Metal dichalcogenide-based 2D materials,gained considerable attention recently as a hydrogen evolution reaction(HER)electrocatalyst.In this work,we synthesized MoSe_(2)-based electrocatalyst via hydrothermal route wit...Metal dichalcogenide-based 2D materials,gained considerable attention recently as a hydrogen evolution reaction(HER)electrocatalyst.In this work,we synthesized MoSe_(2)-based electrocatalyst via hydrothermal route with varying phase contents(1T/2H)and respective HER performances were evaluated under the acidic media(0.5 M H_(2)SO_(4)),where best HER performance was obtained from the sample consisting of mixed 1T/2H phases,which was directly grown on a carbon paper(167 mV at10 mA cm^(-2))Furthermore,HER performance of electrocatalyst was further improved by in-situ electrodeposition of Pt nanoparticles(0.15 wt%)on the MoSe_(2) surface,which lead to significant enhancement in the HER performances(133 mV at 10 mA cm^(-2)).Finally,we conducted density functional theory calculations to reveal the origin of such enhanced performances when the mixed 1T/2H phases were present,where phase boundary region(1T/2H heterojunction)act as a low energy pathway for H_(2)adsorption and desorption via electron accumulation effect.Moreover,presence of the Pt nanoparticles tunes the electronic states of the MoSe_(2)based catalyst,resulting in the enhanced HER activity at heterointerface of 1T/2H MoSe_(2) while facilitating the hydrogen adsorption and desorption process providing a low energy pathway for HER.These results provide new insight on atomic level understanding of the MoSe_(2) based catalyst for HER application.展开更多
Achieving carbon neutrality is urgent due to the critical issue of climate change.To reach this goal,the development of new,breakthrough technologies is necessary and urgent.One such technology involves efficient carb...Achieving carbon neutrality is urgent due to the critical issue of climate change.To reach this goal,the development of new,breakthrough technologies is necessary and urgent.One such technology involves efficient carbon capture and its conversion into useful chemicals or fuels.However,achieving considerable amounts of efficiency in this field is a very challenging task.Even in natural photosynthesis occurring in plant leaves,the CO_(2)conversion efficiency into hydrocarbons cannot exceed a value of 1%.Nevertheless,recently few reports show comparable higher efficiency in CO_(2)to gaseous products such as carbon monoxide(CO),but it is hard to find selective liquid fuel products with a high value of solar to liquid fuel conversion efficiency.Herein,a NiFe-assisted hybrid composite dark cathode is employed for the selective production of solar-to-liquid fuels,in conjunction with a BiVO4 photoanode.This process results in the generation of significant amounts of formaldehyde,ethanol,and methanol selectively.The primary objective of this study is to design and optimize a novel photoelectrochemical(PEC)system to produce solar-to-liquid fuels selectively.This study shows the enhancement of the solar-to-fuel conversion efficiency over 1.5%by employing a hybrid composite cathode composed of NiFe-assisted reduced graphene oxide(rGO),poly(4-vinyl)pyridine(PVP),and Nafion.展开更多
The advanced oxidation system based on peracetic acid(PAA)has been proved to be a green and safe oxidation decontamination technology.Among them,the key challenge and complexity in current research lies in the directi...The advanced oxidation system based on peracetic acid(PAA)has been proved to be a green and safe oxidation decontamination technology.Among them,the key challenge and complexity in current research lies in the directional induction of PAA and its utilization for selective removal of refractory pollutants.This study prepared nitrogen-doped biochar(NBC)using compound pharmaceutical residues commonly found in traditional Chinese medicine as a precursor.A system based on NBC-activated PAA was constructed for sulfamethoxazole(SMX)degradation.The introduction of nitrogen significantly enhanced the degree of graphitization in NBC.The degradation system achieved 87.89%SMX degradation efficiency within 60 min.Furthermore,the formation of the intricate NBC-PAA*complex detected by in-situ Raman was of paramount importance as it facilitates enhanced electron transfer processes within the complex,thereby promoting PAA decomposition through electron loss.The formation of a new complex between SMX and NBC-PAA*facilitated the completion of electron transfer process within the complex.In summary,this study explored a novel approach for treating and disposing of solid waste from Chinese medicine residue by successfully inducing non-free radical degradation pathway using PAA system.It offers fresh insights and ideas in the fields of water treatment and solid waste management.展开更多
Typical p-n junctions have emerged as a promising strategy for contending with charge carrier recombination in solar conversion.However,the photo-corrosion and unsuitable energy band positions still hinder their pract...Typical p-n junctions have emerged as a promising strategy for contending with charge carrier recombination in solar conversion.However,the photo-corrosion and unsuitable energy band positions still hinder their practical application for hydrogen production from water in photoelectrochemical systems.Here,an in-situ photo-oxidation method is proposed for achieving self-adapting activation of BiVO_(4)-based photoanodes with surface-encapsulated CuGaS_(2)particles by the ZnO layer.The self-adapting activation demotes the energy band positions of CuGaS_(2),establishing an S-scheme structure with BiVO_(4),resulting in an efficient p-n junction photoanode.The optimal sample exhibits enhanced photocurrent and an onset potential cathodically shifted by~300 mV compared with BiVO_(4),which is attributed to significantly enhanced charge transport and transfer efficiencies.As expected,it attains the highest photocurrent value of 5.87 mA·cm^(-2),aided by a hole scavenger at 1.23 V versus a reversible hydrogen electrode,which significantly surpasses that of BiVO_(4)(4.32 mA·cm^(-2)).展开更多
Conventional organic coatings often face limitations in providing long-term corrosion protection in aggressive environments.This study introduces a dual-functional polydopamine-zinc oxide(PD-Z)composite incorporated i...Conventional organic coatings often face limitations in providing long-term corrosion protection in aggressive environments.This study introduces a dual-functional polydopamine-zinc oxide(PD-Z)composite incorporated into an epoxy(EP)matrix(PD-Z/EP)to enhance the hydrophobicity and corrosion resistance of aluminum substrates.Characterization analyses confirmed the successful fabrication of the PD-Z composite.Electrochemical measurements,specifically potentiodynamic polarization,are conducted after three days of immersion in a 3.5%(mass)NaCl solution,significantly decreasing corrosion current density(Icorr)from 249.4 nA·cm^(-2)for pure EP to 167 nA·cm^(-2)for PD-Z/EP.Concurrently,the corrosion rate decreased from 0.004 to 0.0002 mm·a^(-1).Additionally,electrochemical impedance spectroscopy(EIS)demonstrated a marked increase in the low-frequency impedance modulus(|Z|_(0.01)_(Hz))from 0.07×10^(6) to 1.2114×10^(6)Ω·cm^(-2),indicating superior corrosion inhibition.The exceptional anodic and cathodic protective performance of the PD-Z/EP coating is attributed to the synergistic effects of polydopamine and ZnO,which enhance chloride ion entrapment,hydrophobic barrier properties,and overall corrosion resistance.展开更多
Humic acid(HA),as a represent of natural organic matter widely existing in water body,dose harm to water quality and human health;however,it was commonly treated as an environmental background substance while not targ...Humic acid(HA),as a represent of natural organic matter widely existing in water body,dose harm to water quality and human health;however,it was commonly treated as an environmental background substance while not targeted contaminant in advanced oxidation processes(AOPs).Herein,we investigated the removal of HA in the alkali-activated biochar(KBC)/peroxymonosulfate(PMS)system.The modification of the original biochar(BC)resulted in an increased adsorption capacity and catalytic activity due to the introduction of more micropores,mesopores,and oxygen-containing functional groups,particularly carbonyl groups.Mechanistic insights indicated that HA is primarily chemically adsorbed on the KBC surface,while singlet oxygen(^(1)O_(2))produced by the PMS decomposition served as the major reactive species for the degradation of HA.An underlying synergistic adsorption and oxidation mechanism involving a local high concentration reaction region around the KBC interface was then proposed.This work not only provides a cost-effective solution for the elimination of HA but also advances our understanding of the nonradical oxidation at the biochar interface.展开更多
Hydrogen evolution reaction(HER)in acidic media has been spotlighted for hydrogen production since it is a favourable kinetics with the supplied protons from a counterpart compared to that within alkaline environment....Hydrogen evolution reaction(HER)in acidic media has been spotlighted for hydrogen production since it is a favourable kinetics with the supplied protons from a counterpart compared to that within alkaline environment.However,there is no choice but to use a platinum-based catalyst yet.As for a noble metal-free electrocatalyst,incorporation of earth-abundant transition metal(TM)atoms into nanocarbon platforms has been extensively adopted.Although a data-driven methodology facilitates the rational design of TM-anchored carbon catalysts,its practical application suffers from either a simplified theoretical model or the prohibitive cost and complexity of experimental data generation.Herein,an effective and facile catalyst design strategy is proposed based on machine learning(ML)and its model verification using electrochemical methods accompanied by density functional theory simulations.Based on a Bayesian genetic algorithm ML model,the Ni-incorporated carbon quantum dots(Ni@CQD)loaded on a three-dimensional reduced graphene oxide conductor are proposed as the best HER catalyst amongst the various TM-incorporated CQDs under the optimal conditions of catalyst loading,electrode type,and temperature and pH of electrolyte.The ML results are validated with electrochemical experiments,where the Ni@CQD catalyst exhibited superior HER activity,requiring an overpotential of 151 mV to achieve 10 mAcm^(−2) with a Tafel slope of 52 mV dec^(−1) and impressive durability in acidic media up to 100 h.This methodology can provide an effective route for the rational design of highly active electrocatalysts for commercial applications.展开更多
With the advent of digital therapeutics(DTx),the development of software as a medical device(SaMD)for mobile and wearable devices has gained significant attention in recent years.Existing DTx evaluations,such as rando...With the advent of digital therapeutics(DTx),the development of software as a medical device(SaMD)for mobile and wearable devices has gained significant attention in recent years.Existing DTx evaluations,such as randomized clinical trials,mostly focus on verifying the effectiveness of DTx products.To acquire a deeper understanding of DTx engagement and behavioral adherence,beyond efficacy,a large amount of contextual and interaction data from mobile and wearable devices during field deployment would be required for analysis.In this work,the overall flow of the data-driven DTx analytics is reviewed to help researchers and practitioners to explore DTx datasets,to investigate contextual patterns associated with DTx usage,and to establish the(causal)relationship between DTx engagement and behavioral adherence.This review of the key components of datadriven analytics provides novel research directions in the analysis of mobile sensor and interaction datasets,which helps to iteratively improve the receptivity of existing DTx.展开更多
A versatile use of a sulfur self-doped biochar derived from Camellia japonica(camellia)flowers is demonstrated as a multifunctional catalyst for overall water splitting and a supercapacitor.The native sulfur content i...A versatile use of a sulfur self-doped biochar derived from Camellia japonica(camellia)flowers is demonstrated as a multifunctional catalyst for overall water splitting and a supercapacitor.The native sulfur content in the camellia flower facilitates in situ self-doping of sulfur,which highly activates the camellia-driven biochar(SA-Came)as a multifunctional catalyst with the enhanced electron-transfer ability and long-term durability.For water splitting,an SA-Came-based electrode is highly stable and shows reaction activities in both hydrogen and oxygen evolution reactions,with overpotentials of 154 and 362 mV at 10 mA cm^(−2),respectively.For supercapacitors,SA-Came achieves a specific capacitance of 125.42 F g^(−1)at 2 A g^(−1)and high cyclic stability in a three-electrode system in a 1 M KOH electrolyte.It demonstrated a high energy density of 34.54 Wh kg^(−1)at a power density of 1600 W kg^(−1)as a symmetric hybrid supercapacitor device with a wide working potential range of 0-1.6 V.展开更多
To demonstrate flexible and tandem device applications,a low-temperature Cu_(2)ZnSnSe_(4)(CZTSe)deposition process,combined with efficient alkali doping,was developed.First,high-quality CZTSe films were grown at 480℃...To demonstrate flexible and tandem device applications,a low-temperature Cu_(2)ZnSnSe_(4)(CZTSe)deposition process,combined with efficient alkali doping,was developed.First,high-quality CZTSe films were grown at 480℃by a single co-evaporation,which is applicable to polyimide(PI)substrate.Because of the alkali-free substrate,Na and K alkali doping were systematically studied and optimized to precisely control the alkali distribution in CZTSe.The bulk defect density was significantly reduced by suppression of deep acceptor states after the(NaF+KF)PDTs.Through the low-temperature deposition with(NaF+KF)PDTs,the CZTSe device on glass yields the best efficiency of 8.1%with an improved Voc deficit of 646 mV.The developed deposition technologies have been applied to PI.For the first time,we report the highest efficiency of 6.92%for flexible CZTSe solar cells on PI.Additionally,CZTSe devices were utilized as bottom cells to fabricate four-terminal CZTSe/perovskite tandem cells because of a low bandgap of CZTSe(~1.0 eV)so that the tandem cell yielded an efficiency of 20%.The obtained results show that CZTSe solar cells prepared by a low-temperature process with in-situ alkali doping can be utilized for flexible thin-film solar cells as well as tandem device applications.展开更多
The discovery of efficient,selective,and stable electrocatalysts can be a key point to produce the largescale chemical fuels via electrochemical CO_(2) reduction(ECR).In this study,an earth-abundant and nontoxic ZnO-b...The discovery of efficient,selective,and stable electrocatalysts can be a key point to produce the largescale chemical fuels via electrochemical CO_(2) reduction(ECR).In this study,an earth-abundant and nontoxic ZnO-based electrocatalyst was developed for use in gas-diffusion electrodes(GDE),and the effect of nitrogen(N)doping on the ECR activity of ZnO electrocatalysts was investigated.Initially,a ZnO nanosheet was prepared via the hydrothermal method,and nitridation was performed at different times to control the N-doping content.With an increase in the N-doping content,the morphological properties of the nanosheet changed significantly,namely,the 2D nanosheets transformed into irregularly shaped nanoparticles.Furthermore,the ECR performance of Zn O electrocatalysts with different N-doping content was assessed in 1.0 M KHCO_(3) electrolyte using a gas-diffusion electrode-based ECR cell.While the ECR activity increased after a small amount of N doping,it decreased for higher N doping content.Among them,the N:ZnO-1 h electrocatalysts showed the best CO selectivity,with a faradaic efficiency(FE_(CO))of 92.7%at-0.73 V vs.reversible hydrogen electrode(RHE),which was greater than that of an undoped Zn O electrocatalyst(FE_(CO)of 63.4%at-0.78 V_(RHE)).Also,the N:ZnO-1 h electrocatalyst exhibited outstanding durability for 16 h,with a partial current density of-92.1 mA cm^(-2).This improvement of N:ZnO-1 h electrocatalyst can be explained by density functional theory calculations,demonstrating that this improvement of N:ZnO-1 h electrocatalyst comes from(ⅰ)the optimized active sites lowering the free energy barrier for the rate-determining step(RDS),and(ⅱ)the modification of electronic structure enhancing the electron transfer rate by N doping.展开更多
The functionalities and diverse metastable phases of multiferroic BiFeO_(3)(BFO)thin films depend on the misfit strain.Although mixed phase-induced strain relaxation in multiphase BFO thin films is well known,it is un...The functionalities and diverse metastable phases of multiferroic BiFeO_(3)(BFO)thin films depend on the misfit strain.Although mixed phase-induced strain relaxation in multiphase BFO thin films is well known,it is unclear whether a singlecrystalline BFO thin film can accommodate misfit strain without the involvement of its polymorphs.Thus,understanding the strain relaxation behavior is key to elucidating the lattice strain–property relationship.In this study,a correlative strain analysis based on dark-field inline electron holography(DIH)and quantitative scanning transmission electron microscopy(STEM)was performed to reveal the structural mechanism for strain accommodation of a single-crystalline BFO thin film.The nanoscale DIH strain analysis results indicated a random combination of multiple strain states that acted as a primary strain relief,forming irregularly strained nanodomains.The STEM-based bond length measurement of the corresponding strained nanodomains revealed a unique strain accommodation behavior achieved by a statistical combination of multiple modes of distorted structures on the unit-cell scale.The globally integrated strain for each nanodomain was estimated to be close to1.5%,irrespective of the nanoscale strain states,which was consistent with the fully strained BFO film on the SrTiO_(3) substrate.Density functional theory calculations suggested that strain accommodation by the combination of metastable phases was energetically favored compared to single-phase-mediated relaxation.This discovery allows a comprehensive understanding of strain accommodation behavior in ferroelectric oxide films,such as BFO,with various low-symmetry polymorphs.展开更多
The conversion of solar energy to produce clean hydrogen fuel through water splitting is an emerging strategy for efficiently storing solar energy in the form of solar fuel.This aligns with the increasing global deman...The conversion of solar energy to produce clean hydrogen fuel through water splitting is an emerging strategy for efficiently storing solar energy in the form of solar fuel.This aligns with the increasing global demand for the development of an ideal energy alternative to fossil fuels that does not emit greenhouse gases.Electrochemical(EC) and photoelectrochemical(PEC) water splitting technologies have garnered significant attention worldwide for advanced hydrogen solar fuel production in recent decades.To achieve sustainable green H_(2) production,it is essential to create efficient catalyst materials that are low-cost and can replace expensive noble metal-based catalysts.These characteristics make them an ideal catalyst material for the process.Two-dimensional MXenes with M_(n+1)X_(n) structure have been identified as a promising option for EC and PEC water splitting due to their superior hydrophilicity,metal-like conductivity,large surface area,and adjustable surface chemistry.Here,we present a summary of recent advancements in the synthesis and performance enhancement methods for MXene hybrid materials in hydrogen production through EC and PEC water splitting.Furthermore,we examine the challenges and insights associated with the rational design of MXene-based hybrid materials to facilitate efficient water splitting for sustainable solar fuel production.展开更多
Electrocatalysis plays a crucial role in the field of clean energy conversion and provides essential support for the development of eco-friendly technology. There is a pressing need for electrocatalysts in renewable e...Electrocatalysis plays a crucial role in the field of clean energy conversion and provides essential support for the development of eco-friendly technology. There is a pressing need for electrocatalysts in renewable energy systems that exhibit exceptional activity, selectivity, stability, and economic viability. The utilization of metal oxides as electrocatalysts for the process of water splitting has made substantial progress in both theoretical and practical aspects and has emerged as a widely explored field of research. Tungsten oxides(WO_(x)) have attracted much attention and are regarded as a highly promising electrocatalytic material due to their exceptional electrocatalytic activity, cost-effectiveness, and ability to withstand extreme conditions. This review introduces the fundamental mechanism of WOx-based electrocatalysts for the hydrogen evolution reaction and the oxygen evolution reaction, providing a comprehensive overview of recent research advancements in their modification. Factors contributing to the catalytic activity and stability of WOxare explored, highlighting their potential for industrial applications. The aim herein is to provide guidelines for the design and fabrication of WOx-based electrocatalysts, thereby facilitating further research on their mechanistic properties and stability improvements in water splitting.展开更多
Electrochemical nitrate reduction(ENR)is an economical and eco-friendly method for converting industrial wastewater into valuable ammonia under atmospheric conditions.The main challenge lies in designing and developin...Electrochemical nitrate reduction(ENR)is an economical and eco-friendly method for converting industrial wastewater into valuable ammonia under atmospheric conditions.The main challenge lies in designing and developing highly durable ENR electrocatalysts.This study introduces defect-rich mesoporous CuO_(x) nanowires electrocatalyst synthesized using a novel solution-flame(sol-flame)hybrid method to control mesoporosity and introduce surface defects,thereby enhancing the electrochemical nitrate-toammonia production performance.We found surface defects(oxygen vacancies and Cu^(+))and unique mesoporous nanowire structure composed of tightly interconnected nanoparticles.The sol-flamesynthesized CuO_(x) nanowires(sf-CuO NWs)achieved superior ammonia yield rate(0.51 mmol h^(-1)cm^(-2)),faradaic efficiency(97.3%),and selectivity(86.2%)in 1 M KOH electrolyte(2000 ppm nitrate).This performance surpasses that of non-porous and less-defective CuO NWs and is attributed to the increased surface area and rapid electron transport facilitated by the distinctive morphology and generated defects.Theoretical calculation further suggests oxygen vacancies enhance NO_(3)^(-)adsorption on the sf-CuO NWs’surface and mitigate the competing hydrogen evolution reaction.This study outlines a strategic design and simple synthesis approach for nanowire electrocatalysts that boost the efficiency of electrochemical nitrate-to-ammonia conversion.展开更多
Ice-assisted synthesis is a facile,effective,and eco-friendly approach for preparing environmental functional materials.The quasi-liquid layer(QLL)or ice grain boundary(IGB)of the ice provides ideal interface-confined...Ice-assisted synthesis is a facile,effective,and eco-friendly approach for preparing environmental functional materials.The quasi-liquid layer(QLL)or ice grain boundary(IGB)of the ice provides ideal interface-confined environments for preparing two-dimensional(2D)sheet-like,three-dimensional(3D)hierarchical porous,polymeric hybrid,and atomically dispersed materials via the in-situ interfacial chemical reactions.Ice-templating physical pretreatment allows directional assembly of preformed materials,sheet exfoliation from bulk materials,transfer or cleaning of 2D materials,uniform dispersion of precursors,and self-assembly of nanoparticles.Additionally,the ice-melting process offers a novel way to prepare nanomaterials of uniform size due to the ultraslow release of reactants from the ice crystals.Furthermore,environmental applications of ice-assisted synthetic materials have been concluded.Advanced membrane materials synthesized based on ice chemistry exhibit superior water permeance,ion selectivity,and disinfection.Also,ice-assisted synthesis has innate advantages for designing environmental functional catalysts or adsorbents dedicated to environmental remediation.Finally,the challenges of the current progress in this field are discussed.展开更多
The synergistic effect of bi-component support catalysts via facile synthesis remains a pivotal challenge in catalysis,particularly under mild conditions.Therefore,this study reports an ultrasonication-plasma strategy...The synergistic effect of bi-component support catalysts via facile synthesis remains a pivotal challenge in catalysis,particularly under mild conditions.Therefore,this study reports an ultrasonication-plasma strategy to produce a PtGaPCoCoO@TiO_(x)site catalyst encapsulated within a high-entropy alloy framework.This approach harnesses instantaneous high-temperature plasma generated using an electrical field and ultrasonication under ambient conditions in H_(2)O.This study also elucidates the origin of the bifunctional effect in high-loading,ultra-stable,and ultra-fine PtGaPCoCoO catalysts,which are coated with a reducible TiO_(x)layer,thereby achieving optimal catalytic activity and hydrogen evolution reaction(HER)performance.PtGaPCo intimacy in PtGaPCoCoO@TiO_(x)is tuned and distributed on the porous titania coating based on strong metal-support interactions by leveraging the instantaneous high-energy input from plasma discharge and ultrasonication under ambient conditions in H_(2)O.PtGaPCoCoO@TiO_(x)exhibits remarkable selectivity and durability in the hydrogenation of 3-nitrophenylacetylene,even after 25 cycles with high conversion rates,significantly outperforming comparative catalysts lacking the ultrasonication plasma treatment and other reported catalysts.Furthermore,the catalyst exhibits exceptional HER activity,demonstrated by an overpotential of 187 mV at a current density of 10 mA cm^(-2)and a Tafel slope of 152 mV dec-1.This enhancement can be attributed to an increased electron density on the Pt surface within the PtGaPCo alloy.These findings highlight the potential of achieving synergistic chemical interactions among active metal sites in stable,industry-applicable catalysts.展开更多
The production of hydrogen using renewable energy sources requires efficient and stable catalysts.However,the development of such catalysts is hindered by the lack of efficient photo/electrocatalysts for the hydrogen ...The production of hydrogen using renewable energy sources requires efficient and stable catalysts.However,the development of such catalysts is hindered by the lack of efficient photo/electrocatalysts for the hydrogen evolution reaction(HER)and the oxygen evolution reaction(OER),as well as an insufficient understanding of the reaction mechanisms.This review comprehensively summarizes recent progress in photo/electrochemical hydrogen production technology and fundamental knowledge of reaction mechanisms.Specifically,it discusses recent developments in carbon-based materials for water splitting,with a focus on photoelectrocatalysts.The review highlights advancements in C-doped metal oxides,carbon quantum dots(CQD),MOF/COF-derived carbon,carbon nanotubes,graphene,carbon nitride-based materials,and strategies to enhance their catalytic activity and conductivity.Furthermore,integrating carbon-based materials with semiconductors and co-catalysts is explored to optimize overall performance.We outline practical routes to improve charge transfer and stability across carbon-based photoelectrocatalysts,providing a concise roadmap toward scalable and sustainable water splitting.展开更多
Hydrogen(H)spillover in nonreducible oxides such as zeolites and Al2O3 has been a highly controversial phenomenon in heterogeneous catalysis.Since industrial catalysts are predominantly prepared using these materials ...Hydrogen(H)spillover in nonreducible oxides such as zeolites and Al2O3 has been a highly controversial phenomenon in heterogeneous catalysis.Since industrial catalysts are predominantly prepared using these materials as supports,it is important to understand the mechanism and catalytic functions of H spillover on their surfaces.In the past decade,fundamental studies on zeolite-encapsulated metal catalysts have revealed that H spillover and reverse spillover can be utilized in the design of hydrogenation and dehydrogenation catalysts with improved properties.Both experimental and theoretical studies have indicated that H spillover can occur in nonreducible oxides when they possess substantial acid sites that aid the surface migration of active H.In the present review,we will discuss the possible mechanisms of H spillover in nonreducible oxides and the unique opportunities of using this phenomenon for the design of advanced hydroprocessing catalysts.展开更多
2D materials are regarded as promising electrocatalysts for water splitting because of their advances in providing ample active sites and improving electrochemical reaction kinetics.2D MoSe_(2)has a greater intrinsic ...2D materials are regarded as promising electrocatalysts for water splitting because of their advances in providing ample active sites and improving electrochemical reaction kinetics.2D MoSe_(2)has a greater intrinsic electrical conductivity and lower Gibbs free energy for reactant adsorption.However,there is still room for improvement in the electrocatalytic performance of MoSe_(2)for high-performance electrochemical water splitting devices.Herein,the in situ preparation of heterostructure made of covalently bonded MoSe_(2)and rGO is reported.The obtained electrocatalyst contains the aggregated 3D structured MoSe_(2)over rGO,which is covalently bonded together with more edge sites.The active edge sites of MoSe_(2)/rGO are dynamically involved in the electrocatalytic activity while facilitating electron transfer.Hence,the MoSe_(2)/rGO heterostructure requires a low cell voltage of 1.64 V to reach 100 mA cm^(−2)in water splitting with high reaction kinetics.The aggregated MoSe_(2)over rGO with more edge sites exposed by the 3D structure of MoSe_(2)and the interfacial covalent bond in between them provides a favorable electronic structure for the HER and OER with low overpotentials and high current densities and enhances the stability of the electrocatalyst.This work presents an attractive and cost-effective electrocatalyst suitable for industrial-scale hydrogen fuel production.展开更多
基金supported by the GRRC program of Gyeonggi Province(GRRC Sungkyunkwan 2023-B01)the support of Korea Institute of Energy Technology Evaluation and Planning(KETEP)and the Ministry of Trade,Industry&Energy(MOTIE)of the Republic of Korea(No.20224000000100)the research support of KENTECH foundation research grant supported by MOTIE。
文摘Metal dichalcogenide-based 2D materials,gained considerable attention recently as a hydrogen evolution reaction(HER)electrocatalyst.In this work,we synthesized MoSe_(2)-based electrocatalyst via hydrothermal route with varying phase contents(1T/2H)and respective HER performances were evaluated under the acidic media(0.5 M H_(2)SO_(4)),where best HER performance was obtained from the sample consisting of mixed 1T/2H phases,which was directly grown on a carbon paper(167 mV at10 mA cm^(-2))Furthermore,HER performance of electrocatalyst was further improved by in-situ electrodeposition of Pt nanoparticles(0.15 wt%)on the MoSe_(2) surface,which lead to significant enhancement in the HER performances(133 mV at 10 mA cm^(-2)).Finally,we conducted density functional theory calculations to reveal the origin of such enhanced performances when the mixed 1T/2H phases were present,where phase boundary region(1T/2H heterojunction)act as a low energy pathway for H_(2)adsorption and desorption via electron accumulation effect.Moreover,presence of the Pt nanoparticles tunes the electronic states of the MoSe_(2)based catalyst,resulting in the enhanced HER activity at heterointerface of 1T/2H MoSe_(2) while facilitating the hydrogen adsorption and desorption process providing a low energy pathway for HER.These results provide new insight on atomic level understanding of the MoSe_(2) based catalyst for HER application.
基金financially supported by the Leader Project at the Korea Institute of Energy Technology(KENTECH)for Environmental and Climate Technology,funded by the Ministry of Science and ICT through the National Research Foundation of Korea(No.2020R1A3B3079715)The large-scale CO_(2)RR for future work is in process and is financially supported by the Korea Evaluation Institute of Industrial Technology(Alchemist Project,NTIS-2410005253,20018904)through the Ministry of Trade,Industry and Energy,Koreasupported by the National Supercomputing Center with supercomputing resources,including technical support(KSC-2022-CRE-0286).
文摘Achieving carbon neutrality is urgent due to the critical issue of climate change.To reach this goal,the development of new,breakthrough technologies is necessary and urgent.One such technology involves efficient carbon capture and its conversion into useful chemicals or fuels.However,achieving considerable amounts of efficiency in this field is a very challenging task.Even in natural photosynthesis occurring in plant leaves,the CO_(2)conversion efficiency into hydrocarbons cannot exceed a value of 1%.Nevertheless,recently few reports show comparable higher efficiency in CO_(2)to gaseous products such as carbon monoxide(CO),but it is hard to find selective liquid fuel products with a high value of solar to liquid fuel conversion efficiency.Herein,a NiFe-assisted hybrid composite dark cathode is employed for the selective production of solar-to-liquid fuels,in conjunction with a BiVO4 photoanode.This process results in the generation of significant amounts of formaldehyde,ethanol,and methanol selectively.The primary objective of this study is to design and optimize a novel photoelectrochemical(PEC)system to produce solar-to-liquid fuels selectively.This study shows the enhancement of the solar-to-fuel conversion efficiency over 1.5%by employing a hybrid composite cathode composed of NiFe-assisted reduced graphene oxide(rGO),poly(4-vinyl)pyridine(PVP),and Nafion.
基金supported by the National Natural Science Foundation of China(No.52200049)the China Postdoctoral Science Foundation(No.2022TQ0089)+2 种基金the Heilongjiang Province Postdoctoral Science Foundation(No.LBH-Z22181)the State Key Laboratory of Urban Water Resource and Environment(Harbin Institute of Technology)(No.2024TS28)the Fundamental Research Funds for the Central Universities。
文摘The advanced oxidation system based on peracetic acid(PAA)has been proved to be a green and safe oxidation decontamination technology.Among them,the key challenge and complexity in current research lies in the directional induction of PAA and its utilization for selective removal of refractory pollutants.This study prepared nitrogen-doped biochar(NBC)using compound pharmaceutical residues commonly found in traditional Chinese medicine as a precursor.A system based on NBC-activated PAA was constructed for sulfamethoxazole(SMX)degradation.The introduction of nitrogen significantly enhanced the degree of graphitization in NBC.The degradation system achieved 87.89%SMX degradation efficiency within 60 min.Furthermore,the formation of the intricate NBC-PAA*complex detected by in-situ Raman was of paramount importance as it facilitates enhanced electron transfer processes within the complex,thereby promoting PAA decomposition through electron loss.The formation of a new complex between SMX and NBC-PAA*facilitated the completion of electron transfer process within the complex.In summary,this study explored a novel approach for treating and disposing of solid waste from Chinese medicine residue by successfully inducing non-free radical degradation pathway using PAA system.It offers fresh insights and ideas in the fields of water treatment and solid waste management.
基金supported by the open fund from Key Lab of Eco-restoration of Regional Contaminated Environment(Shenyang University),Ministry of Education(No.KF-22-08)the National Natural Science Foundation of China(Nos.22003074 and 42177406)+1 种基金the Youth Innovation Promotion Association CAS,Guangdong Basic and Applied Basic Research Foundation(No.2023A1515011410)S.Liu gratefully acknowledges the financial support by the National Natural Science Foundation of China(No.52302223).
文摘Typical p-n junctions have emerged as a promising strategy for contending with charge carrier recombination in solar conversion.However,the photo-corrosion and unsuitable energy band positions still hinder their practical application for hydrogen production from water in photoelectrochemical systems.Here,an in-situ photo-oxidation method is proposed for achieving self-adapting activation of BiVO_(4)-based photoanodes with surface-encapsulated CuGaS_(2)particles by the ZnO layer.The self-adapting activation demotes the energy band positions of CuGaS_(2),establishing an S-scheme structure with BiVO_(4),resulting in an efficient p-n junction photoanode.The optimal sample exhibits enhanced photocurrent and an onset potential cathodically shifted by~300 mV compared with BiVO_(4),which is attributed to significantly enhanced charge transport and transfer efficiencies.As expected,it attains the highest photocurrent value of 5.87 mA·cm^(-2),aided by a hole scavenger at 1.23 V versus a reversible hydrogen electrode,which significantly surpasses that of BiVO_(4)(4.32 mA·cm^(-2)).
基金the Ministry of Higher Education Malaysia for financial support under the Fundamental Research Grant Scheme No.FRGS/1/2021/TKO/UMP/02/75(RDU210141)Universiti Malaysia Pahang Al-Sultan Abdullah for providing laboratory facilities and financial support under Internal Grant RDU210350。
文摘Conventional organic coatings often face limitations in providing long-term corrosion protection in aggressive environments.This study introduces a dual-functional polydopamine-zinc oxide(PD-Z)composite incorporated into an epoxy(EP)matrix(PD-Z/EP)to enhance the hydrophobicity and corrosion resistance of aluminum substrates.Characterization analyses confirmed the successful fabrication of the PD-Z composite.Electrochemical measurements,specifically potentiodynamic polarization,are conducted after three days of immersion in a 3.5%(mass)NaCl solution,significantly decreasing corrosion current density(Icorr)from 249.4 nA·cm^(-2)for pure EP to 167 nA·cm^(-2)for PD-Z/EP.Concurrently,the corrosion rate decreased from 0.004 to 0.0002 mm·a^(-1).Additionally,electrochemical impedance spectroscopy(EIS)demonstrated a marked increase in the low-frequency impedance modulus(|Z|_(0.01)_(Hz))from 0.07×10^(6) to 1.2114×10^(6)Ω·cm^(-2),indicating superior corrosion inhibition.The exceptional anodic and cathodic protective performance of the PD-Z/EP coating is attributed to the synergistic effects of polydopamine and ZnO,which enhance chloride ion entrapment,hydrophobic barrier properties,and overall corrosion resistance.
基金supported by the National Natural Science Foundation of China(No.52200049)the China Postdoctoral Science Foundation(No.2022TQ0089)the Heilongjiang Province Postdoctoral Science Foundation(No.LBHZ22181).
文摘Humic acid(HA),as a represent of natural organic matter widely existing in water body,dose harm to water quality and human health;however,it was commonly treated as an environmental background substance while not targeted contaminant in advanced oxidation processes(AOPs).Herein,we investigated the removal of HA in the alkali-activated biochar(KBC)/peroxymonosulfate(PMS)system.The modification of the original biochar(BC)resulted in an increased adsorption capacity and catalytic activity due to the introduction of more micropores,mesopores,and oxygen-containing functional groups,particularly carbonyl groups.Mechanistic insights indicated that HA is primarily chemically adsorbed on the KBC surface,while singlet oxygen(^(1)O_(2))produced by the PMS decomposition served as the major reactive species for the degradation of HA.An underlying synergistic adsorption and oxidation mechanism involving a local high concentration reaction region around the KBC interface was then proposed.This work not only provides a cost-effective solution for the elimination of HA but also advances our understanding of the nonradical oxidation at the biochar interface.
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korean government(MSIT)(NRF-2022R1A2C1011559,No.RS-2024-00405818 and NRF-2021M3H4A6A01045764)by the National Supercomputing Center with supercomputing resources including technical support(KSC-2024-CRE-0196)by Korea Basic Science Institute(National Research Facilities and Equipment Center)grant funded by the Ministry of Science and ICT(No.RS-2024-00404712).
文摘Hydrogen evolution reaction(HER)in acidic media has been spotlighted for hydrogen production since it is a favourable kinetics with the supplied protons from a counterpart compared to that within alkaline environment.However,there is no choice but to use a platinum-based catalyst yet.As for a noble metal-free electrocatalyst,incorporation of earth-abundant transition metal(TM)atoms into nanocarbon platforms has been extensively adopted.Although a data-driven methodology facilitates the rational design of TM-anchored carbon catalysts,its practical application suffers from either a simplified theoretical model or the prohibitive cost and complexity of experimental data generation.Herein,an effective and facile catalyst design strategy is proposed based on machine learning(ML)and its model verification using electrochemical methods accompanied by density functional theory simulations.Based on a Bayesian genetic algorithm ML model,the Ni-incorporated carbon quantum dots(Ni@CQD)loaded on a three-dimensional reduced graphene oxide conductor are proposed as the best HER catalyst amongst the various TM-incorporated CQDs under the optimal conditions of catalyst loading,electrode type,and temperature and pH of electrolyte.The ML results are validated with electrochemical experiments,where the Ni@CQD catalyst exhibited superior HER activity,requiring an overpotential of 151 mV to achieve 10 mAcm^(−2) with a Tafel slope of 52 mV dec^(−1) and impressive durability in acidic media up to 100 h.This methodology can provide an effective route for the rational design of highly active electrocatalysts for commercial applications.
基金supported by Basic Science Research Program through the National Research Foundation of Korea(NRF)funded by the Korea government(MSIT)(2020R1A4A1018774)。
文摘With the advent of digital therapeutics(DTx),the development of software as a medical device(SaMD)for mobile and wearable devices has gained significant attention in recent years.Existing DTx evaluations,such as randomized clinical trials,mostly focus on verifying the effectiveness of DTx products.To acquire a deeper understanding of DTx engagement and behavioral adherence,beyond efficacy,a large amount of contextual and interaction data from mobile and wearable devices during field deployment would be required for analysis.In this work,the overall flow of the data-driven DTx analytics is reviewed to help researchers and practitioners to explore DTx datasets,to investigate contextual patterns associated with DTx usage,and to establish the(causal)relationship between DTx engagement and behavioral adherence.This review of the key components of datadriven analytics provides novel research directions in the analysis of mobile sensor and interaction datasets,which helps to iteratively improve the receptivity of existing DTx.
基金National Research Foundation of Korea,Grant/Award Numbers:2016M3D1A1021141,2020R1A2C2006077,2022R1A2C1012419,2021R1A4A1024129,2021R1A5A1030054Ministry of Trade,Industry and Energy(MOTIE,Korea),Grant/Award Number:20213030040590。
文摘A versatile use of a sulfur self-doped biochar derived from Camellia japonica(camellia)flowers is demonstrated as a multifunctional catalyst for overall water splitting and a supercapacitor.The native sulfur content in the camellia flower facilitates in situ self-doping of sulfur,which highly activates the camellia-driven biochar(SA-Came)as a multifunctional catalyst with the enhanced electron-transfer ability and long-term durability.For water splitting,an SA-Came-based electrode is highly stable and shows reaction activities in both hydrogen and oxygen evolution reactions,with overpotentials of 154 and 362 mV at 10 mA cm^(−2),respectively.For supercapacitors,SA-Came achieves a specific capacitance of 125.42 F g^(−1)at 2 A g^(−1)and high cyclic stability in a three-electrode system in a 1 M KOH electrolyte.It demonstrated a high energy density of 34.54 Wh kg^(−1)at a power density of 1600 W kg^(−1)as a symmetric hybrid supercapacitor device with a wide working potential range of 0-1.6 V.
基金financially supported by the Korea Institute of Energy Research(KIER)(grant no.C3-2401,2402,2403)the National Research Foundation(grant no.2022M3J1A1063019)funded by the Ministry of Science and ICT
文摘To demonstrate flexible and tandem device applications,a low-temperature Cu_(2)ZnSnSe_(4)(CZTSe)deposition process,combined with efficient alkali doping,was developed.First,high-quality CZTSe films were grown at 480℃by a single co-evaporation,which is applicable to polyimide(PI)substrate.Because of the alkali-free substrate,Na and K alkali doping were systematically studied and optimized to precisely control the alkali distribution in CZTSe.The bulk defect density was significantly reduced by suppression of deep acceptor states after the(NaF+KF)PDTs.Through the low-temperature deposition with(NaF+KF)PDTs,the CZTSe device on glass yields the best efficiency of 8.1%with an improved Voc deficit of 646 mV.The developed deposition technologies have been applied to PI.For the first time,we report the highest efficiency of 6.92%for flexible CZTSe solar cells on PI.Additionally,CZTSe devices were utilized as bottom cells to fabricate four-terminal CZTSe/perovskite tandem cells because of a low bandgap of CZTSe(~1.0 eV)so that the tandem cell yielded an efficiency of 20%.The obtained results show that CZTSe solar cells prepared by a low-temperature process with in-situ alkali doping can be utilized for flexible thin-film solar cells as well as tandem device applications.
基金supported by the Basic Science Research Program through the National Research Foundation of Korea (NRF) (Grant Nos.2018R1A6A1A03024334,2019R1A2C1007637,2021M3I3A1082880,2021R1I1A1A01044174)the Basic Science Research Capacity Enhancement Project through Korea Basic Science Institute (Grant No.2019R1A6C1010024)。
文摘The discovery of efficient,selective,and stable electrocatalysts can be a key point to produce the largescale chemical fuels via electrochemical CO_(2) reduction(ECR).In this study,an earth-abundant and nontoxic ZnO-based electrocatalyst was developed for use in gas-diffusion electrodes(GDE),and the effect of nitrogen(N)doping on the ECR activity of ZnO electrocatalysts was investigated.Initially,a ZnO nanosheet was prepared via the hydrothermal method,and nitridation was performed at different times to control the N-doping content.With an increase in the N-doping content,the morphological properties of the nanosheet changed significantly,namely,the 2D nanosheets transformed into irregularly shaped nanoparticles.Furthermore,the ECR performance of Zn O electrocatalysts with different N-doping content was assessed in 1.0 M KHCO_(3) electrolyte using a gas-diffusion electrode-based ECR cell.While the ECR activity increased after a small amount of N doping,it decreased for higher N doping content.Among them,the N:ZnO-1 h electrocatalysts showed the best CO selectivity,with a faradaic efficiency(FE_(CO))of 92.7%at-0.73 V vs.reversible hydrogen electrode(RHE),which was greater than that of an undoped Zn O electrocatalyst(FE_(CO)of 63.4%at-0.78 V_(RHE)).Also,the N:ZnO-1 h electrocatalyst exhibited outstanding durability for 16 h,with a partial current density of-92.1 mA cm^(-2).This improvement of N:ZnO-1 h electrocatalyst can be explained by density functional theory calculations,demonstrating that this improvement of N:ZnO-1 h electrocatalyst comes from(ⅰ)the optimized active sites lowering the free energy barrier for the rate-determining step(RDS),and(ⅱ)the modification of electronic structure enhancing the electron transfer rate by N doping.
基金Samsung Research Fundings&Incubation Center of Samsung Electronics(Grant No.SRFCMA1702-01)Y.-M.K acknowledges partial support from the National Research Foundation of Korea(NRF)(Grant No.2023R1A2C2002403)funded by the Korean government in KoreaA.Borisevich acknowledges support from FaCT,an Energy Frontier Research Center funded by the U.S.Department of Energy,Office of Science,Office of Basic Energy Science,Collaboratives Research Division.
文摘The functionalities and diverse metastable phases of multiferroic BiFeO_(3)(BFO)thin films depend on the misfit strain.Although mixed phase-induced strain relaxation in multiphase BFO thin films is well known,it is unclear whether a singlecrystalline BFO thin film can accommodate misfit strain without the involvement of its polymorphs.Thus,understanding the strain relaxation behavior is key to elucidating the lattice strain–property relationship.In this study,a correlative strain analysis based on dark-field inline electron holography(DIH)and quantitative scanning transmission electron microscopy(STEM)was performed to reveal the structural mechanism for strain accommodation of a single-crystalline BFO thin film.The nanoscale DIH strain analysis results indicated a random combination of multiple strain states that acted as a primary strain relief,forming irregularly strained nanodomains.The STEM-based bond length measurement of the corresponding strained nanodomains revealed a unique strain accommodation behavior achieved by a statistical combination of multiple modes of distorted structures on the unit-cell scale.The globally integrated strain for each nanodomain was estimated to be close to1.5%,irrespective of the nanoscale strain states,which was consistent with the fully strained BFO film on the SrTiO_(3) substrate.Density functional theory calculations suggested that strain accommodation by the combination of metastable phases was energetically favored compared to single-phase-mediated relaxation.This discovery allows a comprehensive understanding of strain accommodation behavior in ferroelectric oxide films,such as BFO,with various low-symmetry polymorphs.
基金the result of a research project conducted with the funds of the Open R&D program of Korea Electric Power Corporation (R23XO04)supported by the Technology Innovation Program funded by the Ministry of Trade, Industry & Energy (MOTIE, Korea) (K_G012002238601)+2 种基金by “Regional Innovation Strategy (RIS)” through the National Research Foundation of Korea (NRF) funded by the Ministry of Education (MOE) (2021RIS-002)by the National Research Foundation of Korea (NRF) grant funded by the Korea government (MSIT) (No. 2021M3I3A1082880)by the Korea Institute of Energy Technology Evaluation and Planning (KETEP) and the Ministry of Trade, Industry & Energy (MOTIE) of the Republic of Korea (No. 20224000000320)。
文摘The conversion of solar energy to produce clean hydrogen fuel through water splitting is an emerging strategy for efficiently storing solar energy in the form of solar fuel.This aligns with the increasing global demand for the development of an ideal energy alternative to fossil fuels that does not emit greenhouse gases.Electrochemical(EC) and photoelectrochemical(PEC) water splitting technologies have garnered significant attention worldwide for advanced hydrogen solar fuel production in recent decades.To achieve sustainable green H_(2) production,it is essential to create efficient catalyst materials that are low-cost and can replace expensive noble metal-based catalysts.These characteristics make them an ideal catalyst material for the process.Two-dimensional MXenes with M_(n+1)X_(n) structure have been identified as a promising option for EC and PEC water splitting due to their superior hydrophilicity,metal-like conductivity,large surface area,and adjustable surface chemistry.Here,we present a summary of recent advancements in the synthesis and performance enhancement methods for MXene hybrid materials in hydrogen production through EC and PEC water splitting.Furthermore,we examine the challenges and insights associated with the rational design of MXene-based hybrid materials to facilitate efficient water splitting for sustainable solar fuel production.
基金supported by the National Natural Science Foundation of China (grant no. 51902292)the China Postdoctoral Science Foundation (grant no. 2024M752942)the Project funding for Young Backbone Teachers in Colleges and Universities of Henan Province (2020GGJS013)。
文摘Electrocatalysis plays a crucial role in the field of clean energy conversion and provides essential support for the development of eco-friendly technology. There is a pressing need for electrocatalysts in renewable energy systems that exhibit exceptional activity, selectivity, stability, and economic viability. The utilization of metal oxides as electrocatalysts for the process of water splitting has made substantial progress in both theoretical and practical aspects and has emerged as a widely explored field of research. Tungsten oxides(WO_(x)) have attracted much attention and are regarded as a highly promising electrocatalytic material due to their exceptional electrocatalytic activity, cost-effectiveness, and ability to withstand extreme conditions. This review introduces the fundamental mechanism of WOx-based electrocatalysts for the hydrogen evolution reaction and the oxygen evolution reaction, providing a comprehensive overview of recent research advancements in their modification. Factors contributing to the catalytic activity and stability of WOxare explored, highlighting their potential for industrial applications. The aim herein is to provide guidelines for the design and fabrication of WOx-based electrocatalysts, thereby facilitating further research on their mechanistic properties and stability improvements in water splitting.
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korea government(MSIT)(No.-RS-2024-00335976)。
文摘Electrochemical nitrate reduction(ENR)is an economical and eco-friendly method for converting industrial wastewater into valuable ammonia under atmospheric conditions.The main challenge lies in designing and developing highly durable ENR electrocatalysts.This study introduces defect-rich mesoporous CuO_(x) nanowires electrocatalyst synthesized using a novel solution-flame(sol-flame)hybrid method to control mesoporosity and introduce surface defects,thereby enhancing the electrochemical nitrate-toammonia production performance.We found surface defects(oxygen vacancies and Cu^(+))and unique mesoporous nanowire structure composed of tightly interconnected nanoparticles.The sol-flamesynthesized CuO_(x) nanowires(sf-CuO NWs)achieved superior ammonia yield rate(0.51 mmol h^(-1)cm^(-2)),faradaic efficiency(97.3%),and selectivity(86.2%)in 1 M KOH electrolyte(2000 ppm nitrate).This performance surpasses that of non-porous and less-defective CuO NWs and is attributed to the increased surface area and rapid electron transport facilitated by the distinctive morphology and generated defects.Theoretical calculation further suggests oxygen vacancies enhance NO_(3)^(-)adsorption on the sf-CuO NWs’surface and mitigate the competing hydrogen evolution reaction.This study outlines a strategic design and simple synthesis approach for nanowire electrocatalysts that boost the efficiency of electrochemical nitrate-to-ammonia conversion.
基金supported by National Natural Science Foundation of China(Nos.52170030,52200049)China Postdoctoral Science Foundation(No.2022TQ0089)+2 种基金State Key Laboratory of Urban-rural Water Resource and Environment(Harbin Institute of Technology)(No.2024TS28)Young Scientist Studio of Harbin Institute of TechnologyFundamental Research Funds for the Central Universities。
文摘Ice-assisted synthesis is a facile,effective,and eco-friendly approach for preparing environmental functional materials.The quasi-liquid layer(QLL)or ice grain boundary(IGB)of the ice provides ideal interface-confined environments for preparing two-dimensional(2D)sheet-like,three-dimensional(3D)hierarchical porous,polymeric hybrid,and atomically dispersed materials via the in-situ interfacial chemical reactions.Ice-templating physical pretreatment allows directional assembly of preformed materials,sheet exfoliation from bulk materials,transfer or cleaning of 2D materials,uniform dispersion of precursors,and self-assembly of nanoparticles.Additionally,the ice-melting process offers a novel way to prepare nanomaterials of uniform size due to the ultraslow release of reactants from the ice crystals.Furthermore,environmental applications of ice-assisted synthetic materials have been concluded.Advanced membrane materials synthesized based on ice chemistry exhibit superior water permeance,ion selectivity,and disinfection.Also,ice-assisted synthesis has innate advantages for designing environmental functional catalysts or adsorbents dedicated to environmental remediation.Finally,the challenges of the current progress in this field are discussed.
基金supported by two Mid-Level Researcher National Projects of the National Research Foundation(NRF)funded by the Ministry of Science and ICT,Republic of Korea(NRF-2022R1A2C1004392).
文摘The synergistic effect of bi-component support catalysts via facile synthesis remains a pivotal challenge in catalysis,particularly under mild conditions.Therefore,this study reports an ultrasonication-plasma strategy to produce a PtGaPCoCoO@TiO_(x)site catalyst encapsulated within a high-entropy alloy framework.This approach harnesses instantaneous high-temperature plasma generated using an electrical field and ultrasonication under ambient conditions in H_(2)O.This study also elucidates the origin of the bifunctional effect in high-loading,ultra-stable,and ultra-fine PtGaPCoCoO catalysts,which are coated with a reducible TiO_(x)layer,thereby achieving optimal catalytic activity and hydrogen evolution reaction(HER)performance.PtGaPCo intimacy in PtGaPCoCoO@TiO_(x)is tuned and distributed on the porous titania coating based on strong metal-support interactions by leveraging the instantaneous high-energy input from plasma discharge and ultrasonication under ambient conditions in H_(2)O.PtGaPCoCoO@TiO_(x)exhibits remarkable selectivity and durability in the hydrogenation of 3-nitrophenylacetylene,even after 25 cycles with high conversion rates,significantly outperforming comparative catalysts lacking the ultrasonication plasma treatment and other reported catalysts.Furthermore,the catalyst exhibits exceptional HER activity,demonstrated by an overpotential of 187 mV at a current density of 10 mA cm^(-2)and a Tafel slope of 152 mV dec-1.This enhancement can be attributed to an increased electron density on the Pt surface within the PtGaPCo alloy.These findings highlight the potential of achieving synergistic chemical interactions among active metal sites in stable,industry-applicable catalysts.
基金supported by the Outsourced R&D Project of Korea Electric Power Corporation(KEPCO)(Grant number:R23XO04)supported by the Korea Institute for Advancement of Technology(KIAT)grant funded by the Ministry of Trade,Industry,and Energy(MOTIE),Republic of Korea,(P0025273)supported by the Korea Institute of Energy Technology Evaluation and Planning(KETEP)and the Ministry of Trade,Industry&Energy(MOTIE)of the Republic of Korea.(No.RS-2025-07852969).
文摘The production of hydrogen using renewable energy sources requires efficient and stable catalysts.However,the development of such catalysts is hindered by the lack of efficient photo/electrocatalysts for the hydrogen evolution reaction(HER)and the oxygen evolution reaction(OER),as well as an insufficient understanding of the reaction mechanisms.This review comprehensively summarizes recent progress in photo/electrochemical hydrogen production technology and fundamental knowledge of reaction mechanisms.Specifically,it discusses recent developments in carbon-based materials for water splitting,with a focus on photoelectrocatalysts.The review highlights advancements in C-doped metal oxides,carbon quantum dots(CQD),MOF/COF-derived carbon,carbon nanotubes,graphene,carbon nitride-based materials,and strategies to enhance their catalytic activity and conductivity.Furthermore,integrating carbon-based materials with semiconductors and co-catalysts is explored to optimize overall performance.We outline practical routes to improve charge transfer and stability across carbon-based photoelectrocatalysts,providing a concise roadmap toward scalable and sustainable water splitting.
基金supported by the Basic Science Research Program of the National Research Foundation of Korea(No.NRF-2020R1A2C3003694)the KAIST Cross-Generation Collaborative Lab Project.
文摘Hydrogen(H)spillover in nonreducible oxides such as zeolites and Al2O3 has been a highly controversial phenomenon in heterogeneous catalysis.Since industrial catalysts are predominantly prepared using these materials as supports,it is important to understand the mechanism and catalytic functions of H spillover on their surfaces.In the past decade,fundamental studies on zeolite-encapsulated metal catalysts have revealed that H spillover and reverse spillover can be utilized in the design of hydrogenation and dehydrogenation catalysts with improved properties.Both experimental and theoretical studies have indicated that H spillover can occur in nonreducible oxides when they possess substantial acid sites that aid the surface migration of active H.In the present review,we will discuss the possible mechanisms of H spillover in nonreducible oxides and the unique opportunities of using this phenomenon for the design of advanced hydroprocessing catalysts.
基金National Research Foundation of Korea,Grant/Award Number:RS-2023-00248447Ministry of Science and the Korean Government(MSIT),Republic of Korea,Grant/Award Number:RS-2023-00248447+3 种基金The Korea Institute of Energy Technology Evaluation and Planning(KETEP),Grant/Award Numbers:RS-2023-00242227,20224000000320Ministry of Trade,Industry,and Energy,Republic of Korea,Grant/Award Numbers:RS-2023-00242227,20224000000320Korea Electric Power Corporation(KEPCO),Grant/Award Number:R23XO04KENTECH Research Grant,Grant/Award Number:KRG2022-01-016。
文摘2D materials are regarded as promising electrocatalysts for water splitting because of their advances in providing ample active sites and improving electrochemical reaction kinetics.2D MoSe_(2)has a greater intrinsic electrical conductivity and lower Gibbs free energy for reactant adsorption.However,there is still room for improvement in the electrocatalytic performance of MoSe_(2)for high-performance electrochemical water splitting devices.Herein,the in situ preparation of heterostructure made of covalently bonded MoSe_(2)and rGO is reported.The obtained electrocatalyst contains the aggregated 3D structured MoSe_(2)over rGO,which is covalently bonded together with more edge sites.The active edge sites of MoSe_(2)/rGO are dynamically involved in the electrocatalytic activity while facilitating electron transfer.Hence,the MoSe_(2)/rGO heterostructure requires a low cell voltage of 1.64 V to reach 100 mA cm^(−2)in water splitting with high reaction kinetics.The aggregated MoSe_(2)over rGO with more edge sites exposed by the 3D structure of MoSe_(2)and the interfacial covalent bond in between them provides a favorable electronic structure for the HER and OER with low overpotentials and high current densities and enhances the stability of the electrocatalyst.This work presents an attractive and cost-effective electrocatalyst suitable for industrial-scale hydrogen fuel production.
