Electrochemical Cycling Stability Research Articles

Overlithiation-driven structural regulation of lithium nickel manganese oxide for high-performance battery cathode

Spinel LiNi0.5Mn1.5O4 (LNMO) is a promising cathode material due to its high operation voltage, cobalt free nature and low cost. High energy density of batteries could be realized by coupling LNMO with high-capacity Si based anodes, before which large active lithium loss at the anode should be addressed. Pre-insertion of additional lithium (Li, x) into LNMO, namely overlithaition of LNMO (L1+xNMO) here, becomes a promising approach for active Li compensation. Understanding the materials structure and property evolution of L1+xNMO and their further effect on electrochemical behavior is crucial. Although spinel LNMO could endure a certain amount of extra Li, its excessive insertion could cause degradation in materials structure, interfacial stability and electrochemical performance due to the introduction of large strain, grain boundaries and immoderate reduction of Mn element. L1.4NMO showed a tradeoff between donable lithium-ion capacity and electrochemical cycling stability among the investigated L1+xNMO (x = 0, 0.2, 0.4, 0.6 and 1) samples. L1.4NMO||Si/C cell presented a reversible capacity of 121.7 mAh g−1 and energy density of 429 Wh kg−1, achieving over 50 % improvement than that of LNMO||Si/C cell.

Synthesis-Driven Computational Discovery of Organic Redoxmers for Non-Aqueous Redox Flow Batteries

Organic non-aqueous redox flow batteries (RFBs) are promising grid-scale energy storage systems for storing intermittent renewable energy in molecules. For practical applications, low-cost and stable redox active molecules (redoxmers) that display a large redox potential window and long electrochemical cycling stability are required to deliver a high-energy-density RFB with a long battery cycle life. To accelerate the discovery of redoxmer molecules, previous studies have utilized machine learning (ML) methods along with first-principles simulations. Although many ML-suggested molecules show promising electrochemical properties, they are generally difficult to synthesize because of their highly complex structure. To address this challenge, in this work, we propose a new synthesis-driven computational approach to discovering less-complex molecules with a large redox potential window that can deliver high-energy-density RFBs. Specifically, we devised an algorithm to generate an engineered molecular search space and applied a Bayesian optimization-based active learning algorithm to discover promising molecules from a large molecular search space while using a limited number of expensive density functional theory (DFT) calculations. To increase the energy density of RFBs, we focus on maximizing the redox potential window of redoxmer molecules (or cell voltage) by minimizing the reduction potential of anolyte molecules. Precisely, we studied the 2,1,3 Benzothiadiazole (BTZ) molecule, a promising anolyte (redoxmer) candidate for RFBs, and with our synthesis-driven approach discovered new BTZ-based molecules that show 15-43% smaller reduction potential than the BTZ and in principle can deliver organic RFBs with a cell voltage ≈ 3 V.

Li Electrodeposition Modeling for Analyzing the Effect of Li+ Redistribution in Li Metal Secondary Batteries

To meet the high-energy-density requirement of Li secondary batteries for EV applications, Li metal is still being re-examined extensively beyond conventional carbon-based anode active materials. However, unlike intercalation mechanism-based anodes, Li metal anodes (LMAs), suffering from significant surface morphology changes during electroplating and stripping, can accompany several issues such as Li dendrite growth and continuous side reactions, thereby leading to the poor electrochemical performance and cycle stability. Among various reasons of the Li dendrite formation, inhomogeneous and slow Li+ transport to the LMAs are representatively known, accelerating irregular electrodeposition and rapid Li+ depletion on the LMA surface.In this study, we attempted to simulate Li dendrite growth under practical current conditions by developing a 2D Li electrodeposition model. Based on this model, we analyzed the geometric-electrochemical characteristics of Li metal interface depending on Li+ concentration distribution in the electrolyte and SEI. Furthermore, in order to verify a nanomaterial-based micro-convection effect in the electrolyte for improving mass transfer, the Li+ concentration change nearby the interface was calculated while simulating the Li dendritic growth. Also, real 2D morphologies of the Li dendrites were reconstructed and analyzed together in a similar way. As a result, the micro-convection enables relatively uniform Li+ distribution at the LMA interface and enhances the mass transport in the electrolyte, which can suppress the Li dendrite growth even at 5.0 mA cm-2.

Electrochromic conjugated polymers containing benzotriazole and thiophene performing sub-second response time and 916 cm2 C−1 superb coloration efficiency

In pursuit of high-performance electrochromic conjugated polymers (ECPs), three benzotriazole-thiophene ECPs employing benzotriazole as acceptor and different thiophene repeating units as donors, namely, PBTz-T, PBTz-BT, and PBTz-TT, were synthesized via direct (hetero)arylation polymerization (DHAP). Meanwhile, following the above ECPs model, we investigated the effect of corresponding conjugated chain length of monomers on their optical, electrochemical and electrochromic properties. The results showed that along with the increase of the numbers of thiophene in the repeating unit of ECPs, the electronic and optical band gaps decreased, the UV–Vis absorption and fluorescence spectra showed significant bathochromic shift, and the electrochemical cycle stability gradually improved. PBTz-T exhibited giant coloration efficiency (916 cm2 C−1 at 530 nm), which is one of the best results in the visible region. And higher coloration efficiency means less energy consumption, which holds great potential for various applications, including electrochromic back covers of smartphones. PBTz-BT displayed the highest transmittance (28% at 550 nm), and BTz-TT illustrated the fastest switching time (0.6 s/0.5 s for doping/dedoping process). Flexible electrochromic device (ECD) fabricated employed PBTz-T as functional layer gradually changed from red (reduction) to dark green (oxidation), and maintained good cycling stability.

Direct growth of AC@NiCo2S4 composite on nickel foam as binder-free electrodes for supercapacitors

In this study, folded nanotubes were directly grown on Ni foam by two-step hydrothermal method to form activated carbon (AC) and NiCo2S4 composite material with a unique structure like nano-urchin. In addition, the morphology and structure can be controlled by the time of hydrothermal reaction. The resulting samples were characterized by means of XRD, XPS, EDS and SEM. The electrochemical test results show that compared with the 6 h and 24 h hydrothermal composites, the 12 h hydrothermal composites (AC@NiCo2S4–2) form a complete folded nanotube structure, provide a large number of reactive sites, and show better electrochemical properties. And compared with the capacitance of NiCo2S4 (456.14 C g−1), the AC@NiCo2S4–2 exhibited a high specific capacitance of 653.9 C g−1 at a current density of 1 A g−1. In addition, after combination with AC, AC@NiCo2S4 has better electrochemical performance and cycle stability, the capacitance retention rate at 10 A g−1 is 62.84 % of 1 A g−1, and can still maintain 84.96 % of the initial capacitance after 3000 cycles. Moreover, the fabricated hybrid supercapacitor (HSC) based on AC@NiCo2S4–2 and AC electrodes achieved a high energy density of 29.75 Wh kg−1 at the power density of 700 W kg−1 and still maintain the energy density of 16.86 Wh kg−1 at the high power density of 7000 W kg−1.

Highly Stable MWCNT@NVP Composite as a Cathode Material for Na-Ion Batteries.

A 3D framework with Nasicon structured polyanionic Na3V2(PO4)3 (NVP) has been emphasized as a leading cathode material for sodium-ion batteries (SIBs) due to its high working voltage plateau, structural stability, and good rate performance. Herein, pristine NVP and MWCNT@NVP composite synthesized via a facile solid-state method are examined and compared as cathode materials for Na-ion batteries. The morphological study confirms the uniform distribution of MWCNTs in the pristine NVP structure. Impedance spectroscopy clearly confirms more diffusion of Na ions for the MWCNT@NVP composite as compared to pristine NVP, considering its diffusion coefficient which directly implies on an increase in specific capacity. MWCNT@NVP (FNV-2) showed specific discharge capacity 110 mAhg-1 at 0.1C current rate which is almost stable at higher current rates with marginal fading. However, the pristine NVP shows capacity loss at a higher current rate. It is noteworthy that the MWCNT@NVP composite shows stable performance with marginal specific capacity fading (1%) compared to pristine (15%). This is because of the mechanical integrity and stability afforded to the composite by the intertwined MWCNT framework in the MWCNT@NVP composite matrix against electrode degradation during the electrochemical reaction. More significantly, even at a higher current rate, that is, at 10 C, the composite recorded a very stable and excellent Columbic efficiency of 97% with a reversible specific capacity of 94 mAhg-1 after 2000 cycles. An enhanced electrochemical performance, that is, rate capability and cycling stability, demonstrates the high potential of the MWCNT@NVP composite for Na-ion storage. Moreover, a sodium-ion full cell with hard carbon demonstrated a reversible capacity of 103 mAhg-1 at C/20 current rate, which clearly demonstrates that MWCNT@NVP is a promising cathode material for sodium-ion batteries.

Hierarchically cobalt phosphide nanostructures embedded in N, P co-doped porous carbon networks assembled by ultrathin sheets for high-performance Li/Na-ion batteries

Metal phosphides have aroused tremendous interests for energy storages, owing to their unique crystal structure and high theoretical specific capacity. However, poor cycling stability and fast capacity decay inhibit their application. Herein, we successfully synthesized a novel heterostructural architecture with well-dispersed CoP nanoparticles (NPs) embedded in 3-dimential (3D) N, P co-doped porous carbon (NP-PC) networks by a facile polymer-derived route. The unique 3D NP-PC networks can mitigate the volume change, enhance conductivity, and provide electron/ion transport channels. The as-prepared heterostructure exhibits the synergistic effect between CoP NPs and NP-PC, relieves CoP NPs agglomeration, and stabilizes the surface/interface structure. Benefiting from these advantages, the heterostructural architecture exhibits superior electrochemical activities and cycling stability for lithium storage (1056 mAh·g−1 at 0.2 A·g−1 after 200 cycles) and sodium storage (345 mAh·g−1 at 0.2 A·g−1 after 60 cycles). This work aids the construction of high-performance metal phosphide-based anode materials.

In Situ Ion‐Exchange Metathesis Induced Conformal LiF Surface Films on Cathode (NMC811) as a Cathode Electrolyte Interphase

AbstractHigh‐capacity cathodes (LiNi0.8Mn0.1Co0.1O2, NMC811) are promising for vehicle electrification because of their high gravimetric energy density. However, their electrochemical performance still relies upon the stability of the cathode electrolyte interphase (CEI). A highly reactive cathode interface leads to parasitic side reactions with electrolytes, resulting in accelerated capacity fading. Well‐developed LiF and LiF‐like inorganic compounds are believed to be good CEI components for stabilizing such reactive electrode interfaces. However, it is challenging to form an optimal surface sub‐nanolayer of LiF on the cathode surfaces because of the complexity of the electrochemical reaction during battery cycling. Herein, the formation of a conformal LiF layer on the NMC811 electrode surface via an in situ ion‐exchange metathesis process is reported, demonstrating a promising electrochemical performance because of a LiF‐stabilized CEI. In situ generated LiF‐coated NMC811 electrodes exhibit ≈97% capacity retention up to 100 cycles at a 0.3 C rate with average coulombic efficiency of ≈99.9% and ≈80% capacity retention up to 200 cycles at a 1 C rate with average coulombic efficiency of >99.6%. This finding may pave the way for reengineering the CEI to enhance the electrochemical performances and cycling stability of the high‐capacity cathodes.

Tailoring composites via in situ growth of Co-MOF on V2CTx MXene as high-performance anode for lithium-ion batteries

MXenes, as a new family of 2D materials, have attracted extensive attention for their high electrical conductivity and good electrochemical cycling stability. However, due to the self-stacking nature of MXene materials, the actual specific capacity (260 mAh g−1) of V2CTx MXene materials as anodes is much lower than the theoretical specific capacity (940 mAh g−1). Herein, we designed a novel Co-MOF/V2CTx composite (denoted as Co-MOF/V2CTx), where Co-MOF was in situ grown on the surface and interlayer of the V2CTx MXene with larger interlayer spacing. The MOF in the composite provides the additional specific capacity as well as effectively prevented the restacking of V2CTx MXene, which exposed more Li+ active sites. Besides, benefiting from the high conductivity, electrochemical stability, and strong bonding with the Co-MOF at the interface of MXene, the structural stability of Co-MOF itself in composite materials can be better improved. Consequently, the cells with Co-MOF/V2CTx anodes realize a high specific capacity of 484.3 mAh g−1 after 120 cycles at 100 mA g−1 and superior cycling stability even at a higher current density of 500 mA g−1. The unique synergistic design of this work can provide new ideas for the development of MXene-based composites in energy storage applications.

High electrochemical performance of cobalt ions-doped Ni3Se4 boosted by its highly conductive hierarchical framework

Battery-type materials have the intrinsic feature of poor electrical conductivity, significantly affecting their electrochemical performance. At the same time, the low cycling stability of these materials is a key factor weakening the feasibility of their application in supercapacitors (SCs). Although various strategies based on nanoengineering are adopted to address these two issues, it seems that the progress so far does not prove the significant effectiveness of these strategies. In this work, a battery-type material, cobalt ions-doped Ni3Se4, is synthesized using a hydrothermal selenization procedure to address the two issues mentioned above. We preliminarily demonstrate that the electrochemical activity and cycling stability of battery-type materials depend on their intrinsically high conductivity, given that these materials have the proper structure and composition. Based on high electrical conductivity, the cobalt ions-doped Ni3Se4 exhibits high capacitive performance and remarkable cycling stability due to the synergistic effect between Ni and Co and the porous nanosheets self-supported structure. The result of this work proves that the cobalt ions-doped Ni3Se4 with the highly conductive hierarchical framework is a promising electrode material for SCs.

Improving the electrochemical performance of LiNi0.7Mn0.3O2 cathode material by CeO2 coating via Ce doping

This study presents a novel strategy for constructing a stable cathode material by modifying LiNi0.7Mn0.3O2 (NM73) with CeO2 to address the issues of interfacial degradation and significant capacity decay during cycling of Co-free materials. In this approach, Ce3+/Ce4+ is doped within the NM73 bulk material, while CeO2 is coated on the surface of the bulk material to suppress the attack of electrolyte on the particle surface during cycling. As a result, the modified sample, Ce/NM-1.0, exhibits excellent cycling performance compared to the bare sample, NM73, with an initial discharge capacity of 181.7 mAh/g at a rate of 1C within the voltage range of 2.7 V–4.3 V, which is significantly higher than that of NM73 (164.7 mAh/g). Notably, the capacity retention rate of Ce/NM-1.0 after 200 cycles is 85.36%, whereas that of NM73 is only 78.93%. These results demonstrate that the strategy significantly improves the electrochemical performance and cycle stability of the modified material.X-ray photoelectron spectroscopy, X-ray diffraction, scanning electron microscopy, and transmission electron microscopy characterizations indicate that the excellent discharge specific capacity is attributed to the Ce ions doping, while the excellent structural stability is attributed to the CeO2 coating on the particle surface. This work provides valuable insights into the modification of other cathode materials to promote their commercialization.

High-entropy Electrolyte Enables High Reversibility and Long Lifespan for Magnesium Metal Anodes.

The stable cycling of Mg-metal anodes is limited by several problems, including sluggish electrochemical kinetics and passivation at the Mg surface. In this study, we present a high-entropy electrolyte composed of lithium triflate (LiOTf) and trimethyl phosphate (TMP) co-added to magnesium bis(trifluoromethane sulfonyl)imide (Mg(TFSI)2/1,2-dimethoxyethane (DME) to significantly improve the electrochemical performance of Mg-metal anodes. The as-formed high-entropy Mg2+-2DME-OTf--Li+-DME-TMP solvation structure effectively reduced the Mg2+-DME interaction in comparison with that observed in traditional Mg(TFSI)2/DME electrolytes, thereby preventing the formation of insulating components on the Mg-metal anode and promoting its electrochemical kinetics and cycling stability. Comprehensive characterization revealed that the high-entropy solvation structure brought OTf- and TMP to the surface of the Mg-metal anode and promoted the formation of a Mg3(PO4)2-rich interfacial layer, which is beneficial for enhancing Mg2+ conductivity. Consequently, the Mg-metal anode achieved excellent reversibility with a high Coulombic efficiency of 98% and low voltage hysteresis. This study provides new insights into the design of electrolytes for Mg-metal batteries.

High‐entropy Electrolyte Enables High Reversibility and Long Lifespan for Magnesium Metal Anodes

AbstractThe stable cycling of Mg‐metal anodes is limited by several problems, including sluggish electrochemical kinetics and passivation at the Mg surface. In this study, we present a high‐entropy electrolyte composed of lithium triflate (LiOTf) and trimethyl phosphate (TMP) co‐added to magnesium bis(trifluoromethane sulfonyl)imide (Mg(TFSI)2/1,2‐dimethoxyethane (DME) to significantly improve the electrochemical performance of Mg‐metal anodes. The as‐formed high‐entropy Mg2+‐2DME‐OTf−‐Li+‐DME‐TMP solvation structure effectively reduced the Mg2+‐DME interaction in comparison with that observed in traditional Mg(TFSI)2/DME electrolytes, thereby preventing the formation of insulating components on the Mg‐metal anode and promoting its electrochemical kinetics and cycling stability. Comprehensive characterization revealed that the high‐entropy solvation structure brought OTf− and TMP to the surface of the Mg‐metal anode and promoted the formation of a Mg3(PO4)2‐rich interfacial layer, which is beneficial for enhancing Mg2+ conductivity. Consequently, the Mg‐metal anode achieved excellent reversibility with a high Coulombic efficiency of 98 % and low voltage hysteresis. This study provides new insights into the design of electrolytes for Mg‐metal batteries.

Structural, electrical and electrochemical properties of Na2NixMn2−xFe(PO4)3as positive electrode material for sodium-ion batteries

The design of synthetic Alluaudite cathode materials has attracted much interest. However, their poor electrochemical activity and the limited kinetics have prevented them from practical applications, both stationary and mobile. Therefore, we provide in this work, a comprehensive study on the effect of combining 3d multivalent elements (Ni2+, Mn2+, Fe2+) and small particle sizes on structural, electrical and electrochemical properties of a series of Na2NixMn2−xFe(PO4)3 Alluaudite phases using a plethora of techniques. We systematically investigated the impact of the crystal structure, morphology and the density of the samples on Na-ion transport and the associated activation energies. Electrochemical performances of the prepared phases were investigated as positive electrode on a Na-ion battery by means of galvanostatic charge/discharge technique. An enhanced electrochemical performance was obtained by improving the composition of the slurry and the optimization of the electrolyte formulation, thus, affecting the electrochemical performances and cycling stability.

Synergetic Control of Li+ Transport Ability and Solid Electrolyte Interphase by Boron‐Rich Hexagonal Skeleton Structured All‐Solid‐State Polymer Electrolyte

High Li+ transference number electrolytes have long been understood to provide attractive candidates for realizing uniform deposition of Li+. However, such electrolytes with immobilized anions would result in incomplete solid electrolyte interphase (SEI) formation on the Li anode because it suffers from the absence of appropriate inorganic components entirely derived from anions decomposition. Herein, a boron‐rich hexagonal polymer structured all‐solid‐state polymer electrolyte (BSPE+10% LiBOB) with regulated intermolecular interaction is proposed to trade off a high Li+ transference number against stable SEI properties. The Li+ transference number of the as‐prepared electrolyte is increased from 0.23 to 0.83 owing to the boron‐rich cross‐linker (BC) addition. More intriguingly, for the first time, the experiments combined with theoretical calculation results reveal that BOB− anions have stronger interaction with B atoms in polymer chain than TFSI−, which significantly induce the TFSI− decomposition and consequently increase the amount of LiF and Li3N in the SEI layer. Eventually, a LiFePO4|BSPE+10% LiBOB|Li cell retains 96.7% after 400 cycles while the cell without BC‐resisted electrolyte only retains 40.8%. BSPE+10% LiBOB also facilitates stable electrochemical cycling of solid‐state Li‐S cells. This study blazes a new trail in controlling the Li+ transport ability and SEI properties, synergistically.

Epoxy Resin-Reinforced F-Assisted Na3Zr2Si2PO12 Solid Electrolyte for Solid-State Sodium Metal Batteries

Solid sodium ion batteries (SIBs) show a significant amount of potential for development as energy storage systems; therefore, there is an urgent need to explore an efficient solid electrolyte for SIBs. Na3Zr2Si2PO12 (NZSP) is regarded as one of the most potential solid-state electrolytes (SSE) for SIBs, with good thermal stability and mechanical properties. However, NZSP has low room temperature ionic conductivity and large interfacial impedance. F−doped NZSP has a larger grain size and density, which is beneficial for acquiring higher ionic conductivity, and the composite system prepared with epoxy can further improve density and inhibit Na dendrite growth. The composite system exhibits an outstanding Na+ conductivity of 0.67 mS cm−1 at room temperature and an ionic mobility number of 0.79. It also has a wider electrochemical stability window and cycling stability.

Comparison of the capacitance of MnCo2O4 supercapacitor electrode synthesized with different morphologies

In this research, manganese cobaltite (MCO) nanoparticles with different morphologies were synthesized by a simple hydrothermal method with excellent electrochemical properties. To investigate the physical features of prepared samples, XRD analysis was used to study the crystalline structure. The SEM and TEM proved that the morphology of synthesized materials formed as flake and nanoplane structures. The electrode of samples was prepared using the hydrothermal method and the electrochemical properties of samples were investigated by cyclic voltammetry (CV), galvanostatic charge–discharge (GCD), electrochemical impedance spectroscopy (EIS) and cyclic stability analysis. Results showed that the flake structures of nanoparticles revealed the highest capacitance of 1971.98[Formula: see text][Formula: see text] at 0.5[Formula: see text]Ag[Formula: see text] as well as longer stability compared to the others with the nanoplane structure. The high cyclic stability of 91.47% after 5000 cycles introduces this electrode as a durable and promising electrode for use in energy storage devices.

Anomalous Inferior Zn Anode in High-Concentration Electrolyte: Leveraging Solid-Electrolyte-Interface for Stabilized Cycling of Aqueous Zn-Metal Batteries.

Aqueous Zn-metal batteries (AZMBs) are promising large-scale energy storage devices for their high safety and theoretical capacity. However, unstable Zn-electrolyte interface and severe side reactions have excluded AZMBs from long cycling required by practically reversible energy storage. Traditional high-concentration electrolyte is an effective strategy to suppress dendrites growth and resolve the poor electrochemical stability and reversibility of Zn-metal anodes, yet how scientifically universal such strategy is for hybrid electrolyte of different concentrations remains unclear. Herein, we studied the electrochemical behaviors of AZMBs comprising a ZnCl2-based DMSO/H2O electrolyte of two distinct concentrations (1 M vs 7 M). The electrochemical stability/reversibility of Zn anodes in both symmetric and asymmetric cells with high-concentration electrolytes are unusually inferior to the ones with low-concentration electrolyte. It was found that more DMSO components in the solvation sheath of low-concentration electrolyte exist at the Zn-electrolyte interface than in high-concentration counterpart, enabling higher organic compositions in SEI. The rigid inorganic and flexible organic compositions of SEI decomposed from the low-concentration electrolyte is accounted for improved cycling and reversibility of Zn metal anodes and the respective batteries. This work reveals the critical role of SEI than the high concentration itself in delivering stable electrochemical cycling in AZMBs.

Heterointerface Engineering‐Induced Oxygen Defects for the Manganese Dissolution Inhibition in Aqueous Zinc Ion Batteries

Manganese‐based material is a prospective cathode material for aqueous zinc ion batteries (ZIBs) by virtue of its high theoretical capacity, high operating voltage, and low price. However, the manganese dissolution during the electrochemical reaction causes its electrochemical cycling stability to be undesirable. In this work, heterointerface engineering‐induced oxygen defects are introduced into heterostructure MnO2 (δa‐MnO2) by in situ electrochemical activation to inhibit manganese dissolution for aqueous zinc ion batteries. Meanwhile, the heterointerface between the disordered amorphous and the crystalline MnO2 of δa‐MnO2 is decisive for the formation of oxygen defects. And the experimental results indicate that the manganese dissolution of δa‐MnO2 is considerably inhibited during the charge/discharge cycle. Theoretical analysis indicates that the oxygen defect regulates the electronic and band structure and the Mn‐O bonding state of the electrode material, thereby promoting electron transport kinetics as well as inhibiting Mn dissolution. Consequently, the capacity of δa‐MnO2 does not degrade after 100 cycles at a current density of 0.5 A g−1 and also 91% capacity retention after 500 cycles at 1 A g−1. This study provides a promising insight into the development of high‐performance manganese‐based cathode materials through a facile and low‐cost strategy.

Hybrid Ag/Ni mesh/PH 1000 transparent electrodes for high performance flexible electrochromic devices with exceptional stability

Flexible electrochromic technology has gained numerous attentions in flexible smart wearable devices and flexible displays. For large-area flexible electrochromic devices (FECDs), highly conductive transparent electrodes with advanced stability at a prolonged redox cycling process are indispensable. In this work, a silver (Ag)/nickel (Ni) mesh/PH 1000 hybrid transparent film were successfully fabricated by selectively electrodepositing an 800 nm-thick dense metallic Ni layer and coating PH 1000 on an embedded Ag mesh to improve its electrochemical stability. The prepared hybrid transparent film presented high conductivity with a sheet resistance of below 1.5 Ω sq−1 at over 80% optical transmittance. The Ag/Ni mesh/PH 1000 was successfully utilized as current collectors for all-solid-state FECDs, showing fast coloration switching with a bleaching/coloring time of 0.7 s/0.9 s. In addition, the device demonstrated an exceptional electrochemical cycling stability, which could sustain 89% of its initial optical modulation after 25 000 cycles. More importantly, a remarkable mechanical durability was also achieved with a small optical modulation decay of 15% and an invariable response time after 1000 rolling cycles. In addition, uniform coloration were realized on a 6 × 6 cm2 FECD, demonstrating its great potential for applications of next-generation up-scaling FECDs.