Fast Charge Transfer Kinetics Research Articles

Electrochemically co-deposited WO3-V2O5 composites for electrochromic energy storage applications

In this study, a W-V mixed metal oxide composite thin-film structure comprising tungsten oxide (WO3) and vanadium oxide (V2O5) is prepared using a one-step electrochemical co-deposition method. The electrochromic and electrochemical energy storage applications of the prepared thin films comprising different compositions of WO3 and V2O5 are systematically investigated. The films of the W-V mixed composite, comprising WO3 and V2O5 in the ratio of 1:1, exhibits remarkable electrochromic properties, such as an optimum optical contrast of 60%, a fast coloration response of 4.9 s, and the highest coloration efficiency of 61.5 cm2/C. Furthermore, for the electrochemical energy storage application, a maximum areal capacitance of 38.75 mF/cm2 at an applied current of 0.5 mA/cm2 is obtained. Furthermore, it displays a capacitive retention of 78.5%, even after 5000 charge/discharge cycles. The ameliorated characteristics of both electrochromic and electrochemical energy storage applications are attributed to the (a) unique morphology containing more active sites introduced by both WO3 and V2O5, (b) fast charge transfer kinetics, and (c) redox behavior of both metal ions present in the synthesized W-V mixed metal composite.

Design metal-free single-atom catalyst P@BN for CO oxidation: A DFT-D study

Single-atom catalysts (SACs) have arisen significant interest in catalysis and have the superior advantage for CO oxidation. In the current study, beyond the normal single-metal atom catalyst, we designed a new type of metal-free single-atom catalyst based on P doped BN surface. The catalytic mechanism and electronic analysis of CO oxidation on P doped BN metal-free single-atom catalyst is studied by using DFT-D simulation. We found that the phosphorus is preferable to anchor on the boron vacancy of h-BN, and the 3p states of the P dopant would be the key to activate the pre-adsorbed O2. Due to the high catalytic performance and stability of metal-free single-atom, fast charge-transfer kinetics is permissible via catalysis. CO oxidation on the P doped Bv/BN is found to be feasible with the direct formation of CO2 from the cleavage of P–O bonds (ER2 pathway: O2 + CO → CO2 + O) and followed by the reaction process (O + CO → CO2) with low activation energy barriers, indicating that the CO oxidation might be ready at a low temperature. Our work is helpful to reveal the significant role of P dopant for the CO oxidation and shed light on design the new type metal-free single-atom catalyst with low cost, high-performance catalytic activities.

Multi-pathway mechanism of polydopamine film formation at vertically aligned diamondised boron-doped carbon nanowalls

Boron-doped carbon nanowall (B:CNW) electrodes were used as a platform for studying the electropolymerisation of dopamine. Due to the unique properties of B:CNW, including the fast charge-transfer kinetics and high surface conductivity, a high degree of reversibility of redox reactions was achieved. Three separated redox peaks were observed on voltammograms and attributed to three fundamental reactions in the dopamine polymerisation mechanism: dopamine/dopamine quinone, leukodopaminechrome/dopaminechrome, and dihydroxyindole/indolequinone. The mechanism was also supported by the density functional theory calculations of the single point energy of the polydopamine structural units. Moreover, the electrochemical impedance spectroscopy experiments strongly suggest that the majority of th epolymerisation occurs only in the narrow range of potentials between +0.0 and +0.4 V vs. the silver chloride reference electrode. The concept of a resistor-like CPE element is introduced to facilitate the description of the electrochemical properties of B:CNW electrodes in a neutral electrolyte. Further, it is shown that electropolymerisation differs significantly as a function of pH. In acidic environments (pH 3–6) mostly the dopamine/dopamine quinone reaction can be seen, whereas in a more alkaline pH (8–10), the leukodopaminechrome/dopaminechrome reaction becomes dominant. The dihydroxyindole/indolequinone redox pair is seen only in a short pH interval between 7 and 8. Additionally, the kinetics of polymerisation is significantly boosted when the pH is more than 7. Together, these results provide insight into the complexity of the formation of polydopamine and can assist in better controlling the properties of electropolymerised dopamine films.

Graphdiyne/graphene heterostructure supported NiFe layered double hydroxides for oxygen evolution reaction

Graphdiyne (GDY) with the characteristic delocalized sp and sp2 electronic structure is an excellent carbon carrier for metal-based catalysts. However, the semiconductor properties limited its electrocatalytic activity. Herein, a two-dimensional (2D) few-layered graphdiyne/graphene (GDY/G) heterostructure was employed to anchor NiFe layered double hydroxides (NiFe-LDH) for enhanced oxygen evolution reaction (OER). This heterostructure not only exhibits excellent conductivity for charge transfer due to the graphene layer, but also significantly regulates the electronic structure of NiFe-LDH for enhanced intrinsic activity on account of the strong covalent bond between the Ni/Fe active site and GDY. Remarkably, the NiFe-LDH/GDY/G catalyst achieved a competitive low overpotential of 215 mV @ 10 mA cm−2 as well as a small Tafel slope of 22 mV dec−1. The improved OER kinetics could be attributed to the unique few-layered GDY/G heterostructure with a larger electrochemical active surface area, faster charge transfer kinetics, and higher intrinsic activity.

Defect‐Selectivity and “Order‐in‐Disorder” Engineering in Carbon for Durable and Fast Potassium Storage

Defect-rich carbon materials possess high gravimetric potassium storage capability due to the abundance of active sites, but their cyclic stability is limited because of the low reversibility of undesirable defects and the deteriorative conductivity. Herein, in situ defect-selectivity and order-in-disorder synergetic engineering in carbon via a self-template strategy is reported to boost the K+ -storage capacity, rate capability and cyclic stability simultaneously. The defect-sites are selectively tuned to realize abundant reversible carbon-vacancies with the sacrifice of poorly reversible heteroatom-defects through the persistent gas release during pyrolysis. Meanwhile, nanobubbles generated during the pyrolysis serve as self-templates to induce the surface atom rearrangement, thus in situ embedding nanographitic networks in the defective domains without serious phase separation, which greatly enhances the intrinsic conductivity. The synergetic structure ensures high concentration of reversible carbon-vacancies and fast charge-transfer kinetics simultaneously, leading to high reversible capacity (425 mAh g-1 at 0.05 A g-1 ), high-rate (237.4 mAh g-1 at 1 A g-1 ), and superior cyclic stability (90.4% capacity retention from cycle 10 to 400 at 0.1 A g-1 ). This work provides a rational and facile strategy to realize the tradeoff between defect-sites and intrinsic conductivity, and gives deep insights into the mechanism of reversible potassium storage.

Organic-inorganic hybrid ferrocene/AC as cathodes for wide temperature range aqueous Zn-ion supercapacitors.

Organic and inorganic materials have their own advantages and limitations, and new properties can be displayed in organic–inorganic hybrid materials by uniformly combining the two categories of materials at small scale. The objective of this study is to hybridize activated carbon (AC) with ferrocene to obtain a new material, ferrocene/AC, as the cathode for Zn-ion hybrid supercapacitors (ZHSCs). The optimized ferrocene/AC material owns fast charge transfer kinetics and can obtain pseudo-capacitance through redox reaction. Due to the introduction of ferrocene/AC, the ZHSCs exhibit remarkable electrochemical performances relative to that using ferrocene cathode, including high discharge specific capacity of 125.1 F g−1, high energy density (up to 44.8 Wh kg−1 at 0.1 A g−1) and large power density (up to 1839 W kg−1 at 5 A g−1). Meanwhile, the capacity retention rate remains 73.8% after 10 000 charge and discharge cycles. In particular, this cathode material can be used at low temperatures (up to −30 °C) with 60% capacity remained, which enlarges the application temperature range of ZHSCs. These results of this study can help understand new properties of organic–inorganic hybrid materials.

Fast charge transfer kinetics in an inorganic–organic S-scheme heterojunction photocatalyst for cooperative hydrogen evolution and furfuryl alcohol upgrading

Inorganic Znln2S4 nanosheets were grown in situ on organic Tp-Tta COF nanoplates to construct an inorganic–organic S-scheme photocatalyst for synergetic hydrogen precipitation and furfuryl alcohol upgrading oxidation.

Nanocrystals of CuCoO2 derived from MOFs and their catalytic performance for the oxygen evolution reaction.

In this work, two different solvothermal synthesis routes were employed to prepare MOF-derived CuCoO2 (CCO) nanocrystals for electrocatalytic oxygen evolution reaction (OER) application. The effects of the reductants (ethylene glycol, methanol, ethanol, and isopropanol), NaOH addition, the reactants, and the reaction temperature on the structure and morphology of the reaction product were investigated. In the first route, Cu-BTC derived CCO (CCO1) nanocrystals with a size of ∼214 nm and a specific surface area of 4.93 m2 g-1 were prepared by using Cu-BTC and Co(NO3)2·6H2O as the Cu and Co source, respectively. In the second route, ZIF-67 derived CCO (CCO2) nanocrystals with a size of ∼146 nm and a specific surface area of 11.69 m2 g-1 were prepared by using ZIF-67 and Cu(NO3)2·3H2O as the Co and Cu source, respectively. Moreover, the OER performances of Ni foam supported CCO1 (Ni@CCO1) and CCO2 (Ni@CCO2) electrodes were evaluated in 1.0 M KOH solution. Ni@CCO2 demonstrates a better OER catalytic performance with a lower overpotential of 394.5 mV at 10 mA cm-2, a smaller Tafel slope of 82.6 mV dec-1, and long-term durability, which are superior to those of some previously reported delafossite oxide or perovskite oxide catalysts. This work reveals the preparation method and application potential of CCO electrocatalysts by using Cu-BTC/ZIF-67 as the precursor, providing a new approach for the preparation of delafossite oxide CCO and the enhancement of their OER performances.

The fast nucleation/growth of Co3O4 nanowires on cotton silk: the facile development of a potentiometric uric acid biosensor.

In this study, we have used cotton silk as a source of abundant hydroxyl groups for the fast nucleation/growth of cobalt oxide (Co3O4) nanowires via a hydrothermal method. The crystal planes of the Co3O4 nanowires well matched the cubic phase. The as-synthesized Co3O4 nanowires mainly contained cobalt and oxygen elements and were found to be highly sensitive towards uric acid in 0.01 M phosphate buffer solution at pH 7.4. Importantly, the Co3O4 nanowires exhibited a large surface area, which was heavily utilized during the immobilization of the enzyme uricase via a physical adsorption method. The potentiometric response of the uricase-immobilizing Co3O4 nanowires was measured in the presence of uric acid (UA) against a silver/silver chloride (Ag/AgCl) reference electrode. The newly fabricated uric acid biosensor possessed a low limit of detection of 1.0 ± 0.2 nM with a wide linear range of 5 nM to 10 mM and sensitivity of 30.6 mV dec−1. Additionally, several related parameters of the developed uric acid biosensor were investigated, such as the repeatability, reproducibility, storage stability, selectivity, and dynamic response time, and these were found to be satisfactory. The good performance of the Co3O4 nanowires was verified based on the fast charge-transfer kinetics, as confirmed via electrochemical impedance spectroscopy. The successful practical use of the uric acid biosensor was demonstrated based on the recovery method. The observed performance of the uricase-immobilizing Co3O4 nanowires revealed that they could be considered as a promising and alternative tool for the detection of uric acid under both in vitro and in vivo conditions. Also, the use of cotton silk as a source of abundant hydroxyl groups may be considered for the remarkably fast nucleation/growth of other metal-oxide nanostructures, thereby facilitating the fabrication of functional electrochemical devices, such as batteries, water-splitting devices, and supercapacitors.

Atomic-level coupled spinel@perovskite dual-phase oxides toward enhanced performance in Zn–air batteries

The interfacial synergy of Co3O4@LaCoO3 provides fast charge transfer paths and kinetics in the oxide/solution interface, which exhibit exceptional bifunctional catalytic activity and robust stability for Zn–air batteries.

Zn2SiO4@C submicro-ellipsoids assembled from oriented nanorods with outstanding rate performance for Li-ion capacitors

A Zn2SiO4@C network with fast charge transfer kinetics assembled from submicro-ellipsoids containing uniformly aligned nanorods is designed and prepared. The assembled Zn2SiO4@C//graphene hydrogel LIC exhibits excellent electrochemical properties.

Controlled moderative sulfidation-fabricated hierarchical heterogeneous nickel sulfides-based electrocatalyst with tripartite Mo doping for efficient oxygen evolution

An electrocatalyst with heterogeneous nanostructure, especially the hierarchical one, generally shows a more competitive activity than that of its single-component counterparts for oxygen evolution reaction (OER), due to the synergistically enhanced kinetics on enriched active sites and reconfigured electronic band structure. Here this work introduces hierarchical heterostructures into a NiMo@NiS/MoS2@Ni3S2/MoOx (NiMoS) composite by one-pot controlled moderative sulfidation. The optimal solvent composition and addition of NaOH enable NiMoS to own loose and porous structures, smaller nanoparticle sizes, optimal phase composition and chemical states of elements, improving the OER activity of NiMoS. To achieve current densities of 50 and 100 mA cm−2, small overpotentials of 275 and 306 mV are required respectively, together with a minor Tafel slope of 58 mV dec−1, which outperforms most reported sulfide catalysts and IrO2. The synergistic effects in the hierarchical heterostructures expose more active sites, adjust the electronic band structure, and enable the fast charge transfer kinetics, which construct an optimized local coordination environment for high OER electrocatalytic activity. Furthermore, the hierarchical heterostructures suppress the distinct lowering of electrical conductivity and collapse of pristine structures resulted from the metal oxidation and synchronous S leaching during OER, yielding competitive catalytic stability.

Controllable and high-yielding synthesis of ZIF-8 hollow structures for electrochemical energy storage

Well-designed architectures are of great significance for metal–organic frameworks (MOFs) to explore new applications, but the controllable and industrial-scale synthesis remains a great challenge so far. We herein develop a general and facile route for preparing ZIF-8 hollow structures, by adjusting the balance between old bond breakage of starting MOFs and new bond reassembly of targeted ZIF-8. With a simple carbonization treatment, hollow ZIF-8-derived nanoporous carbon can be fabricated, which inherit hollow structures of their original precursors. Due to the unique double-shelled hollow architecture which affords more active sites and fast charge transfer kinetics as well as structural stability, the double-shelled hollow ZIF-8-derived nanoporous carbon exhibits remarkable electrochemical energy storage performances. It is believed that the present synthesis strategy will give a significant insight into the controllable synthesis of hollow MOF structures and other more complicated MOF architectures, which would further exploit new application areas of MOF materials.

An Electrochemically Activated Nanofilm for Sustainable Mg Anode with Fast Charge Transfer Kinetics

Highly reversible Mg plating/stripping is key for rechargeable Mg batteries and has typically been successfully demonstrated using transient electrochemical techniques such as cyclic voltammetry measurements. However, little effort has been invested in studying the stability of the electrode/electrolyte interface over an extended time. We report here the development of an in situ generated surface film for Mg anodes based on electrodeposited bismuth (E_Bi). This film improves the interfacial stability of Mg in contact with the electrolyte, particularly over an extended time, and possesses fast charge-transfer kinetics (<30 Ω∙cm2) and low non-time-sensitive interfacial film resistance (ca. 5 Ω∙cm2) for active Mg species.

Improved Photoelectrochemical Performance of Chemically Grown Pristine Hematite Thin Films

The alpha phase of hematite (α-Fe2O3) is one of the most promising catalysts for photoelectrochemical (PEC) water splitting among several photoanode materials due to its suitable band gap and stability in aqueous solutions. The surface structure and morphology of films play pivotal roles in the enhancement of water oxidation reaction kinetics. In this work, α-Fe2O3 films were produced via either spray pyrolysis (SP), chemical vapor deposition (CVD), or aerosol-assisted chemical vapor deposition (AACVD). Their structural and morphological properties were subsequently characterized by powder x-ray diffraction (PXD), scanning electron microscopy (SEM), and Raman spectroscopy. High-quality thin films were best achieved by AACVD annealed at 525 °C, possessing an average thickness of 0.75 µm with 85% transmittance and an optical absorption onset at 650 nm. The results showed that the thermal oxidation process achieved at 525 °C eliminated undesired impurity phases, such as FeO and Fe3O4 , and enabled the microstructure to be optimized to facilitate the generation and transport of photogenerated charge carriers. The optimized α-Fe2O3 film showed a stable PEC water oxidation current density of ~1.23 mA cm-2 at 1.23 V (vs. RHE), with an onset potential of 0.76 V, under AM 1.5 irradiation. The obtained higher current density of pristine α-Fe2O3 thin films obtained by the AACVD method is unique, and the films presented good photocurrent stability with 92% retention after 6 h. Data from electrochemical impedance spectroscopy (EIS) corroborated these results, identifying fast charge transfer kinetics with decreased resistance and an electron lifetime of 175 µs. Quantitative measurements showed that 1.2 μmol cm-2 of oxygen could be produced at the photoanode in 6 h.Graphical Abstract

Dianhydride-based polyimide as organic electrode materials for aqueous hydronium-ion battery

Organic materials are promising materials for anode electrodes in aqueous hydronium-ion battery due to their flexible of structural, the abundant resources and the tunable electrochemical properties. However, the dissolution of the organic materials in the electrolytes is still inevitable. Polyimide (PI) possesses stable aromatic core, π–π stacking interaction, and increased conjugated system, which are favorable for fast charge transfer kinetics and stable cycling performance of aqueous hydronium-ion battery. Here, the synthesis PI by 1,4,5,8-naphthalenetetracarboxylic dianhydride (NTCDA) and urea is reported. In this work, the capacity of full cell can retain about 67.9% at the current of 5 A•g−1 after charging-discharging over 5000 cycles. Therefore, our studies are suggesting a potential feasibility of these NTCDA-based carbonyl PI as promising organic anode materials for aqueous hydronium-ion battery.

High-performance Zn battery with transition metal ions co-regulated electrolytic MnO2

Electrolytic MnO2/Zn batteries have attracted extensive attention for use in large-scale energy storage applications due to their low cost, high output voltage, safety, and environmental friendliness. However, the poor electrical conductivity of MnO2 limits its deposition and dissolution at large capacities, which leads to sluggish reaction kinetics and drastic capacity decay. Here, we report a theory-guided design principle for an electrolytic MnO2/Zn battery co-regulated with transition metal ions that has improved electrochemical performance in terms of deposition and stripping chemistries. We start with first-principles calculations to predict the electrolytic effects of regulating transition metal ions in the deposition/stripping chemistry of the MnO2 cathode. The results indicate that with the simultaneous incorporation of strongly electronegative Co and Ni, the MnO2 cathode tends to possess more active electron states, faster charge-transfer kinetics, and better electrical conductivity than either MnO2 regulated with Co or Ni on their own, or pristine MnO2; hence, this co-regulation is beneficial for the cathode solid/liquid MnO2/Mn2+ reactions. We then fabricate and demonstrate a novel Co2+ and Ni2+ co-regulated MnO2/Zn (Co–Ni–MnO2/Zn) battery that yields significantly better electrochemical performance, finding that the synergistic regulation of Co and Ni on MnO2 can significantly increase its intrinsic conductivity and achieve high rates and Coulombic efficiencies at large capacities. The aqueous Co–Ni–MnO2/Zn battery exhibits a high rate (10C, 100 ​mA ​cm–2), high Coulombic efficiency (91.89%), and excellent cycling stability (600 cycles without decay) at a large areal capacity of 10 mAh cm–2. Our proposed strategy of co-regulation with transition metal ions offers a versatile approach for improving the electrochemical performance of aqueous electrolytic MnO2/Zn batteries in large-scale energy storage applications.

Bipolar Membranes for Ion Management in (Photo)Electrochemical Energy Conversion

Conspectus(Photo)electrochemical energy conversion is important in the development of a carbon-neutral energy economy because it can provide a pathway for mitigating the intermittency of renewable energy sources such as wind and solar. In order to operate efficiently, these technologies, which include photoelectrochemical cells, water and CO2 electrolyzers, fuel cells, and redox flow batteries, require fast charge transfer kinetics at the electrode/electrolyte interface as well as robust ion management in the electrolyte.In conventional electrolyzers and fuel cells, the electrolyte is strongly acidic or basic and ionic current is carried by H+ or OH– ions. In contrast, photoelectrodes and electrocatalysts for water splitting are often studied in buffered solutions. The question of ion balance in these systems led us to analyze the polarization losses due to ion concentration gradients in cells that employed various buffer–membrane combinations. Continuously driving the buffer ions across an ionomer membrane not only lowers the buffer capacity of an aqueous electrolyte but also introduces pH gradients that result in significant energy losses.To address the problem, we and other groups have studied the use of reverse-biased bipolar membranes (BPMs) in (photo)electrolytic cells. BPMs consist of an anion exchange layer (AEL) laminated with a cation exchange layer (CEL) and are usually equipped with a catalytic layer in between to accelerate the water dissociation reaction. At the AEL/CEL interface, water dissociates into protons and hydroxide ions, which replenish those consumed at the cathode and anode. Compared to conventional water electrolyzers with proton/anion exchange membranes (PEM/AEM), BPM electrolyzers provide the unique advantage of continuously operating the cathode and anode under different pH conditions, which is desirable when the two electrode reactions have different pH requirements.BPMs also enable the use of buffered electrolytes at pH values that are optimized for electrode stability and product selectivity in applications such as CO2 electrolysis. Product crossover losses and CO2 pumping can be dramatically reduced in BPM-based CO2 electrolyzers, relative to conventional alkaline membranes, by electrostatic repulsion (of anionic products) and electroosmotic drag (for neutral products). BPM-based gas fed CO2 electrolyzers can achieve high current density, but they suffer from low Faradaic efficiency (FE) due to the acidic local environment of the CEL. This problem can be mitigated by adding an aqueous buffering layer or by creating a weak acid cation exchange film on the CEL face of the membrane.The use of BPMs in fuel cells and redox flow batteries offers some interesting advantages. Configurations with both reverse and forward bias have been studied, but forward bias has been favored due to material compatibility, reaction kinetics, and thermodynamic considerations. The net reaction at the AEL/CEL interface is the acid–base neutralization reaction, which has a high inherent reaction rate constant, but in the BPM is limited to a nanometric space-charge layer and requires efficient catalysis to achieve high current density. Understanding the mechanism of the acid–base neutralization and the opposite process, the water dissociation reaction, will be essential for improving the performance of forward-biased BPMs. This Account reviews our current understanding of the working mechanisms of BPMs and discusses how we can use them to effectively manage ions for various (photo)electrochemical applications.

Synergetic Layer-By-Layer Deposition for Highly Capacitive CNT Electrodes

While inorganic materials are currently dominating in energy storage, organic redox active molecules and polymers are sustainable and low-cost alternatives. Thin layer redox active polymers and molecules are often deposited onto high surface area carbonaceous substrates to form high-performance composite electrodes. Layer-by-layer (LbL) deposition has been widely used in such deposition to provide versatile electrochemical properties for specific applications [1, 2]. The advantages of LbL are its easy and effective processes and, more importantly, allowing design and engineering of novel composites. Through simple superimposing and overlapping of organic molecules, combined supplementary effects and even synergies can be achieved.In this study, a composite electrode based on CNT modified with two previously investigated organic layers, a chemically polymerized luminol (CpLum) [3] and a tetraphenylporphyrin sulfonate (TPPS), was developed via an in-situ polymerization/layer-by-layer process. Fig 1 a) depicts the CVs of CNT, CpLum-CNT, TPPS-CNT as well as TPPS-CpLum-CNT electrodes in 1 M H2SO4 electrolyte. TPPS-CNT showed clear increase in capacitive current from CNT baseline due to the redox contribution from TPPS. CpLum-CNT had a much greater faradaic current but with much less “mirror-image” CV profile, indicating a slower kinetics. When combining CpLum and TPPS by LbL deposition, a new pseudocapacitive CV profile with highly reversible redox peaks was obtained. The TPPS-CpLum-CNT composite electrode not only had higher current and capacitance (Fig. 1b) than those of the individual composite electrodes but also a much faster charge transfer kinetics. The synergy within the composite promoted the complementary electrochemical contribution between the CpLum and the TPPS layer with fast surface capacitive charge storage. Detailed analyses of this composite from first-principles adsorption and energy level, vibrational spectroscopy as well as surface and morphology were carried out to understand the origin of the synergistic effect of the TPPS-CpLum-CNT composite and will be presented in the talk.

Synergistic Effect of Fe2O3/NC-Gdl Interlayer and Partially Exfoliated Carbon Nanotubes/Sulfur Cathode for Efficient Polysulphide Confinement in High Performance Lithium–Sulfur Batteries

Lithium sulfur batteries have gained considerable research interest for electric vehicles and portable electronic devices due to their high theoretical energy density (2600 Wh/Kg) compared to existing metal ion batteries. In addition, the low cost, high abundance and high theoretical specific capacity (1675 mAh/g) of sulfur have made Li-S batteries to be the potential replacement for lithium ion batteries. However, the low electrical conductivity of sulfur (5 × 10−30 S/cm), Li2S, low sulfur loading (<70%) at the composite cathode, large volume expansion during S to Li2S conversion and multistep reduction of sulfur to lithium polysulphides (LPS) act as the prohibitor for the commercialization. Elemental sulfur undergoes a various structural variation during the charge–discharge and forms soluble higher order lithium polysulfides Li2S n (8 ≤ n ≤ 3) and lower order insoluble sulfides Li2S2/Li2S in liquid. The poor conductivity of the intermediates formed and their structural changes result in high polarization. Also, the consecutive shuttling of the soluble polysulfides between the anode and cathode results in reoxidation at the cathode and further leads to capacity fading of the Li-S battery. To mitigate these, researchers have developed several types of conducting carbon matrix i.e., acetylene black, super P, carbon nanotubes, graphene, carbon paper etc. However, due to poor interaction of polar polysulfides with non-polar carbon matrix, polysulfide migrates into the electrolyte and increases the shuttle effect. Metal oxides (TiO2, Fe2O3 , MgO, Co3O4, SiO2) based interlayer though offer abundant polar active sites for polysulfides adsorption, but suffers from low electrical conductivity and high binding energy between oxides and sulphides, which results degradation in the electrochemical performance. Hence optimization of oxide interlayers are necessary to increase the performance of Li-S batteries.So, in our work, further to minimize the LPS confinement and conversion, we have proposed an efficient cathode where partially exfoliated carbon nanotubes are used as sulfur host. Due to the high surface area, and high electrical conductivity, it serves as an efficient cathode material with high sulfur loading (>75%) and results in high sulfur utilization. In addition, we have also considered the effect of polar sites and designed Fe2O3/NC nanoparticles coated on the polytetrafluoroethylene ethylene coated carbon paper (GDL paper) as interlayer between separator and cathode, which can efficiently adsorb the polysulphides and effectively mitigates the shuttling effect due to the active polar sites and oxygen vacancy. From our electrochemical studies, we have observed with PECNT/S cathode without interlayer initial discharge capacity of 900 mAh/g can be obtained at 0.1 C rate. However, with only GDL interlayer this capacity increases to ~1400 mAh/g. Further, on coating of Fe2O3/NC nanoparticles on GDL paper the capacity can further be enhanced and reached to 1610 mAh/g. For GDL-Fe2O3/NC interlayer better reversibility and faster charge transfer kinetics are confirmed from the CV curves. Cyclic stability of 500 cycles is carried out for PECNT/S, PECNT/S/GDL and PECNT/S/GDL- Fe2O3/NC at 0.5 C rate. ~80% of initial capacity retention can be obtained even after 500 cycles. This substantiate that with PECNT/S and GDL-Fe2O3/NC as cathode and interlayer respectively can synergistically result in a high capacity and stable lithium-sulfur batteries.