenesulfonyl isocyanate (PTSI) is used as the electrolyte additive to overcome the above problem of LNMO. The results show that the specific capacity of LNMO/Li cell with 0.5 wt.% PTSI at the first cycle is effectively enhanced by 36.0 mAh/g and has better cycling performance than that without PTSI at 4.98 V. Also, a stable solid electrolyte interface (SEI) film derived from PTSI is generated on the electrode surface, which could alleviate the strike of hydrofluoric acid (HF) caused by electrolyte decomposition. These results are explained by the molecular structure of PTSI, which contains SO3. The S=O groups can delocalize the nitrogen nucleus to block the reactivity of PF5.

Although the electrochemical properties of porous LiMn2O4 microspheres are usually improved compared to those of irregular LiMn2O4 particles, the effects of the different synthesis conditions on the preparation of the porous LiMn2O4 microspheres are rarely discussed in detail. In the present work, porous LiMn2O4 microspheres were successfully synthesized by using molten LiOH and porous Mn2O3 spheres as a template. Multiple factors were considered in the preparation process, including reagent concentration, pH, adding mode, heating time, etc. The morphology of the MnCO3 template was crucial for the preparation of porous LiMn2O4 microspheres and it was mainly affected by the concentration of reactants and the pH value of the solution during the precipitation process. During the lithiation of Mn2O3 microspheres, the heating temperature and the ratio between Mn2O3 and lithium salt were the most significant variables in terms of control over the morphology and purity of the LiMn2O4 microspheres. Furthermore, we demonstrated that the porous LiMn2O4 microspheres presented better rate capability and cyclability compared to commercial LiMn2O4 powder as cathode materials for lithium-ion batteries (LIBs). This study not only highlights the shape-controllable synthesis of LiMn2O4 microspheres as promising cathode materials, but also provides some useful guidance for the synthesis of porous LiMn2O4 microspheres and other LIB' electrode materials.

In this work, Al, Si and Ti oxides are used to modify the surface of LiNi 0.6 Co 0.2 Mn 0.2 O 2 (NCM622) electrode through the hydrolysis coating technology. SEM and TEM results revealed that three prepared oxide layers have different uniformity and morphology. Also, charge-discharge results showed different initial discharge capacity and cycle ability of three different oxide coatings. It is shown that when the temperature is increased from 25 to 50 °C, the capacity retention of Al 2 O 3 -coated NCM622 is reduced by only 4 %, what demonstrated the best ability of this oxide to restrain cycle deterioration. Additionally, when the charge cutoff voltage is increased to 4.6 V, Al 2 O 3 -coated NCM622 showed 74 % of capacity retention. As the number of charge-discharge cycles increases, the dissolution of some transition metal ions may be restrained by Al 2 O 3 layer. Generally, the enhanced electrochemical performance of Al 2 O 3 -coated NCM622 could be ascribed to the suppression of mutual reaction between electrode and electrolyte and improvement of structural stability of the material by Al 2 O 3 coating.

The current study investigated the effects of active material, conductive additives, and binder in a composite electrode on battery performance. In addition, the parameters related to cell performance as well as side reactions were integrated in an electrochemical model. In order to predict the cell performance, key parameters including manganese dissolution, electronic conductivity, and resistance were first measured through experiments. Experimental results determined that a higher ratio of polymer binder to conductive additives increased the interfacial resistance, and a higher ratio of conductive additives to polymer binder in the electrode resulted in an increase in dissolved transition metal ions from the LiMn2O4 composite electrode. By performing a degradation simulation with these parameters, battery capacity was predicted with various fractions of constituents in the composite electrode. The present study shows that by using this integrated prediction method, the optimal ratio of constituents for a particular cathode composite electrode can be specified that will maximize battery performance.

Rational design of high performance anode material with outstanding rate capability and cycling stability is of great importance for lithium ion batteries (LIBs). Herein, a series of NiO/NiFe2O4 hetero-structures with adjustable porosity, particle size, and shell/internal structure have been synthesized via a controllable annealing process. The optimized NiO/NiFe2O4 (S-NFO) is hierarchical hollow nanocube that is composed of ~5 nm subunits and high porosity. When being applied as anode for LIBs, the S-NFO exhibits high rate capability and excellent cycle stability, which remains high capacity of 1,052 mAh g−1 after 300 cycles at 5.0 A g−1 and even 344 mAh g−1 after 2,000 cycles at 20 A g−1. Such impressive electrochemical performance of S-NFO is mainly due to three reasons. One is high porosity of its hierarchical hollow shell, which not only promotes the penetration of electrolyte, but also accommodates the volume change during cycling. Another is the small particle size of its subunits, which can effectively shorten the electron/ion diffusion distance and provide more active sites for Li+ storage. Besides, the hetero-interfaces between NiO and NiFe2O4 also contribute toitsfast charge transport.

WOS: 000448031900047 PubMed ID: 30360177 Scientists have been working to replace graphite, the state-of-art anode material, to improve battery performances. In this sense, transitional metals and their oxides become attractive due to their capacities, widespread availabilities, and environmental benignity. In this paper, first in literature, a progressive study has been followed to evaluate the possible uses of pristine, partially oxidized and reduced Mo oxide films (with glucose droplets on top of the oxide layer gives the hybride and the film without glucose droplets on top of the oxide film gives merely reduced Mo oxide film) as anodes in lithium ion batteries. Unlike to conventional studies, herein the oxidation of molybdenum (Mo) atoms is restricted with the surface atoms to benefit the advantages of metallic Mo atoms at the electrode/current collector interface. These Mo atoms which are inactive versus Li and insoluble in copper are expected to create conductive pathway in the oxide (or hybride) films as well as minimize volume changes in cycling. Knowing that carbonaceous materials have been used as efficient additives to improve the electrochemical performance of electrodes, the best performance is achieved when the hybrid molydenbum oxide (C film on top of the reduced molybdenum oxide film as a result of the reduction of the glucose droplet) sample is cycled between 0.005-3.0 V versus Li/Li+.

Red phosphorus (RP) has attracted extensive attention as an anodic material for lithium-ion batteries (LIBs) due to its high theoretical specific capacity of 2596 mA h g− 1 and earth abundance. However, the facile and large-scale preparation of the red phosphorus nanomaterials via a solution synthesis remains a challenge. Herein, we develop a simple and facile solution method to prepare red phosphorus nanoparticles (RP NPs). PCl3 readily reacts with HSiCl3 in the presence of amines at room temperature to produce amorphous RP NPs with sizes about 100–200 nm in high yields. When used as an anode for rechargeable lithium ion battery, the RP NP electrode exhibits good electrochemical performance with a reversible capacity of 1380 mA h g− 1 after 100 cycles at a current density of 100 mA g− 1, and Coulombic efficiencies reaching almost 100% for each cycle. The study shows that this solution synthesis is a facile and convenient approach for large-scale production of RP NP materials for use in high-performance Li-ion batteries. Electronic supplementary material The online version of this article (10.1186/s11671-018-2770-4) contains supplementary material, which is available to authorized users.

As one of the common life garbages, about 4.5 trillion waste cigarette butts are produced and randomly discarded every year due to the addiction to the nicotine and the need of the social intercourse. Such a treatment would result in the waste of the resources and the environmental pollution if they weren't reasonably recycled in time. Herein, the waste cigarette butts were recycled in form of N-doped carbon powders with high economic value-added via one-step facile carbonization at 800°C for 2 h in the inert N2 atmosphere. The waste-cigarette-butts-derived black carbon powders were characterized by scanning electron microscope (SEM), N2 adsorption/desorption, and X-ray photoelectron spectroscopy (XPS). Furthermore, the corresponding electrochemical performances as the anode in lithium ion battery (LIB) were also investigated by galvanostatic charge/discharge, cyclic voltammetry (CV), and alternating current (AC) impedance. The results suggested that the recycled N-doped waste cigarette butts carbon (WCBC) powders consisted of major carbon and minor residual N-containing and O-containing functional groups, and the corresponding specific surface area was about 1,285 m2·g−1. Furthermore, the reversible specific discharge capacity was about 528 mAh·g−1 for 100 cycles at 25 mA·g−1 and about 151 mAh·g−1 even at 2,000 mA·g−1 for 2,500 cycles. Additionally, full cell performances were also satisfactory, indicating high feasibility. N-doping effect (such as additional active sites and higher electronic conductivity) and the residual O-containing functional groups may be responsible for the satisfactory electrochemical performances, which offered good inspiration and strategy to develop the green energy and circular economy.

Batteries as a multi-disciplinary field have been analyzed from the electrical, material science and electrochemical engineering perspectives. The first principle-based four-dimensional degradation model (4DM) of the battery is used in the article to connect the interdisciplinary sciences that deal with batteries. The 4DM is utilized to identify the physical manifestation that electrolyte degradation has on the battery and the response observed in the terminal voltage. This paper relates the different kinds of side reactions in the electrolyte and the material properties affected due to these side reactions. It goes on to explain the impact the material property changes has on the electrochemical reactions in the battery. This paper discusses how these electrochemical reactions affect the voltage across the terminals of the battery. We determine the relationship the change in the terminal voltage has due to the change in the design properties of the electrolyte. We also determine the impact the changes in the electrolyte material property have on the terminal voltage. In this paper, the lithium ion concentration and the transference number of the electrolyte are analyzed and the impact of their degradation is studied.

In this study, MnO nanocrystals incorporated in a N-containing carbon matrix were fabricated by the facile thermal decomposition of manganese nitrate-glycine gels. MnO/C composites with different carbon contents were prepared by controlling the initial ratio of manganese to glycine. The composition, phase structure and morphology of the composites were characterized by X-ray diffraction, X-ray photoelectron spectroscopy, Raman spectroscopy, scanning and transmission electron microscopy, and thermogravimetric analysis. The results indicated that MnO nanocrystals were uniformly embedded in the N-doped carbon matrix. The carbon matrix could effectively enhance the electrical conductivity of MnO and alleviate the strain arising from the discharge/charge cycling. The composite materials exhibited high discharge/charge capacities, superior cycling performance, and excellent rate capability. A high reversible capacity of 556 mA h g(-1) was obtained after 110 cycles of discharging and charging at a current rate of 0.5 A g(-1). Even at a high current rate of 3 A g(-1), the sample still delivered a capacity of around 286 mA h g(-1). The easy production and superior electrochemical properties enables the composites to be a promising candidate as an anode alternative for high-performance lithium-ion batteries.

Nano-sized hollow spindle LiMnPO4 with a well-developed olivine-type structure was synthesized with the assistance of glucose in dimethyl sulfoxide (DMSO)/H2O under ambient pressure and 108 °C. The scanning electron microscopy (SEM) and transmission electron microscope (TEM) images show that the LiMnPO4 particles consist of hollow spindles with a mean width of 200 nm, length of 500-700 nm, and wall thickness of about 30-60 nm. The LiMnPO4/C nanocomposite was obtained by sintering nano-sized LiMnPO4 with glucose at 650 °C under an inert atmosphere for 4 h. With a coated carbon thickness of about 10 nm, the obtained composite maintained the morphology and size of the hollow spindle. The electrochemical tests show the specific capacity of LiMnPO4/C nanocomposite is 161.8 mAh g−1 at 0.05C, 137.7 mAh g−1 at 0.1C and 110.8 mAh g−1 at 0.2 C. The retention of discharge capacity maintains 92% after 100 cycles at 0.2 C. After different rate cycles the high capacity of the LiMnPO4/C nanocomposite can be recovered. This high performance is attributed to the composite material's hollow spindle structure, which facilitates the electrolyte infiltration, resulting in an increased solid-liquid interface. The carbon layer covering the hollow spindle also contributes to the high performance of the LiMnPO4/C material as the carbon layer improves its electronic conductivity and the nano-scaled wall thickness decreases the paths of Li deintercalation.

We construct successfully a porous antimony-doped tin oxide (ATO)/nitrogen-doped graphene 3-dimensional (3D) frameworks (denoted as ATO/NG/TEPA; TEPA refers to tetraethylenepentamine) by a one-pot hydrothermal process, with which TEPA aqueous solution is adopted to easily re-disperse commercial ATO precursor forming a transparent hydrosol. The results show that TEPA plays a key role in the construction of ATO/NG/TEPA, not only acting as a peptization reagent to re-disperse ATO precursor nanoparticles, and as a linker to combine ATO with graphene sheets. The as-fabricated ATO/NG/TEPA hybrid as the negative electrode of lithium ion batteries exhibits excellent lithium storage capacity and cycling stability. With the advantage of easily re-dispersing commercial ATO, the present synthetic route may be put into use for the large-scale production of the titled nanocomposites as the anode material of lithium ion batteries. Refereed/Peer-reviewed

The development of facile preparation methods and novel three-dimensional structured anodes to improve cycling stability of lithium ion batteries (LIBs) is urgently needed. Herein, a dual-network ferroferric oxide/nickel oxide (Fe3O4/NiO) anode was synthesized through a facile dealloying technology, which is suitable for commercial mass manufacturing. The dual-network with high specific surface area contains a nanoplate array network and a bimodal nanoporous urchin network. It exhibits excellent electrochemical performance as an anode material for LIB, delivering a reversible capacity of 721 mAh g&minus, 1 at 100 mA g&minus, 1 after 100 cycles. The good lithium storage performance is related to the ample porous structure, which can relieve stress and mitigate the volume change in the charge/discharge process, the interconnected porous network that enhances ionic mobility and permeability, and synergistic effects of two kinds of active materials. The paper provides a new idea for the design and preparation of anode materials with a novel porous structure by a dealloying method and may promote the development of the dealloying field.

N-doped porous carbon encapsulated NiO/Ni composite nanomaterials (N-doped NiO/Ni@C) was successfully obtained by a one-step solution combustion method. This study demonstrates a one-step combustion method to synthesize n-doped porous carbon encapsulated NiO/Ni composite nanomaterials, using carbon dioxide as the carbon source, nickel nitrate as the nickel source, and hydrazine hydrate as the reaction solution. Spherical NiO nanoparticles with a particle size of 20 nm were uniformly distributed in the carbon matrix. The load of NiO/Ni can be controlled by the amount of nickel nitrate. The range of carbon content of recovered samples is 69&ndash, 87 at%. The content of incorporated nitrogen for recovered samples is 1.94 at%. As the anode of lithium ion battery, the composite material exhibits high capacity, excellent multiplier performance and stable circulation performance. N-doped NiO/Ni@C-2 was applied to lithium ion batteries, and its reversible capacity maximum is 980 mAh g&minus, 1 after 100 cycles at the current density of 0.1 A g&minus, 1. Its excellent electrochemical properties imply its high potential application for high-performance lithium-ion battery anode materials.

Solid polymer electrolytes for bipolar lithium ion batteries requiring electrochemical stability of 4.5 V vs. Li/Li+ are presented. Thus, imidazolium-containing poly(ionic liquid) (PIL) networks were prepared by crosslinking UV-photopolymerization in an in situ approach (i.e., to allow preparation directly on the electrodes used). The crosslinks in the network improve the mechanical stability of the samples, as indicated by the free-standing nature of the materials and temperature-dependent rheology measurements. The averaged mesh size calculated from rheologoical measurements varied between 1.66 nm with 10 mol% crosslinker and 4.35 nm without crosslinker. The chemical structure of the ionic liquid (IL) monomers in the network was varied to achieve the highest possible ionic conductivity. The systematic variation in three series with a number of new IL monomers offers a direct comparison of samples obtained under comparable conditions. The ionic conductivity of generation II and III PIL networks was improved by three orders of magnitude, to the range of 7.1 &times, 10&minus, 6 Scm&minus, 1 at 20 &deg, C and 2.3 &times, 4 Scm&minus, 1 at 80 &deg, C, compared to known poly(vinylimidazolium&middot, TFSI) materials (generation I). The transition from linear homopolymers to networks reduces the ionic conductivity by about one order of magnitude, but allows free-standing films instead of sticky materials. The PIL networks have a much higher voltage stability than PEO with the same amount and type of conducting salt, lithium bis(trifluoromethane sulfonyl)imide (LiTFSI). GII-PIL networks are electrochemically stable up to a potential of 4.7 V vs. Li/Li+, which is crucial for a potential application as a solid electrolyte. Cycling (cyclovoltammetry and lithium plating-stripping) experiments revealed that it is possible to conduct lithium ions through the GII-polymer networks at low currents. We concluded that the synthesized PIL networks represent suitable candidates for solid-state electrolytes in lithium ion batteries or solid-state batteries.

In this study, we propose a mass production-able and low-cost method to fabricate the anodes of Li-ion battery. Carbonaceous anodes, integrated with thin amorphous silicon layers by plasma enhanced chemical vapor deposition, can improve the performance of specific capacity and coulombic efficiency for Li-ion battery. Three different thicknesses of a-Si layers (320, 640, and 960 nm), less than 0.1 wt% of anode electrode, were deposited on carbonaceous electrodes at low temperature 200 °C. Around 30 mg of a-Si by plasma enhanced chemical vapor deposition (PECVD) can improve the specific capacity ~42%, and keep coulombic efficiency of the half Li-ion cells higher than 85% after first cycle charge-discharge test. For the thirty cyclic performance and rate capability, capacitance retention can maintain above 96%. The thicker a-Si layers on carbon anodes, the better electrochemical performance of anodes with silicon-carbon composites we get. The traditional carbonaceous electrodes can be deposited a-Si layers easily by plasma enhanced chemical vapor deposition, which is a method with high potential for industrialization.

Limited by the development of energy storage technology, the utilization ratio of renewable energy is still at a low level. Lithium/sodium ion batteries (LIBs/SIBs) with high-performance electrochemical performances, such as large-scale energy storage, low costs and high security, are expected to improve the above situation. Currently, developing anode materials with better electrochemical performances is the main obstacle to the development of LIBs/SIBs. Recently, a variety of studies have focused on cobalt-based anode materials applied for LIBs/SIBs, owing to their high theoretical specific capacity. This review systematically summarizes the recent status of cobalt-based anode materials in LIBs/SIBs, including Li+/Na+ storage mechanisms, preparation methods, applications and strategies to improve the electrochemical performance of cobalt-based anode materials. Furthermore, the current challenges and prospects are also discussed in this review. Benefitting from these results, cobalt-based materials can be the next-generation anode for LIBs/SIBs.

The LiNi0.5Mn1.5O4 ||Li4Ti5O12 (LMNO||LTO) battery possesses a relatively-high energy density and cycle performance, with further enhancement possible by application of an AlF3 coating on the LTO electrode particles. We measure the performance enhancement to the LMNO||LTO battery achieved by a AlF3 coating on the LTO particles through electrochemical testing and use in-operando neutron powder diffraction to study the changes to the evolution of the bulk crystal structure during battery cycling. We find that the AlF3 coating along with parasitic Al doping slightly increases capacity and greatly increases rate capability of the LTO electrode, as well as significantly reducing capacity loss on cycling, facilitating a gradual increase in capacity during the first 50 cycles. Neutron powder diffraction reveals a structural response of the LTO and LNMO electrodes consistent with a greater availability of lithium in the battery containing AlF3-coated LTO. Further, the coating increases the rate of structural response of the LNMO electrode during charge, suggesting faster delithiation, and enhanced Li diffusion. This work demonstrates the importance of studying such battery performance effects within full configuration batteries.

Cu2Se nanoflake arrays supported by Cu foams are synthesized by a facile hydrothermal method in this study. The Cu2Se materials are directly used as an anode for lithium ion batteries, which show superior cycle performance with significant capacity increase. Combining with previous reports and scanning electron microscope images after cycling, the capacity increase caused by the reversible growth of a polymeric film is discussed. Electrochemical impedance spectroscopy is used to test the reversible growth of the polymeric film. By analyzing the three-dimensional Nyquist plots at different potentials during the discharge/charge process, detailed electrochemical reaction information can be obtained, which can further verify the reversible formation of a polymeric film at low potential.

Accurate diagnosis of lithium ion battery state-of-health (SOH) is of significant value for many applications, to improve performance, extend life and increase safety. However, in-situ or in-operando diagnosis of SOH often requires robust models. There are many models available however these often require expensive-to-measure ex-situ parameters and/or contain unmeasurable parameters that were fitted/assumed. In this work, we have developed a new empirically parameterised physics-informed equivalent circuit model. Its modular construction and low-cost parametrisation requirements allow end users to parameterise cells quickly and easily. The model is accurate to 19.6 mV for dynamic loads without any global fitting/optimisation, only that of the individual elements. The consequences of various degradation mechanisms are simulated, and the impact of a degraded cell on pack performance is explored, validated by comparison with experiment. Results show that an aged cell in a parallel pack does not have a noticeable effect on the available capacity of other cells in the pack. The model shows that cells perform better when electrodes are more porous towards the separator and have a uniform particle size distribution, validated by comparison with published data. The model is provided with this publication for readers to use.

An amorphous iron oxide–carbon composite has been fabricated through an effective, inexpensive, and scalable method employing solution combustion synthesis. Amorphous iron oxide nanoparticles with diameters of about 5 nm were synthesized and uniformly embedded in a dense carbon matrix. The synthesized composite exhibits enhanced cyclability and rate capability, showing a high reversible capacity of 687 mA h g − 1 after 200 discharge/charge cycles at a current rate of 0.5 A g − 1 , compared to the 400 mA h g − 1 observed for Fe 2 O 3 nanoparticles. This enhanced performance was retained despite more demanding conditions, delivering a high capacity of about 525 mA h g − 1 and a nearly perfect coulombic efficiency even after 400 cycles at 1 A g − 1 . The easy production and superior electrochemical properties of this composite suggest that it is a promising material for use as an anode material in high performance lithium ion batteries.

This review deals with the recent developments and present status of the theoretical models for the simulation of the performance of lithium ion batteries. Preceded by a description of the main materials used for each of the components of a battery -anode, cathode and separator- and how material characteristics affect battery performance, a description of the main theoretical models describing the operation and performance of a battery are presented. The influence of the most relevant parameters of the models, such as boundary conditions, geometry and material characteristics are discussed. Finally, suggestions for future work are proposed., This work is funded by FEDER funds through the “Programa Operacional Factores de Competitividade—COMPETE” and by national funds from FCT—Fundação para a Ciência e a Tecnologia, in the framework of the strategic project Strategic Project PEST-C/FIS/UI607/2011, project F-COMP-01-0124-FEDER-022716 and grant SFRH/BD/68499/2010 (C.M.C.). The authors also thank funding from Matepro – Optimizing Materials and Processes”, ref. NORTE-07-0124-FEDER-000037”, cofunded by the “Programa Operacional Regional do Norte” (ON.2 – O Novo Norte), under the “Quadro de Referência Estratégico Nacional” (QREN), through the “Fundo Europeu de Desenvolvimento Regional” (FEDER). The authors thank Celgard LLC, Timcal, Solvay, Arkema and Clariant for kindly supplying their high quality membranes and excellent materials, respectively.

Degradation mechanism of surface coating effects at the cathode/electrolyte interface is investigated using thin-film model electrodes combined with operando X-ray absorption spectroscopy (XAS). MgO-coated LiCoO[2] thin-film electrodes prepared via pulsed laser deposition at room temperature and high temperature are used as model systems. The MgO coating improves the durability of the cathode during high-potential cycling. Operando total reflection fluorescence XAS reveals that initial deterioration due to reduction of Co ions at the surface of the uncoated-LiCoO[2] thin film upon electrolyte immersion is inhibited by the MgO coating. Operando depth-resolved XAS reveals that the MgO coating suppresses drastic distortions of local structure at the LiCoO[2] surface as observed in the uncoated-LiCoO[2] during charging process. The electronic and local structure changes at the electrode/electrolyte interface for two types of surface coating morphologies are discussed.

The requirement of energy-storage equipment needs to develop the lithium ion battery (LIB) with high electrochemical performance. The surface modification of commercial LiFePO4 (LFP) by utilizing zeolitic imidazolate frameworks-8 (ZIF-8) offers new possibilities for commercial LFP with high electrochemical performances. In this work, the carbonized ZIF-8 (CZIF-8) was coated on the surface of LFP particles by the in situ growth and carbonization of ZIF-8. Transmission electron microscopy indicates that there is an approximate 10 nm coating layer with metal zinc and graphite-like carbon on the surface of LFP/CZIF-8 sample. The N2 adsorption and desorption isotherm suggests that the coating layer has uniform and simple connecting mesopores. As cathode material, LFP/CZIF-8 cathode-active material delivers a discharge specific capacity of 159.3 mAh g−1 at 0.1C and a discharge specific energy of 141.7 mWh g−1 after 200 cycles at 5.0C (the retention rate is approximate 99%). These results are attributed to the synergy improvement of the conductivity, the lithium ion diffusion coefficient, and the degree of freedom for volume change of LFP/CZIF-8 cathode. This work will contribute to the improvement of the cathode materials of commercial LIB. Highlights: 1 A surface modification layer, which has 10 nm with metal zinc and graphite-like carbon, was synthesized on commercial LiFePO4 (LFP) using ZIF-8.2 As-prepared LFP/CZIF-8 possesses prominent electrochemical performances with a discharge specific capacity of 159.3 mAh g−1 at 0.1C and a discharge specific energy of 141.7 mWh g−1 after 200 cycles at 5.0C.