Free Electrode Research Articles

Cigarette filter butts-derived activated carbon with free binder electrode design for solid-state supercapacitor application

The aim of this research is to formulate activated carbon monolith from hazardous waste of cigarette filter butts (CFB) for electrode material monolith design in solid-state supercapacitor application. Potassium hydroxide (KOH) was selected for activation. The ratio of CFB to KOH varied in terms of weight between 1:2 and 1:4, thereby obtaining activated cigarette filter carbon (ACFC). The carbon that has been obtained is designed to be solidly in the form of an additive-free monolith. Monolith-activated carbon is physically characterized to examine thermal decomposition profiles (pre-carbonized), structure, composition, morphology, surface area adsorption, and electrochemical measurements. The optimum precursor was marked with high wettability with self-O-doped of 5.44%.in carbon content of 94.56%. Activated carbon electrodes prepared from ACFCs showed an optimum specific capacitance of ~87.17 F g-1, which is a more ecologically responsible method of producing supercapacitors.

Facilitation polysulfides adsorption/catalysis by nitrogen/phosphorous co-doped carbon nanofibers networks for advanced lithium/polysulfides batteries

The development of lithium‑sulfur batteries was hindered due to the shuttling of lithium polysulfides in electrolytes and sluggish electrochemical kinetics of polysulfides transformation. Herein, multi heteroatoms (nitrogen and phosphorus) co-doped carbon nanofibers (NP-CF) is elaborately designed, which acted as the current collector and binder free membrane electrode containing Li2S6 catholyte for lithium/polysulfides batteries. The conductivity of mesoporous NP-CF provide fast electronic transport and polarity of substrate possess a strong affinity to sulfur species, which could effectively anchor lithium polysulfides, boost their redox reaction catalytically-accelerate the reversible soluble/insolube phases conversion process, and greatly improve the utilization of active material. On the basis of density functional theory calculations on the bonding energies between NP-CF and lithium polysulfides (Li2Sn, n = 4, 6), it is found the NP-CF possesses higher binding energies toward polysulfides than N-CF. As a result, the cell with NP-CF membrane electrode with 4.6 mg cm−2 sulfur loading exhibits stability cycling capacity, which delivers a high intial capacity of 1023.3 mAh g−1 at 0.2C and sustains a capacity of 709.2 mAh g−1 over 300 cycles. NP-CF/Li2S6 electrode also performs well in cyclic performance with a sulfur loading of 8.4 mg cm−2, delivers a high specific capacity of 7.8 mAh and still maintains 6.4 mAh after 100 cycles.

Zn-In Alloying Powder Solvent Free Electrode Toward High-Load Ampere-Hour Aqueous Zn-Mn Secondary Batteries.

Aqueous Zn-ion batteries (ZIBs) are promising candidates for large-scale energy storage due to high safety, abundant reserves, low-cost, and high energy density. However, the reversibility of the metallic Zn anode in the mild electrolyte is still unsatisfactory, due to the Zn dendrite growth, hydrogen evolution, and corrosion passivation. Herein, a Zn-In alloying powder solvent free electrode is proposed to replace the Zn foil in ZIBs. The novel Zn anodes are constructed by a solvent-free manufacturing process with carbons, forming a 3D Zn deposition network and providing uniformly electric field distribution. The In on the Zn powder surface can increase the overpotential for hydrogen evolution and further improve the morphology of Zn deposition against dendrite growth. The Zn solvent-free electrodes enable the Zn-MnO2 batteries with high cathode loading mass of 10-20mg cm-2 to achieve >380 stable cycles. Furthermore, the assembled soft package batteries of 2.4 Ah (52Wh kg-2) is evaluated and the capacity retention is maintained at 80% after 200 cycles at a high areal capacity of 5 mAh cm-2 without gas evolution. This work offers a workable strategy to develop a durable Zn anode for the eventually commercial applications of aqueous Zn-Mn secondary batteries.

Construction of Low Cost, and Platinum‐Free Counter Electrode for Dye‐Sensitized Solar Cells

AbstractRecently, design and fabrication of platinum free counter electrodes have received enormous attention of the scientific community. In this work, we have fabricated manganese dioxide/reduced graphene oxide (MnO2@Gr) counter electrode based DSSCs. Hydrothermal method was utilized for the synthesis of MnO2@Gr. Further, X‐ray diffraction technique (XRD), scanning electron microscopy (SEM), and energy dispersive X‐ray spectroscopy (XPS) were employed as physiochemical characterization technique. Surface structural investigations showed that MnO2 has rods like surface morphology which are attached with Gr. The fabricated DSSCs demonstrated good open circuit voltage (Voc) and reasonable efficiency of 0.72 V and 5.87 %, respectively.

Electro‐elucidation and quantification of olopatadine hydrochloride in bulk form and eye drops using modification free glassy carbon electrode with its development by different electrolytes and surfactants

AbstractThe electro‐oxidation pathway of olopatadine hydrochloride which is used in eye drops as antihistaminic agent was proposed and discussed in detail as the first time using different voltammetry methods at the modification free glassy carbon electrode surface. The oxidation process of olopatadine hydrochloride based on the presence of electro‐active tertiary amine group was irreversible. The dissociation constants were attained by the dependence of peak current and potential on the pH values. Some kinetic parameters were also estimated. Depending on the oxidation of olopatadine hydrochloride in citrate buffer (pH 5.5; 0.1 M) and sodium dodecyl sulfate (3×10−5 M) as supporting electrolyte and a modifier, respectively, sensitive, simple, accurate and inexpensive a novel square wave voltammetry method was achieved. The method was validated for linearity, precision, accuracy, ruggedness, specificity and stability. Limit of detection of 9×10−7 M in bulk form was attained. The characterized method was successfully used for routine analysis of olopatadine hydrochloride in pharmaceutical eye drops (Olohistine® and olopalite). No electroactive interferences from the inactive ingredients present in eye drops were noticed. So the proposed method does not necessitate any extraction step preceding the drug analysis. Also, the obtained data of the calibration curve and standard addition methods were compared statistically with a reported spectrophotometrically method showing no differences between them with respect to accuracy and precision, what proved the reproducibility, suitability and reliability of the described voltammetric method for assay of olopatadine hydrochloride in its formulation.

Activation and Stabilization of Mn‐Based Positive Electrode Materials by Doping Nonmetallic Elements

AbstractDisordered rock‐salt (DRS) type active materials are highly significant because of their large reversible capacities, which are due to their unique Li+ diffusion pathway and the redox capabilities of cationic transition metals (TMs) and anionic O ions. Loosely crystalline DRS materials have weak covalent bonds between TMs and O, increasing the O redox contribution and thereby enhancing their capacities. In this study, Mn‐based positive electrode materials with DRS structures are activated and stabilized by mechanochemical doping of nonmetallic elements P and B into interstitial sites. Synthesized Li0.90Mn0.84P0.04O2 (LMPO5) exhibits an initial discharge capacity of 346 mAh g−1 (1050 Wh kg−1) during charging/discharging. Li0.91Mn0.83B0.10O2 (LMBO5) has a moderately expanded lattice size, which facilitates high‐capacity retention during cycling (≈284 mAh g−1 at the 30th cycle). The structural properties of the synthesized active materials are extensively characterized. By introducing nonmetallic elements into the interstitial sites of Mn‐based materials, inexpensive, high‐capacity, and long‐cycling/calendar‐life Co/Ni‐free monometallic positive electrode materials may be further developed.

La0.6Sr0.4MnO3-Based Fuel Electrode Materials for Solid Oxide Electrolysis Cells Operating under Steam, CO2, and Co-Electrolysis Conditions

The conventional Ni–YSZ (yttria-stabilized zirconia) fuel electrode experiences severe degradation due to Ni- agglomeration and migration away from the electrolyte. Therefore, herein, we have considered Ni free electrodes, i.e., La0.6Sr0.4MnO3-δ (LSM)-based perovskite oxides as fuel electrodes. The LSM perovskite phase transforms into a Ruddlesden–Popper LSM (RP-LSM) phase with exsolved MnOx under reducing atmospheres. The RP-LSM is mainly interesting due to its good electrical conductivity, redox stability, and acceptable electrochemical behaviour. In this work, we synthesized the LSM powder and characterized it using several methods including X-ray diffraction (XRD), thermogravimetry analyses (TGA), four-probe conductivity, and scanning electron microscope with energy-dispersive X-ray spectroscopy (SEM-EDX). Finally, the electrolyte-supported single cells were fabricated and electrochemically characterized using AC and DC techniques under electrolysis conditions. In addition to pure LSM fuel electrodes, we have also investigated the electrochemical behaviour of LSM + YSZ (50:50) and LSM + GDC (50:50) composite fuel electrodes. The single cells containing LSM and LSM + GDC fuel electrodes show higher cell performance than LSM + YSZ. For instance, current densities of 1, 1.03, and 0.51 A·cm−2 at 1.5 V are obtained for LSM, LSM + GDC, and LSM + YSZ fuel electrodes containing single cells, respectively, with a 50% N2 and 50% H2O feed gas mixture. Moreover, the performance of the cell was also investigated under co-electrolysis with 50% CO2 and 50% H2O and under direct CO2 electrolysis conditions with 100% CO2 fuel gas.

Improved electrochemical performance of nanostructured binder free Cu2CoSnS4 electrode using redox additive electrolyte

Improved electrochemical performance of nanostructured binder free Cu2CoSnS4 electrode using redox additive electrolyte

Engineering of nickel, cobalt oxides and nickel/cobalt binary oxides by electrodeposition and application as binder free electrodes in supercapacitors

Cobalt oxide, nickel oxide and cobalt/nickel binary oxides were synthesised by electrodeposition. To fine tune composition of CoNi alloys, growth parameters including voltage, electrolyte pH/concentration and deposition time were varied. These produced nanomaterials were used as binder free electrodes in supercapacitor cells and tested using three electrode setup in 2 MKOH aqueous electrolyte. Cyclic voltammetry and galvanostatic charge/discharge were used at different scan rates (5–100 mV/s) and current densities (1–10 A/g) respectively to investigate the capacitive behaviour and measure the capacitance of active material. Electrochemical impedance spectroscopy was used to analyse the resistive/conductive behaviours of these electrodes in frequency range of 100 kHz to 0.01 Hz at applied voltage of 10 mV. Binary oxide electrode displayed superior electrochemical performance with the specific capacitance of 176 F/g at current density of 1 A/g. This hybrid electrode also displayed capacitance retention of over 83% after 5000 charge/discharge cycles. Cell displayed low solution resistance of 0.35 Ω along with good conductivity. The proposed facile approach to synthesise binder free blended metal electrodes can result in enhanced redox activity of pseudocapacitive materials. Consequently, fine tuning of these materials by controlling the cobalt and nickel contents can assist in broadening their applications in electrochemical energy storage in general and in supercapacitors in particular.

Hierarchical porous nickel tin sulfide nanosheets as a binder free electrode for hybrid supercapacitor

The utilization of free-standing sulfide-based hybrid nanostructures plays a paramount role in supplying the steadily increasing demand for energy storage devices. Herein, this report presents the growth of outstanding binder-free Ni-Sn sulfide thin films for high-performance supercapacitors via the revised successive ionic layer adsorption and reaction (r-SILAR) method. Molar concentration ratios between Ni/Sn have been studied, and the optimum designed mesoporous Nix-Sn1.0xS/Ni foam (NF), a single cathode electrode material, successfully achieved outstanding specific capacitance of 2890 F/g at 5 A/g, capacitance retention of 85 %, and coulombic efficiency of 100 % after 10,000 cycles. Moreover, the constructed Nix-Sn1.0xS/NF//activated carbon (AC) hybrid supercapacitor device delivers an ultrahigh power density of 53.469 KW/Kg and capacitance retention of 95 % with robust long-term cycling stability up to1000 cycles. The superior electrochemical performance of the prepared Nix-Sn1.0xS electrode could be attributed to: (i) the synergistic effect of the two binary metal sulfides (Ni/Sn) into reversible faradaic redox reaction; (ii) the growing mechanism of the ultra-thin film (1.2 nm) as a binder-free electrode, enhance the ions insertion/extraction, and (iii) the formation of hierarchically flower-like architecture with uniform mesopores provides a high surface area (62.2 m2/g) and intensifies active sites for faradaic redox reactions. These encouraging results present a novel avenue for constructing advanced free-standing electrode materials for high-performance supercapacitors.

Hydrogen Reconversion from Ammonia through Anion Exchange Membrane Electrolysis

Nitrogen-based compounds, especially ammonia, is a promising alternative for the storage and transport of renewable hydrogen over long distances [1]. Considering ammonia as a hydrogen carrier will require studying the conversion (ammonia to hydrogen) and reconversion steps (hydrogen to ammonia). The reconversion of ammonia can take place through electrolysis under alkaline conditions [2] and needs the development of more efficient catalysts. For this, we started studying the electro-oxidation of ammonia in an anion exchange membrane electrolyser over platinum-based and PGM free electrodes with KOH as electrolyte. We have prepared several catalysts, carbon supported platinum, platinum-iridium, and nickel nanoparticles using the polyol technique. Commercial carbon supported platinum nanoparticles was used as catalyst for the cathodes. Catalyst coated substrates (CCS) were then prepared by spraying a catalytic ink over stainless-steel fiber paper for the anode side. The formulation of the ink requires optimizing parameters such as the type of ionomer (nafion, sustanion) and the ratio of ionomer to carbon. Anodes obtained have been assembled with anion exchange membranes and commercial cathodes for ammonia electro-oxidation in single cell. We have compared the performance of these different membrane electrodes assemblies (MEAs) to commercially available ones integrating nickel-iron-cobalt based anodes. The performance of MEAs was analyzed based on polarization curves, cyclic voltammograms and impedance spectroscopy data. Different testing conditions were investigated by varying the ammonia concentration from 0.1 to 1 M, the temperature from 25 °C to 60°C, and the KOH concentration from 0.1 to 5 M.

Hydrothermally modified tin(II) sulfide binder-free battery grade electrode for supercapattery

In the initiative of diminishing the current research gap related to the limited electrochemical performance of supercapacitor, various hybrid supercapacitor combinations were introduced. However, the energy storage capacity and power are still limited. Thus, a new type of hybrid device known as supercapattery was introduced by combining a battery grade electrode with capacitive type electrode to improve the energy and power densities. In the midst of material exploration on battery grade materials suited for supercapattery, transition metal sulfides have grabbed intense attention for their excellent electrochemical properties and conductivity. Herein, a novel tin (II) sulfide (SnS) binder free electrode materials were synthesized through hydrothermal method as a battery grade material for supercapattery. In this work, the electrodes were fabricated by differing metal precursor to reducing agent ratios (1:2,1:4, and 1:6) followed by fine tuning the physio-chemical characteristics of SnS by differing hydrothermal temperature. The synthesized materials were structurally characterized using X-ray diffraction analysis. The surface morphology and particle size were investigated through field emission scanning electron microscopy (FESEM) and high-resolution transmission electron microscopy (HRTEM). The SnS fabricated using ratio 1:4 at 150 °C exhibited fascinating specific capacity/specific capacitance (325.20Cg−1/668.45Fg−1) with 89.73% rate capability. The SnS was then combined with activated carbon (AC) to produce supercapattery. The fabricated supercapattery demonstrated fascinating stability of 98.61% over 15,000 cycles with maximum energy and power density of 8.77 Wh kg-1 and 3,095.20 W kg−1, respectively.

Synthesis of CuMoS micro‐rods material as efficient bifunctional electrocatalyst for overall water splitting

AbstractIn oxygen evolution reactions (OER) metal sulfides are the subject of extensive research. Copper‐molybdenum sulfides (CuMoS) that can be made a simple hydrothermal treatment are designed to reduce catalyst costs even more. Here, we demonstrate that binder free electrode composed of micro‐rod structure copper‐molybdenum sulfides on nickel foam (CuMoS/NF) can be employed as an active and robust bifunctional electrocatalyst for water splitting. CuMoS/NF catalyst displays an overpotential for OER of 358 mV (121 mV dec−1) and HER of 129 mV (101 mV dec−1) at current density of 10 mA cm−2. CuMoS/NF is stable for 60 hours with potential deviations in OER and HER of 2.8 % and 3.2 %, respectively. The active bifunctional CuMoS/NF electrode combination helps to fabricate a water electrolyser with 10 mA cm−2 current density at 1.65 V. CuMoS/NF//CuMoS/NF shows good stability over 60 hours with a potential deviation of 2.7 %. The earth‘s abundant non‐precious metal‐based electrode, and solar cell delivered continuous hydrogen and oxygen (1.65 V), making it possible to produce a significant quantity of hydrogen at a low‐cost and on a large‐scale.

Highly scalable and low cost binder free electrode of Zinc modified NiO nanofoam for dual role of supercapacitor and its free radical scavenging activity

In this study, pristine nickel oxide (NiO) and Zinc modified NiO nanofoams were prepared by green approach using camellia sinensis leaves extract. Pristine nickel oxide and Zn2+ modified NiO nanofoam were characterized by XRD, FTIR, FL, UV and FESEM. FE-SEM micrographs were clearly shows that the synthesised porous nanofoam with spherical shaped were constant distribution. The as prepared foam electrodes showed excellent supercapacitive behaviour with increase in specific capacitance with decrease in scan rate. The maximum specific capacitance 1530, 1706 and 1847Fg-1 was obtained at scan rate of 10 mVs-1 for increasing the Zn concentrations. After 3,000 cycles at 1 A g−1, the cyclic stability remains excellent at 88.1% of the initial capacitance. Moreover, the as-prepared asymmetric supercapacitor exhibits a high energy density of 30.6 W h·kg−1 at power density of 398 W kg−1. This study is expected to provide new insights into exploring the potential mechanism of catalyst action. These findings show that Zinc @ NiO nanofoam could be a potentially useful electrode material for energy storage devices.

Performance and Electrochemical Behavior of LSM Based Fuel Electrode Materials Under High Temperature Electrolysis Conditions

Ni-YSZ is known as the state-of-the-art fuel electrode material for solid oxide cells. However, this conventional fuel electrode experiences severe degradation due to Ni- agglomeration and migration away from the electrolyte. Therefore, to avoid such issues, we have considered Ni free electrodes i.e. La0.6Sr0.4MnO3 (LSM) based perovskite oxides as fuel electrode. Under reducing atmosphere, the LSM perovskite phase transforms into a Ruddlesden-Popper (La0.6Sr0.4)2MnO4±δ phase. In addition to pure LSM fuel electrode, we have also investigated the performance of LSM+YSZ (50:50 wt %) and LSM+GDC (50:50 wt %) composite electrodes. The electrolyte-supported single cells were prepared using 8YSZ electrolyte supports, and in all cases, LSM+YSZ/LSM oxygen electrodes were used. The current-voltage characteristics show good performance for LSM and LSM+GDC fuel electrode containing single cells. However, a lower performance is observed for LSM+YSZ fuel electrode containing single cell. For instance, a current density of 997, 1025, and 511 mA.cm-2 at 1.5 V, are obtained for LSM, LSM+GDC, and LSM+YSZ fuel electrode containing single cells respectively, with 50% N2 and 50% H2O feed gas mixture.

Nafion-based label-free immunosensor as a reliable warning system: The case of AFB1 detection in cattle feed

This study presents a simple method for the rapid and versatile fabrication of label-free immunosensors on Nafion-modified screen-printed platforms. Herein, Nafion is exploited both as an immobilization matrix and as a weak (unexpectedly) electrochemical enhancer for the first time. The electrochemical characteristics in terms of diffusivity and conductivity of thin cation-exchange polymer membrane-modified screen-printed electrodes were investigated using cyclic voltammetry and electrochemical impedance spectroscopy. The free electrode surface area, the diffusion coefficient, the peak-to-peak separation, the heterogeneous electron transfer constant, and the charge transfer resistance for Nafion-modified and bare SPE have been calculated and compared. Then, Nafion-SPEs were employed to develop a competitive label-free immunoassay for the quantitative detection of Aflatoxin B1. Morphological characterization of the proposed immunosensor was performed using Scanning Electron Microscopy, and its analytical performance was evaluated using square wave voltammetry as a detection technique and [Fe(CN)6]3−/4− as a redox probe. The immunosensor showed satisfactory results in spiked cattle feed in terms of limit of detection (3.8 ngmL−1), linear range (LR 10–100 ngmL−1), sensitivity (33.0 ngmL−1) and reproducibility (RSD%<10%). The comparison of performance to that of a labelled immunosensor and a conventional chromatographic technique revealed a strong correlation between the respective results, but with shorter analysis time for the proposed tool. Furthermore, The present study achieved evidence of the dependability of the proposed method, proving that its use as an early warning system for the detection of AFB1 in cattle feed is something doable and not an abstract idea.

Fabrication of 3D bi-functional binder-free electrode by hydrothermal growth of MIL-101(Fe) framework on nickel foam: A supersensitive electrochemical sensor and highly stable supercapacitor

In present investigation, we report unique and successful fabrication of 3D bi-functional binder free electrode by hydrothermal growth of Fe based metal organic frameworks on nickel foam (MIL-101(Fe)/NF) for supersensitive electrochemical sensor and high capacitance supercapacitor. The materials characteristics were investigated by XRD, FTIR, RAMAN, FE-SEM, and BET techniques. The FE-SEM results revealed the formation of octahedral spindles nanosheets of MIL-101(Fe) fully covered on the nickel foam. In applications involving an electrochemical sensor or a supercapacitor, the binder-free MIL-101(Fe)/NF electrode provided excellent results by modestly avoiding dead mass of binders. The determination capability of MIL-101(Fe)/NF electrode as an electrochemical sensor of lead (Pb2+) ions has been investigated by differential pulse voltammetry (DPV) technique. According to the findings, the MIL-101(Fe)/NF exhibits excellent sensing performance towards Pb2+ ions with low detection limit of 0.169 nM and high sensitivity of 22.6 µA/M. Moreover, the electrode exhibits ideal sensor characteristics such as good selectivity, reproducibility, repeatability and stability. In addition, the structure of MIL-101(Fe)/NF electrode provides elevated electro-active sites, which altogether provides shorter path for electron passage and electrolyte diffusion process, which resulted in a high specific capacitance. At a scan rate of 10 mVs−1, the MIL-101(Fe)/NF electrode exhibits a specific capacitance of 210 Fg−1. Capacitance retention of greater than 98% is demonstrated by the fabricated electrode, even after 1000 cycles. The present investigated results and novel strategies to develop multifunctional materials will open innovative avenues for material scientist.

Highly stable electrodeposited 2D Mn0.2Co0.8 LDH nanoplatelets based symmetric supercapacitor electrode

High performance Mn0.2Co0.8 layered double hydroxide (LDH)-based binder free supercapacitor symmetric electrode is fabricated via single step electrochemical deposition. The synthesized Mn0.2Co0.8 electrode shows specific capacitance of 370.58–141.17 F/g (315–120 C/g) at 2–40 A/g within potential range −0.45–0.4 V along with 172.72% capacitance retention for 9000 GCD cycles. Additionally, a symmetric supercapacitor is also made utilizing Mn0.2Co0.8 LDH both as cathode and anode. The high potential of synthesized electrode as a supercapacitor material is shown by achieving a specific capacitance of 106.91–34.57 F/g at 0.5–3 A/g within a cell voltage of 0 to 0.8 V, as well as outstanding cyclic stability over 5000 GCD cycles. Red LEDs are used to analyze the real world application of the fabricated symmetric supercapacitor for energy storage and it is assumed that the future portable electrical systems and gadgets might benefit from the device based on the reported material and synthesis technique.

A Novel OpenBCI Framework for EEG-Based Neurophysiological Experiments.

An Open Brain-Computer Interface (OpenBCI) provides unparalleled freedom and flexibility through open-source hardware and firmware at a low-cost implementation. It exploits robust hardware platforms and powerful software development kits to create customized drivers with advanced capabilities. Still, several restrictions may significantly reduce the performance of OpenBCI. These limitations include the need for more effective communication between computers and peripheral devices and more flexibility for fast settings under specific protocols for neurophysiological data. This paper describes a flexible and scalable OpenBCI framework for electroencephalographic (EEG) data experiments using the Cyton acquisition board with updated drivers to maximize the hardware benefits of ADS1299 platforms. The framework handles distributed computing tasks and supports multiple sampling rates, communication protocols, free electrode placement, and single marker synchronization. As a result, the OpenBCI system delivers real-time feedback and controlled execution of EEG-based clinical protocols for implementing the steps of neural recording, decoding, stimulation, and real-time analysis. In addition, the system incorporates automatic background configuration and user-friendly widgets for stimuli delivery. Motor imagery tests the closed-loop BCI designed to enable real-time streaming within the required latency and jitter ranges. Therefore, the presented framework offers a promising solution for tailored neurophysiological data processing.

Flexible, stripe-patterned organic solar cells and modules based on multilayer-printed Ag fibers for smart textile applications

Rapid advancement in the fabrication technologies of stripe/fiber-shaped optoelectronic devices has driven the performance of smart textile electronics to a new height. In the development of high-performance smart textile electronics, indium tin oxide (ITO)-free flexible transparent conductive electrodes (TCEs) are particularly desirable because they offer superior flexibility and lower manufacturing cost than the brittle ITO-based counterparts. Herein, we innovatively combine spin-coating and three-dimensional direct-ink writing (three-dimensional-DIW) techniques to develop large-area (5 × 5 cm2) PEDOT:PSS/Ag-fibers hybrid TCEs (denoted as DIW-TCEs) for application in flexible organic solar cells (OSCs). Through a multilayer printing strategy, high aspect-ratio Ag-fibers are successfully deposited on top of the planar PEDOT:PSS film. The resulting DIW-TCEs, when fully embedded in a colorless polyimide substrate, exhibit excellent electrical conductivity (sheet resistance ∼ 4 Ω/□), superior optical transmittance, and mechanical flexibility. One-dimensional stripe-patterned OSCs (stripe-OSCs) based on DIW-TCEs achieved power conversion efficiency of 9.3% and 8.2% at an active area of 0.11 cm2 and 0.31 cm2, respectively. For real-life application, a flexible power module was constructed using eight stripe-OSCs. When attached on textile, the module successfully lit up a commercial light-emitting diode upon photocharging. The unique DIW-TCE fabricated herein can be the ITO-free alternative for the production of smart textile electronics.