Metal-doped(Cu,Zn)Fe2O4 from integral utilization of toxic Zn-containing electric arc furnace dust: An environment-friendly heterogeneous Fenton-like catalyst

Pure metal-doped(Cu,Zn)Fe2O4 was synthesized from Zn-containing electric arc furnace dust(EAFD)by solid-state reaction using copper salt as additive.The effects of pretreated EAFD-to-Cu2(OH)2CO3·6H2O mass ratio,calcination time,and calcination temperature on the structure and catalytic ability were systematically studied.Under the optimum conditions,the decolorization efficiency and total organic carbon(TOC)removal efficiency of the as-prepared ferrite for treating a Rhodamine B solution were approximately 90.0%and 45.0%,respectively,and the decolorization efficiency remained 83.0%after five recycles,suggesting that the as-prepared(Cu,Zn)Fe2O4 was an efficient heterogeneous Fenton-like catalyst with high stability.The high catalytic activity mainly depended on the synergistic effect of iron and copper ions occupying octahedral positions.More importantly,the toxicity characteristic leaching procedure(TCLP)analysis illustrated that the toxic Zncontaining EAFD was transformed into harmless(Cu,Zn)Fe2O4 and that the concentrations of toxic ions in the degraded solution were all lower than the national emission standard(GB/31574-2015),further confirming that the as obtained sample is an environment-friendly heterogeneous Fenton-like catalyst.

Synthesis of Magnetically Modified Fe-Al Pillared Bentonite and Heterogeneous Fenton-like Degradation of Orange II

Magnetically modified Fe-Al pillared bentonite（Fe3O4/ Fe-Al-Bent） was prepared via chemical co-precipitation method and characterized by powder X-ray diffraction（XRD）, Brunauer-EmmettTeller（BET）, Fourier transform infrared spectroscopy（FTIR） and scanning electron microscopy（SEM）. A series of experiments were carried out to investigate the degradation of Orange II by the obtained heterogeneous catalysts in the presence of H2O2. The experimental result indicated that the synthetic materials had a high catalytic activity and good reusability.

Iron-glutamate-silicotungstate ternary complex as highly active heterogeneous Fenton-like catalyst for 4-chlorophenol degradation

A novel iron-glutamate-silicotungstate ternary complex（FeШGluS iW） was synthesized from ferric chloride（FeI II）,glutamic acid（Glu）,and silicotungstic acid（SiW）,and used as a heterogeneous Fenton-like catalyst for 4-chlorophenol（4-CP） degradation at neutral pH value. The prepared FeШGluS iW was characterized using inductively coupled plasma atomic emission spectroscopy,thermogravimetry,Fourier-transform infrared spectroscopy,ultraviolet-visible diffuse reflectance spectroscopy,X-ray diffraction,and field-emission scanning electron microscopy. The results showed that FeШGluS iW has the formula [Fe（C5H8NO4）（H2O）]2SiW 12O40？13H2O,with glutamate moiety and Keggin-structured SiW 12O404- heteropolyanion. The catalyst showed high catalytic activity in 4-CP degradation in the dark and under irradiation. Under the conditions of 4-CP 100 mg/L,FeШGluS iW 1.0 g/L,H2O2 20 mmol/L,and pH = 6.5,4-CP was completely decomposed in 40 min in the dark and in 15 min under irradiation. When the reaction time was prolonged to 2 h,the corresponding total organic carbon removals under dark and irradiated conditions were ca. 27% and 72%,respectively. The high catalytic activity of FeI IIGluS iW is resulted from hydrogen bonding of H2O2 on the FeI IIGluS iW surface. The enhanced degradation of 4-CP under irradiation arises from simultaneous oxidation of 4-CP through Fenton-like and photocatalytic processes respectively catalyzed by ferric iron and the SiW 12O404- hetropolyanion in FeШGluS iW.

Degradation of n-butyl xanthate using fly ash as heterogeneous Fenton-like catalyst

Heterogeneous Fenton-like process using fly ash as a catalyst was studied to degrade n-butyl xanthate form aqueous solution. The different reaction parameters on the degradation efficiency of the process were investigated. The fly ash/H2O2 catalyst possesses a high oxidation activity for n-butyl xanthate degradation in aqueous solution. It is found that both the dosage of catalyst and initial solution pH significantly affect the n-butyl xanthate conversion efficient. The results indicate that by using 1.176 mmol/L H2O2 and 1.0 g/L fly ash catalyst with mass fraction of 4.14% Fe(III) oxide at pH 3.0, almost 96.90% n-butyl xanthate conversion and over 96.66% COD removal can be achieved within 120 min with heterogeneous catalysis by fly ash. CS2 as an intermediate of n-butyl xanthate oxidation. Finally, it is demonstrated that the fly ash/H2O2 catalytic oxidation process can be an efficient method for the treatment of n-butyl xanthate containing wastewater.

Green synthesis of bentonite-supported iron nanoparticles as a heterogeneous Fenton-like catalyst:Kinetics of decolorization of reactive blue 238 dye

This study aimed to synthesize green tea nano zero-valent iron(GT-NZVI)and bentonite-supported green tea nano zero-valent iron(BGT-NZVI)nanoparticles using green tea extracts in an environmentally sustainable way.Bentonite was used as a support material because it disperses and stabilizes GT-NZVI,and it helps to reduce the cost,increase the adsorption capacity of GT-NZVI,and decrease the optimum amount of GT-NZVI used in Fenton-like oxidation.A scanning electron microscope,an atomic force microscope,and a Fourier transform infrared spectroscope were used to characterize GT-NZVI and B-GT-NZVI,while the zeta potential was measured to evaluate the stability of iron nanoparticles.The decolorization kinetics of reactive blue 238(RB 238)dye in the aqueous phase in the Fenton-like oxidation process were investigated as well.The effects of various experimental conditions such as reaction time,dosages of catalysts,concentration of H2O2,temperature,addition of inorganic salts,and other parameters were investigated.The results show that the oxidative degradation efficiencies of RB 238 dye catalyzed by GT-NZVI and B-GT-NZVI were 93.5%and 96.2%,respectively,at the optimum reaction conditions as follows:c(H2O2)¼5 mmol/L,r(GT-NZVI)¼0.5 g/L or r(B-GT-NZVI)¼0.5 g/L,c(RB 238 dye)¼0.05 mmol/L,and pH¼2.5 at 180 min.The best catalytic performance was exhibited when B-GT-NZVI was used.Three kinetic models were employed,and the second-order model was found to be the best model representing the experimental kinetic data of RB 238 dye.The value of activation energy decreased from 38.22 kJ/mol for GT-NZVI to 14.13 kJ/mol for B-GT-NZVI.This indicates that the effect of B-GT-NZVI in decreasing the energy barrier is more pronounced than that of the GT-NZVI catalyst,leading to improved Fenton-like oxidation processes.©2020 Hohai University.Production and hosting by Elsevier B.V.This is an open access article under the CC BY-NC-ND license(http://creativecommons.org/licenses/by-nc-nd/4.0/).

Reactive species in resin supported heterogeneous Fenton-like oxidation of Malachite green solution

During the oxidative degradation of nonbiodegradable Malachite green (MG) by means of H2O2 /FeIIIR (iron supported on ion-exchage resin) in a dynamic column,the binding energy of the Fe(2p3/2) region for XPS spectra was found to be different between the top layer and the bottom layer in this column. Based on the data from XPS spectra and DMPO-OH·signal by EPR spectra,it is shown that the formation of ferryl (IV) is the key step for the oxidation of MG. The ferryl (IV) species can oxidize MG,and its redox potential is about 0. 739 - 0. 803 V measured by cyclic voltammograms (CV) . The catalytic capability of ferryl (IV) species was also evaluated,and it is found that it can promote the decomposition of H2O2 more efficiently than ferric iron. The removal rate of MG mainly depends on the adsorption of catalyst. Both ferryl (IV) and HO·radicals are the reactive species in the system. The oxidation of HO·is only a small part of the overall removal rate. Based on the obtained results,a possible mechanism for a resin-supported Fenton-like oxidation reaction is proposed.

Discarded Carbon-Zinc Batteries as Source of an Efficient Heterogeneous Fenton-Like Catalyst Employed to Degrade Organic Molecules in an Aqueous Medium

The present work evaluates the feasibility of using the raw material collected from discarded zinc-carbon batteries as heterogeneous catalyst to degrade the dye Indigo Carmine in an aqueous solution. Besides the evident environmental application, this work also presents an economic alternative for the production of new catalysts used to remediate polluted waters. For this, discarded carbon-zinc batteries were gathered, disassembled and their anodic paste collected. After acidic treatment and calcination at 500°C, characterization measurements, i.e. flame atomic absorption spectroscopy (FAAS), nitrogen sorption, X-ray diffraction (XRD) and scanning electron microscopy (SEM), revealed that the so-obtained material consisted mainly of ZnMn2O4. This material acts as a heterogeneous catalyst in a Fenton-like process that degrades the dye Indigo Carmine in water. That is probably due to the presence of Mn(III) (manganese in the +3 oxidation state) in this material that triggers the decomposition of hydrogen peroxide (H2O2) to yield hydroxyl radicals (HO·). Moreover, direct infusion electrospray ionization coupled to high resolution mass spectrometry (ESI-HRMS) was employed to characterize the main by-products resulting from such degradation process. These initial results thus indicate that raw materials from waste batteries can therefore be potentially employed as efficient Fenton-like catalysts to degrade organic pollutants in an aqueous solution.

Selective oxidation of emerging organic contaminants in heterogeneous Fenton-like systems

Heterogeneous Fenton-like reaction shows great potential for eliminating organic substances (e.g. emerging organic contaminants (EOCs)) in water, which has been widely explored in recent decades. However, the catalytic mechanisms reported in current studies are extremely complicated because multiple mechanisms coexist and contribute to the removal efficiencies. Most importantly, heterogeneous systems show selective oxidation properties, which are crucial for improving the efficiencies in the catalytic elimination of organic substances. Thus, this critical review summarizes and compares the diverse existing mechanisms (non-radical and radical pathways) in heterogeneous catalytic processes based on recent studies. The typical oxidation mechanisms during selective advanced oxidation of EOCs were systematically discussed based on the following sections, including the selective adsorption and generation of reactive oxygen species (ROS) in photo/electron-Fenton and Fenton-like systems. Moreover, the non-radical pathways are discussed in depth by the singlet oxygen, high-valent metal-oxo, electron transfer process, etc. Moreover, the direct oxidative transfer process for the removal of EOCs was introduced in recent studies. Finally, the cost, feasibility as well as the sustainability of heterogeneous Fenton-like catalysts are summarized. This review offers useful guidance for developing suitable strategies to develop materials for decomposing the organic substrates.

Application of response surface methodology for optimization of Orange Ⅱ removal by heterogeneous Fenton-like process using Fe_3O_4nanoparticles

In this study, Fe3O4nanoparticles（Fe3O4NPs） were successfully prepared via oxidation–precipitation method and characterized by scanning electron microscopy（SEM）, X-ray diffraction（XRD） and Fourier transform infrared spectroscopy（FT-IR）. The characterization results indicated that Fe3O4 NPs with regular crystal structure and a narrow of diameters had been synthesized successfully and had high purity. A series of experiments were carried out to investigate the degradation of Orange II by the obtained heterogeneous Fe3O4 catalysts in the presence of H2O2. The response surface methodology（RSM） based on Box–Behnken design（BBD） was employed to design and optimize individual and interactive effects of the four main independent parameters（catalyst loading, initial p H, reaction temperature and H2O2concentration） on decolorization efficiency of Orange II. A significant quadratic model（p-value 〈0.0001, R2= 0.9369） was derived using analysis of variance（ANOVA）. Optimum conditions were catalyst loading of 1.5 g/L, initial p H of 2.7, reaction temperature of 42 8C and H2O2 concentration of 22 mmol/L, respectively. The predicted decolorization rate under the optimum conditions as determined by the proposed model was 99.55%. Confirmatory tests were carried out and the decolorization rate of 99.49% was observed under the optimum conditions, which agreed well with the model prediction.

Enabling heterogeneous catalysis to achieve carbon neutrality: Directional catalytic conversion of CO_(2) into carboxylic acids

The increase in anthropogenic carbon dioxide(CO_(2))emissions has exacerbated the deterioration of the global environment,which should be controlled to achieve carbon neutrality.Central to the core goal of achieving carbon neutrality is the utilization of CO_(2) under economic and sustainable conditions.Recently,the strong need for carbon neutrality has led to a proliferation of studies on the direct conversion of CO_(2) into carboxylic acids,which can effectively alleviate CO_(2) emissions and create high-value chemicals.The purpose of this review is to present the application prospects of carboxylic acids and the basic principles of CO_(2) conversion into carboxylic acids through photo-,electric-,and thermal catalysis.Special attention is focused on the regulation strategy of the activity of abundant catalysts at the molecular level,inspiring the preparation of high-performance catalysts.In addition,theoretical calculations,advanced technologies,and numerous typical examples are introduced to elaborate on the corresponding process and influencing factors of catalytic activity.Finally,challenges and prospects are provided for the future development of this field.It is hoped that this review will contribute to a deeper understanding of the conversion of CO_(2) into carboxylic acids and inspire more innovative breakthroughs.

Synergy of heterogeneous Co/Ni dual atoms enabling selective C-O bond scission of lignin coupling with in-situ N-functionalization

Selective cleavage of Csp^(2)-OCH_(3)bond in lignin without breaking other types of C-O bonds followed by N-functionalization is fascinating for on-purpose valorization of biomass.Here,a Co/Ni-based dual-atom catalyst CoNiDA@NC prepared by in-situ evaporation and acid-etching of metal species from tailor-made metal–organic frameworks was efficient for reductive upgrading of various lignin-derived phenols to cyclohexanols(88.5%–99.9%yields),which had ca.4 times higher reaction rate than the single-atom catalyst and was superior to state-of-the-art heterogeneous catalysts.The synergistic catalysis of Co/Ni dual atoms facilitated both hydrogen dissociation and hydrogenolysis steps,and could optimize adsorption configuration of lignin-derived methoxylated phenols to further favor the Csp^(2)-OCH_(3)cleavage,as elaborated by theoretical calculations.Notably,the CoNi_(DA)@NC catalyst was highly recyclable,and exhibited excellent demethoxylation performance(77.1%yield)in real lignin monomer mixtures.Via in-situ cascade conversion processes assisted by dual-atom catalysis,various high-value N-containing chemicals,including caprolactams and cyclohexylamines,could be produced from lignin.

Development of a convolutional neural network based geomechanical upscaling technique for heterogeneous geological reservoir

Geomechanical assessment using coupled reservoir-geomechanical simulation is becoming increasingly important for analyzing the potential geomechanical risks in subsurface geological developments.However,a robust and efficient geomechanical upscaling technique for heterogeneous geological reservoirs is lacking to advance the applications of three-dimensional(3D)reservoir-scale geomechanical simulation considering detailed geological heterogeneities.Here,we develop convolutional neural network(CNN)proxies that reproduce the anisotropic nonlinear geomechanical response caused by lithological heterogeneity,and compute upscaled geomechanical properties from CNN proxies.The CNN proxies are trained using a large dataset of randomly generated spatially correlated sand-shale realizations as inputs and simulation results of their macroscopic geomechanical response as outputs.The trained CNN models can provide the upscaled shear strength(R^(2)>0.949),stress-strain behavior(R^(2)>0.925),and volumetric strain changes(R^(2)>0.958)that highly agree with the numerical simulation results while saving over two orders of magnitude of computational time.This is a major advantage in computing the upscaled geomechanical properties directly from geological realizations without the need to perform local numerical simulations to obtain the geomechanical response.The proposed CNN proxybased upscaling technique has the ability to(1)bridge the gap between the fine-scale geocellular models considering geological uncertainties and computationally efficient geomechanical models used to assess the geomechanical risks of large-scale subsurface development,and(2)improve the efficiency of numerical upscaling techniques that rely on local numerical simulations,leading to significantly increased computational time for uncertainty quantification using numerous geological realizations.

Catalytic effect in lithium metal batteries: From heterogeneous catalyst to homogenous catalyst

Lithium metal batteries are regarded as prominent contenders to address the pressing needs owing to the high theoretical capacity.Toward the broader implementation,the primary obstacle lies in the intricate multi-electron,multi-step redox reaction associated with sluggish conversion kinetics,subsequently giving rise to a cascade of parasitic issues.In order to smooth reaction kinetics,catalysts are widely introduced to accelerate reaction rate via modulating the energy barrier.Over past decades,a large amount of research has been devoted to the catalyst design and catalytic mechanism exploration,and thus the great progress in electrochemical performance has been realized.Therefore,it is necessary to make a comprehensive review toward key progress in catalyst design and future development pathway.In this review,the basic mechanism of lithium metal batteries is provided along with corresponding advantages and existing challenges detailly described.The main catalysts employed to accelerate cathode reaction with emphasis on their catalytic mechanism are summarized as well.Finally,the rational design and innovative direction toward efficient catalysts are suggested for future application in metal-sulfur/gas battery and beyond.This review is expected to drive and benefit future research on rational catalyst design with multi-parameter synergistic impacts on the activity and stability of next-generation metal battery,thus opening new avenue for sustainable solution to climate change,energy and environmental issues,and the potential industrial economy.

Removing lignin model pollutants with BiFeO_3–g-C_3N_4 compound as an efficient visible-light-heterogeneous Fenton-like catalyst

BiFeO3-g-C3N4 nanoscaled composite was prepared with a hydrothermal method and evaluated as a highly efficient photo-Fenton like catalyst under visible light irradiation. The BiFeO3-g-CHN4 composite exhibited much stronger adsorption ability to lignin model pollutant （guaiacol） than that of BiFeO3, which may be due to the higher specific surface area （BiFeO3-g-C3N4：35.59 m2/g 〉 BiFeO3：7.42 m2/g） and the adsorption form of π-π stack between g-C3N4 and guaiacol. The composite exhibited excellent visible light-Fenton like catalysis activity, being influenced by the solution pH value and the proportions of BiFe03 and g-C3N4 nanosheets. Under optimal conditions with visible light irradiation, the BiFeO3- g-C3N4 composite yielded fast degradation of guaiacol with an apparent rate constant of 0.0452 rain-I, which were 5.21 and 6.80 folds of that achieved by using BiFeO3 and the mixture of BiFeO3 and g-C3N4 nanosheets, respectively. The significantly enhanced visible light-Fenton like catalytic properties of the BiFeO3-g-C3N4 composite in comparison with that of BiFeO3 was attributed to a large surface area, much increased adsorption capacity and the semiconductor coupling effect between BiFe03 and g-C3N4 in the composite.

Silicon-based optoelectronic heterogeneous integration for optical interconnection

The performance of optical interconnection has improved dramatically in recent years.Silicon-based optoelectronic heterogeneous integration is the key enabler to achieve high performance optical interconnection,which not only provides the optical gain which is absent from native Si substrates and enables complete photonic functionalities on chip,but also improves the system performance through advanced heterogeneous integrated packaging.This paper reviews recent progress of silicon-based optoelectronic heterogeneous integration in high performance optical interconnection.The research status,development trend and application of ultra-low loss optical waveguides,high-speed detectors,high-speed modulators,lasers and 2D,2.5D,3D and monolithic integration are focused on.

Intelligent Dynamic Heterogeneous Redundancy Architecture for IoT Systems

The conventional dynamic heterogeneous redundancy(DHR)architecture suffers from the security threats caused by the stability differences and similar vulnerabilities among the executors.To overcome these challenges,we propose an intelligent DHR architecture,which is more feasible by intelligently combining the random distribution based dynamic scheduling algorithm(RD-DS)and information weight and heterogeneity based arbitrament(IWHA)algorithm.In the proposed architecture,the random distribution function and information weight are employed to achieve the optimal selection of executors in the process of RD-DS,which avoids the case that some executors fail to be selected due to their stability difference in the conventional DHR architecture.Then,through introducing the heterogeneity to restrict the information weights in the procedure of the IWHA,the proposed architecture solves the common mode escape issue caused by the existence of multiple identical error output results of similar vulnerabilities.The experimental results characterize that the proposed architecture outperforms in heterogeneity,scheduling times,security,and stability over the conventional DHR architecture under the same conditions.

Blockchain-Enabled Cybersecurity Provision for Scalable Heterogeneous Network:A Comprehensive Survey

Blockchain-enabled cybersecurity system to ensure and strengthen decentralized digital transaction is gradually gaining popularity in the digital era for various areas like finance,transportation,healthcare,education,and supply chain management.Blockchain interactions in the heterogeneous network have fascinated more attention due to the authentication of their digital application exchanges.However,the exponential development of storage space capabilities across the blockchain-based heterogeneous network has become an important issue in preventing blockchain distribution and the extension of blockchain nodes.There is the biggest challenge of data integrity and scalability,including significant computing complexity and inapplicable latency on regional network diversity,operating system diversity,bandwidth diversity,node diversity,etc.,for decision-making of data transactions across blockchain-based heterogeneous networks.Data security and privacy have also become the main concerns across the heterogeneous network to build smart IoT ecosystems.To address these issues,today’s researchers have explored the potential solutions of the capability of heterogeneous network devices to perform data transactions where the system stimulates their integration reliably and securely with blockchain.The key goal of this paper is to conduct a state-of-the-art and comprehensive survey on cybersecurity enhancement using blockchain in the heterogeneous network.This paper proposes a full-fledged taxonomy to identify the main obstacles,research gaps,future research directions,effective solutions,andmost relevant blockchain-enabled cybersecurity systems.In addition,Blockchain based heterogeneous network framework with cybersecurity is proposed in this paper tomeet the goal of maintaining optimal performance data transactions among organizations.Overall,this paper provides an in-depth description based on the critical analysis to overcome the existing work gaps for future research where it presents a potential cybersecurity design with key requirements of blockchain across a heterogeneous network.

Carbon-doped CuFe_(2)O_(4) with C-O-M channels for enhanced Fenton-like degradation of tetracycline hydrochloride: From construction to mechanism

Carbon-doped copper ferrite(C–CuFe_(2)O_(4))was synthesized by a simple two-step hydrothermal method,which showed enhanced tetracycline hydrochloride(TCH)removal efficiency as compared to the pure CuFe_(2)O_(4) in Fenton-like reaction.A removal efficiency of 94%was achieved with 0.2 g L^(-1) catalyst and 20 mmol L^(-1) H_(2)O_(2) within 90 min.We demonstrated that 5%C–CuFe_(2)O_(4) catalyst in the presence of H_(2)O_(2) was significantly efficient for TCH degradation under the near-neutral pH(5–9)without buffer.Multiple techniques,including SEM,TEM,XRD,FTIR,Raman,XPS M€ossbauer and so on,were conducted to investigate the structures,morphologies and electronic properties of as-prepared samples.The introduction of carbon can effectively accelerate electron transfer by cooperating with Cu and Fe to activate H_(2)O_(2) to generate·OH and·O_(2)^(-).Particularly,theoretical calculations display that the p,p,d orbital hybridization of C,O,Cu and Fe can form C–O–Cu and C–O–Fe bonds,and the electrons on carbon can transfer to metal Cu and Fe along the C–O–Fe and C–O–Cu channels,thus forming electron-rich reactive centers around Fe and Cu.This work provides lightful reference for the modification of spinel ferrites in Fenton-like application.

Dynamics and synchronization in a memristor-coupled discrete heterogeneous neuron network considering noise

Research on discrete memristor-based neural networks has received much attention.However,current research mainly focuses on memristor–based discrete homogeneous neuron networks,while memristor-coupled discrete heterogeneous neuron networks are rarely reported.In this study,a new four-stable discrete locally active memristor is proposed and its nonvolatile and locally active properties are verified by its power-off plot and DC V–I diagram.Based on two-dimensional(2D)discrete Izhikevich neuron and 2D discrete Chialvo neuron,a heterogeneous discrete neuron network is constructed by using the proposed discrete memristor as a coupling synapse connecting the two heterogeneous neurons.Considering the coupling strength as the control parameter,chaotic firing,periodic firing,and hyperchaotic firing patterns are revealed.In particular,multiple coexisting firing patterns are observed,which are induced by different initial values of the memristor.Phase synchronization between the two heterogeneous neurons is discussed and it is found that they can achieve perfect synchronous at large coupling strength.Furthermore,the effect of Gaussian white noise on synchronization behaviors is also explored.We demonstrate that the presence of noise not only leads to the transition of firing patterns,but also achieves the phase synchronization between two heterogeneous neurons under low coupling strength.

Phase reconfiguration of heterogeneous CoFeS/CoNiS nanoparticles for superior battery-type supercapacitors

Developing advanced battery-type materials with abundant active sites,high conductivity,versatile morphologies,and hierarchically porous structures is crucial for realizing high-quality hybrid supercapacitors.Herein,heterogeneous FeS@NiS is synthesized by cationic Co doping via surface-structure engineering.The density functional theory(DFT)theoretical calculations are firstly performed to predict the advantages of Co dopant by improving the OH^(−)adsorption properties and adjusting electronic structure,benefiting ions/electron transfer.The dynamic surface evolution is further explored which demonstrates that CoFeS@CoNiS could be quickly reconstructed to Ni(Co)Fe_(2)O_(4)during the charging process,while the unstable structure of the amorphous Ni(Co)Fe_(2)O_(4)results in partial conversion to Ni/Co/FeOOH at high potentials,which contributes to the more reactive active site and good structural stability.Thus,the free-standing electrode reveals excellent electrochemical performance with a superior capacity(335.6 mA h g^(−1),2684 F g^(−1))at 3 A g^(−1).Furthermore,the as-fabricated device shows a quality energy density of 78.1 W h kg^(−1)at a power density of 750 W kg^(−1)and excellent cycle life of 92.1%capacitance retention after 5000 cycles.This work offers a facile strategy to construct versatile morphological structures using electrochemical activation and holds promising applications in energy-related fields.