Bioethanol produced via valorisation of renewable biomass is of great interest to many industries.The increased availability and decreased cost of bioethanol make it a promising platform molecule to produce a wide ran...Bioethanol produced via valorisation of renewable biomass is of great interest to many industries.The increased availability and decreased cost of bioethanol make it a promising platform molecule to produce a wide range of value-added chemicals and fuels via the catalytic conversions.This paper provides a comprehensive review of catalytic conversions of bioethanol to a variety of chemicals/fuels such as hydrogen,C_(2)-C_(4)olefins,gasoline and small oxygenates.Specifically,the focus was placed on the relationship between the catalyst property(such as pore structure,acidity,active metal sites,and catalyst supports)and the catalytic performance(including catalyst activity and stability),as well as the reaction mechanisms involved.Future research avenues on the catalyst design for improving catalytic valorisation of bioethanol are also discussed.展开更多
With the rapid development of flexible wearable electronics,the demand for stretchable energy storage devices has surged.In this work,a novel gradient-layered architecture was design based on single-pore hollow lignin...With the rapid development of flexible wearable electronics,the demand for stretchable energy storage devices has surged.In this work,a novel gradient-layered architecture was design based on single-pore hollow lignin nanospheres(HLNPs)-intercalated two-dimensional transition metal carbide(Ti_(3)C_(2)T_(x) MXene)for fabricating highly stretchable and durable supercapacitors.By depositing and inserting HLNPs in the MXene layers with a bottom-up decreasing gradient,a multilayered porous MXene structure with smooth ion channels was constructed by reducing the overstacking of MXene lamella.Moreover,the micro-chamber architecture of thin-walled lignin nanospheres effectively extended the contact area between lignin and MXene to improve ion and electron accessibility,thus better utilizing the pseudocapacitive property of lignin.All these strategies effectively enhanced the capacitive performance of the electrodes.In addition,HLNPs,which acted as a protective phase for MXene layer,enhanced mechanical properties of the wrinkled stretchable electrodes by releasing stress through slip and deformation during the stretch-release cycling and greatly improved the structural integrity and capacitive stability of the electrodes.Flexible electrodes and symmetric flexible all-solid-state supercapacitors capable of enduring 600%uniaxial tensile strain were developed with high specific capacitances of 1273 mF cm^(−2)(241 F g^(−1))and 514 mF cm^(−2)(95 F g^(−1)),respectively.Moreover,their capacitances were well preserved after 1000 times of 600%stretch-release cycling.This study showcased new possibilities of incorporating biobased lignin nanospheres in energy storage devices to fabricate stretchable devices leveraging synergies among various two-dimensional nanomaterials.展开更多
The increasing demand for electronics has led to a desire to recover rare earth elements(REEs) from nonconventional sources,including mining and liquid waste effluents.Biosorption could be a promising method for adsor...The increasing demand for electronics has led to a desire to recover rare earth elements(REEs) from nonconventional sources,including mining and liquid waste effluents.Biosorption could be a promising method for adsorbing REEs onto microalgae,but biomass immobilization and light delivery challenges remain.It was recently shown that REEs biosorb 160% more on algal biofilms than suspended biomass due to the extracellular polymeric substance(EPS) matrix that grows abundantly in biofilms.In this work,we present findings on biosorption selectivity for different REEs in sulfate solutions.The maximum adsorption capacities of Euglena mutabilis suspensions and biofilms were determined for a mixed REE sulfate solution at an equimolar initial concentration range of 0.1-1 mol/L of each REE ion.The highest adsorption capacities for the suspension are for Sm and Eu which are 57% and 46% higher,respectively,compared to the average REE adsorption capacity.The biofilms also preferentially adsorb Sm,Eu,Yb and Lu at 0.035,0.033,0.033,and 0.031 mmol/g,respectively.The impact of dissolved divalent ions of Ca,Mg,and Fe on REE adsorption was also assessed.When Ca and Mg are added in equimolar amounts to0.1-1 mmol/L solutions of equimolar La,Eu,and Yb sulfate,the amount of REEs adsorbed onto suspensions increases by 30% while when Fe is added,it decreases by 10%.No change is observed in biofilms except when Fe is added resulting in a reduction of the adsorption capacity by 40%.A possible explanation for the role of Fe is attributed to the formation of stronger bonds at the binding sites compared to Ca and Mg.展开更多
In an era where technological advancement and sustainability converge,developing renewable materials with multifunctional integration is increasingly in demand.This study filled a crucial gap by integrating energy sto...In an era where technological advancement and sustainability converge,developing renewable materials with multifunctional integration is increasingly in demand.This study filled a crucial gap by integrating energy storage,multi-band electromagnetic interference(EMI)shielding,and structural design into bio-based materials.Specifically,conductive polymer layers were formed within the 2,2,6,6-tetramethylpiperidine-1-oxide(TEMPO)-oxidized cellulose fiber skeleton,where a mild TEMPO-mediated oxidation system was applied to endow it with abundant macropores that could be utilized as active sites(specific surface area of 105.6 m2 g-1).Benefiting from the special hierarchical porous structure of the material,the constructed cellulose fiber-derived composites can realize high areal-specific capacitance of 12.44 F cm^(-2)at 5 m A cm^(-2)and areal energy density of 3.99 m Wh cm^(-2)(2005 m W cm^(-2))with an excellent stability of maintaining 90.23%after 10,000 cycles at 50 m A cm^(-2).Meanwhile,the composites showed a high electrical conductivity of 877.19 S m-1 and excellent EMI efficiency(>99.99%)in multiple wavelength bands.The composite material’s EMI values exceed 100 d B across the L,S,C,and X bands,effectively shielding electromagnetic waves in daily life.The proposed strategy paves the way for utilizing bio-based materials in applications like energy storage and EMI shielding,contributing to a more sustainable future.展开更多
The practical application of lithium(Li)metal batteries(LMBs)faces challenges due to the irreversible Li deposition/dissolution process,which promotes Li dendrite growth with severe parasitic reactions during cycling....The practical application of lithium(Li)metal batteries(LMBs)faces challenges due to the irreversible Li deposition/dissolution process,which promotes Li dendrite growth with severe parasitic reactions during cycling.To address these issues,achieving uniform Li‐ion flux and improving Li‐ion conductivity of the separator are the top priorities.Herein,a separator(PCELS)with enhanced Li‐ion conductivity,composed of polymer,ceramic,and electrically conductive carbon,is proposed to facilitate fast Li‐ion transport kinetics and increase Li deposition uniformity of the LMBs.The PCELS immobilizes PF6–anions with high adsorption energies,leading to a high Li‐ion transference number.Simultaneously,the PCELS shows excellent electrolyte wettability on both its sides,promoting rapid ion transport.Moreover,the electrically conductive carbon within the PCELS provides additional electron transport channels,enabling efficient charge transfer and uniform Li‐ion flux.With these advantages,the PCELS achieves rapid Li‐ion transport kinetics and uniform Li deposition,demonstrating excellent cycling stability over 100 cycles at a high current density of 12.0 mA cm^(-2).Furthermore,the PCELS shows stable cycling performances in Li–S cell tests and delivers an excellent capacity retention of 95.45%in the Li|LiFePO_(4) full‐cell test with a high areal capacity of over 5.5 mAh cm^(-2).展开更多
Heterogeneously catalyzed hydrolytic dehydrogenation of ammonia borane is a remarkable structure sensitive reaction. In this work, a strategy by using polyoxometalates(POMs) as the ligands is proposed to engineer the ...Heterogeneously catalyzed hydrolytic dehydrogenation of ammonia borane is a remarkable structure sensitive reaction. In this work, a strategy by using polyoxometalates(POMs) as the ligands is proposed to engineer the surface and electronic properties of Pt/CNT catalysts toward the enhanced hydrogen generation rate and durability. Three kinds of POMs, i.e., silicotungstic acid(STA), phosphotungstic acid(PTA)and molybdophosphoric acid(PMA), are comparatively studied, among which the STA shows positive effects on the catalytic activity and durability. A catalyst structure-performance relationship is established by a combination of kinetic and isotopic analyses with multiple characterization techniques, such as HAADF-STEM, EDS, Raman spectroscopy and XPS. It is shown that the STA compared to the other two POMs can increase the Pt binding energy and thus promote the reaction. The insights demonstrated here could open a new avenue for boosting the reaction by employing the POMs as the ligands to engineer the catalyst electronic properties.展开更多
Objective The wetland at Dalian Bay in the Northeast of China has been polluted by oil severely. The effect of various microbes and operation parameters on the bioremediation of oil-polluted wetlands at Dalian Bay was...Objective The wetland at Dalian Bay in the Northeast of China has been polluted by oil severely. The effect of various microbes and operation parameters on the bioremediation of oil-polluted wetlands at Dalian Bay was investigated and reported previously. In the study, other operation conditions related to the status of medium were investigated via statistical experimental design and analysis and a necessary information is involved to use micro-technology in the application. Methods The method used involved the direct inoculation of selected bacteria, which were capable of degrading oil. The operation conditions were further optimized and evaluated by gravimetrical assay. Results The optimal pH and temperature for the studied bacteria to degrade the existing oil pollutants were established as pH 8.0 and 27℃. The mixed of various bacteria showed better results in terms of oil degradation than any single one. Among the selected four factors, disturbance, oxidant, nutrients, and biosurfactant, the former two contributed more impacts on the oil degradation in the early stage of process, while the latter two became the limiting factors in the late stage. Three sets of optimal conditions were obtained for each individual stage, but no one was suitable for the overall process. Conclusion The study demonstrated the technical feasibility of using direct inoculation into the contaminated soil samples to remove oil pollutants. It suggested that the operation conditions should be monitored and adjusted during the different stages of bio-reactions in the process to achieve the best result of oil degradation.展开更多
The dry deposition process refers to the flux loss of an atmospheric pollutant due to uptake of the pollutant by the earth’s surfaces.Dry deposition flux of a chemical species is typically calculated as the product o...The dry deposition process refers to the flux loss of an atmospheric pollutant due to uptake of the pollutant by the earth’s surfaces.Dry deposition flux of a chemical species is typically calculated as the product of its surface-layer concentration and its dry deposition velocity(V_(d)).Field measurement based V_(d) data are very scarce or do not exist for many chemical species considered in chemistry transport models.In the present study,gaseous and particulate dry deposition schemes were applied to generate a database of hourly V_(d) for 45 gaseous species and three particle size ranges for two years(2016–2017)at a 15 kmby 15 km horizontal resolution across North America.Hourly V_(d) of the 45 gaseous species ranged from<0.001 to 4.6 cm/sec across the whole domain,with chemical species-dependentmedian(mean)values being in the range of 0.018–1.37 cm/sec(0.05–1.43 cm/sec).The spatial distributions of the two-year average V_(d) showed values higher than 1–3 cm/sec for those soluble and reactive species over certain land types.Soluble species have the highest V_(d) over water surfaces,while insoluble but reactive species have the highest V_(d) over forests.Hourly V_(d) of PM_(2.5) across the whole domain ranged from 0.039 to 0.75 cm/sec with median(mean)value of 0.18(0.20)cm s^(−1),while the mean V_(d) for PM_(2.5)–10 is twice that of PM_(2.5).Uncertainties in the modeled V_(d) are typically on the order of a factor of 2.0 or larger,which needs to be considered when applying the dataset in other studies.展开更多
Double fortified salt containing both potassium iodate and ferrous fumarate microcapsules was produced at an Indian commercial facility. The packaged product became discolored, turning yellow, to a degree that would i...Double fortified salt containing both potassium iodate and ferrous fumarate microcapsules was produced at an Indian commercial facility. The packaged product became discolored, turning yellow, to a degree that would impact consumer acceptance. Therefore, there was a need for an investigation into the cause and possible remedy for this discoloration. The components of the fortified salt product, storage conditions, and processing characteristics were taken into consideration. Canadian and Indian salt samples were prepared unfortified as well as with iodine and/or iron microcapsules;stored at 25°C and 45°C in glass, polyethylene, or commercial polymer film. Some samples were heat treated prior to storage. Salt samples containing iodine that were heated before storage in packaging material turned yellow in color. From this study, it was found that due to heat and the presence of a sacrificial antioxidant component in the packaging film, potassium iodate was reduced to elemental iodine (I<sub>2</sub>) turning packaged salt samples to a yellow/orange color. Hence it is recommended that in the manufacture of foods containing potassium iodate, the packaging material selected should be free from readily accessible antioxidants.展开更多
A three-dimensional direct numerical simulation is carried out to predict the surface oscillation and flow structure of isothermal liquid bridges of 5 cSt silicone oil held vertically between solid disks. By subjectin...A three-dimensional direct numerical simulation is carried out to predict the surface oscillation and flow structure of isothermal liquid bridges of 5 cSt silicone oil held vertically between solid disks. By subjecting liquid bridges to various horizontal vibrations, the surface resonance frequencies are clearly determined numerically and compared well with the existing analytical model predictions. The investigation on the flow structure inside the liquid bridge reveals, for the first time, the flow structure and the existence of transw＇,rsal vortices inside the liquid bridge when a horizontal vibration is applied.展开更多
Water often presents significant challenges in catalysts by deactivating active sites,poisoning the reaction,and even degrading composite structure.These challenges are amplified when the water participates as a react...Water often presents significant challenges in catalysts by deactivating active sites,poisoning the reaction,and even degrading composite structure.These challenges are amplified when the water participates as a reactant and is fed as a liquid phase,such as trickle bed-type reactors in a hydrogen-water isotope exchange(HIE)reaction.The key balance in such multiphase reactions is the precise control of catalyst design to repel bulk liquid water while diffusing water vapor.Herein,a platinum-incorporated metal-organic framework(MIL-101)based bifunctional hydrophobic catalyst functionalized with long alkyl chains(C_(12),dodecylamine)and further manufactured with poly(vinylidene fluoride),Pt@MIL-101-12/PVDF,has been developed which can show dramatically improved catalytic activity under multi-phase reactions involving hydrogen gas and liquid water.Pt@MIL-101-12/PVDF demonstrates enhanced macroscopic water-blocking properties,with a notable reduction of over 65%in water adsorption capacity and newly introduced liquid water repellency.while exhibiting a negligible increase in mass transfer resistance,i.e.,bifunctional hydrophobicity.Excellent catalytic activity,evaluated via HIE reaction,and its durability underscore the impact of bifunctional hydrophobicity.In situ DRIFTS analysis elucidates water adsorption/desorption dynamics within the catalyst composite,highlighting reinforced water diffusion at the microscopic level,affirming the catalyst's bifunctionality in different length scales.With demonstrated radiation resistance,Pt@MIL-101-12/PVDF emerges as a promising candidate for isotope exchange reactions.展开更多
Artificial photosynthesis presents a sustainable and cost-effective approach to harnessing solar energy to produce value-added chemicals[1,2].In particular,the simultaneous photocatalytic conversion of CO_(2)and H_(2)...Artificial photosynthesis presents a sustainable and cost-effective approach to harnessing solar energy to produce value-added chemicals[1,2].In particular,the simultaneous photocatalytic conversion of CO_(2)and H_(2)O into formic acid(HCOOH)and hydrogen peroxide(H2O2)has emerged as a promising strategy to mitigate global warming driven by CO_(2)emissions.HCOOH is a versatile chemical and hydrogen carrier,offering economic and practical advantages due to its compatibility with existing industrial processes and energy storage/conversion systems.Meanwhile,H_(2)O_(2)is among the world’s top 100 essential chemicals,with a global market valued at$4.0 billion in 2020 and projected to grow to$5.2 billion by 2026.展开更多
Lithium metal batteries(LMBs)offer high energy densities but face challenges including poor reversibility and Li dendrite growth.Herein,we evaluate two flexible composite current collectors composed of reduced graphen...Lithium metal batteries(LMBs)offer high energy densities but face challenges including poor reversibility and Li dendrite growth.Herein,we evaluate two flexible composite current collectors composed of reduced graphene oxide and carbon nanotubes(rGO/CNT)to investigate how Li storage mechanisms influence electrochemical performance.By modulating the number of layers in rGO,the few-layered rGO/CNT collector(FL-CC)stores Li through a pure plating mechanism,whereas the multi-layered rGO/CNT collector(ML-CC)stores lithium via a hybrid intercalation/plating mechanism.The hybrid mechanism in ML-CC promotes reversible Li-ion storage,reduces active Li-ion loss,and suppresses dendrite formation.As a result,ML-CC achieves superior cycling stability compared to FLCC in both LMBs and anode-free LMB tests paired with LiFePO_(4)cathodes at a practical areal capacity of 4.5 mAh cm^(-2).This study highlights the importance of structural design in current collectors and demonstrates that incorporating lithiatable materials can significantly enhance the electrochemical stability of anode-free LMBs.展开更多
Geometric and structural integrity often deteriorate in 3D printed cell-laden constructs over time due to cellular compaction and hydrogel shrinkage.This study introduces a new approach that synergizes the advantages ...Geometric and structural integrity often deteriorate in 3D printed cell-laden constructs over time due to cellular compaction and hydrogel shrinkage.This study introduces a new approach that synergizes the advantages of cell compatibility of biological hydrogels and mechanical stability of elastomeric polymers for structure fidelity maintenance upon stereolithography and extrusion 3D printing.Enabling this advance is the composite bioink,formulated by integrating elastomeric microparticles from poly(octamethylene maleate(anhydride)citrate)(POMaC)into biologically derived hydrogels(fibrin,gelatin methacryloyl(GelMA),and alginate).The composite bioink enhanced the elasticity and plasticity of the 3D printed constructs,effectively mitigating tissue compaction and swelling.It exhibited a low shear modulus and a rapid crosslinking time,along with a high ultimate compressive strength and resistance to deformation from cellular forces and physical handling;this was attributed to packing and stress dissipation of elastomeric particles,which was confirmed via mathematical modelling.Enhanced functional assembly and stability of human iPSC-derived cardiac tissues and primary vasculature proved the utility of the composite bioink in tissue engineering.In vivo implantation studies revealed that constructs containing POMaC particles exhibited improved resilience against host tissue stress,enhanced angiogenesis,and infiltration of pro-reparative macrophages.展开更多
Ionic clays,formed by the natural weathering of REE-bearing minerals and the adsorption of the resulting liberated REE ions onto the clay surface,are an important resource for critical rare earth elements(REEs).Here,a...Ionic clays,formed by the natural weathering of REE-bearing minerals and the adsorption of the resulting liberated REE ions onto the clay surface,are an important resource for critical rare earth elements(REEs).Here,a two-step desorption process using ammonium sulfate with active pH adjustment using sulfuric acid was developed to extract REEs from a South American clay.The desorption process was optimized using response surface methodology approach and the optimum operating conditions were determined to be 0.15 mol/L ammonium sulfate,pH 3,liquid to solid ratio of 3/1,and 25℃ with20 min residence time.It is shown that this ionic clay is significantly different from previously reported clays,e.g.,from southern China,as it consists of three modes of REEs,including ion-exchanged REEs physically adsorbed on the clay surface,hydrolyzed REEs chemically adsorbed on the clay surface,and mineralized(non-desorbable) REEs within the clay.Mechanistic investigations through progressive acidification during desorption and adsorption isotherms show that REE desorption/adsorption occurs due to the combined action of physical ion exchange adsorption and surface complexation chemical adsorption,with their relative importance depending on the pH of the system and the amount of sulfate anions present within the solution.This work supports overall efforts to utilize ionic clays as a relatively new resource for REEs to empower the development and adoption of modern green technologies such as wind turbines and electric vehicles.展开更多
Traffic-related pollutants adversely affect air quality, especially in regions near major roadways. The vehicleinduced turbulence(VIT) is a significant factor that controls the initial dilution, dispersion, and ultima...Traffic-related pollutants adversely affect air quality, especially in regions near major roadways. The vehicleinduced turbulence(VIT) is a significant factor that controls the initial dilution, dispersion, and ultimately the chemical and physical fate of pollutants by altering the conditions in the microenvironment. This study used a computational fluid dynamics(CFD) software FLUENT to model the vehicle-induced turbulence(VIT) generated on roadways, with a focus on impact of vehicle-vehicle interactions, traffic density and vehicle composition on turbulent kinetic energy(TKE). We show, for the first time, that the overall TKE from multiple vehicles traveling in series can be estimated by superimposing the TKE of each vehicle, without considering the distance between them while the distance is greater than one vehicle length. This finding is particularly significant since it enables a new approach to VIT simulations where the overall TKE is calculated as a function of number of vehicles. We found that the interactions between vehicles traveling next to each other in adjacent lanes are insignificant,regardless the directions of the traffic flow. Consequently, simulations of different traffic scenarios can be substantially simplified by treating two-way traffic as one-way traffic, with less than 5% difference in the overall volume-averaged TKE. We also developed equations that allow the estimation of the overall volume-averaged TKE as a function of the number and the type of vehicles.展开更多
Froth flotation is an essential processing technique for upgrading low-grade ores.Flotation separation would not be efficient without chemical surfactants(collectors,depressants,frothers,etc.).Depressants play a criti...Froth flotation is an essential processing technique for upgrading low-grade ores.Flotation separation would not be efficient without chemical surfactants(collectors,depressants,frothers,etc.).Depressants play a critical role in the selective separation of minerals in that they deactivate unfavorable mineral surfaces and hinder them from floating into the flotation concentration zone.Pyrite is the most common and challenging sulfide gangue,and its conventional depressants could be highly harmful to nature and humans.Therefore,using available,affordable,eco-friendly polymers to assist or replace hazardous reagents is mandatory for a green transition.Polysaccharide-based(starch,dextrin,carboxymethyl cellulose,guar gum,etc.)polymers are one of the most used biodegradable depressant groups for pyrite depression.Despite the satisfactory flotation results obtained using these eco-friendly depressants,several gaps still need to be addressed,specifically in investigating surface interactions,adsorption mechanisms,and parameters affecting their depression performance.As a unique approach,this review comprehensively discussed previously conducted studies on pyrite depression with polysaccharide-based reagents.Additionally,practical suggestions have been provided for future assessments and developments of polysaccharide-based depressants,which pave the way to green flotation.This robust review also explored the depression efficiency and various adsorption aspects of naturally derived depressants on the pyrite surface to create a possible universal trend for each biodegradable depressant derivative.展开更多
The main purpose of this study was to optimize microwave assisted alkaline extraction of the hemicellulose, xylan, from birch wood. The simultaneous effects of process variables such as time (10 - 30 minutes), concent...The main purpose of this study was to optimize microwave assisted alkaline extraction of the hemicellulose, xylan, from birch wood. The simultaneous effects of process variables such as time (10 - 30 minutes), concentration of sodium hydroxide solution (4 - 8 wt%), solid to liquid ratio (1:8 to 1:20, g:mL), and sample size (5 - 10 g) on the temperature of the wood slurry, wood dissolution, and yield of extraction were evaluated. A central composite design (CCD) and response surface methodology (RSM) were used for the optimization of the extraction process. Based on the CCD, quadratic models were developed to correlate the extraction process variables with the responses such as temperature of wood slurry, wood dissolution, and yield of xylan and the models were analyzed using appropriate statistical methods (ANOVA). Statistical analysis showed that all the models developed were found to be adequate for the prediction of the respective responses. Optimization of the process was performed using a numerical optimization available in the software to maximize the yield of xylan and the optimum process variables for the maximum yield of xylan was found to be: 10 g of wood fibres, 8 wt% of NaOH solution, 1:10 solid to liquid ratio (g:mL) and 25 minutes of irradiation time. About 72.5% of the xylan present in the birch wood was extracted using the optimized extraction parameters.展开更多
基金funding from the European Union’s Hori-zon 2020 research and innovation programme under grant agree-ment No 872102H.X.thanks The University of Manchester Presi-dent’s Doctoral Scholar Award and the China Scholarship Council(file no.201606150068)for supporting her PhD research.
文摘Bioethanol produced via valorisation of renewable biomass is of great interest to many industries.The increased availability and decreased cost of bioethanol make it a promising platform molecule to produce a wide range of value-added chemicals and fuels via the catalytic conversions.This paper provides a comprehensive review of catalytic conversions of bioethanol to a variety of chemicals/fuels such as hydrogen,C_(2)-C_(4)olefins,gasoline and small oxygenates.Specifically,the focus was placed on the relationship between the catalyst property(such as pore structure,acidity,active metal sites,and catalyst supports)and the catalytic performance(including catalyst activity and stability),as well as the reaction mechanisms involved.Future research avenues on the catalyst design for improving catalytic valorisation of bioethanol are also discussed.
基金supported by Natural Science and Engineering Research Council of Canada(RGPIN-2017-06737)Canada Research Chairs program,the National Key Research and Development Program of China(2017YFD0601005,2022YFD0904201)+1 种基金the National Natural Science Foundation of China(51203075)the China Scholarship Council(Grant No.CSC202208320361).
文摘With the rapid development of flexible wearable electronics,the demand for stretchable energy storage devices has surged.In this work,a novel gradient-layered architecture was design based on single-pore hollow lignin nanospheres(HLNPs)-intercalated two-dimensional transition metal carbide(Ti_(3)C_(2)T_(x) MXene)for fabricating highly stretchable and durable supercapacitors.By depositing and inserting HLNPs in the MXene layers with a bottom-up decreasing gradient,a multilayered porous MXene structure with smooth ion channels was constructed by reducing the overstacking of MXene lamella.Moreover,the micro-chamber architecture of thin-walled lignin nanospheres effectively extended the contact area between lignin and MXene to improve ion and electron accessibility,thus better utilizing the pseudocapacitive property of lignin.All these strategies effectively enhanced the capacitive performance of the electrodes.In addition,HLNPs,which acted as a protective phase for MXene layer,enhanced mechanical properties of the wrinkled stretchable electrodes by releasing stress through slip and deformation during the stretch-release cycling and greatly improved the structural integrity and capacitive stability of the electrodes.Flexible electrodes and symmetric flexible all-solid-state supercapacitors capable of enduring 600%uniaxial tensile strain were developed with high specific capacitances of 1273 mF cm^(−2)(241 F g^(−1))and 514 mF cm^(−2)(95 F g^(−1)),respectively.Moreover,their capacitances were well preserved after 1000 times of 600%stretch-release cycling.This study showcased new possibilities of incorporating biobased lignin nanospheres in energy storage devices to fabricate stretchable devices leveraging synergies among various two-dimensional nanomaterials.
基金supported by Natural Sciences and Engineering Research Council of Canada Strategic Grants program(463037-14)Discovery Grants program(2016-05524,2022-04881,2020-04262)。
文摘The increasing demand for electronics has led to a desire to recover rare earth elements(REEs) from nonconventional sources,including mining and liquid waste effluents.Biosorption could be a promising method for adsorbing REEs onto microalgae,but biomass immobilization and light delivery challenges remain.It was recently shown that REEs biosorb 160% more on algal biofilms than suspended biomass due to the extracellular polymeric substance(EPS) matrix that grows abundantly in biofilms.In this work,we present findings on biosorption selectivity for different REEs in sulfate solutions.The maximum adsorption capacities of Euglena mutabilis suspensions and biofilms were determined for a mixed REE sulfate solution at an equimolar initial concentration range of 0.1-1 mol/L of each REE ion.The highest adsorption capacities for the suspension are for Sm and Eu which are 57% and 46% higher,respectively,compared to the average REE adsorption capacity.The biofilms also preferentially adsorb Sm,Eu,Yb and Lu at 0.035,0.033,0.033,and 0.031 mmol/g,respectively.The impact of dissolved divalent ions of Ca,Mg,and Fe on REE adsorption was also assessed.When Ca and Mg are added in equimolar amounts to0.1-1 mmol/L solutions of equimolar La,Eu,and Yb sulfate,the amount of REEs adsorbed onto suspensions increases by 30% while when Fe is added,it decreases by 10%.No change is observed in biofilms except when Fe is added resulting in a reduction of the adsorption capacity by 40%.A possible explanation for the role of Fe is attributed to the formation of stronger bonds at the binding sites compared to Ca and Mg.
基金the financial support of a special fund from the Beijing Key Laboratory of Lignocellulosic Chemistry,College of Materials Science and Technology,Beijing Forestry UniversityFinancial support from NSERC Discovery grant(RGPIN-2017-06737)+1 种基金Canada Research Chair program is also acknowledgedthe China Scholarship Council(CSC)for its financial support(CSC No.202306510047)。
文摘In an era where technological advancement and sustainability converge,developing renewable materials with multifunctional integration is increasingly in demand.This study filled a crucial gap by integrating energy storage,multi-band electromagnetic interference(EMI)shielding,and structural design into bio-based materials.Specifically,conductive polymer layers were formed within the 2,2,6,6-tetramethylpiperidine-1-oxide(TEMPO)-oxidized cellulose fiber skeleton,where a mild TEMPO-mediated oxidation system was applied to endow it with abundant macropores that could be utilized as active sites(specific surface area of 105.6 m2 g-1).Benefiting from the special hierarchical porous structure of the material,the constructed cellulose fiber-derived composites can realize high areal-specific capacitance of 12.44 F cm^(-2)at 5 m A cm^(-2)and areal energy density of 3.99 m Wh cm^(-2)(2005 m W cm^(-2))with an excellent stability of maintaining 90.23%after 10,000 cycles at 50 m A cm^(-2).Meanwhile,the composites showed a high electrical conductivity of 877.19 S m-1 and excellent EMI efficiency(>99.99%)in multiple wavelength bands.The composite material’s EMI values exceed 100 d B across the L,S,C,and X bands,effectively shielding electromagnetic waves in daily life.The proposed strategy paves the way for utilizing bio-based materials in applications like energy storage and EMI shielding,contributing to a more sustainable future.
基金supported by Ministry of Science and ICT,South Korea(RS‐2024‐00407282)National Research Foundation of Korea(RS‐2024‐00408156).
文摘The practical application of lithium(Li)metal batteries(LMBs)faces challenges due to the irreversible Li deposition/dissolution process,which promotes Li dendrite growth with severe parasitic reactions during cycling.To address these issues,achieving uniform Li‐ion flux and improving Li‐ion conductivity of the separator are the top priorities.Herein,a separator(PCELS)with enhanced Li‐ion conductivity,composed of polymer,ceramic,and electrically conductive carbon,is proposed to facilitate fast Li‐ion transport kinetics and increase Li deposition uniformity of the LMBs.The PCELS immobilizes PF6–anions with high adsorption energies,leading to a high Li‐ion transference number.Simultaneously,the PCELS shows excellent electrolyte wettability on both its sides,promoting rapid ion transport.Moreover,the electrically conductive carbon within the PCELS provides additional electron transport channels,enabling efficient charge transfer and uniform Li‐ion flux.With these advantages,the PCELS achieves rapid Li‐ion transport kinetics and uniform Li deposition,demonstrating excellent cycling stability over 100 cycles at a high current density of 12.0 mA cm^(-2).Furthermore,the PCELS shows stable cycling performances in Li–S cell tests and delivers an excellent capacity retention of 95.45%in the Li|LiFePO_(4) full‐cell test with a high areal capacity of over 5.5 mAh cm^(-2).
基金supported by the National Natural Science Foundation of China(21776077)the Program for Professor of Special Appointment(Eastern Scholar)at Shanghai Institutions of Higher Learning+3 种基金the Shanghai Rising-Star Program(17QA1401200)the Open Project of SKLOCE(SKL-Che-15C03)the Shanghai Natural Science Foundation(17ZR1407300 and 17ZR1407500)the State Key Laboratory of Organic-Inorganic Composites(oic201801007)。
文摘Heterogeneously catalyzed hydrolytic dehydrogenation of ammonia borane is a remarkable structure sensitive reaction. In this work, a strategy by using polyoxometalates(POMs) as the ligands is proposed to engineer the surface and electronic properties of Pt/CNT catalysts toward the enhanced hydrogen generation rate and durability. Three kinds of POMs, i.e., silicotungstic acid(STA), phosphotungstic acid(PTA)and molybdophosphoric acid(PMA), are comparatively studied, among which the STA shows positive effects on the catalytic activity and durability. A catalyst structure-performance relationship is established by a combination of kinetic and isotopic analyses with multiple characterization techniques, such as HAADF-STEM, EDS, Raman spectroscopy and XPS. It is shown that the STA compared to the other two POMs can increase the Pt binding energy and thus promote the reaction. The insights demonstrated here could open a new avenue for boosting the reaction by employing the POMs as the ligands to engineer the catalyst electronic properties.
基金This research was supported by the National Key and Fundamental ResearchDevelopment Programming Projects 863 (No. 2002AA648010).
文摘Objective The wetland at Dalian Bay in the Northeast of China has been polluted by oil severely. The effect of various microbes and operation parameters on the bioremediation of oil-polluted wetlands at Dalian Bay was investigated and reported previously. In the study, other operation conditions related to the status of medium were investigated via statistical experimental design and analysis and a necessary information is involved to use micro-technology in the application. Methods The method used involved the direct inoculation of selected bacteria, which were capable of degrading oil. The operation conditions were further optimized and evaluated by gravimetrical assay. Results The optimal pH and temperature for the studied bacteria to degrade the existing oil pollutants were established as pH 8.0 and 27℃. The mixed of various bacteria showed better results in terms of oil degradation than any single one. Among the selected four factors, disturbance, oxidant, nutrients, and biosurfactant, the former two contributed more impacts on the oil degradation in the early stage of process, while the latter two became the limiting factors in the late stage. Three sets of optimal conditions were obtained for each individual stage, but no one was suitable for the overall process. Conclusion The study demonstrated the technical feasibility of using direct inoculation into the contaminated soil samples to remove oil pollutants. It suggested that the operation conditions should be monitored and adjusted during the different stages of bio-reactions in the process to achieve the best result of oil degradation.
文摘The dry deposition process refers to the flux loss of an atmospheric pollutant due to uptake of the pollutant by the earth’s surfaces.Dry deposition flux of a chemical species is typically calculated as the product of its surface-layer concentration and its dry deposition velocity(V_(d)).Field measurement based V_(d) data are very scarce or do not exist for many chemical species considered in chemistry transport models.In the present study,gaseous and particulate dry deposition schemes were applied to generate a database of hourly V_(d) for 45 gaseous species and three particle size ranges for two years(2016–2017)at a 15 kmby 15 km horizontal resolution across North America.Hourly V_(d) of the 45 gaseous species ranged from<0.001 to 4.6 cm/sec across the whole domain,with chemical species-dependentmedian(mean)values being in the range of 0.018–1.37 cm/sec(0.05–1.43 cm/sec).The spatial distributions of the two-year average V_(d) showed values higher than 1–3 cm/sec for those soluble and reactive species over certain land types.Soluble species have the highest V_(d) over water surfaces,while insoluble but reactive species have the highest V_(d) over forests.Hourly V_(d) of PM_(2.5) across the whole domain ranged from 0.039 to 0.75 cm/sec with median(mean)value of 0.18(0.20)cm s^(−1),while the mean V_(d) for PM_(2.5)–10 is twice that of PM_(2.5).Uncertainties in the modeled V_(d) are typically on the order of a factor of 2.0 or larger,which needs to be considered when applying the dataset in other studies.
文摘Double fortified salt containing both potassium iodate and ferrous fumarate microcapsules was produced at an Indian commercial facility. The packaged product became discolored, turning yellow, to a degree that would impact consumer acceptance. Therefore, there was a need for an investigation into the cause and possible remedy for this discoloration. The components of the fortified salt product, storage conditions, and processing characteristics were taken into consideration. Canadian and Indian salt samples were prepared unfortified as well as with iodine and/or iron microcapsules;stored at 25°C and 45°C in glass, polyethylene, or commercial polymer film. Some samples were heat treated prior to storage. Salt samples containing iodine that were heated before storage in packaging material turned yellow in color. From this study, it was found that due to heat and the presence of a sacrificial antioxidant component in the packaging film, potassium iodate was reduced to elemental iodine (I<sub>2</sub>) turning packaged salt samples to a yellow/orange color. Hence it is recommended that in the manufacture of foods containing potassium iodate, the packaging material selected should be free from readily accessible antioxidants.
基金Supported by the National Natural Science Foundation of China under Grant Nos 11072057 and 51376040, the Foundation of Canadian Space Agency under Grant No 9F007-02-6019, and the Research Fund of Japan Aerospace Exploration Agency.
文摘A three-dimensional direct numerical simulation is carried out to predict the surface oscillation and flow structure of isothermal liquid bridges of 5 cSt silicone oil held vertically between solid disks. By subjecting liquid bridges to various horizontal vibrations, the surface resonance frequencies are clearly determined numerically and compared well with the existing analytical model predictions. The investigation on the flow structure inside the liquid bridge reveals, for the first time, the flow structure and the existence of transw＇,rsal vortices inside the liquid bridge when a horizontal vibration is applied.
基金supported by grants from the National Research Foundation of Korea(NRF)under grant No.RS-2022-00155422 and No.2021R1C1C102014。
文摘Water often presents significant challenges in catalysts by deactivating active sites,poisoning the reaction,and even degrading composite structure.These challenges are amplified when the water participates as a reactant and is fed as a liquid phase,such as trickle bed-type reactors in a hydrogen-water isotope exchange(HIE)reaction.The key balance in such multiphase reactions is the precise control of catalyst design to repel bulk liquid water while diffusing water vapor.Herein,a platinum-incorporated metal-organic framework(MIL-101)based bifunctional hydrophobic catalyst functionalized with long alkyl chains(C_(12),dodecylamine)and further manufactured with poly(vinylidene fluoride),Pt@MIL-101-12/PVDF,has been developed which can show dramatically improved catalytic activity under multi-phase reactions involving hydrogen gas and liquid water.Pt@MIL-101-12/PVDF demonstrates enhanced macroscopic water-blocking properties,with a notable reduction of over 65%in water adsorption capacity and newly introduced liquid water repellency.while exhibiting a negligible increase in mass transfer resistance,i.e.,bifunctional hydrophobicity.Excellent catalytic activity,evaluated via HIE reaction,and its durability underscore the impact of bifunctional hydrophobicity.In situ DRIFTS analysis elucidates water adsorption/desorption dynamics within the catalyst composite,highlighting reinforced water diffusion at the microscopic level,affirming the catalyst's bifunctionality in different length scales.With demonstrated radiation resistance,Pt@MIL-101-12/PVDF emerges as a promising candidate for isotope exchange reactions.
文摘Artificial photosynthesis presents a sustainable and cost-effective approach to harnessing solar energy to produce value-added chemicals[1,2].In particular,the simultaneous photocatalytic conversion of CO_(2)and H_(2)O into formic acid(HCOOH)and hydrogen peroxide(H2O2)has emerged as a promising strategy to mitigate global warming driven by CO_(2)emissions.HCOOH is a versatile chemical and hydrogen carrier,offering economic and practical advantages due to its compatibility with existing industrial processes and energy storage/conversion systems.Meanwhile,H_(2)O_(2)is among the world’s top 100 essential chemicals,with a global market valued at$4.0 billion in 2020 and projected to grow to$5.2 billion by 2026.
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korea goverment(MSIT)(RS-2025-02218301)supported by the Nano&Material Technology Development Program through the National Research Foundation of Korea(NRF)funded by Ministry of Science and ICT(No.RS-2024-00412289).
文摘Lithium metal batteries(LMBs)offer high energy densities but face challenges including poor reversibility and Li dendrite growth.Herein,we evaluate two flexible composite current collectors composed of reduced graphene oxide and carbon nanotubes(rGO/CNT)to investigate how Li storage mechanisms influence electrochemical performance.By modulating the number of layers in rGO,the few-layered rGO/CNT collector(FL-CC)stores Li through a pure plating mechanism,whereas the multi-layered rGO/CNT collector(ML-CC)stores lithium via a hybrid intercalation/plating mechanism.The hybrid mechanism in ML-CC promotes reversible Li-ion storage,reduces active Li-ion loss,and suppresses dendrite formation.As a result,ML-CC achieves superior cycling stability compared to FLCC in both LMBs and anode-free LMB tests paired with LiFePO_(4)cathodes at a practical areal capacity of 4.5 mAh cm^(-2).This study highlights the importance of structural design in current collectors and demonstrates that incorporating lithiatable materials can significantly enhance the electrochemical stability of anode-free LMBs.
文摘Geometric and structural integrity often deteriorate in 3D printed cell-laden constructs over time due to cellular compaction and hydrogel shrinkage.This study introduces a new approach that synergizes the advantages of cell compatibility of biological hydrogels and mechanical stability of elastomeric polymers for structure fidelity maintenance upon stereolithography and extrusion 3D printing.Enabling this advance is the composite bioink,formulated by integrating elastomeric microparticles from poly(octamethylene maleate(anhydride)citrate)(POMaC)into biologically derived hydrogels(fibrin,gelatin methacryloyl(GelMA),and alginate).The composite bioink enhanced the elasticity and plasticity of the 3D printed constructs,effectively mitigating tissue compaction and swelling.It exhibited a low shear modulus and a rapid crosslinking time,along with a high ultimate compressive strength and resistance to deformation from cellular forces and physical handling;this was attributed to packing and stress dissipation of elastomeric particles,which was confirmed via mathematical modelling.Enhanced functional assembly and stability of human iPSC-derived cardiac tissues and primary vasculature proved the utility of the composite bioink in tissue engineering.In vivo implantation studies revealed that constructs containing POMaC particles exhibited improved resilience against host tissue stress,enhanced angiogenesis,and infiltration of pro-reparative macrophages.
基金Aclara Resources Inc.for providing financial support for this study。
文摘Ionic clays,formed by the natural weathering of REE-bearing minerals and the adsorption of the resulting liberated REE ions onto the clay surface,are an important resource for critical rare earth elements(REEs).Here,a two-step desorption process using ammonium sulfate with active pH adjustment using sulfuric acid was developed to extract REEs from a South American clay.The desorption process was optimized using response surface methodology approach and the optimum operating conditions were determined to be 0.15 mol/L ammonium sulfate,pH 3,liquid to solid ratio of 3/1,and 25℃ with20 min residence time.It is shown that this ionic clay is significantly different from previously reported clays,e.g.,from southern China,as it consists of three modes of REEs,including ion-exchanged REEs physically adsorbed on the clay surface,hydrolyzed REEs chemically adsorbed on the clay surface,and mineralized(non-desorbable) REEs within the clay.Mechanistic investigations through progressive acidification during desorption and adsorption isotherms show that REE desorption/adsorption occurs due to the combined action of physical ion exchange adsorption and surface complexation chemical adsorption,with their relative importance depending on the pH of the system and the amount of sulfate anions present within the solution.This work supports overall efforts to utilize ionic clays as a relatively new resource for REEs to empower the development and adoption of modern green technologies such as wind turbines and electric vehicles.
基金financial support from Environment Canada and the Government of Ontario (72021622) for a scholarship to YK
文摘Traffic-related pollutants adversely affect air quality, especially in regions near major roadways. The vehicleinduced turbulence(VIT) is a significant factor that controls the initial dilution, dispersion, and ultimately the chemical and physical fate of pollutants by altering the conditions in the microenvironment. This study used a computational fluid dynamics(CFD) software FLUENT to model the vehicle-induced turbulence(VIT) generated on roadways, with a focus on impact of vehicle-vehicle interactions, traffic density and vehicle composition on turbulent kinetic energy(TKE). We show, for the first time, that the overall TKE from multiple vehicles traveling in series can be estimated by superimposing the TKE of each vehicle, without considering the distance between them while the distance is greater than one vehicle length. This finding is particularly significant since it enables a new approach to VIT simulations where the overall TKE is calculated as a function of number of vehicles. We found that the interactions between vehicles traveling next to each other in adjacent lanes are insignificant,regardless the directions of the traffic flow. Consequently, simulations of different traffic scenarios can be substantially simplified by treating two-way traffic as one-way traffic, with less than 5% difference in the overall volume-averaged TKE. We also developed equations that allow the estimation of the overall volume-averaged TKE as a function of the number and the type of vehicles.
基金a project financially supported by CAMM3,the Center of Advanced Mining and Metallurgy,a center of excellence at the Lule?University of Technology。
文摘Froth flotation is an essential processing technique for upgrading low-grade ores.Flotation separation would not be efficient without chemical surfactants(collectors,depressants,frothers,etc.).Depressants play a critical role in the selective separation of minerals in that they deactivate unfavorable mineral surfaces and hinder them from floating into the flotation concentration zone.Pyrite is the most common and challenging sulfide gangue,and its conventional depressants could be highly harmful to nature and humans.Therefore,using available,affordable,eco-friendly polymers to assist or replace hazardous reagents is mandatory for a green transition.Polysaccharide-based(starch,dextrin,carboxymethyl cellulose,guar gum,etc.)polymers are one of the most used biodegradable depressant groups for pyrite depression.Despite the satisfactory flotation results obtained using these eco-friendly depressants,several gaps still need to be addressed,specifically in investigating surface interactions,adsorption mechanisms,and parameters affecting their depression performance.As a unique approach,this review comprehensively discussed previously conducted studies on pyrite depression with polysaccharide-based reagents.Additionally,practical suggestions have been provided for future assessments and developments of polysaccharide-based depressants,which pave the way to green flotation.This robust review also explored the depression efficiency and various adsorption aspects of naturally derived depressants on the pyrite surface to create a possible universal trend for each biodegradable depressant derivative.
文摘The main purpose of this study was to optimize microwave assisted alkaline extraction of the hemicellulose, xylan, from birch wood. The simultaneous effects of process variables such as time (10 - 30 minutes), concentration of sodium hydroxide solution (4 - 8 wt%), solid to liquid ratio (1:8 to 1:20, g:mL), and sample size (5 - 10 g) on the temperature of the wood slurry, wood dissolution, and yield of extraction were evaluated. A central composite design (CCD) and response surface methodology (RSM) were used for the optimization of the extraction process. Based on the CCD, quadratic models were developed to correlate the extraction process variables with the responses such as temperature of wood slurry, wood dissolution, and yield of xylan and the models were analyzed using appropriate statistical methods (ANOVA). Statistical analysis showed that all the models developed were found to be adequate for the prediction of the respective responses. Optimization of the process was performed using a numerical optimization available in the software to maximize the yield of xylan and the optimum process variables for the maximum yield of xylan was found to be: 10 g of wood fibres, 8 wt% of NaOH solution, 1:10 solid to liquid ratio (g:mL) and 25 minutes of irradiation time. About 72.5% of the xylan present in the birch wood was extracted using the optimized extraction parameters.
