Co3O4 Anode Research Articles

Nanostructure-Mediated Phase Evolution in Lithiation/Delithiation of Co3O4.

Nanostructured transition-metal oxides have been under intensive investigation for their tantalizing potential as anodes of next-generation lithium-ion batteries (LIBs). However, the exact mechanism for nanostructures to influence the LIB performance remains largely elusive. In this work, we discover the nanostructure-mediated lithiation mechanism in Co3O4 anodes using ex situ transmission electron microscopy (TEM) and X-ray diffractometry: while Co3O4 nanosheets exhibit a typical two-step conversion reaction (from Co3O4 to CoO and then to Co0), Co3O4 nanoarrays can go through a direct conversion from Co3O4 to Co0 at a high discharge rate. Such nanostructure-dependent lithiation can be rationalized by the slow lithiation kinetics intrinsic to Co3O4 nanoarrays, which at a high discharge rate may cause local accumulation of lithium to initiate a one-step Co3O4-to-Co0 conversion. Combined with the larger volume change observed in Co3O4 nanoarrays, the slow lithiation kinetics can lead to inhomogeneous expansion with large stress developed at the reaction front, which can eventually cause structure failure and irreversible capacity loss, as explicitly observed by in situ TEM as well as galvanostatic discharge-charge measurement. Our observation resolves the nanostructure-dependent lithiation mechanism of Co3O4 and provides important insights into the interplay among lithiation kinetics, phase evolution, and lithium-storage performance, which can be translated into electrode design strategies for next-generation LIBs.

CNTs embedded in layered Zn-doped Co3O4 nano-architectures as an efficient hybrid anode material for SIBs

Advantageous utilization of sodium-ion batteries (SIBs) requires superior performance, enriched with cost-effective anode materials, having excellent storage capability, high conductivity, and structural stability. Hybrid structures based on inorganic metal oxides and organic nano-carbons are evolving as satisfactory electrode materials for the next-generation SIBs owing to their exceptional properties. In this study, Co2.98Zn0.02O4/CNTs hybrid is synthesized using a facile hydrothermal followed by a solvothermal route. As prepared hybrid has been utilized as an anode in a Na half cell and the results are compared with Co2.98Zn0.02O4 and bare Co3O4 anodes. Galvanostatic charge-discharge profiles revealed a high reversible capacity of 721 mAh g−1 for the electrode containing carbon nanotubes (CNTs) i.e. Co2.98Zn0.02O4/CNTs exhibiting remarkable coulombic efficiency of 99% as compared to the other two electrodes. The hybrid anode showed improved capacity retention (289 mAh g−1) after 100 cycles as computed from the cyclic test which is much higher than bare Co3O4. The rate capability test of Co2.98Zn0.02O4/CNTs showed that specific capacity retained as high as 138 mAh g−1@10 C which is an outstanding rate performance, whereas bare Co3O4 couldn’t perform even after 0.5 C. Sodium insertion/extraction is also improved for Co2.98Zn0.02O4/CNTs, as revealed by electrochemical impedance and diffusion coefficient. From these findings, it is inferred that carbon-based Zn-doped Co3O4 hybrid electrode materials can be a superior combination for high-performance and fast charging future SIBs.

Electrochemical Performance of Co3O4 Anode Material with Conductive Binder

A water-soluble conductive binder consisting of poly-3,4-ethylenedioxythiophene:polysterne sulfonate and carboxymethyl cellulose was proposed for conversion Co3O4 anode material. This type of electrode shows ultrahigh specific capacity value and brilliant C-rate capability in comparison with Co3O4 electrode with poly(acrylic acid) and carboxymethyl cellulose was used. It also demonstrates better stability during continuous cycling at 0.2 C. Long-term cycling voltammetry measurements show that using of conducting polymer as binder component lead to superior stability of the Co3O4 electrodes.

Highly efficient Co3O4/CeO2 heterostructure as anode for lithium-ion batteries

Co3O4 has been extensively studied as an anode material for lithium-ion batteries (LIBs) because of its high theoretical capacity. However, during the charging-discharging processes, the issues of large volume change and low electric conductivity arise, which significantly limit the practical applications of Co3O4. To solve these issues, a Co3O4/CeO2 heterostructure derived from metal-organic frameworks (MOFs) was designed and synthesized through one-step microwave synthesis. Benefiting from the mesoporous structure and presence of hetero-components, Co3O4/CeO2 having the molar ratio of Co/Ce = 5:1 (denoted as 5Co3O4/CeO2) exhibits high reversible capacity and excellent cycling stability when used as an anode material for LIBs. Specifically, compared to a single-phase Co3O4 anode, which shows a capacity of 538.6 mAh/g after 100 cycles, 5Co3O4/CeO2 exhibits a higher capacity (1131.2 mAh/g at 100 mA/g). This study provides a novel strategy for using rare earth components to modify electrode materials.

Carbon coated porous Co3O4 polyhedrons as anode materials for highly reversible lithium-ion storage

Co3O4 is considered a promising anode candidate for lithium ion batteries (LIBs) owing to its high theoretical capacitance. However, the electrochemical properties of bare Co3O4 for LIBs remain seriously limited by poor electronic conductivity and large volume expansion. Herein, carbon-coated porous Co3O4 polyhedrons with (220) facets are fabricated through a hydrothermal method and subsequent calcination process. The size of Co3O4 polyhedrons ranges from 70 nm to 170 nm. The continuous amorphous carbon layer is approximately 3 nm thick, and uniformly covers the surface of Co3O4. Moreover, the discharge capacity of carbon-coated porous Co3O4 anode reaches 1463 and 596 mA h g−1 at 100 and 5000 mA g−1, respectively. After 150 charge discharge cycles, the carbon-coated Co3O4 anode still exhibits a reversible capacity of 840 mA h g−1 at 1000 mA g−1. Carbon nano-coating, mixed conductive matrix, and crystalline texture design can enhance the electrochemical performance of Co3O4.

Enhanced electrochemical properties of Co3O4 anode with PEDOT:PSS/CMC binder for lithium-ion batteries

A superior electrochemical performance of Co3O4 anode with water-soluble binder consisting of a combination of intrinsically conducting polymer poly-3,4-ethylenedioxythiophene:polystyrene sulfonate (PEDOT:PSS) dispersion and carboxymethyl cellulose (CMC) is presented. This type of electrode material shows ultrahigh capacity value of 1200 mA·h·g−1. It also demonstrates an excellent stability during continuous cycling at 0.2 C (capacity loss is near 4–5%) and has no significant capacity fading at high current densities. Cyclic voltammetry measurements show that Co3O4-electrode containing conducting polymer has smaller changes in shape of the curves than in the case of anode material where polyvinylidene fluoride (PVDF) binder was used.

Poplar branch bio-template synthesis of mesoporous hollow Co3O4 hierarchical architecture as an anode for long-life lithium ion batteries

Mesoporous hollow hierarchical structures play an important role in enhancing the lithium storage performances of Co3O4 anode materials. In this work, Co3O4 with mesoporous hollow structure has been successfully fabricated by simple impregnation and subsequently air calcination using poplar branch as bio-template. The product calcined at 600 °C (PB-Co600) perfectly duplicates the 3D aligned microchannels structure of poplar branch. Importantly, the wall of aligned microchannels in PB-Co600 is constructed by a lot of irregular cross-linked Co3O4 nanoparticles and there are abundant mesopores on the surface. As an anode, it exhibits high reversible capacity and remarkable long-cycle stability. At 0.1 A g-1, it can deliver a high specific capacity of 1153.7 mA h g-1 after 100 cycles, and even at 1 A g-1, the reversible specific capacity of 555.7 mA h g-1 can be retained after cycling 1000 times. The excellent lithium storage performance of PB-Co600 may be attributed to its unique hierarchical structure, which is not only favorable to the rapid transfer of substances and Li+ ion diffusion, but also alleviates the volume change during the charge/discharge cycle. Furthermore, the existence of oxygen vacancies and pseudo-capacitance also contributes significantly to the superior lithium storage performance of the PB-Co600 electrode. Therefore, the PB-Co600 prepared by a large-scale and eco-friendly route can be used as a potential candidate anode for LIBs.

Lithium and potassium storage behavior comparison for porous nanoflaked Co3O4 anode in lithium-ion and potassium-ion batteries

Rising cost has generated extended interest from lithium-ion (LIBs) to potassium-ion batteries (PIBs). Here, attempts are concentrated on comparative study on electrochemical Li and K storage behavior features for porous nanoflaked (PNF) Co3O4 anode in LIBs and PIBs. PNF–Co3O4 is synthesized by a facile solution-combustion route and its growth-mechanism is proposed as “bubble-gum fracturing effect”. Such PNF–Co3O4 presents both encouraging Li and K storage reactivity. But considering larger-sized K+, it presents a slightly lower reversible capacity (417 mAh g−1) and obviously higher charge-transfer-resistance (516.8 Ω) in PIBs than LIBs (743.9 mAh g−1, 46.0 Ω), implying moderate K+ electrode-kinetics. However, this capacity in PIBs is better than most explored carbon/alloy-based PIBs-anodes. Additionally, first, the substantially lower (nearly 1 V difference) discharge-plateau in PIBs than LIBs indicates a higher operating-voltage full-cell for PIBs than LIBs; Second, this discharge-plateau (0.3 V vs. K+/K) in PIBs slightly higher than potassium-plating-potential could potentially alleviate partial dendrite-formation. Also, enhanced performance for PNF–Co3O4 compared with bulk-Co3O4 confirms marked benefits of PNF-structure in both LIBs and PIBs on shortening Li+/K+ diffusion-distance and enduring volume-swelling. These findings demonstrate extended advantages from LIBs to PIBs for nanostructured Co3O4 and offer a better understanding of its Li and K storage behavior.

Preaddition of Cations to Electrolytes for Aqueous 2.2 V High Voltage Hybrid Supercapacitor with Superlong Cycling Life and Its Energy Storage Mechanism.

Electrolyte solutions and electrode active materials, as core components of energy storage devices, have a great impact on the overall performance. Currently, supercapacitors suffer from the drawbacks of low energy density and poor cyclic stability in typical alkaline aqueous electrolytes. Herein, the ultrathin Co3O4 anode material is synthesized by a facile electrodeposition, followed by postheat treatment process. It is found that the decomposition of active materials induces reduction of energy density and specific capacitance during electrochemical testing. Therefore, a new strategy of preadding Co2+ cations to achieve the dissolution equilibrium of cobalt in active materials is proposed, which can improve the cyclic lifetime of electrode materials and broaden the operation window of electrochemical devices. Co2+ and Li+ embedded in carbon electrode during charging can enhance H+ desorption energy barrier, further hampering the critical step of bulk water electrolysis. More importantly, the highly reversible chemical conversion mechanism between Co3O4 and protons is demonstrated to be the fact that a large amount of quantum dots and second-order flaky CoO layers were in situ formed in the electrochemical reaction process, which is first discovered and reported in neutral solutions. The as-assembled device achieves a high operation voltage (2.2 V), excellent cycling stability (capacitance retention of 168% after 10 000 cycles) and ultrahigh energy density (99 W h kg-1 at a power density of 1100 W kg-1). The as-prepared electrolytes and highly active electrode materials will open up new opportunities for aqueous supercapacitors with high safety, high voltage, high energy density, and long-lifespan.

Unique Double Carbon Protection Structured Co<sub>3</sub>O<sub>4</sub> Anode for Lithium Ion Battery

In this study, novel Carbon aerogel (CA)/Co3O4/Carbon (C) composites with a double protective structure are synthesized through a solvothermal method and in-situ polymerization. The morphology and structure are characterized by X-ray diffraction, scanning electron microscopy (SEM), high-resolution transmission electron microscopy (HRTEM), and Fourier transform infrared spectroscopy (FTIR). The loading content of active anode material Co3O4 in the composite is investigated by thermogravimetry, and the electrochemical properties of the composite are characterized by electrochemical impedance spectroscopy (EIS). The SEM results show that the nano-sized spherical Co3O4 particle is adhered to the inner Carbon aerogel (CA). The HRTEM result indicates the thickness of the prepared Carbon (C) up to 40 nm. Nano-sheet is coated on the surface of the Co3O4 particle. Compared with the pure Co3O4 anode materials, the Carbon aerogel (CA)/Co3O4/Carbon (C) composites have better transport kinetics for both electron and lithium-ion in EIS testing results, which may contribute to its higher specific capacity and higher first coulomb efficiency. Due to the unique structure of the composite material with double protection against the volume expansion of Co3O4 when charged, the Carbon aerogel (CA)/Co3O4/Carbon (C) composite material exhibits better cycle stability with a discharge capacity of 1180 mAh/g after 50 cycles. Therefore, the double protection strategy is verified as an effective method to improve the electrochemical performance of transition metal oxide with carbon composite as an anode material in lithium battery.

Microstructures and electrochemical properties of Co3O4 anodes coated by silane coupling agents

The surface of a Co3O4 anode for lithium ion batteries (LIBs) was treated by a facile solid-state method using a silane coupling agent. Characterization by X-ray diffraction (XRD), scanning electron microscopy (SEM), energy-dispersive X-ray spectroscopy (EDS) mapping, and transmission electron microscopy (TEM) indicate that amorphous SiO2 with an average thickness of 5–8 nm was uniformly coated on the surfaces of Co3O4 particles. The SiO2 coating did not induce any change in the crystal lattice and morphology, but reduced the crystallite size of Co3O4 slightly. Electrochemical tests demonstrate that the electrochemical performances of the Co3O4 anode were significantly improved by coating with 2 wt% SiO2. Specifically, when coated with 2 wt% SiO2 using a silane coupling agent, the charge capacity of pure Co3O4 under a constant current density of 50 mA g−1 was increased to 169.54 and 183.09 mA h g−1 at room temperature (RT) and 55 °C, respectively, and improved by 1.99 and 2.68 times under a high current density of 800 mA g−1 at RT and 55 °C respectively. Furthermore, the charge capacity of coated Co3O4 was 1.35 times higher than that of the untreated material after 50 cycles at 55 °C. Cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS) tests showed that the improved performance is mainly due to the unique coating layer of amorphous SiO2 on the surface, which effectively reduces the direct contact between the anode material and the electrolyte and suppresses the side reactions between Co3O4 and the electrolyte.

Oxygen-defective Co3O4 for pseudo-capacitive lithium storage

Transition metal oxide is widely studied type of high-capacity anode material for lithium ion batteries. Herein, oxygen-defective cobalt oxide with attractive lithium storage performance is prepared via a two-step strategy. Experimental results shows that there is certain amount of oxygen vacancies in Co3O4. Reversible conversion between metallic Co and CoO during the charge-discharge process was revealed by ex-situ XRD. Reversible morphology evolution is also confirmed by the ex-situ FE-SEM. The oxygen-defective Co3O4 anode shows attractive stability and rate performance. It possesses a discharge capacity of 1006 mAh∙g−1 in the first cycle, with a high initial Coulombic efficiency of 73.9%. A reversible capacity of 896 mAh∙g−1 can be maintained after 200 cycles at 250 mA g−1. It could even stably operate at an elevated current density of 5000 mA g−1 for 500 times. Further kinetic analysis reveals that pseudo-capacitance plays a dominant role in the lithium storage of oxygen-defective Co3O4. Existence of oxygen vacancies could not only facilitate Li+ migration but also enhance electric conductivity to a certain extent, resulting in improved lithium storage performance.

Aggregation-Morphology-Dependent Electrochemical Performance of Co3O4 Anode Materials for Lithium-Ion Batteries.

The aggregation morphology of anode materials plays a vital role in achieving high performance lithium-ion batteries. Herein, Co3O4 anode materials with different aggregation morphologies were successfully prepared by modulating the morphology of precursors with different cobalt sources by the mild coprecipitation method. The fabricated Co3O4 can be flower-like, spherical, irregular, and urchin-like. Detailed investigation on the electrochemical performance demonstrated that flower-like Co3O4 consisting of nanorods exhibited superior performance. The reversible capacity maintained 910.7 mAh·g−1 at 500 mA·g−1 and 717 mAh·g−1 at 1000 mA·g−1 after 500 cycles. The cyclic stability was greatly enhanced, with a capacity retention rate of 92.7% at 500 mA·g−1 and 78.27% at 1000 mA·g−1 after 500 cycles. Electrochemical performance in long-term storage and high temperature conditions was still excellent. The unique aggregation morphology of flower-like Co3O4 yielded a reduction of charge-transfer resistance and stabilization of electrode structure compared with other aggregation morphologies.

Recycling LiCoO2 with methanesulfonic acid for regeneration of lithium-ion battery electrode materials

With the massive consumption of lithium-ion batteries in portable consumer electronics and electric vehicles, proper disposal of spent batteries is of paramount importance for sustainable development. In this study, biodegradable organic methanesulfonic acid (MSA) is investigated for the first time to leach valuable metals from waste LiCoO2 powders for battery material regeneration. Under the optimal conditions, leaching efficiencies of lithium and cobalt are achieved at nearly ∼100% and ∼100%, respectively. Comparison experiment indicates that MSA can achieve better leaching performance than previously reported organic acids (e.g. citric acid, malonic acid, succinic acid, oxalic acid) under the same conditions. Besides, strong leaching capability of MSA at high solid-to-liquid ratios (e.g. 81.2 g L−1 and 163 g L−1) is confirmed with satisfactory leaching efficiencies (ca. 92.4%–100%). Feasibility test of MSA utilization for proper treatment of spent batteries is demonstrated at the optimized conditions. Importantly, regeneration study suggests that the as-obtained leachate can be employed to synthesize Co3O4 anode and LiCoO2 cathode materials with micro/nanostructures. Excellent cycling performance and rate capability of the regenerated electrode materials are demonstrated in the repeated charge-discharge cycles. Overall, the proposed recycling strategy is of great significance for rational resource utilization of spent lithium-ion batteries.

Tuning lithium storage properties of cubic Co3O4 crystallites: The effect of oxygen vacancies

Transition metal oxides show unique physical and chemical properties, and thus have a wide range of applications, including the electrodes for batteries, supercapacitors, and catalysts. However, poor electrical conductivity of the metal oxides hinder the above applications. In this work, we report a facile method to generate oxygen vacancies in cubic Co3O4 particles by thermal annealing in Ar atmosphere. By carefully controlling annealing condition, the oxygen vacancies can be well modulated while the formation of any other phases is avoided. The microstructure and chemical composition of the Co3O4 particles are studied by different methods. Lithium storage measurements show that the Co3O4 anodes with optimized oxygen vacancies (Co3O4-250) show a specific capacity of 904.2 mAhg−1 at a current density of 0.1 Ag−1, and charge/discharge rate capability of 530.5 mAhg−1 at 5.0 Ag−1. Well controlled oxygen vacancies together with sub-micrometer scale morphology in the annealed Co3O4 electrodes are responsible for the enhanced lithium storage properties. The current oxygen vacancy modulation strategy can also be used for other energy related applications, such as sodium ion batteries and electrocatalysts, with improved performance.

Electrochemical oxidation and advanced oxidation processes using a 3D hexagonal Co3O4 array anode for 4-nitrophenol decomposition coupled with simultaneous CO2 conversion to liquid fuels via a flower-like CuO cathode

A novel electrocatalytic system was developed to realize one-pot conversion of organic pollutants into liquid fuels such as methanol (CH3OH) and ethanol (C2H5OH). The process combines the catalytic oxidation of organic pollutants with electrocatalytic reduction of CO2. We first coupled the electrocatalytic process with SO4•−-based advanced oxidation processes (AOPs) for the degradation of 4-nitrophenol (4-NP) using a 3D-hexagonal Co3O4 anode. In this step, 4-NP was mineralized to CO2, and then the CO2 was converted to CH3OH and C2H5OH by electrocatalytic reduction using a flower-like CuO cathode. The experimental results show the destruction of 4-NP (60 mL, 10 mg/L) can be as high as 99%. In addition, the yields of CH3OH and C2H5OH were 98.29 μmol/L and 40.95 μmol/L, respectively, which represents a conversion of 41.8% of 4-NP into liquid fuels; the electron efficiency was 73.1%. In addition, we found that 3D-hexagonal arrays of Co3O4 with different morphologies can be obtained by adding different amounts of urea. We also investigated the formation mechanism of novel 3D-hexagonal Co3O4 arrays for the first time. A mechanism was proposed to explain the electrocatalytic steps involved in the conversion of 4-NP to CH3OH and C2H5OH and the synergetic effects between AOPs and electrocatalysis.

Synthesis of Co3O4/nitrogen-doped carbon composite from metal-organic framework as anode for Li-ion battery

In order to overcome the disadvantages of low electrical conductivity and pulverization of Co3O4 anode material, a novel Co3O4/nitrogen-doped carbon composite (Co3O4/N-C) was prepared by annealing a cobalt-based metal-organic framework (MOF) precursor. In this Co3O4/N-C composite, the Co3O4 particles are dispersed uniformly in the matrix of the nitrogen-doped carbon with an average diameter of approximately 10 nm and a mass content of 22.6%. This approach has the advantages that first, the dispersed Co3O4 nanoparticles could increase the lithium ions storage capacity and alleviate the electrode pulverization during the lithium ions insertion/extraction processes; second, the nitrogen-doped carbon material could increase the electrical conductivity of the electrode material and meanwhile serve as a buffer to relieve the structure collapse induced by the large volume change. The as-prepared Co3O4/N-C composite maintains a high reversible discharge capacity of 423 mAhg−1 after 100 cycles at the current density of 100 mAg−1, which is 129% times higher than that of the contrastive nitrogen-doped carbon material. Moreover, this strategy was verified to be effective to produce other transition metal oxides/carbon composite for improving the performance of LIBs.

Electrochemical Oxidation and Advanced Oxidation Processes Using 3D Hexagonal Co3O4 Arrays Anode for 4-Nitrophenol Decomposition Coupled with Simultaneous CO2 Conversion to Liquid Fuels Via Flower-like CuO Cathode

A novel electrocatalytic system was developed to realize one-pot conversion of organic pollutants into liquid fuels, such as methanol (CH3OH) and ethanol (C2H5OH). The process combines the catalytic oxidation of organic pollutants with electrocatalytic reduction of CO2. We first coupled the electrocatalytic process with SO4 •− based advanced oxidation processes (AOPs) for the degradation of 4-Nitrophenol (4-NP) using a 3D-hexagonal Co3O4 anode. In this step, 4-NP was mineralized to CO2 and then the CO2 was converted into CH3OH and C2H5OH by electrocatalytic reduction using a flower-like CuO cathode. Experimental results show the destruction of 4-NP (60 mL, 10 mg/L) can be as high as 99 %. And the yield of CH3OH and C2H5OH was 98.29 μmol L− 1 and 40.95 μmol L− 1, respectively, which represents a conversion of 41.8 % of 4-NP into liquid fuels and the electron efficiency was 73.1%. In addition, we found that 3D-hexagonal arrays of Co3O4 with different morphologies can be obtained by adding different amounts of urea. Also, we investigated the formation mechanism of the novel 3D-hexagonal Co3O4 arrays for the first time. A mechanism was proposed to explain the electrocatalytic steps involved in the conversion of 4-NP to CH3OH and C2H5OH and the synergetic effects between AOPs and electrocatalysis. Figure 1

Rate-dependent electrochemical reaction mechanism of spinel metal oxide anode studied by in situ TEM

Spinel Co3O4, as conversion-type transitional metal oxide, has attracted extensive interest for LIBs anode due to its high theoretical capacity. The application of transitional metal oxide including Co3O4 anode has been proved challenging due to voltage hysteresis, bad rate capability, extremely low initial Coulombic efficiency (typically 65∼70%), and volume change induced mechanical failure. Among the facing problems, the fundamental understanding of severe capacity fading at high C-rate is clearly needed to be unveiled. In this paper, we utilized in situ transmission electron microscopy (TEM) to study the electrochemical reaction process of spinel Co3O4 anode and firstly unveiled the rate-dependent morphological and structural evolution process. It has been demonstrated that the structural evolution from pristine Co3O4 phase to the formation of Co/Li2O composites during lithiation (bias = −3 V). Impressively, the Co/Li2O composites could fully delithiated into pure tightly-contacted CoO crystals (∼1.45 nm) at lower delithiated bias (+3 V); while the lithiated products partially transformed into the CoO crystals, and further suffered a severe aggregation (∼6 nm) at higher delithiated bias (+8 V). These findings advance the understanding of the mechanism of capacity fading at high current density (C-rate) in conversion-type spinel Co3O4 anode for lithium ion batteries.

Embedding Co3O4 nanoparticles into graphene nanoscrolls as anode for lithium ion batteries with superior capacity and outstanding cycling stability

Co3O4 is a promising high-performance anode for lithium ion batteries (LIBs), but suffers from unsatisfied cyclability originating duo to low electrical conductivity and large volume expansion during charge and discharge process. Herein, we successfully constructed the Co3O4 nanoparticles embedded into graphene nanoscrolls (GNSs) as advanced anode for high-performance LIBs with large capacity and exceptional cyclability. The one-dimensional (1D) Co3O4/GNSs were synthesized via liquid nitrogen cold quenching of large-size graphene oxide nanosheets and sodium citrate (SC) modified Co3O4 nanoparticles, followed by freeze drying and annealing at 400 °C for 2 h in nitrogen atmosphere. Benefiting from the interconnected porous network constructed by 1D Co3O4/GNSs for fast electron transfer and rapid ion diffusion, and wrinkled graphene shell for significantly alleviating the huge volume expansion of Co3O4 during lithiation and delithiation. The resultant Co3O4/GNSs exhibited ultrahigh reversible capacity of 1200 mAh g−1 at 0.1 C, outperforming most reported Co3O4 anodes. Moreover, they showed high rate capability of 600 mAh g−1 at 5 C, and outstanding cycling stability with a high capacity retention of 90% after 500 cycles. Therefore, this developed strategy could be extended as an universal and scalable approach for intergrating various metal oxide materials into GNSs for energy storage and conversion applications.