Performance Improvement and Application of Degradable Poly-l-lactide and Yttrium-Doped Zinc Oxide Hybrid Films for Energy Harvesting.

Piezoelectric nanogenerators (PENGs) are booming for energy collection and wearable energy supply as one of the next generations of green energy-harvesting devices. Balancing the output, safety, degradation, and cost is the key to solving the bottleneck of PENG application. In this regard, yttrium (Y)-doped zinc oxide (ZnO) (Y-ZnO) was synthesized and embedded into polylactide (PLLA) for developing degradable piezoelectric composite films with an enhanced energy-harvesting performance. The synthesized Y-ZnO exhibits high piezoelectric properties benefiting from the stronger polarity of the Y-O bond and regulation of oxygen vacancy concentration, which improve the output performance of the composite film with Y-ZnO and PLLA (Y-Z-PLLA). The obtained open-circuit voltage (Voc), short-circuit current (Isc), and instantaneous power density of the optimized Y-Z-PLLA PENG reach 17.52 V, 2.45 µA, and 1.76 µW/cm2, respectively. The proposed PENG also shows good degradability. In addition, practical applications of the proposed PENG were demonstrated by converting biomechanical energy, such as walking, running, and jumping, into electricity.

Rational synthesis of 3D coral-like ZnCo2O4 nanoclusters with abundant oxygen vacancies for high-performance supercapacitors.

Transition metal oxides with high theoretical capacitance are regarded as desired electrode materials for supercapacitors, however, the poor conductivity and sluggish charge transfer kinetics constrain their electrochemical performance. The three-dimensional (3D) coral-like ZnCo2O4 nanomaterials with abundant oxygen vacancies were synthesized through a facile hydrothermal method and chemical reduction approach. The introduced oxygen vacancies can provide more active sites and lower the energy barrier, thereby facilitating the kinetics of surface reactions. Furthermore, the abundant oxygen vacancies in metal oxides can function as shallow donors to facilitate charge carrier diffusion, resulting in a faster ion diffusion rate and superior electrochemical conductivity. The electrochemical performance of ZnCo2O4 was optimized by the introduction of oxygen vacancies. The ZnCo2O4 nanoclusters, reduced by 0.5 M NaBH4 (ZnCo2O4-0.5), exhibit a specific capacitance of 2685.7 F g-1 at 1 A g-1, which is nearly twice that of the pristine ZnCo2O4 (1525.7 F g-1 at 1 A g-1). The ZnCo2O4-0.5 exhibits an excellent rate capacity (81.9% capacitance retention at 10 A g-1) and a long cycling stability (72.6% specific capacitance retention after 10 000 cycles at 3 A g-1). Furthermore, the asymmetric supercapacitor (ASC, ZnCo2O4-0.5 nanoclusters//active carbon) delivers a maximum energy density of 50.2 W h kg-1 at the power density of 493.7 W kg-1 and an excellent cycling stability (75.3% capacitance retention after 3000 cycles at 2 A g-1), surpassing the majority of previously reported ZnCo2O4-based supercapacitors. This work is important for revealing the pivotal role of implementing the defect engineering regulation strategy in achieving optimization of both electrochemical activity and conductivity.

Cyanuric Acid-Assisted Synthesis of Hierarchical Amorphous Carbon Nitride Assembled by Ultrathin Oxygen-Doped Nanosheets for Excellent Photocatalytic Hydrogen Generation.

Amorphous carbon nitride with typical short-range order arrangement as an effective photocatalyst is worth exploring but remains a great challenge because its disordered structure induces severe recombination of photogenerated charge carriers. Herein, for the first time, we demonstrate that a hierarchical amorphous carbon nitride (HACN) with structural oxygen incorporation can be synthesized via a cyanuric acid-assisted melem hydrothermal process, accompanied by freeze-drying and pyrolysis. The complex composed of melem and cyanuric acid exhibiting a unique 3D self-supporting skeleton and significant phase transformation is responsible for the formation of an interconnected hierarchical framework and amorphous structure for HACN. These features are beneficial to enhance its visible light harvesting by the multiple-reflection effect within the architecture consisting of more exposed porous nanosheets and introducing a long band tail absorption. The well-designed morphology, band tail state, and oxygen doping effectively inhibit rapid band-to-band recombination of the photogenerated electrons and holes and facilitate subsequent separation. Accordingly, the HACN catalyst exhibits exceptional visible light (λ > 420 nm)-driven photoreduction for hydrogen production with a rate of 82.4 µmol h-1, which is 21.7 and 9.5 times higher than those of melem-derived carbon nitride and crystalline nanotube carbon nitride counterparts, respectively, and significantly surpasses those of most reported amorphous carbon nitrides. Our controlling of rearrangement of the in situ supramolecular self-assembly of melem oligomer using cyanuric acid directly instructs the development of highly efficient amorphous photocatalysts for converting solar energy into hydrogen fuel.

Regulating Crystal Orientation in VO2 for Aqueous Zinc Batteries with Enhanced Pseudocapacitance.

Although aqueous zinc batteries have attracted extensive interest, they are limited by relatively low rate capabilities and poor cyclic stability of cathodes. The crystal orientation of the cathode is one important factor influencing electrochemical properties. However, it has rarely been investigated. Herein, VO2 cathodes with different crystal orientations are developed via tuning the number of hydroxyl groups in polyol, such as using glycerol, erythritol, xylitol, or mannitol. The polyols serve as a reductant as well as a structure-directing agent through a hydrothermal reaction. Xylitol-derived VO2 shows a (110)-orientated crystalline structure and ultrathin nanosheet morphology. Such features greatly enhance the pseudocapacitance to 76.1% at a scan rate of 1.0 mV s-1, which is significantly larger than that (61.6%) of the (001)-oriented VO2 derived from glycerol. The corresponding aqueous zinc batteries exhibit a high energy storage performance with a reversible specific capacity of 317 mAh g-1 at 0.5 A g-1, rate ability of 220 mAh g-1 at 10 A g-1, and capacity retention of 81.0% at 10 A g-1 over 2000 cycles. This work demonstrates a facile method for tailoring VO2 crystal orientations, offers an understanding of the Zn2+ storage mechanism upon different VO2 facets, and provides a novel method to develop cathode materials toward advanced aqueous zinc batteries.

Facile synthesis of morphology-controlled hybrid structure of ZnCo2O4 nanosheets and nanowires for high-performance asymmetric supercapacitors.

Controllable synthesis of electrode materials with desirable morphology and size is of significant importance and challenging for high-performance supercapacitors. Herein, we propose an efficient hydrothermal approach to controllable synthesis of hierarchical porous three-dimensional (3D) ZnCo2O4 composite films directly on Ni foam substrates. The composite films consisted of two-dimensional (2D) nanosheets array anchored with one-dimensional (1D) nanowires. The morphologies of ZnCo2O4 arrays can be easily controlled by adjusting the concentration of NH4F. The effect of NH4F in the formation of these 3D hierarchical porous ZnCo2O4 nanosheets@nanowires films is systematically investigated based on the NH4F-independent experiments. This unique 3D hierarchical structure can help enlarge the electroactive surface area, accelerate the ion and electron transfer, and accommodate structural strain. The as-prepared hierarchical porous ZnCo2O4 nanosheets@nanowires films exhibited inspiring electrochemical performance with high specific capacitance of 1289.6 and 743.2 F g-1 at the current density of 1 and 30 A g-1, respectively, and a remarkable long cycle stability with 86.8% capacity retention after 10 000 cycles at the current density of 1 A g-1. Furthermore, the assembled asymmetric supercapacitor using the as-prepared ZnCo2O4 nanosheets@nanowires films as the positive electrode and active carbon as negative electrode delivered a high energy density of 39.7 W h kg-1 at a power density of 400 W kg-1. Our results show that these unique hierarchical porous 3D ZnCo2O4 nanosheets@nanowires films are promising candidates as high-performance electrodes for energy storage applications.

Oxygen vacancies induced by lanthanum-doped indium oxide nanofibers for promoted temperature-dependent triethylamine and formaldehyde sensing.

A novel TEA and HCHO dual-function temperature-dependent sensing material (3La-In2O3) with ultra-high sensitivity was developed via a facile electrospinning process. Though rare earth doped in In2O3-based sensors have been widely reported, the low sensitivity, poor selectivity and high operating temperature remain restrict their application. Herein, the In2O3 nanofibers with different contents of La3+ ions are firstly obtained by a facile electrospinning process. The sensing performance investigation confirms that the 3% La/In molar ratio of La3+ doped in In2O3 nanofibers are more appropriate as the sensing material for TEA and HCHO detection. The 3La-In2O3 exhibits greatest response value of 3721.60-10 ppm TEA and 1469.65-10 ppm HCHO at their best working temperature (100 â„ƒ and 160 â„ƒ), approximately 23.85-fold and 10.85-fold higher than that of pristine In2O3 nanofibers. In addition, the excellent selectivity, repeatability, and long-term stability ensure the further application of the 3La-In2O3-based sensor in actual environment. The promoted sensing performance is mainly ascribed to the more oxygen vacancies, the increasing specific surface area, the smaller grain size of In2O3 nanofibers induced by La3+ doping. The DFT results demonstrate the beneficial effect of La and oxygen vacancies on the improved target gas adsorption energy.

A New Structure with Localized sp2 Bonding for Fivefold Twinning in Diamond.

Changes in atomic bonding configuration in carbon from sp3 to sp2 are known to exist in certain structural defects in diamond, such as twin boundaries, grain boundaries, and dislocations, which have a significant impact on many properties of diamond. In this work, the atomic structure of fivefold twinning in detonation synthesized ultra-dispersed diamonds is investigated using a combination of techniques, including spherical aberration-corrected high-resolution electron microscopy (HREM), HREM image simulations, and molecular mechanics (MM) calculations. The experimental HREM images reveal clearly that the fivefold twinning in diamond has two distinct structures. In addition to the concentric fivefold twins, where the core structure is the intersection of five {111} twinning boundaries, a new extended core structure with co-hybridization of bonding is identified and analyzed in fivefold twinning. The atomic structure forming these fivefold twinning boundaries and their respective core structures is proposed to involve both the tetrahedral sp3 and planar graphitic sp2 bonding configurations, in which a co-hybridized planar hexagon of carbon serves as a fundamental structural unit. The presence of this sp2 -bonded planar unit of hexagonal carbon rings in general grain boundaries is also discussed.

Aqueous Zinc Batteries with Ultra-Fast Redox Kinetics and High Iodine Utilization Enabled by Iron Single Atom Catalysts.

Rechargeable aqueous zinc iodine (ZnǀǀI2) batteries have been promising energy storage technologies due to low-cost position and constitutional safety of zinc anode, iodine cathode and aqueous electrolytes. Whereas, on one hand, the low-fraction utilization of electrochemically inert host causes severe shuttle of soluble polyiodides, deficient iodine utilization and sluggish reaction kinetics. On the other hand, the usage of high mass polar electrocatalysts occupies mass and volume of electrode materials and sacrifices device-level energy density. Here, we propose a "confinement-catalysis" host composed of Fe single atom catalyst embedding inside ordered mesoporous carbon host, which can effectively confine and catalytically convert I2/I- couple and polyiodide intermediates. Consequently, the cathode enables the high capacity of 188.2 mAh g-1 at 0.3 A g-1, excellent rate capability with a capacity of 139.6 mAh g-1 delivered at high current density of 15 A g-1 and ultra-long cyclic stability over 50,000 cycles with 80.5% initial capacity retained under high iodine loading of 76.72 wt%. Furthermore, the electrocatalytic host can also accelerate the [Formula: see text] conversion. The greatly improved electrochemical performance originates from the modulation of physicochemical confinement and the decrease of energy barrier for reversible I-/I2 and I2/I+ couples, and polyiodide intermediates conversions.

La2Ti2O7 nanosheets modified by Pt quantum dots for efficient NO removal avoiding NO2 secondary pollutant.

Two-dimensional La2Ti2O7 nanosheets with regular morphology and good dispersion were prepared by the hydrothermal method under a magnetic field. Zero-dimensional Pt quantum dots (Pt-QDs) were loaded on the La2Ti2O7 nanosheets. The electron-hole separation and carrier transfer in the Pt-loaded La2Ti2O7 nanosheets were significantly enhanced. The La2Ti2O7 nanosheets loaded with 3 wt% Pt-QDs exhibit the largest NO removal efficiency of 51% and less than 3.2 ppb NO2 intermediate pollutant in 30 min. The high photocatalytic ability was attributed to the surface plasmon resonance in Pt-QDs and the enhanced electron-hole separation. A large number of e-, h+, •OH and •O2- active species were formed on the surface of Pt-loaded La2Ti2O7 nanosheets under light irradiation. The conversion pathway from NO to NO3- was verified by the in situ diffuse reflectance infrared Fourier-transform spectroscopy and DFT calculation. This work supplies a feasible approach to responsive photocatalysts for efficient, stable, and selective NO removal avoiding the NO2 secondary pollutant.

Surface-assisted synthesis of biomass carbon-decorated polymer carbon nitride for efficient visible light photocatalytic hydrogen evolution.

Template is frequently studied as a structure-directing agent to tune the nanomorphology of photocatalysts. However, the influences of template on the polymerization of precursors and compositions of the resulting samples are rarely considered. Herein, a biomass carbon-modified graphitic carbon nitride (CCNx) with a thin-layer morphology is synthesized via one-pot surface-assisted polymerization of melamine precursor on organic yeast. The formation of the hydrogen bond between melamine and yeast induces a strong interfacial confinement, giving rise to small-sized CCNx. In addition, the carbon materials derived from yeast dramatically broaden n â†’ π* visible light harvesting, improve electron delocalization, and greatly enhance charge carrier separation. The optimized CCNx presents a much higher photocatalytic hydrogen production rate of 2704 µmol g-1h-1 under visible light irradiation (λ ≥ 420 nm), which is nearly 11-fold that of its pristine counterpart. This work realizes the synergistic effect between morphology tunning and composition tailoring by using biomass template, which shows a great potential in developing efficient metal-free photocatalysts.

Synergism between chemisorption and unique electron transfer pathway in S-scheme AgI/g-C3N4 heterojunction for improving the photocatalytic H2 evolution.

AgI/g-C3N4 S-scheme heterojunction with a unique electron transfer pathway was developed as a catalyst for H2 evolution. We discussed the behavior of chemisorption and photoexcited charge carriers in photocatalytic reduction on the S-scheme AgI/g-C3N4 heterojunction. It was demonstrated that the path of charge transfer mediated by S-scheme AgI/g-C3N4 heterojunction was favorable for the improvement of electron utilization in photocatalysis. The advantage of S-scheme heterojunction was that the holes in the valence band (VB) of g-C3N4 could recombine with the electrons in the conduction band (CB) of AgI due to the built-in electric field. Electrons on the CB of g-C3N4 and holes on the VB of AgI were preserved for further photocatalytic reaction. Therefore, a distinctive electron transfer pathway was introduced in the S-scheme heterojunction. In addition, the lifetime of charge carriers was prolonged, and the reduced ability of electrons was increased as compared to reference g-C3N4. It not only decreased the energy required for electron excitation, but also reduced the energy consumption for the charge transfer. This paper provided a new strategy to improve the utilization of photogenerated electrons and chemisorption of water for photocatalytic H2O splitting.

Porous (K0.5Na0.5)0.94Li0.06NbO3-polydimethylsiloxane piezoelectric composites harvesting mechanical energy for efficient decomposition of dye wastewater.

Piezoelectricity as a physical property has received great attention due to its excellently functional applications, especially in piezoelectric catalysis and mechanical energy harvesting. To take full advantage of the functions of piezoelectric materials, (K0.5Na0.5)0.94Li0.06NbO3 (KNN6L) piezoelectric powders were compounded with polydimethylsiloxane (PDMS) in this work. The developed KNN6L-PDMS porous piezoelectric composites with flexible and recyclable characteristics could achieve âˆ¼ 91% degradation rate of Rhodamine B (RhB) dye wastewater under mechanical vibration, and the outstanding piezocatalytic activity was still maintained after repeated decomposition multiple times. Besides, the relationship between piezoelectric potential and piezocatalysis was validated by COMSOL simulations. The content of piezoelectric powders played a positive effect on the magnitude of piezoelectric potential generated by the KNN6L-PDMS porous composites. Moreover, the catalytic mechanism was found to be originated by generation of various reactive oxygen species (mainly •O2- and •OH) in water environment as a result of strong piezoelectric effect by the porous composites. The porous piezoelectric composites with flexible and recyclable characteristics exhibited excellent performance in piezoelectric catalysis which has promising applications in the field of environmental remediation.

Solid Electrolyte Interface in Zn-Based Battery Systems.

Due to its high theoretical capacity (820 mAh g-1), low standard electrode potential (- 0.76 V vs. SHE), excellent stability in aqueous solutions, low cost, environmental friendliness and intrinsically high safety, zinc (Zn)-based batteries have attracted much attention in developing new energy storage devices. In Zn battery system, the battery performance is significantly affected by the solid electrolyte interface (SEI), which is controlled by electrode and electrolyte, and attracts dendrite growth, electrochemical stability window range, metallic Zn anode corrosion and passivation, and electrolyte mutations. Therefore, the design of SEI is decisive for the overall performance of Zn battery systems. This paper summarizes the formation mechanism, the types and characteristics, and the characterization techniques associated with SEI. Meanwhile, we analyze the influence of SEI on battery performance, and put forward the design strategies of SEI. Finally, the future research of SEI in Zn battery system is prospected to seize the nature of SEI, improve the battery performance and promote the large-scale application.

Segmented Structure Design of Carbon Ring In-Plane Embedded in g-C3 N4 Nanotubes for Ultra-High Hydrogen Production.

The photocatalytic water splitting capability of metal-free graphitic carbon nitride (g-C3 N4 ) photocatalyst is determined by its microstructure and photoexcited electrons transfer. Herein, a segmented structure was developed, consisting of alternant g-C3 N4 nanotubes and graphitic carbon rings (denoted as Cr -CN-NT). The Cr -CN-NT showed ordered structure and ultralong length/diameter ratio of 150 nm in diameter and a few microns in lengths, which promoted electron transport kinetics and elongated photocarrier diffusion length and lifetime. Meanwhile, the local in-plane π-conjugation was formed and extended in Cr -CN-NT, which could improve charge carrier density and prohibit electron-hole recombination. Accordingly, the average hydrogen evolution rate of Cr -CN-NT reached 9245 µmol h-1 g-1 , which was 61.6 times that of pristine CN, and the remarkable apparent quantum efficiency (AQE) of Cr -CN-NT reached up to 12.86 % at 420 nm. This work may provide a pathway for simultaneous morphology regulation and in-plane modification of high-performance photocatalysts.

Simultaneous and Efficient Removal of Oleophilic and Hydrophilic Stains from Polyurethane by the Combination of Easy-Cleaning and Self-Cleaning.

The simultaneous and efficient removal of oleophilic and hydrophilic stains from polyurethane (PU) is realized by combining the easy-cleaning from the hydrophilic thermoresponsive hydrogel coating containing acrylamide (AAm), gum arabic (GA), and (ethylene glycol) methyl ether methacrylate (OEGMA300) P(GA/AAm/OEGMA300) and the self-cleaning from the embedded nonmetallic photocatalyst g-C3N4. Due to the existence of strong hydrogen bonds between the hydroxyl groups in the hybrid hydrogel coating and the hydroxyl/carboxyl groups in the plasma-treated PU, the hybrid hydrogel coating is very stable on PU. Simultaneously, the acrylamide network in the hybrid hydrogel coating enhances its mechanical strength. Because the transition temperature of OEGMA300 is well above the room temperature, the cross-linked coating remains hydrophilic in ambient conditions. Thus, oleophilic stains, such as oil and grease, can be easily removed from the coating surface. In addition, the embedded photocatalyst g-C3N4 in the hybrid hydrogel coating introduces the extra capability of decomposing organic compounds under sunshine, which favors the removal of hydrophilic stains such as dyes and wines. After sunlight illumination and simply rinsing with water, both hydrophilic and oleophilic stains can be easily removed. Moreover, this joint cleaning performance can work for a long time. Even after four consecutive cycles, both the easy-cleaning to oleophilic stains by the hydrophilic hydrogel surface and self-cleaning to the hydrophilic stains by the embedded g-C3N4 remain unchanged.

Experimental Investigation and Numerical Simulation for Corrosion Rate of Amorphous/Nano-Crystalline Coating Influenced by Temperatures.

A high-velocity oxygen fuel (HVOF) system was employed to prepare a Fe49.7Cr18Mn1.9Mo7.4W1.6B15.2C3.8Si2.4 amorphous coating on mild steel. The electrochemical behavior of the resultant coatings, namely as-sprayed coating and vacuum heat-treated coating (at 650 °C and 800 °C), were investigated in a 3.5% NaCl solution at variable temperatures using scanning electron microscopy (SEM), electrochemical impedance spectroscopy (EIS), potentiodynamic polarization, optical microscopy (OM), and XRD diffraction. Moreover, COMSOL Multiphysics version 5.5 software were employed for predicting the galvanic corrosion of amorphous material immersed in an aqueous NaCl solution, using the software finite element kit. The experiments demonstrated that the coatings' pitting resistance was significantly affected by temperature. The results also showed that temperature affected the pitting corrosion rate and changed the shape of the pits. However, the changes were not as extreme as those observed in stainless steel. Furthermore, there was no significant difference between the as-sprayed coating and the vacuum-heat-treated coating at 650 °C. At low NaCl concentrations at and temperatures below the critical pitting temperature, the resulting pits were significantly small with a hemisphere-like. By contrast, at a higher NaCl concentration at 70 °C, particularly in the case of heating at 650 °C, the pits appearing on the Fe-based amorphous coating were vast and sometimes featured a lacy cover.

Roles of water in the formation and preparation of graphene oxide.

The functional groups and physical properties of graphene oxide (GO) are found to be sensitive to and can be controlled by the water content in the reactions when GO samples are prepared at different concentrations of sulfuric acid using a modified Hummers method. GO prepared with 93% sulfuric acid (H2SO4) showed fewer structural defects, less π-π conjugation, and larger interlayer spacing than GO prepared with 99% H2SO4. The intensity ratio of the D-band to the G-band of the Raman spectrum is 0.89 ± 0.01 and 1.02 ± 0.01, corresponding to average interlayer spacing of 0.91 nm and 0.86 nm, respectively. The yield and carbon to oxygen ratio of the GO sheets prepared from different concentrations of H2SO4 are nearly identical. More importantly, compared with GO synthesized with 99% H2SO4, GO prepared with 93% H2SO4 contains more carbon-oxygen single bonds, such as epoxy groups and hydroxyl groups, but fewer carbonyl groups.

Correction: Roles of water in the formation and preparation of graphene oxide.

[This corrects the article DOI: 10.1039/D0RA10026A.].

Wearable Bracelet Monitoring the Solar Ultraviolet Radiation for Skin Health Based on Hybrid IPN Hydrogels.

The risk of extensive exposure of the human epidermis to solar ultraviolet radiation is significantly increased nowadays. It not only induces skin aging and solar erythema but also increases the possibility of skin cancer. Therefore, a simply prepared, highly sensitive, and optically readable device for monitoring the solar ultraviolet radiation is highly desired for the skin health management. Because of the photoinitiated polymerization triggered by graphene-carbon nitride (g-C3N4) under ultraviolet radiation, g-C3N4 is homogeneously distributed in the hybrid hydrogels containing N-isopropylacrymide (NIPAM), poly(ethylene glycol) methyl ether methacrylate (OEGMA300), and sodium alginate (SA). By further immersing the hybrid hydrogels into calcium chloride solution, hybrid alginate-Ca2+/P(NIPAM-co-OEGMA300)/g-C3N4 interpenetrating polymeric network (IPN) hydrogels are obtained. Due to the homogeneous distribution of g-C3N4 and the existence of thermoresponsive polymers, the hybrid IPN hydrogels present good adsorption capability and high degradation efficiency for methylene blue (MB) especially at high temperature under ultraviolet radiation. Based on this unique property, the bracelet monitoring skin health is prepared by simply immersing the hybrid IPN hydrogels into the MB solution and then wrapping it with PET foil. Because the immersion time for the top, middle, and bottom parts of the hybrid IPN hydrogels is gradually increased, their colors vary from light to dark blue. A longer time is required for the discoloration of the darker part under solar ultraviolet radiation. Thus, the bracelet can be used to conveniently monitor the dose of solar ultraviolet radiation by simply checking the discoloration in the bracelet under sunshine. Due to the facile preparation and low cost of the bracelet, it is a promising candidate for wearable devices for skin health management.

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.