Tensile Strain-Mediated Spinel Ferrites Enable Superior Oxygen Evolution Activity.

Exploring efficient strategies to overcome the performance constraints of oxygen evolution reaction (OER) electrocatalysts is vital for electrocatalytic applications such as H2O splitting, CO2 reduction, N2 reduction, etc. Herein, tunable, wide-range strain engineering of spinel oxides, such as NiFe2O4, is proposed to enhance the OER activity. The lattice strain is regulated by interfacial thermal mismatch during the bonding process between thermally expanding NiFe2O4 nanoparticles and the nonexpanding carbon fiber substrate. The tensile lattice strain causes energy bands to flatten near the Fermi level, lowering eg orbital occupancy, effectively increasing the number of electronic states near the Fermi level, and reducing the pseudoenergy gap. Consequently, the energy barrier of the rate-determining step for strained NiFe2O4 is reduced, achieving a low overpotential of 180 mV at 10 mA/cm2. A total water decomposition voltage range of 1.52-1.56 V at 10 mA/cm2 (without iR correction) was achieved in an asymmetric alkaline electrolytic cell with strained NiFe2O4 nanoparticles, and its robust stability was verified with a voltage retention of approximately 99.4% after 100 h. Furthermore, the current work demonstrates the universality of tuning OER performance with other spinel ferrite systems, including cobalt, manganese, and zinc ferrites.

Covalently Interlayer-Confined Organic-Inorganic Heterostructures for Aqueous Potassium Ion Supercapacitors.

Artificial assembly of organic-inorganic heterostructures for electrochemical energy storage at the molecular level is promising, but remains a great challenge. Here, a covalently interlayer-confined organic (polyaniline [PANI])-inorganic (MoS2 ) hybrid with a dual charge-storage mechanism is developed for boosting the reaction kinetics of supercapacitors. Systematic characterizations reveal that PANI induces a partial phase transition from the 2H to 1T phases of MoS2 , expands the interlayer spacing of MoS2 , and increases the hydrophilicity. More in-depth insights from the synchrotron radiation-based X-ray technique illustrate that the covalent grafting of PANI to MoS2  induces the formation of MoN bonds and unsaturated Mo sites, leading to increased active sites. Theoretical analysis reveals that the covalent assembly facilitates cross-layer electron transfer and decreases the diffusion barrier of K+ ions, which favors reaction kinetics. The resultant hybrid material exhibits high specific capacitance and good rate capability. This design provides an effective strategy to develop organic-inorganic heterostructures for superior K-ion storage. The K-ion storage mechanism concerning the reversible insertion/extraction upon charge/discharge is revealed through ex situ X-ray photoelectron spectroscopy.

Electronic and Structural Engineering of Atomically Dispersed Isolated Single-Atom and Alloy Architectures.

Precise configurations of isolated metal atoms in nitrogen-doped carbon materials with 2D single or multilayers and 3D nanoarchitectures are gaining attention owing to their good stability and activity at high current densities. Atomic metal-Nx moieties, which utilize maximum atoms to attain high intrinsic activity and novel electronic architecture of support materials, facilitate strong interaction between the central metal atom and support matrix. However, resource consumption is considerably high due to the inferior atomic utilization of active sites. Therefore, energy-efficient electrochemical processes are needed to develop advanced isolated single-atom architecture, which would provide high atom-utilization and good durability. Herein, the concepts of atomically dispersed metal sites in single-atom and alloy architectures and their electronic features associated with structural evolution are discussed. Opportunities and challenges associated with the use of isolated single-atoms in 2D materials are discussed based on their unique electronic defects, low-valence central metals, mechanical flexibility, and maximum access to metal sites. This insightful revisit into the engineering of single-atom and alloy architectures would provide a profound understanding of electronic modulations and regulation of geometric characteristics, and unravels potential directions for electrochemical energy conversion, charge storage, and sensing processes.

Emerging Pristine MOF-Based Heterostructured Nanoarchitectures: Advances in Structure Evolution, Controlled Synthesis, and Future Perspectives.

Metal-organic frameworks (MOFs) can be customized through modular assembly to achieve a wide range of potential applications, based on their desired functionality. However, most of the initially reported MOFs are limited to microporous systems and are not sufficiently stable, which restricts their popularization. Heterogeneity is introduced into a simple MOF framework to create MOF-based heterostructures with fascinating properties and interesting functions. Heterogeneity can be introduced into the MOFs via postsynthetic/ligand exchange. Although the ligand exchange has shown potential, it is difficult to precisely control the degree of exchange or position. Among the various synthesis strategies, hierarchical assembly is particularly attractive for constructing MOF-based heterostructures, as it can achieve precise regulation of MOF-based heterostructured nanostructures. The hierarchical assembly significantly expands the compositional diversity of MOF-based heterostructures, which has high elasticity for lattice matching during the epitaxial growth of MOFs. This review focuses on the synthetic evolution mechanism of hierarchical assemblies of MOF-based nanoarchitectures. Subsequently, the precise control of pore structure, pore size, and morphology of MOF-based nanoarchitectures by hierarchical assembly is emphasized. Finally, possible solutions to address the challenges associated with heterogeneous interfaces are presented, and potential opportunities for innovative applications are proposed.

Stabilizing Zn Metal Anode Through Regulation of Zn Ion Transfer and Interfacial Behavior with a Fast Ion Conductor Protective Layer.

Aqueous Zn-ion batteries (AZIBs) attract intensive attention owing to their environmental friendliness, cost-effectiveness, innate safety, and high specific capacity. However, the practical applications of AZIBs are hindered by several adverse phenomena, including corrosion, Zn dendrites, and hydrogen evolution. Herein, a Zn anode decorated with a 3D porous-structured Na3 V2 (PO4)3 (NVP@Zn) is obtained, where the NVP reconstruct the electrolyte/anode interface. The resulting NVP@Zn anode can provide a large quantity of fast and stable channels, facilitating enhanced Zn ion deposition kinetics and regulating the Zn ions transport process through the ion confinement effect. The NASICON-type NVP protective layer promote the desolvation process due to its nanopore structure, thus effectively avoiding side reactions. Theoretical calculations indicate that the NVP@Zn electrode has a higher Zn ion binding energy and a higher migration barrier, which demonstrates that NVP protective layer can enhance Zn ion deposition kinetics and prevent the unfettered 2D diffusion of Zn ions. Therefore, the results show that NVP@Zn/MnO2 full cell can maintain a high specific discharge capacity of 168 mAh g-1 and a high-capacity retention rate of 74.6% after cycling. The extraordinary results obtained with this strategy have confirmed the promising applications of NVP in high-performance AZIBs.

Reconfiguring the Electronic Structure of Heteroatom Doped Carbon Supported Bimetallic Oxide@Metal Sulfide Core-Shell Heterostructure via In Situ Nb Incorporation toward Extrinsic Pseudocapacitor.

High-energy-density battery-type materials have sparked considerable interest as supercapacitors electrode; however, their sluggish charge kinetics limits utilization of redox-active sites, resulting in poor electrochemical performance. Here, the unique core-shell architecture of metal organic framework derived N-S codoped carbon@Cox Sy micropetals decorated with Nb-incorporated cobalt molybdate nanosheets (Nb-CMO4 @Cx Sy NC) is demonstrated. Coordination bonding across interfaces and π-π stacking interactions between CMO4 @Cx Sy and N and, S-C can prevent volume expansion during cycling. Density functional theory analysis reveals that the excellent interlayer and the interparticle conductivity imparted by Nb doping in heteroatoms synergistically alter the electronic states and offer more accessible species, leading to increased electrical conductivity with lower band gaps. Consequently, the optimized electrode has a high specific capacity of 276.3 mAh g-1 at 1 A g-1 and retains 98.7% of its capacity after 10 000 charge-discharge cycles. A flexible quasi-solid-state SC with a layer-by-layer deposited reduced graphene oxide /Ti3 C2 TX anode achieves a specific energy of 75.5 Wh kg-1 (volumetric energy of 1.58 mWh cm-3 ) at a specific power of 1.875 kWh kg-1 with 96.2% capacity retention over 10 000 charge-discharge cycles.

Electronic Structure Engineered Heteroatom Doped All Transition Metal Sulfide Carbon Confined Heterostructure for Extrinsic Pseudocapacitor.

Ultra-high energy density battery-type materials are promising candidates for supercapacitors (SCs); however, slow ion kinetics and significant volume expansion remain major barriers to their practical applications. To address these issues, hierarchical lattice distorted α-/γ-MnS@Cox Sy core-shell heterostructure constrained in the sulphur (S), nitrogen (N) co-doped carbon (C) metal-organic frameworks (MOFs) derived nanosheets (α-/γ-MnS@Cox Sy @N, SC) have been developed. The coordination bonding among Cox Sy , and α-/γ-MnS nanoparticles at the interfaces and the π-π stacking interactions developed across α-/γ-MnS@Cox Sy and N, SC restrict volume expansion during cycling. Furthermore, the porous lattice distorted heteroatom-enriched nanosheets contain a sufficient number of active sites to allow for efficient electron transportation. Density functional theory (DFT) confirms the significant change in electronic states caused by heteroatom doping and the formation of core-shell structures, which provide more accessible species with excellent interlayer and interparticle conductivity, resulting in increased electrical conductivity. . The α-/γ-MnS@Cox Sy @N, SC electrode exhibits an excellent specific capacity of 277 mA hg-1 and cycling stability over 23 600 cycles. A quasi-solid-state flexible extrinsic pseudocapacitor (QFEPs) assembled using layer-by-layer deposited multi-walled carbon nanotube/Ti3 C2 TX nanocomposite negative electrode. QFEPs deliver specific energy of 64.8 Wh kg-1 (1.62 mWh cm-3 ) at a power of 933 W kg-1 and 92% capacitance retention over 5000 cycles.

Zinc-Bismuth Binary Alloy Enabling High-Performance Aqueous Zinc Ion Batteries.

Reconfiguration of zinc anodes efficiently mitigates dendrite formation and undesirable side reactions, thus favoring the long-term cycling performance of aqueous zinc ion batteries (AZIBs). This study synthesizes a Zn@Bi alloy anode (Zn@Bi) using the fusion method, and find that the anode surfaces synthesized using this method have an extremely high percentage of Zn(002) crystalline surfaces. Experimental results indicate that the addition of bismuth inhibits the hydrogen evolution reaction and corrosion of zinc anodes. The finite-element simulation results indicate that Zn@Bi can effectively achieve a uniform anodic electric field, thereby regulating the homogeneous depositions of zinc ions and reducing the production of Zn dendrite. Theoretical calculations reveal that the incorporation of Bi favors the anode structure stabilization and higher adsorption energy of Zn@Bi corresponds to better Zn deposition kinetics. The Zn@Bi//Zn@Bi symmetric cell demonstrates an extended cycle life of 1000 h. Furthermore, when pairing Zn@Bi with an α-MnO2 cathode to construct a Zn@Bi//MnO2 cell, a specific capacity of 119.3 mAh g-1 is maintained even after 1700 cycles at 1.2 A g-1 . This study sheds light on the development of dendrite-free anodes for advanced AZIBs.

Realizing Superior Redox Kinetics of Hollow Bimetallic Sulfide Nanoarchitectures by Defect-Induced Manipulation toward Flexible Solid-State Supercapacitors.

As a typical battery-type material, CuCo2 S4 is a promising candidate for supercapacitors due to the high theoretical specific capacity. However, its practical application is plagued by inherently sluggish ion diffusion kinetics and inferior electrical transport properties. Herein, sulfur vacancies are incorporated in CuCo2 S4 hollow nanoarchitectures (HNs) to accelerate redox reactivity. Experimental analyses and theoretical investigations uncover that the generated sulfur vacancies increase the active electron states, reduce the adsorption barriers of electrolyte ions, and enrich reactive redox species, thus achieving enhanced electrochemical performance. Consequently, the deficient CuCo2 S4 with optimized vacancy concentration presents a high specific capacity of 231 mAh g-1 at 1 A g-1 , a ≈1.78 times increase compared to that of pristine CuCo2 S4 , and exhibits a superior rate capability (73.8% capacity retention at 20 A g-1 ). Furthermore, flexible solid-state asymmetric supercapacitor devices assembled with the deficient CuCo2 S4 HNs and VN nanosheets deliver a high energy density of 61.4 W h kg-1 at 750 W kg-1 . Under different bending states, the devices display exceptional mechanical flexibility with no obvious change in CV curves at 50 mV s-1 . These findings provide insights for regulating electrode reactivity of battery-type materials through intentional nanoarchitectonics and vacancy engineering.

A reversible and stable doping technique to invert the carrier polarity of MoTe2.

Two-dimensional (2D) materials can be implemented in several functional devices for future optoelectronics and electronics applications. Remarkably, recent research on p-n diodes by stacking 2D materials in heterostructures or homostructures (out of plane) has been carried out extensively with novel designs that are impossible with conventional bulk semiconductor materials. However, the insight of a lateral p-n diode through a single nanoflake based on 2D material needs attention to facilitate the miniaturization of device architectures with efficient performance. Here, we have established a physical carrier-type inversion technique to invert the polarity of MoTe2-based field-effect transistors (FETs) with deep ultraviolet (DUV) doping in (oxygen) O2and (nitrogen) N2gas environments. A p-type MoTe2nanoflake transformed its polarity to n-type when irradiated under DUV illumination in an N2gaseous atmosphere, and it returned to its original state once irradiated in an O2gaseous environment. Further, Kelvin probe force microscopy (KPFM) measurements were employed to support our findings, where the value of the work function changed from ∼4.8 and ∼4.5 eV when p-type MoTe2inverted to the n-type, respectively. Also, using this approach, an in-plane homogeneous p-n junction was formed and achieved a diode rectifying ratio (If/Ir) up to ∼3.8 × 104. This effective approach for carrier-type inversion may play an important role in the advancement of functional devices.

Phosphorus Regulated Cobalt Oxide@Nitrogen-Doped Carbon Nanowires for Flexible Quasi-Solid-State Supercapacitors.

Battery-type materials are promising candidates for achieving high specific capacity for supercapacitors. However, their slow reaction kinetics hinders the improvement in electrochemical performance. Herein, a hybrid structure of P-doped Co3 O4 (P-Co3 O4 ) ultrafine nanoparticles in situ encapsulated into P, N co-doped carbon (P, N-C) nanowires by a pyrolysis-oxidation-phosphorization of 1D metal-organic frameworks derived from Co-layered double hydroxide as self-template and reactant is reported. This hybrid structure prevents active material agglomeration and maintains a 1D oriented arrangement, which exhibits a large accessible surface area and hierarchically porous feature, enabling sufficient permeation and transfer of electrolyte ions. Theoretical calculations demonstrate that the P dopants in P-Co3 O4 @P, N-C could reduce the adsorption energy of OH- and regulate the electrical properties. Accordingly, the P-Co3 O4 @P, N-C delivers a high specific capacity of 669 mC cm-2 at 1 mA cm-2 and an ultralong cycle life with only 4.8% loss over 5000 cycles at 30 mA cm-2 . During the fabrication of P-Co3 O4 @P, N-C, Co@P, N-C is simultaneously developed, which can be integrated with P-Co3 O4 @P, N-C for the assembly of asymmetric supercapacitors. These devices achieve a high energy density of 47.6 W h kg-1 at 750 W kg-1 and impressive flexibility, exhibiting a great potential in practical applications.

Phosphorus-Mediated MoS2 Nanowires as a High-Performance Electrode Material for Quasi-Solid-State Sodium-Ion Intercalation Supercapacitors.

Molybdenum disulfide (MoS2 ) is a promising electrode material for electrochemical energy storage owing to its high theoretical specific capacity and fascinating 2D layered structure. However, its sluggish kinetics for ionic diffusion and charge transfer limits its practical applications. Here, a promising strategy is reported for enhancing the Na+ -ion charge storage kinetics of MoS2 for supercapacitors. In this strategy, electrical conductivity is enhanced and the diffusion barrier of Na+ ion is lowered by a facile phosphorus-doping treatment. Density functional theory results reveal that the lowest energy barrier of dilute Na-vacancy diffusion on P-doped MoS2 (0.11 eV) is considerably lower than that on pure MoS2 (0.19 eV), thereby signifying a prominent rate performance at high Na intercalation stages upon P-doping. Moreover, the Na-vacancy diffusion coefficient of the P-doped MoS2 at room temperatures can be enhanced substantially by approximately two orders of magnitude (10-6 -10-4 cm2 s-1 ) compared with pure MoS2 . Finally, the quasi-solid-state asymmetrical supercapacitor assembled with P-doped MoS2 and MnO2 , as the positive and negative electrode materials, respectively, exhibits an ultrahigh energy density of 67.4 W h kg-1 at 850 W kg-1 and excellent cycling stability with 93.4% capacitance retention after 5000 cycles at 8 A g-1 .

Vertical and In-Plane Current Devices Using NbS2/n-MoS2 van der Waals Schottky Junction and Graphene Contact.

A van der Waals (vdW) Schottky junction between two-dimensional (2D) transition metal dichalcogenides (TMDs) is introduced here for both vertical and in-plane current devices: Schottky diodes and metal semiconductor field-effect transistors (MESFETs). The Schottky barrier between conducting NbS2 and semiconducting n-MoS2 appeared to be as large as ∼0.5 eV due to their work-function difference. While the Schottky diode shows an ideality factor of 1.8-4.0 with an on-to-off current ratio of 103-105, Schottky-effect MESFET displays little gate hysteresis and an ideal subthreshold swing of 60-80 mV/dec due to low-density traps at the vdW interface. All MESFETs operate with a low threshold gate voltage of -0.5 ∼ -1 V, exhibiting easy saturation. It was also found that the device mobility is significantly dependent on the condition of source/drain (S/D) contact for n-channel MoS2. The highest room temperature mobility in MESFET reaches to approximately more than 800 cm2/V s with graphene S/D contact. The NbS2/n-MoS2 MESFET with graphene was successfully integrated into an organic piezoelectric touch sensor circuit with green OLED indicator, exploiting its predictable small threshold voltage, while NbS2/n-MoS2 Schottky diodes with graphene were applied to extract doping concentrations in MoS2 channel.

Tension assisted metal transfer of graphene for Schottky diodes onto wafer scale substrates.

We developed an effective graphene transfer method for graphene/silicon Schottky diodes on a wafer as large as 6 inches. Graphene grown on a large scale substrate was passivated and sealed with a gold layer, protecting graphene from any possible contaminant and keeping good electrical contact. The Au/graphene was transferred by the tension-assisted transfer process without polymer residues. The gold film itself was used directly as the electrodes of a Schottky diode. We demonstrated wafer-scale integration of graphene/silicon Schottky diode using the proposed transfer process. The transmission electron microscopy analysis and relatively low ideality factor of the diodes indicated fewer defects on the interface than those obtained using the conventional poly(methyl methacrylate)-assisted transfer method. We further demonstrated gas sensors as an application of graphene Schottky diodes.

Phosphorus-Doped Graphene Oxide Layer as a Highly Efficient Flame Retardant.

A simple and easy process has been developed to efficiently dope phosphorus into a graphene oxide surface. Phosphorus-doped graphene oxide (PGO) is prepared by the treatment of polyphosphoric acid with phosphoric acid followed by addition of a graphene oxide solution while maintaining a pH of around 5 by addition of NaOH solution. The resulting materials are characterized by X-ray photoelectron spectroscopy (XPS), Fourier transform infrared spectroscopy (FT-IR), X-ray diffraction (XRD), Raman spectroscopy, thermogravimetric analysis (TGA), and scanning electron microscopy (SEM). The as-made PGO solution-coated cloth exhibits excellent flame retardation properties. The PGO-coated cloth emits some smoke at the beginning without catching fire for more than 120 s and maintains its initial shape with little shrinkage. In contrast, the pristine cloth catches fire within 5 s and is completely burned within 25 s, leaving trace amounts of black residue. The simple technique of direct introduction of phosphorus into the graphene oxide surface to produce phosphorus-doped oxidized carbon nanoplatelets may be a general approach towards the low-cost mass production of PGO for many practical applications, including flame retardation.

Heterometallic Electrocatalysts Derived from High-Nuclearity Metal Clusters for Efficient Overall Water Splitting.

The development of cost-effective electrocatalysts with an optimal surface affinity for intermediates is essential for sustainable hydrogen fuel production, but this remains insufficient. Here we synthesize Ni2P/MoS2-CoMo2S4@C heterometallic electrocatalysts based on the high-nuclearity cluster {Co24(TC4A)6(MoO4)8Cl6}, in which Ni2P nanoparticles were anchored to the surface of the MoS2-CoMo2S4@C nanosheets via strong interfacial interactions. Theoretical calculations revealed that the introduction of Ni2P phases induces significant disturbances in the surface electronic configuration of Ni2P/MoS2-CoMo2S4@C, resulting in more relaxed d-d orbital electron transfers between the metal atoms. Moreover, continuous electron transport was established by the formation of multiple heterojunction interfaces. The optimized Ni2P/MoS2-CoMo2S4@C electrocatalyst exhibited ultralow overpotentials of 198 and 73 mV for oxygen and hydrogen evolution reactions, respectively, in alkaline media, at 10 mA cm-2. The alkali electrolyzer constructed using Ni2P/MoS2-CoMo2S4@C required a cell voltage of only 1.45 V (10 mA cm-2) to drive overall water splitting with excellent long-term stability.

Mechanical Activation of Graphite for Na-Ion Battery Anodes: Unexpected Reversible Reaction on Solid Electrolyte Interphase via X-Ray Analysis.

Although sodium-ion batteries (SIBs) offer promising low-cost alternatives to lithium-ion batteries (LIBs), several challenges need to be overcome for their widespread adoption. A primary concern is the optimization of carbon anodes. Graphite, vital to the commercial viability of LIBs, has a limited capacity for sodium ions. Numerous alternatives to graphite are explored, particularly focusing on disordered carbons, including hard carbon. However, compared with graphite, most of these materials underperform in LIBs. Furthermore, the reaction mechanism between carbon and sodium ions remains ambiguous owing to the structural diversity of disordered carbon. A straightforward mechanical approach is introduced to enhance the sodium ion storage capacity of graphite, supported by comprehensive analytical techniques. Mechanically activated graphite delivers a notable reversible capacity of 290.5 mAh·g-1 at a current density of 10 mA·g-1. Moreover, it maintains a capacity of 157.7 mAh·g-1 even at a current density of 1 A·g-1, benefiting from the defect-rich structure achieved by mechanical activation. Soft X-ray analysis revealed that this defect-rich carbon employs a sodium-ion storage mechanism distinct from that of hard carbon. This leads to an unexpected reversible reaction on the solid electrolyte surface. These insights pave the way for innovative design approaches for carbon electrodes in SIB anodes.

Heterostructured grafting of NiFe-layered double hydroxide@TiO2 for boosting photoelectrochemical cathodic protection.

Accelerating the oxidation process at photoanode-electrolyte interfaces can prolong the lifetime of photoexcited electrons and improve the efficiency of photoelectrochemical cathodic protection (PECCP) systems without relying on hole scavengers. However, the systematic design of precisely structured heterostructures for efficient photoanodes remains challenging. Here we meticulously engineered a type-II heterostructure featuring precise spatial organization, wherein NiFe-layered double hydroxide nanosheets (NiFe-LDH NSs) were assembled onto annealed TiO2 nanorod arrays (ATNAs), demonstrating their effectiveness in achieving efficient PECCP. The interfacial electronic coupling and appropriate energy alignment between the NiFe-LDH NSs and ATNAs allowed rapid hole extraction from the ATNAs to the NiFe-LDH NSs. Furthermore, the uniform distribution of the NiFe-LDH NSs on top of ATNAs drastically reduced the overpotential of oxygen evolution reactions (OER) from 370 to 200 mV and Tafel slope from 162 to 56 mV dec-1, leading to significantly improved cathodic protection of 304 stainless steel (SS) under extended illumination and interesting post-illumination protection. In addition, with the increase of testing cycles, the as-prepared NiFe-LDH NSs@ATNAs demonstrated a progressively enhanced cathodic protection potential from 0.15 to 0.13 V vs. RHE over 50 cycles. These findings provide important guidelines for the design of future high-efficiency green metal protection through rational photoanode design.

Hierarchical Spatial Confinement Unlocking the Storage Limit of MoS2 for Flexible High-Energy Supercapacitors.

Molybdenum sulfide (MoS2) is a promising electrode material for supercapacitors; however, its limited Mo/S edge sites and intrinsic inert basal plane give rise to sluggish active electronic states, thus constraining its electrochemical performance. Here we propose a hierarchical confinement strategy to develop ethylene molecule (EG)-intercalated Co-doped sulfur-deficient MoS2 (Co-EG/SV-MoS2) for efficient and durable K-ion storage. Theoretical analyses suggest that the intercalation-confined EG and lattice-confined Co can enhance the interfacial K-ion storage capacity while reducing the K-ion diffusion barrier. Experimentally, the intercalated EG molecules with mildly reducing properties induced the creation of sulfur vacancies, expanded the interlayer spacing, regulated the 2H-1T phase transition, and strengthened the structural grafting between layers, thereby facilitating ion diffusion and ensuring structural durability. Moreover, the Co dopants occupying the initial Mo sites initiated charge transfer, thus activating the basal plane. Consequently, the optimized Co-EG/SV-MoS2 electrode exhibited a substantially improved electrochemical performance. Flexible supercapacitors assembled with Co-EG/SV-MoS2 delivered a notable areal energy density of 0.51 mW h cm-2 at 0.84 mW cm-2 with good flexibility. Furthermore, supercapacitor devices were integrated with a strain sensor to create a self-powered system capable of real-time detection of human joint motion.