Activated carbon nanofibers(ACNFs)with small diameter can significantly increase the accessibility of intra pores and accelerate adsorption of molecules from water.In this study,ACNFs were made by blending K_(2)CO_(3)...Activated carbon nanofibers(ACNFs)with small diameter can significantly increase the accessibility of intra pores and accelerate adsorption of molecules from water.In this study,ACNFs were made by blending K_(2)CO_(3)or ZnCl_(2)as the activating agent into the polyacrylonitrile(PAN)in dimethylformamide solution for electrospinning prior to pyrolysis.Bisphenol-A(BPA),an endocrine disruption pollutant,is widely applied in the production of polycarbonate plastics and epoxy resins.Accordingly,BPA is often used as a model contaminant commonly removed via adsorption.Batch adsorption studies were used to evaluate the kinetics and adsorption capacity of the ACNFs.Redlich-Peterson(R-P)and Langmuir models were found to fit the isotherm of BPA adsorption better than Freundlich model,showing the homogeneous nature of the PAN originated ACNFs.The adsorption kinetics was better described by the pseudo second-order model than that by the pseudo first-order model.The fitting by intraparticle diffusion model indicates the adsorption of BPA onto ACNFs is mainly controlled by pore diffusion.High pH value and ionic strength reduced BPA adsorption from aqueous solution.The breakthrough curves studied in two different fixed bed systems(cross flow bed system and packed flow bed system)confirmed the scalability of BPA removal by ACNFs in dynamic adsorption processes.The modified dose-response model predicted well the fixed-bed outlet concentration profiles.展开更多
Despite the proficiency of lithium(Li)-7 NMR spectroscopy in delineating the physical and chemical states of Li metal electrodes,challenges in specimen preparation and interpretation impede its progress.In this study,...Despite the proficiency of lithium(Li)-7 NMR spectroscopy in delineating the physical and chemical states of Li metal electrodes,challenges in specimen preparation and interpretation impede its progress.In this study,we conducted a comprehensive postmortem analysis utilizing ^(7)Li NMR,employing a stan-dard magic angle spinning probe to examine protective-layer coated Li metal electrodes and LiAg alloy electrodes against bare Li metal electrodes within Li metal batteries(LMBs).Our investigation explores the effects of sample burrs,alignment with the magnetic field,the existence of liquid electrolytes,and precycling on the ^(7)Li NMR signals.Through contrasting NMR spectra before and after cycling,we identi-fied alterations in Li^(0) and Li^(+) signals attributable to the degradation of the Li metal electrode.Our NMR analyses decisively demonstrate the efficacy of the protective layer in mitigating dendrite and solid elec-trolyte interphase formation.Moreover,we noted that Li*ions near the Li metal surface exhibit magnetic susceptibility anisotropy,revealing a novel approach to studying diamagnetic species on Li metal elec-trodes in LMBs.This study provides valuable insights and practical guidelines for characterizing distinct lithium states within LMBs.展开更多
Powered by electricity from renewable energies,electrochemical reduction of CO_(2)could not only efficiently alleviate the excess emission of CO_(2),but also produce many kinds of valuable chemical feedstocks.Among va...Powered by electricity from renewable energies,electrochemical reduction of CO_(2)could not only efficiently alleviate the excess emission of CO_(2),but also produce many kinds of valuable chemical feedstocks.Among various catalysts,single atom catalysts(SACs)have attracted much attention due to their high atom utilization efficiency and expressive catalytic performances.Additionally,SACs serve as an ideal platform for the investigation of complex reaction pathways and mechanisms thanks to their explicit active sites.In this review,the possible re-action pathways for the generation of various products(mainly C1 products for SACs)were firstly summarized.Then,recent progress of SACs for electrochemical reduction of CO_(2)was discussed in aspect of different central metal sites.As the most popular and efficient coordination modulation strategy,introducing heteroatom was then reviewed.Moreover,as an extension of SACs,the development of dual atom catalysts was also briefly discussed.At last,some issues and challenges regarding the SACs for CO_(2)reduction reaction(CO_(2)RR)were listed,followed by corresponding suggestions.展开更多
Plastic,renowned for its versatility,durability,and cost-effectiveness,is indispensable in modern society.Nevertheless,the annual production of nearly 400 million tons of plastic,coupled with a recycling rate of only ...Plastic,renowned for its versatility,durability,and cost-effectiveness,is indispensable in modern society.Nevertheless,the annual production of nearly 400 million tons of plastic,coupled with a recycling rate of only 9%,has led to a monumental environmental crisis.Plastic recycling has emerged as a vital response to this crisis,offering sustainable solutions to mitigate its environmental impact.Among these recycling efforts,plastic upcycling has garnered attention,which elevates discarded plastics into higher-value products.Here,electrocatalytic and photoelectrocatalytic treatments stand at the forefront of advanced plastic upcycling.Electrocatalytic or photoelectrocatalytic treatments involve chemical reactions that facilitate electron transfer through the electrode/electrolyte interface,driven by electrical or solar energy,respectively.These methods enable precise control of chemical reactions,harnessing potential,current density,or light to yield valuable chemical products.This review explores recent progress in plastic upcycling through electrocatalytic and photoelectrocatalytic pathways,offering promising solutions to the plastic waste crisis and advancing sustainability in the plastics industry.展开更多
The scaled-up synthesis of organic-free monolayer nanomaterials is highly desirable,especially in obtaining green energy by electrocatalysis.In this study,a method for the scaled-up synthesis of the series of monolaye...The scaled-up synthesis of organic-free monolayer nanomaterials is highly desirable,especially in obtaining green energy by electrocatalysis.In this study,a method for the scaled-up synthesis of the series of monolayer layered double hydroxides(LDHs)without the addition of organic solvents is reported via the separate nucleation and aging steps process.The resulting monolayer LDHs with the thicknesses of less than 1 nm showed a narrow thickness distribution.X-ray absorption fine-structure revealed that monolayer NiFe-LDH nanosheets have a number of oxygen and metal vacancies defects.As a practical application,monolayer NiFe-LDH nanosheets containing defects showed an enhanced electrocatalytic water oxidation activity compared with that of bulk NiFe-LDH.Density functional theory calculations uncovered that excellent catalytic activity is attributed to vacancies defects.The proposed method is an economical and universally applicable strategy for the scaled-up production of monolayer LDHs.展开更多
Surface modification of natural cellulose fibers with nanomaterials is an effective strategy for producing functional textiles for multiple applications.A4-sized printing paper is a commonly used,cheap,and easily acqu...Surface modification of natural cellulose fibers with nanomaterials is an effective strategy for producing functional textiles for multiple applications.A4-sized printing paper is a commonly used,cheap,and easily acquirable office supply which is mainly made of cellulose fibers.Here,we report green and simple nanofabrication of A4 paper to endow it with high capability for fragrance encapsulation and sustained release,and strong adsorption to indoor air pollutants.The method utilizes the sugar molecule of cellulose for in-situ growth ofγ-cyclodextrin(γ-CD)metal-organic frameworks(MOFs)on A4 paper.The obtainedγ-CD-MOF/A4 nanocomposites have superior specific surface area and high porous structure.Theγ-CD-MOF/A4 nanocomposites can effectively encapsulate fragrant molecules through host-guest interaction.Theγ-CD-MOF/A4 nanocomposites also show strong absorption capability to formaldehyde and carbon dioxide through the formation of hydrogen bonding and chemical bonds.Theseγ-CD-MOF/A4nanocomposites combine the advantages of both A4 paper andγ-CD-MOF,which can be used in indoor air freshening and cleaning.展开更多
The Ni-Nb_(2)O_(5)nanocatalysts have been prepared by the solgel method,and the catalytic hydrodeoxygenation(HDO)performance of anisole as model compound is studied.The results show that Nb exists as amorphous Nb_(2)O...The Ni-Nb_(2)O_(5)nanocatalysts have been prepared by the solgel method,and the catalytic hydrodeoxygenation(HDO)performance of anisole as model compound is studied.The results show that Nb exists as amorphous Nb_(2)O_(5)species,which can promote Ni dispersion.The addition of Nb_(2)O_(5)increases the acidity of the catalyst.However,when the content of niobium is high,there is an inactive Nb-Ni-O mixed phase.The size and morphology of Ni grains in catalysts are different due to the difference of Nb/Ni molar ratio.The Ni_(0.9)Nb_(0.1)sample has the largest surface area of 170.8 m^(2)·g^(-1)among the catalysts prepared in different Nb/Ni molar ratios,which is mainly composed of spherical nanoparticles and crack pores.The HDO of anisole follows the reaction route of the hydrogenation HYD route.The Ni_(0.9)Nb_(0.1)catalyst displayed a higher HDO performance for anisole than Ni catalyst.The selectivity to cyclohexane over the Ni_(0.9)Nb_(0.1)sample is about 10 times that of Ni catalyst at 220℃and 3 MPa H_(2).The selectivity of cyclohexane is increased with the increase of reaction temperature.The anisole is almost completely transformed into cyclohexane at 240℃,3 MPa H_(2)and 4 h.展开更多
The development of multifunctional and efficient electromagnetic wave absorbing materials is a challenging research hotspot.Here,the magnetized Ni flower/MXene hybrids are successfully assembled on the surface of mela...The development of multifunctional and efficient electromagnetic wave absorbing materials is a challenging research hotspot.Here,the magnetized Ni flower/MXene hybrids are successfully assembled on the surface of melamine foam(MF)through electrostatic self-assembly and dip-coating adsorption process,realizing the integration of microwave absorption,infrared stealth,and flame retardant.Remarkably,the Ni/MXene-MF achieves a minimum reflection loss(RLmin)of−62.7 dB with a corresponding effective absorption bandwidth(EAB)of 6.24 GHz at 2 mm and an EAB of 6.88 GHz at 1.8 mm.Strong electromagnetic wave absorption is attributed to the three-dimensional magnetic/conductive networks,which provided excellent impedance matching,dielectric loss,magnetic loss,interface polarization,and multiple attenuations.In addition,the Ni/MXene-MF endows low density,excellent heat insulation,infrared stealth,and flame-retardant functions.This work provided a new development strategy for the design of multifunctional and efficient electromagnetic wave absorbing materials.展开更多
Ultra-thin flexible films have attracted wide attention because of their excellent ductility and potential versatility.In particular,the energy-harvesting films(EHFs)have become a research hotspot because of the indis...Ultra-thin flexible films have attracted wide attention because of their excellent ductility and potential versatility.In particular,the energy-harvesting films(EHFs)have become a research hotspot because of the indispensability of power source in various devices.However,the design and fabrication of such films that can capture or transform di erent types of energy from environments for multiple usages remains a challenge.Herein,the multifunctional flexible EHFs with e ective electro-/photo-thermal abilities are proposed by successive spraying Ag microparticles and MXene suspension between on waterborne polyurethane films,supplemented by a hot-pressing.The optimal coherent film exhibits a high electrical conductivity(1.17×10^(4)S m^(-1)),excellent Joule heating performance(121.3℃)at 2 V,and outstanding photo-thermal performance(66.2℃ within 70 s under 100 mW cm^(-1)).In addition,the EHFs-based single-electrode triboelectric nanogenerators(TENG)give short-circuit transferred charge of 38.9 nC,open circuit voltage of 114.7 V,and short circuit current of 0.82μA.More interestingly,the output voltage of TENG can be further increased via constructing the double triboelectrification layers.The comprehensive ability for harvesting various energies of the EHFs promises their potential to satisfy the corresponding requirements.展开更多
Hybrid adsorbents for COcapture were prepared by coassembling laponite(LP) nanosheets and 1-nbutyl-3-methylimidazolium chloride(BMIMCl). The prepared BMIMCl/LP layered hybrids were systematically characterized. Th...Hybrid adsorbents for COcapture were prepared by coassembling laponite(LP) nanosheets and 1-nbutyl-3-methylimidazolium chloride(BMIMCl). The prepared BMIMCl/LP layered hybrids were systematically characterized. The interlayer distance of the BMIMCl/LP layered hybrids expanded with an increasing concentration of BMIMCl, indicating that cumulative BMIMCl was intercalated into the LP layers. The efficiency of BMIMCl toward COcapture was significantly enhanced after it was immobilized within LP layers.展开更多
Polyvinyl alcohol(PVA)/laponite(LP)nanocomposite coatings were fabricated via a facile one-step coassembly process.The formed nanocoatings contain a high concentration of LP nanosheets,which can be well aligned along ...Polyvinyl alcohol(PVA)/laponite(LP)nanocomposite coatings were fabricated via a facile one-step coassembly process.The formed nanocoatings contain a high concentration of LP nanosheets,which can be well aligned along the substrate surface during the coassembly process.Due to the highly orientated structure,the flexible nanocoatings exhibit ultra-high transparency and superior mechanical properties,and can also act as excellent gas barriers.Such nanocoatings can be exceptional candidates for a variety of applications,such as food packaging.展开更多
Biomass-derived 2,5-bis(hydroxymethyl)furan(BHMF)has received great attention and interest due to its broad application prospects in polyesters and medicine.Over the past decades,the catalytic systems including thermo...Biomass-derived 2,5-bis(hydroxymethyl)furan(BHMF)has received great attention and interest due to its broad application prospects in polyesters and medicine.Over the past decades,the catalytic systems including thermocatalytic,biocatalytic,electrocatalytic,and photocatalytic hydrogenation of 5-hydroxymethylfurfural(HMF)into BHMF have been developed to a great extent.To understand the present status and challenges of BHMF production,this review systematically evaluates recent findings and developments of HMF hydrogenation through various reaction systems,with an emphasis on catalyst screening,synthesis processes,and reaction mechanism.Furthermore,a few potential research trends are also proposed,in order to provide innovative ideas for further exploration of BHMF synthesis in a simpler,efficient,and economical way.展开更多
Every three years the world's leaders in solvent extraction get together at the International Solvent Extraction Conference and in2014 it was held in Wurzburg in Germany.The following are 9 papers that were picked...Every three years the world's leaders in solvent extraction get together at the International Solvent Extraction Conference and in2014 it was held in Wurzburg in Germany.The following are 9 papers that were picked out that show an overview of the work presented and provide an update on some of the research being undertaken in solvent extraction today.For me the trend to environmentally sustainable bio derived solvents is a key展开更多
The original version of this article unfortunately contained some mistakes.The corrections are updated as follows:Error 1:We found that Equations 3,4 and 6 were wrong in the published paper:Error 2:In the page 7,“Sin...The original version of this article unfortunately contained some mistakes.The corrections are updated as follows:Error 1:We found that Equations 3,4 and 6 were wrong in the published paper:Error 2:In the page 7,“Since N Ni/MXene-MF possessed numer-ous heterogeneous interfaces and abundant functional groups,the dielectric loss mechanism was explored.”展开更多
An active bacterial anti-adhesion strategy based on directional transportation of bacterial droplets driven by a triboelectric nanogenerator(TENG)has not been reported to date,although passive defense approaches can p...An active bacterial anti-adhesion strategy based on directional transportation of bacterial droplets driven by a triboelectric nanogenerator(TENG)has not been reported to date,although passive defense approaches can prevent bacterial adhesion by regulating superwetting surfaces combined with incorporated antibacterial substances.Here a triboelectric nanogenerator driving droplet system(TNDDS)was built to drive directional transportation of bacterial droplets to be eliminated,which comprises TENG with periodical frictional Kapton film and aluminum foils and a superhydrophobic driving platform(SDP)with paralleled driving electrodes.The current generated by the TENG triboelectricity is transmitted to the paralleled driving electrodes to form an electric field driving the directional transportation of charged droplets.The critical value of the driven droplet volume on SDP is closely related to the distributed electrodes’distance and width,and the driving distance of droplets is related to the number of electrodes.More crucially,TNDDS can actively drive the charged droplets of prepared triangular silver nanoprisms(Ag NPs)forward and back to mix with and remove a tiny bacterial droplet on an open SDP or in a tiny semi-enclosed channel.Bacteria could be killed by releasing Ag+and effectively removed by TNDDS by regulating the motion direction.Generally,this approach offers a promising application for removing bacteria from material surfaces driven by TENG and opens a new avenue for bacterial anti-adhesion.展开更多
Single-atomic transition metal-nitrogen codoped carbon(M-N-C)are efficient substitute catalysts for noble metals to catalyze the electrochemical CO_(2) reduction reaction(CO_(2)RR).However,the uncontrolled aggregation...Single-atomic transition metal-nitrogen codoped carbon(M-N-C)are efficient substitute catalysts for noble metals to catalyze the electrochemical CO_(2) reduction reaction(CO_(2)RR).However,the uncontrolled aggregations of metal and serious loss of nitrogen species constituting the M-N_(x) active sites are frequently observed in the commonly used pyrolysis procedure.Herein,single-atomic nickel(Ni)-based sheet-like electrocatalysts with abundant Ni-N_(4) active sites were created by using a novel ammonium chloride(NH_(4)Cl)-assited pyrolysis method.Spherical aberration correction electron microscopy and X-ray absorption fine structure analysis clearly revealed that Ni species are atomically dispersed and anchored by N in Ni-N_(4) structure.The addition of NH_(4)Cl optimized the mesopore size to 7-10 nm and increased the concentrations of pyridinic N(3.54 wt%)and Ni-N_(4)(3.33 wt%)species.The synergistic catalytic effect derived from Ni-N_(4) active sites and pyridinic N species achieved an outstanding CO_(2) RR performance,presenting a high CO Faradaic efficiency(FE_(CO))up to 98% and a large CO partial current density of 8.5 mA cm^(-2) at a low potential of-0.62 V vs.RHE.Particularly,the FE_(CO) maintains above 80% within a large potential range from -0.43 to -0.73 V vs.RHE.This work provides a practical and feasible approach to building highly active single-atomic catalysts for CO_(2) conversion systems.展开更多
Atomic dispersion of Rh on phosphotungstic acid(PTA)salts was achieved by a self-assembled precipitation method using alkali metal ions as coprecipitation reagents.During styrene hydroformylation,the supported Rh sing...Atomic dispersion of Rh on phosphotungstic acid(PTA)salts was achieved by a self-assembled precipitation method using alkali metal ions as coprecipitation reagents.During styrene hydroformylation,the supported Rh single-atom catalyst(Rh1/M-PTA,M refers to an alkali metal ion)demonstrated an optimum turnover frequency(TOF)of 1076 h−1.With increasing ionic radius,the pore size of the catalysts increased in the following order:Rh1/K-PTA<Rh1/Rb-PTA<Rh1/Cs-PTA.The catalytic activity showed the same trend,suggesting a positive correlation between pore size and hydroformylation perfor-mance.Further experimental data suggested that temperature is an important factor affecting not only the activity but also the selectivity.This study enriches the understanding of the structure and catalytic properties of PTA-supported single-atom materials.The cation-controlled synthesis of catalysts may also be applied to prepare other single-atom catalysts with tunable pore size distributions.展开更多
Advanced model-based control strategies,e.g.,model predictive control,can offer superior control of key process variables for multiple-input multiple-output systems.The quality of the system model is critical to contr...Advanced model-based control strategies,e.g.,model predictive control,can offer superior control of key process variables for multiple-input multiple-output systems.The quality of the system model is critical to controller performance and should adequately describe the process dynamics across its operating range while remaining amenable to fast optimization.This work articulates an integrated system identification procedure for deriving black-box nonlinear continuous-time multiple-input multiple-output system models for nonlinear model predictive control.To showcase this approach,five candidate models for polynomial and interaction features of both output and manipulated variables were trained on simulated data and integrated into a nonlinear model predictive controller for a highly nonlinear continuous stirred tank reactor system.This procedure successfully identified system models that enabled effective control in both servo and regulator problems across wider operating ranges.These controllers also had reasonable per-iteration times of ca.0.1 s.This demonstration of how such system models could be identified for nonlinear model predictive control without prior knowledge of system dynamics opens further possibilities for direct data-driven methodologies for model-based control which,in the face of process uncertainties or modelling limitations,allow rapid and stable control over wider operating ranges.展开更多
Generation of large strains upon Na^(+) intercalation is one of the prime concerns of the mechanical degradation of Prussian blue(PB)and its analogs.Structural construction from the atomic level is imperative to maint...Generation of large strains upon Na^(+) intercalation is one of the prime concerns of the mechanical degradation of Prussian blue(PB)and its analogs.Structural construction from the atomic level is imperative to maintain structural stability and ameliorate the long-term stability of PB.Herein,an inter nickel hexacyanoferrate(NNiFCN)is successfully introduced at the out layer of iron hexacyanoferrate(NFFCN)through ion exchange to improve structural stability through compressive stress locking by forming NNiFCN shell.Furthermore,the kinetics of sodium ion diffusion is enhanced through the built-in electric pathway.The electrochemical performance is therefore significantly improved with a remarkable long-term cycling stability over 3,000 cycles at 500 mA·g^(–1) in the full sodium-ion batteries(SIBs)with a maximum energy density of 91.94 Wh·g^(–1),indicating that the core-shell structured NNiFCN/NFFCN could be the low-cost and high-performance cathode for full SIBs in large-scale EES applications.展开更多
Zwitterionic glycine was employed to modify Fe/Mg-layered double hydroxides(LDH)to realize an GFe/Mg-LDH adsorbent with high adsorption capacities of oxygen-containing anions including As(Ⅴ),P(Ⅴ)and Cr(Ⅵ).When the ...Zwitterionic glycine was employed to modify Fe/Mg-layered double hydroxides(LDH)to realize an GFe/Mg-LDH adsorbent with high adsorption capacities of oxygen-containing anions including As(Ⅴ),P(Ⅴ)and Cr(Ⅵ).When the Fe/Mg mole ratio was 0.02 mol/0.02 mol,the G-Fe/Mg-LDH has a good adsorption performance.The optimum adsorption pH value of G-Fe/Mg-LDH for oxygen-containing anions was 6.The selectivity of three oxygen-containing anions was Cr(Ⅵ)展开更多
基金financially supported by the National Science Foundation(1438518)。
文摘Activated carbon nanofibers(ACNFs)with small diameter can significantly increase the accessibility of intra pores and accelerate adsorption of molecules from water.In this study,ACNFs were made by blending K_(2)CO_(3)or ZnCl_(2)as the activating agent into the polyacrylonitrile(PAN)in dimethylformamide solution for electrospinning prior to pyrolysis.Bisphenol-A(BPA),an endocrine disruption pollutant,is widely applied in the production of polycarbonate plastics and epoxy resins.Accordingly,BPA is often used as a model contaminant commonly removed via adsorption.Batch adsorption studies were used to evaluate the kinetics and adsorption capacity of the ACNFs.Redlich-Peterson(R-P)and Langmuir models were found to fit the isotherm of BPA adsorption better than Freundlich model,showing the homogeneous nature of the PAN originated ACNFs.The adsorption kinetics was better described by the pseudo second-order model than that by the pseudo first-order model.The fitting by intraparticle diffusion model indicates the adsorption of BPA onto ACNFs is mainly controlled by pore diffusion.High pH value and ionic strength reduced BPA adsorption from aqueous solution.The breakthrough curves studied in two different fixed bed systems(cross flow bed system and packed flow bed system)confirmed the scalability of BPA removal by ACNFs in dynamic adsorption processes.The modified dose-response model predicted well the fixed-bed outlet concentration profiles.
基金the Basic Research Project(C123000,C210200,C310200,&C421000)of the Korea Basic Science Institute(KBSI)funded by the Korea Ministry of Science and ICT(MSIT)the Technology Development Program to Solve Climate Changes through the National Research Foundation of Korea(NRF)funded by MSIT(NRF-2021M1A2A2038141).O.H.Han thanks to Prof.I.S.Yang at Ewha Womans University for insightful discussion.
文摘Despite the proficiency of lithium(Li)-7 NMR spectroscopy in delineating the physical and chemical states of Li metal electrodes,challenges in specimen preparation and interpretation impede its progress.In this study,we conducted a comprehensive postmortem analysis utilizing ^(7)Li NMR,employing a stan-dard magic angle spinning probe to examine protective-layer coated Li metal electrodes and LiAg alloy electrodes against bare Li metal electrodes within Li metal batteries(LMBs).Our investigation explores the effects of sample burrs,alignment with the magnetic field,the existence of liquid electrolytes,and precycling on the ^(7)Li NMR signals.Through contrasting NMR spectra before and after cycling,we identi-fied alterations in Li^(0) and Li^(+) signals attributable to the degradation of the Li metal electrode.Our NMR analyses decisively demonstrate the efficacy of the protective layer in mitigating dendrite and solid elec-trolyte interphase formation.Moreover,we noted that Li*ions near the Li metal surface exhibit magnetic susceptibility anisotropy,revealing a novel approach to studying diamagnetic species on Li metal elec-trodes in LMBs.This study provides valuable insights and practical guidelines for characterizing distinct lithium states within LMBs.
文摘Powered by electricity from renewable energies,electrochemical reduction of CO_(2)could not only efficiently alleviate the excess emission of CO_(2),but also produce many kinds of valuable chemical feedstocks.Among various catalysts,single atom catalysts(SACs)have attracted much attention due to their high atom utilization efficiency and expressive catalytic performances.Additionally,SACs serve as an ideal platform for the investigation of complex reaction pathways and mechanisms thanks to their explicit active sites.In this review,the possible re-action pathways for the generation of various products(mainly C1 products for SACs)were firstly summarized.Then,recent progress of SACs for electrochemical reduction of CO_(2)was discussed in aspect of different central metal sites.As the most popular and efficient coordination modulation strategy,introducing heteroatom was then reviewed.Moreover,as an extension of SACs,the development of dual atom catalysts was also briefly discussed.At last,some issues and challenges regarding the SACs for CO_(2)reduction reaction(CO_(2)RR)were listed,followed by corresponding suggestions.
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korea government(MSIT)(RS-2023-00302697,2022H1D3A3A01077254)。
文摘Plastic,renowned for its versatility,durability,and cost-effectiveness,is indispensable in modern society.Nevertheless,the annual production of nearly 400 million tons of plastic,coupled with a recycling rate of only 9%,has led to a monumental environmental crisis.Plastic recycling has emerged as a vital response to this crisis,offering sustainable solutions to mitigate its environmental impact.Among these recycling efforts,plastic upcycling has garnered attention,which elevates discarded plastics into higher-value products.Here,electrocatalytic and photoelectrocatalytic treatments stand at the forefront of advanced plastic upcycling.Electrocatalytic or photoelectrocatalytic treatments involve chemical reactions that facilitate electron transfer through the electrode/electrolyte interface,driven by electrical or solar energy,respectively.These methods enable precise control of chemical reactions,harnessing potential,current density,or light to yield valuable chemical products.This review explores recent progress in plastic upcycling through electrocatalytic and photoelectrocatalytic pathways,offering promising solutions to the plastic waste crisis and advancing sustainability in the plastics industry.
基金supported by the National Nature Science Foundation of China(U1707603,21878008,21625101,U1507102,21922801)the Beijing Natural Science Foundation(2182047,2202036)the Fundamental Research Funds for the Central Universities(XK1802-6,XK1902,12060093063,2312018RC07)。
文摘The scaled-up synthesis of organic-free monolayer nanomaterials is highly desirable,especially in obtaining green energy by electrocatalysis.In this study,a method for the scaled-up synthesis of the series of monolayer layered double hydroxides(LDHs)without the addition of organic solvents is reported via the separate nucleation and aging steps process.The resulting monolayer LDHs with the thicknesses of less than 1 nm showed a narrow thickness distribution.X-ray absorption fine-structure revealed that monolayer NiFe-LDH nanosheets have a number of oxygen and metal vacancies defects.As a practical application,monolayer NiFe-LDH nanosheets containing defects showed an enhanced electrocatalytic water oxidation activity compared with that of bulk NiFe-LDH.Density functional theory calculations uncovered that excellent catalytic activity is attributed to vacancies defects.The proposed method is an economical and universally applicable strategy for the scaled-up production of monolayer LDHs.
基金supported by the National Key Research and Development Program of China(2016YFA0200301)the National Natural Science Foundation of China(21875211,52073249,51833008,and51603181)the Zhejiang Provincial Key Research and Development Program(2020C01123)。
文摘Surface modification of natural cellulose fibers with nanomaterials is an effective strategy for producing functional textiles for multiple applications.A4-sized printing paper is a commonly used,cheap,and easily acquirable office supply which is mainly made of cellulose fibers.Here,we report green and simple nanofabrication of A4 paper to endow it with high capability for fragrance encapsulation and sustained release,and strong adsorption to indoor air pollutants.The method utilizes the sugar molecule of cellulose for in-situ growth ofγ-cyclodextrin(γ-CD)metal-organic frameworks(MOFs)on A4 paper.The obtainedγ-CD-MOF/A4 nanocomposites have superior specific surface area and high porous structure.Theγ-CD-MOF/A4 nanocomposites can effectively encapsulate fragrant molecules through host-guest interaction.Theγ-CD-MOF/A4 nanocomposites also show strong absorption capability to formaldehyde and carbon dioxide through the formation of hydrogen bonding and chemical bonds.Theseγ-CD-MOF/A4nanocomposites combine the advantages of both A4 paper andγ-CD-MOF,which can be used in indoor air freshening and cleaning.
基金Major Science and Technology Project of Yunnan Province(202102AE090042)National Natural Science Foundation of China(21766016)+1 种基金the Science and Technology Talent and Platform Program of Yunnan Provincial Science and Technology Department(202005AF150037)the financial support of Taif University Researchers Supporting Project(TURSP-2020/27),Taif University,Taif,Saudi Arabia。
文摘The Ni-Nb_(2)O_(5)nanocatalysts have been prepared by the solgel method,and the catalytic hydrodeoxygenation(HDO)performance of anisole as model compound is studied.The results show that Nb exists as amorphous Nb_(2)O_(5)species,which can promote Ni dispersion.The addition of Nb_(2)O_(5)increases the acidity of the catalyst.However,when the content of niobium is high,there is an inactive Nb-Ni-O mixed phase.The size and morphology of Ni grains in catalysts are different due to the difference of Nb/Ni molar ratio.The Ni_(0.9)Nb_(0.1)sample has the largest surface area of 170.8 m^(2)·g^(-1)among the catalysts prepared in different Nb/Ni molar ratios,which is mainly composed of spherical nanoparticles and crack pores.The HDO of anisole follows the reaction route of the hydrogenation HYD route.The Ni_(0.9)Nb_(0.1)catalyst displayed a higher HDO performance for anisole than Ni catalyst.The selectivity to cyclohexane over the Ni_(0.9)Nb_(0.1)sample is about 10 times that of Ni catalyst at 220℃and 3 MPa H_(2).The selectivity of cyclohexane is increased with the increase of reaction temperature.The anisole is almost completely transformed into cyclohexane at 240℃,3 MPa H_(2)and 4 h.
基金The authors thank National Natural Science Foundation of China(51803190)National Key R&D Program of China(2019YFA0706802)financial support.
文摘The development of multifunctional and efficient electromagnetic wave absorbing materials is a challenging research hotspot.Here,the magnetized Ni flower/MXene hybrids are successfully assembled on the surface of melamine foam(MF)through electrostatic self-assembly and dip-coating adsorption process,realizing the integration of microwave absorption,infrared stealth,and flame retardant.Remarkably,the Ni/MXene-MF achieves a minimum reflection loss(RLmin)of−62.7 dB with a corresponding effective absorption bandwidth(EAB)of 6.24 GHz at 2 mm and an EAB of 6.88 GHz at 1.8 mm.Strong electromagnetic wave absorption is attributed to the three-dimensional magnetic/conductive networks,which provided excellent impedance matching,dielectric loss,magnetic loss,interface polarization,and multiple attenuations.In addition,the Ni/MXene-MF endows low density,excellent heat insulation,infrared stealth,and flame-retardant functions.This work provided a new development strategy for the design of multifunctional and efficient electromagnetic wave absorbing materials.
基金National Natural Science Foundation of China(51803190)National Key R&D Program of China(2019YFA0706802)for financial support。
文摘Ultra-thin flexible films have attracted wide attention because of their excellent ductility and potential versatility.In particular,the energy-harvesting films(EHFs)have become a research hotspot because of the indispensability of power source in various devices.However,the design and fabrication of such films that can capture or transform di erent types of energy from environments for multiple usages remains a challenge.Herein,the multifunctional flexible EHFs with e ective electro-/photo-thermal abilities are proposed by successive spraying Ag microparticles and MXene suspension between on waterborne polyurethane films,supplemented by a hot-pressing.The optimal coherent film exhibits a high electrical conductivity(1.17×10^(4)S m^(-1)),excellent Joule heating performance(121.3℃)at 2 V,and outstanding photo-thermal performance(66.2℃ within 70 s under 100 mW cm^(-1)).In addition,the EHFs-based single-electrode triboelectric nanogenerators(TENG)give short-circuit transferred charge of 38.9 nC,open circuit voltage of 114.7 V,and short circuit current of 0.82μA.More interestingly,the output voltage of TENG can be further increased via constructing the double triboelectrification layers.The comprehensive ability for harvesting various energies of the EHFs promises their potential to satisfy the corresponding requirements.
基金sponsored by the National Science Foundation(CMMI-1562907)the financial support from the National Natural Science Foundation of China(51678511 and 51308484)+4 种基金the Open Fund of Key Laboratory of Mineralogy and Metallogeny in Chinese Academy of Sciences(KLMM20150104)the Natural Science Foundation of Hunan Province(13JJ4049)the Education Department Fund of Hunan Province(14C1094)the Major Talent Training Program of Xiangtan University(16PYZ09)the Specialized Research Fund for the Doctoral Program of Xiangtan University(12QDZ18)
文摘Hybrid adsorbents for COcapture were prepared by coassembling laponite(LP) nanosheets and 1-nbutyl-3-methylimidazolium chloride(BMIMCl). The prepared BMIMCl/LP layered hybrids were systematically characterized. The interlayer distance of the BMIMCl/LP layered hybrids expanded with an increasing concentration of BMIMCl, indicating that cumulative BMIMCl was intercalated into the LP layers. The efficiency of BMIMCl toward COcapture was significantly enhanced after it was immobilized within LP layers.
文摘Polyvinyl alcohol(PVA)/laponite(LP)nanocomposite coatings were fabricated via a facile one-step coassembly process.The formed nanocoatings contain a high concentration of LP nanosheets,which can be well aligned along the substrate surface during the coassembly process.Due to the highly orientated structure,the flexible nanocoatings exhibit ultra-high transparency and superior mechanical properties,and can also act as excellent gas barriers.Such nanocoatings can be exceptional candidates for a variety of applications,such as food packaging.
基金the financial support of the National Natural Science Foundation of China(22278121,21975070)Hunan Provincial Innovation Foundation for Postgraduate(QL20210132)the funding offered by China Scholarship Council(202106720021).
文摘Biomass-derived 2,5-bis(hydroxymethyl)furan(BHMF)has received great attention and interest due to its broad application prospects in polyesters and medicine.Over the past decades,the catalytic systems including thermocatalytic,biocatalytic,electrocatalytic,and photocatalytic hydrogenation of 5-hydroxymethylfurfural(HMF)into BHMF have been developed to a great extent.To understand the present status and challenges of BHMF production,this review systematically evaluates recent findings and developments of HMF hydrogenation through various reaction systems,with an emphasis on catalyst screening,synthesis processes,and reaction mechanism.Furthermore,a few potential research trends are also proposed,in order to provide innovative ideas for further exploration of BHMF synthesis in a simpler,efficient,and economical way.
文摘Every three years the world's leaders in solvent extraction get together at the International Solvent Extraction Conference and in2014 it was held in Wurzburg in Germany.The following are 9 papers that were picked out that show an overview of the work presented and provide an update on some of the research being undertaken in solvent extraction today.For me the trend to environmentally sustainable bio derived solvents is a key
文摘The original version of this article unfortunately contained some mistakes.The corrections are updated as follows:Error 1:We found that Equations 3,4 and 6 were wrong in the published paper:Error 2:In the page 7,“Since N Ni/MXene-MF possessed numer-ous heterogeneous interfaces and abundant functional groups,the dielectric loss mechanism was explored.”
基金This work was supported by the National Natural Science Foundation of China(No.22078077).
文摘An active bacterial anti-adhesion strategy based on directional transportation of bacterial droplets driven by a triboelectric nanogenerator(TENG)has not been reported to date,although passive defense approaches can prevent bacterial adhesion by regulating superwetting surfaces combined with incorporated antibacterial substances.Here a triboelectric nanogenerator driving droplet system(TNDDS)was built to drive directional transportation of bacterial droplets to be eliminated,which comprises TENG with periodical frictional Kapton film and aluminum foils and a superhydrophobic driving platform(SDP)with paralleled driving electrodes.The current generated by the TENG triboelectricity is transmitted to the paralleled driving electrodes to form an electric field driving the directional transportation of charged droplets.The critical value of the driven droplet volume on SDP is closely related to the distributed electrodes’distance and width,and the driving distance of droplets is related to the number of electrodes.More crucially,TNDDS can actively drive the charged droplets of prepared triangular silver nanoprisms(Ag NPs)forward and back to mix with and remove a tiny bacterial droplet on an open SDP or in a tiny semi-enclosed channel.Bacteria could be killed by releasing Ag+and effectively removed by TNDDS by regulating the motion direction.Generally,this approach offers a promising application for removing bacteria from material surfaces driven by TENG and opens a new avenue for bacterial anti-adhesion.
基金financially supported by the National Natural Science Foundation of China(Nos.21571159 and U1704256)the Natural Science Foundation of Henan Province,China(No.212300410299)the Doctoral Research Fund of Zhengzhou University of Light Industry(No.2018BSJJ024).
文摘Single-atomic transition metal-nitrogen codoped carbon(M-N-C)are efficient substitute catalysts for noble metals to catalyze the electrochemical CO_(2) reduction reaction(CO_(2)RR).However,the uncontrolled aggregations of metal and serious loss of nitrogen species constituting the M-N_(x) active sites are frequently observed in the commonly used pyrolysis procedure.Herein,single-atomic nickel(Ni)-based sheet-like electrocatalysts with abundant Ni-N_(4) active sites were created by using a novel ammonium chloride(NH_(4)Cl)-assited pyrolysis method.Spherical aberration correction electron microscopy and X-ray absorption fine structure analysis clearly revealed that Ni species are atomically dispersed and anchored by N in Ni-N_(4) structure.The addition of NH_(4)Cl optimized the mesopore size to 7-10 nm and increased the concentrations of pyridinic N(3.54 wt%)and Ni-N_(4)(3.33 wt%)species.The synergistic catalytic effect derived from Ni-N_(4) active sites and pyridinic N species achieved an outstanding CO_(2) RR performance,presenting a high CO Faradaic efficiency(FE_(CO))up to 98% and a large CO partial current density of 8.5 mA cm^(-2) at a low potential of-0.62 V vs.RHE.Particularly,the FE_(CO) maintains above 80% within a large potential range from -0.43 to -0.73 V vs.RHE.This work provides a practical and feasible approach to building highly active single-atomic catalysts for CO_(2) conversion systems.
基金supported by the National Natural Science Foundation of China(92061109 and 22273053)the Natural Science Basic Research Program of Shaanxi(2021JCW-20 and 2022KJXX-18).
文摘Atomic dispersion of Rh on phosphotungstic acid(PTA)salts was achieved by a self-assembled precipitation method using alkali metal ions as coprecipitation reagents.During styrene hydroformylation,the supported Rh single-atom catalyst(Rh1/M-PTA,M refers to an alkali metal ion)demonstrated an optimum turnover frequency(TOF)of 1076 h−1.With increasing ionic radius,the pore size of the catalysts increased in the following order:Rh1/K-PTA<Rh1/Rb-PTA<Rh1/Cs-PTA.The catalytic activity showed the same trend,suggesting a positive correlation between pore size and hydroformylation perfor-mance.Further experimental data suggested that temperature is an important factor affecting not only the activity but also the selectivity.This study enriches the understanding of the structure and catalytic properties of PTA-supported single-atom materials.The cation-controlled synthesis of catalysts may also be applied to prepare other single-atom catalysts with tunable pore size distributions.
基金The authors thank the MOE AcRF Grant in Singapore for financial support of the projects on Precision Healthcare Development,Manufacturing and Supply Chain Optimization(Grant No.R-279-000-513-133)Advanced Process Control and Machine Learning Methods for Enhanced Continuous Manufacturing of Pharmaceutical Products(Grant No.R-279-000-541-114).
文摘Advanced model-based control strategies,e.g.,model predictive control,can offer superior control of key process variables for multiple-input multiple-output systems.The quality of the system model is critical to controller performance and should adequately describe the process dynamics across its operating range while remaining amenable to fast optimization.This work articulates an integrated system identification procedure for deriving black-box nonlinear continuous-time multiple-input multiple-output system models for nonlinear model predictive control.To showcase this approach,five candidate models for polynomial and interaction features of both output and manipulated variables were trained on simulated data and integrated into a nonlinear model predictive controller for a highly nonlinear continuous stirred tank reactor system.This procedure successfully identified system models that enabled effective control in both servo and regulator problems across wider operating ranges.These controllers also had reasonable per-iteration times of ca.0.1 s.This demonstration of how such system models could be identified for nonlinear model predictive control without prior knowledge of system dynamics opens further possibilities for direct data-driven methodologies for model-based control which,in the face of process uncertainties or modelling limitations,allow rapid and stable control over wider operating ranges.
基金J.G.S.wants to thanks China Scholarship Council(CSC)for the scholarship support(No.201706050153)。
文摘Generation of large strains upon Na^(+) intercalation is one of the prime concerns of the mechanical degradation of Prussian blue(PB)and its analogs.Structural construction from the atomic level is imperative to maintain structural stability and ameliorate the long-term stability of PB.Herein,an inter nickel hexacyanoferrate(NNiFCN)is successfully introduced at the out layer of iron hexacyanoferrate(NFFCN)through ion exchange to improve structural stability through compressive stress locking by forming NNiFCN shell.Furthermore,the kinetics of sodium ion diffusion is enhanced through the built-in electric pathway.The electrochemical performance is therefore significantly improved with a remarkable long-term cycling stability over 3,000 cycles at 500 mA·g^(–1) in the full sodium-ion batteries(SIBs)with a maximum energy density of 91.94 Wh·g^(–1),indicating that the core-shell structured NNiFCN/NFFCN could be the low-cost and high-performance cathode for full SIBs in large-scale EES applications.
文摘Zwitterionic glycine was employed to modify Fe/Mg-layered double hydroxides(LDH)to realize an GFe/Mg-LDH adsorbent with high adsorption capacities of oxygen-containing anions including As(Ⅴ),P(Ⅴ)and Cr(Ⅵ).When the Fe/Mg mole ratio was 0.02 mol/0.02 mol,the G-Fe/Mg-LDH has a good adsorption performance.The optimum adsorption pH value of G-Fe/Mg-LDH for oxygen-containing anions was 6.The selectivity of three oxygen-containing anions was Cr(Ⅵ)