Coal gasification fine slag(FS)is a typical solid waste generated in coal gasification.Its current disposal methods of stockpil-ing and landfilling have caused serious soil and ecological hazards.Separation recovery a...Coal gasification fine slag(FS)is a typical solid waste generated in coal gasification.Its current disposal methods of stockpil-ing and landfilling have caused serious soil and ecological hazards.Separation recovery and the high-value utilization of residual carbon(RC)in FS are the keys to realizing the win-win situation of the coal chemical industry in terms of economic and environmental benefits.The structural properties,such as pore,surface functional group,and microcrystalline structures,of RC in FS(FS-RC)not only affect the flotation recovery efficiency of FS-RC but also form the basis for the high-value utilization of FS-RC.In this paper,the characteristics of FS-RC in terms of pore structure,surface functional groups,and microcrystalline structure are sorted out in accordance with gasification type and FS particle size.The reasons for the formation of the special structural properties of FS-RC are analyzed,and their influence on the flotation separation and high-value utilization of FS-RC is summarized.Separation methods based on the pore structural characterist-ics of FS-RC,such as ultrasonic pretreatment-pore-blocking flotation and pore breaking-flocculation flotation,are proposed to be the key development technologies for improving FS-RC recovery in the future.The design of low-cost,low-dose collectors containing polar bonds based on the surface and microcrystalline structures of FS-RC is proposed to be an important breakthrough point for strengthening the flotation efficiency of FS-RC in the future.The high-value utilization of FS should be based on the physicochemical structural proper-ties of FS-RC and should focus on the environmental impact of hazardous elements and the recyclability of chemical waste liquid to es-tablish an environmentally friendly utilization method.This review is of great theoretical importance for the comprehensive understand-ing of the unique structural properties of FS-RC,the breakthrough of the technological bottleneck in the efficient flotation separation of FS,and the expansion of the field of the high value-added utilization of FS-RC.展开更多
Studying the relationship between ionic interactions and salt solubility in seawater has implications for seawater desalination and mineral extraction.In this paper,a new method of expressing ion-to-ion interaction is...Studying the relationship between ionic interactions and salt solubility in seawater has implications for seawater desalination and mineral extraction.In this paper,a new method of expressing ion-to-ion interaction is proposed by using molecular dynamics simulation,and the relationship between ion-to-ion interaction and salt solubility in a simulated seawater water-salt system is investigated.By analyzing the variation of distance and contact time between ions in an electrolyte solution,from both spatial and temporal perspectives,new parameters were proposed to describe the interaction between ions:interaction distance(ID),and interaction time ratio(ITR).The best correlation between characteristic time ratio and solubility was found for a molar ratio of salt-to-water of 10:100 with a correlation coefficient of 0.96.For the same salt,a positive correlation was found between CTR and the molar ratio of salt and water.For type 1-1,type 2-1,type 1-2,and type 2-2 salts,the correlation coefficients between CTR and solubility were 0.93,0.96,0.92,and 0.98 for a salt-to-water molar ratio of 10:100,respectively.The solubility of multiple salts was predicted by simulations and compared with experimental values,yielding an average relative deviation of 12.4%.The new ion-interaction parameters offer significant advantages in describing strongly correlated and strongly hydrated electrolyte solutions.展开更多
Yolk-shell SiO2 particles(YP)with center-radial meso-channels were fabricated through a simple and effective method.Al-containing YP-supported NiMo catalysts with different Al amounts(NiMo/AYP-x,x=Si/Al molar proporti...Yolk-shell SiO2 particles(YP)with center-radial meso-channels were fabricated through a simple and effective method.Al-containing YP-supported NiMo catalysts with different Al amounts(NiMo/AYP-x,x=Si/Al molar proportion)were prepared and dibenzothiophene(DBT)and 4,6-dimethyl-dibenzothiophene(4,6-DMDBT)were employed as the probes to evaluate the hydrodesulfurization(HDS)catalytic performance.The as-prepared AYP-x carriers and corresponding catalysts were characterized by some advanced characterizations to obtain deeper correlations between physicochemical properties and the HDS performance.The average pore sizes of series AYP-x supports are above 6.0 nm,which favors the mass transfer of organic sulfides.The cavity between the yolk and the shell is beneficial for the enrichment of S-containing compounds and the accessibility between reactants and active metals.Aluminum embedded into the silica framework could facilitate the formation of Lewis(L)and Brønsted(B)acid sites and adjust the metal-support interaction(MSI).Among all the as-synthesized catalysts,NiMo/AYP-20 catalyst shows the highest HDS activities.The improved HDS activity of NiMo/AYP-20 catalyst is attributed to the perfect combination of excellent structural properties of the yolk-shell mesoporous silica,enhanced acidity,moderate MSI,and good accessibility/dispersion of active components.展开更多
To simplify the composite propellant formulation and address the current issue of the single-functionality present in existing additives,the multi-cyano,amine-based polybutadiene(AEHTPB-CN)was prepared based on AEHTPB...To simplify the composite propellant formulation and address the current issue of the single-functionality present in existing additives,the multi-cyano,amine-based polybutadiene(AEHTPB-CN)was prepared based on AEHTPB by adopting appropriate synthesis strategies.By replacing 10% of HTPB binder in the propellant formulation,it can effectively enhance the interfacial bond strength between the propellant binder matrix and solid fillers(AP(ammonium perchlorate)and RDX(cyclotrimethylene-trinitramine)),the mechanical properties of the HTPB/AP/RDX/Al propellant were superior to blank control propellant with an improvement of 35.4% in tensile strength,62.0% enhancement in elongation at break,and reduce the propellant burn rate by 10.7% with any energy loss.The function mechanism of AEHTPB-CN was systematically elucidated through experiments and computer simulation techniques.The results show that the tertiary amine group in AEHTPB-CN can react with AP to form ammonium ionic bonds,and the hydroxyl and cyano groups can form hydrogen bonding interactions with AP,which enables AEHTPB-CN to be firmly adsorbed on the AP surface through chemical and physical interactions.For RDX,the interfacial bonding effect of AEHTPB-CN is attributed to their ability to form C-H···N≡C weak hydrogen bonding interaction between the cyano group and RDX methylene group.展开更多
Exploitation of oxygen evolution reaction(OER)and urea oxidation reaction(UOR)catalysts with high activity and stability at large current density is a major challenge for energy-saving H_(2) production in water electr...Exploitation of oxygen evolution reaction(OER)and urea oxidation reaction(UOR)catalysts with high activity and stability at large current density is a major challenge for energy-saving H_(2) production in water electrolysis.Herein,we use the pyridinic-N doping carbon layers coupled with tensile strain of FeNi alloy activated by NiFe_(2)O_(4)(FeNi/NiFe_(2)O_(4)@NC)for efficiently increasing the performance of water and urea oxidation.Due to the tensile strain effect on FeNi/NiFe_(2)O_(4)@NC,it provides a favorable modulation on the electronic properties of the active center,thus enabling amazing OER(η_(100)=196 mV)and UOR(E_(10)=1.32 V)intrinsic activity.Besides,the carbon-coated layers can be used as armor to prevent FeNi alloy from being corroded by the electrolyte for enhancing the OER/UOR stability at large current density,showing high industrial practicability.This work thus provides a simple way to prepare high-efficiency catalyst for activating water and urea oxidation.展开更多
The pursuit of high-performance is worth considerable effort in catalysis for energy efficiency and environmental sustainability. To develop redox catalysts with superior performance for soot combustion, a series of M...The pursuit of high-performance is worth considerable effort in catalysis for energy efficiency and environmental sustainability. To develop redox catalysts with superior performance for soot combustion, a series of Mn_(x)Co_(y) oxides were synthesized using MgO template substitution.This method greatly improves the preparation and catalytic efficiency and is more in line with the current theme of green catalysts and sustainable development. The resulting Mn_(1)Co_(2.3) has a strong activation capability of gaseous oxygen due to a high concentration of Co^(3+) and Mn^(3+). The Mn doping enhanced the intrinsic activity by prompting oxygen vacancy formation and gaseous oxygen adsorption. The nanosheet morphology with abundant mesoporous significantly increased the solid–solid contact efficiency and improved the adsorption capability of gaseous reactants. The novel design of Mn_(1)Co_(2.3)oxide enhanced its catalytic performance through a synergistic effect of Mn doping and the porous nanosheet morphology, showing significant potential for the preparation of high-performance soot combustion catalysts.展开更多
Implementing a new energy-saving electrochemical synthesis system with high commercial value is a strategy of the sustainable development for upgrading the bulk chemicals preparation technology in the future.Here,we r...Implementing a new energy-saving electrochemical synthesis system with high commercial value is a strategy of the sustainable development for upgrading the bulk chemicals preparation technology in the future.Here,we report a multiple redox-mediated linear paired electrolysis system,combining the hydrogen peroxide mediated cathode process with the I2 mediated anode process,and realize the conversion of furfural to furoic acid in both side of the dividedflow cell simultaneously.By reasonably controlling the cathode potential,the undesired water splitting reaction and furfural reduction side reactions are avoided.Under the galvanostatic electrolysis,the two-mediated electrode processes have good compatibility,which reduce the energy consumption by about 22%while improving the electronic efficiency by about 125%.This system provides a green electrochemical synthesis route with commercial prospects.展开更多
Two-dimensional(2D)magnetic materials have been demonstrated to have excellent chemical,optical,electrical,and magnetic properties,particularly in the development of multifunctional electronic and spin electronic devi...Two-dimensional(2D)magnetic materials have been demonstrated to have excellent chemical,optical,electrical,and magnetic properties,particularly in the development of multifunctional electronic and spin electronic devices,showcasing tremendous potential.Therefore,corresponding synthesis techniques for 2D magnetic materials that offer high quality,high yield,low cost,time-saving,and simplicity are highly desired.This review provides a comprehensive overview of recent research advances in preparation of magnetic 2D materials,with a particular focus on the preparation methods employed.Moreover,the characteristics and applications of these magnetic materials are also discussed.Finally,the challenges and prospects of synthesis methods for magnetic 2D materials are briefly addressed.This review serves as a guiding reference for the controlled synthesis of 2D magnetic materials.展开更多
The autotetraploid Carassius auratus(4nRR,4n=200,RRRR)is derived from whole-genome duplication of Carassius auratus red var.(RCC,2n=100,RR).In the current study,we demonstrated that chromatophores and pigment changes ...The autotetraploid Carassius auratus(4nRR,4n=200,RRRR)is derived from whole-genome duplication of Carassius auratus red var.(RCC,2n=100,RR).In the current study,we demonstrated that chromatophores and pigment changes directly caused the coloration and variation of 4nRR skin(red in RCC,brownish-yellow in4nRR).To further explore the molecular mechanisms underlying coloration formation and variation in 4nRR,we performed transcriptome profiling and molecular functional verification in RCC and 4nRR.Results revealed that scarb1,associated with carotenoid metabolism,underwent significant down-regulation in 4nRR.Efficient editing of this candidate pigment gene provided clear evidence of its significant role in RCC coloration.Subsequently,we identified four divergent scarb1 homeologs in 4nRR:two original scarb1 homeologs from RCC and two duplicated ones.Notably,three of these homeologs possessed two highly conserved alleles,exhibiting biased and allelespecific expression in the skin.Remarkably,after precise editing of both the original and duplicated scarb1homeologs and/or alleles,4nRR individuals,whether singly or multiply mutated,displayed a transition from brownishyellow skin to a cyan-gray phenotype.Concurrently,the proportional areas of the cyan-gray regions displayed a gene-dose correlation.These findings illustrate the subfunctionalization of duplicated scarb1,with all scarb1genes synergistically and equally contributing to the pigmentation of 4nRR.This is the first report concerning the functional differentiation of duplicated homeologs in an autopolyploidfish,substantiallyenrichingour understanding of coloration formation and change within this group of organisms.展开更多
A silylated melamine sponge(SMS)was prepared by two simple steps,namely,immersion and dehydration of a melamine sponge coated with methyltrichlorosilane.The silylated structure of SMS was characterized by FT-IR(Fourie...A silylated melamine sponge(SMS)was prepared by two simple steps,namely,immersion and dehydration of a melamine sponge coated with methyltrichlorosilane.The silylated structure of SMS was characterized by FT-IR(Fourier-transform infrared)spectroscopy,SEM(Scanning electron microscopy)and in terms of water contact angles.Its oil-water absorption and separation capacities were measured by FT-IR and UV-visible spectrophoto-metry.The experimental results have shown that oligomeric silanol covalently bonds by Si-N onto the surface of melamine sponge skeletons.SMS has shown superhydrophobicity with a water contact angle exceeding 150°±1°,a better separation efficiency with regard to diesel oil(by 99.31%(wt/wt%)in oil-water mixture and even up to 99.99%(wt/wt%)for diesel oil in its saturated aqueous solution.Moreover,SMS inherited the intrinsicflame retardancy of the melamine sponge.In general,SMS has shown superhydrophobicity,high porosity,excellent selectivity,remarkable recyclability,and better absorption capacity for various oils and organic solvents,and a high separation efficiency for oil in saturated aqueous solutions.展开更多
In this article,a series of high refractive indices(1.50-1.53)thiol phenyl polysiloxane(TPS)were synthesized via hydrolytic sol-gel reaction.The Fourier transform infrared spectra(FT-IR)and nuclear magnetic resonance ...In this article,a series of high refractive indices(1.50-1.53)thiol phenyl polysiloxane(TPS)were synthesized via hydrolytic sol-gel reaction.The Fourier transform infrared spectra(FT-IR)and nuclear magnetic resonance spectra(NMR)results showed that TPS conformed to the predicted structures.Natural terpene linalool was exploited as photocrosslinker to fabricate UV-curing linalool-polysiloxane hybrid films(LPH)with TPS via photoinitiated thiol-ene reaction.LPH rapidly cured under UV irradiation at the intensity of 80 mW/cm2 in 30 s,exhibiting good UV-curing properties.The optical transmittance of LPH in the wavelength of 300-800 nm was over 90%,exhibiting good optical transparency.The water contact angle and water vapor permeability results showed that the introduction of phenyl groups enhance the hydrophobicity and water vapor barrier properties of LPH.The results indicated the potential of LPHs in the applications of optical functional coatings.展开更多
Plasticizers are essential additives in the processing of polyvinyl chloride(PVC),with phthalate plasticizers being widely used.However,these conventional plasticizers have been shown to be harmful to human health and...Plasticizers are essential additives in the processing of polyvinyl chloride(PVC),with phthalate plasticizers being widely used.However,these conventional plasticizers have been shown to be harmful to human health and environmentally unfriendly,necessitating the exploration of eco-friendly bio-based alternatives.In this study,Camellia oleifera seed oil,a specialty resource in China,was utilized as a raw material and reacted with 4,4′-Methylenebis(N,N-diglycidylaniline)(AG-80)to synthesize Phenyl Camellia seed Oil Ester(PCSOE).PCSOE was employed as a plasticizer to prepare modified PVC films with varying concentrations,with the conventional plasticizer dioctyl phthalate(DOP)serving as a control.Experimental results demonstrate that PSCOE-plasticized PVC films exhibit enhanced hydrophilicity,tensile strength,and thermal stability compared to DOP-modified PVC films.The contact angle of PSCOE-plasticized PVC films ranges from 66.26°to 78.48°,which is generally lower than the contact angle of DOP-modified PVC films at 78.40°,indicating improved hydrophilicity due to the modification with PCSOE.The tensile strength of PSCOE-plasticized PVC films ranges from 17.73 to 20.17 MPa,all surpassing the value of 16.41 MPa for DOP-modified PVC films.Moreover,the temperatures corresponding to 5%,10%,and 50%weight loss for PVC samples modified with PCSOE are higher than those for DOP.Hence,PCSOE presents a viable alternative to DOP as a plasticizer for PVC materials.展开更多
In the search of alternative resources to make commodity chemicals and transportation fuels for a low carbon future,lignocellulosic biomass with over 180-billion-ton annual production rate has been identified as a pro...In the search of alternative resources to make commodity chemicals and transportation fuels for a low carbon future,lignocellulosic biomass with over 180-billion-ton annual production rate has been identified as a promising feedstock.This review focuses on the state-of-the-art catalytic transformation of lignocellulosic biomass into value-added chemicals and fuels.Following a brief introduction on the structure,major resources and pretreatment methods of lignocellulosic biomass,the catalytic conversion of three main components,i.e.,cellulose,hemicellulose and lignin,into various compounds are comprehensively discussed.Either in separate steps or in one-pot,cellulose and hemicellulose are hydrolyzed into sugars and upgraded into oxygen-containing chemicals such as 5-HMF,furfural,polyols,and organic acids,or even nitrogen-containing chemicals such as amino acids.On the other hand,lignin is first depolymerized into phenols,catechols,guaiacols,aldehydes and ketones,and then further transformed into hydrocarbon fuels,bioplastic precursors and bioactive compounds.The review then introduces the transformations of whole biomass via catalytic gasification,catalytic pyrolysis,as well as emerging strategies.Finally,opportunities,challenges and prospective of woody biomass valorization are highlighted.展开更多
Electrochemical carbon dioxide reduction reaction(CO_(2)RR)provides an attractive approach to carbon capture and utilization for the production high-value-added products.However,CO_(2)RR still suffers from poor select...Electrochemical carbon dioxide reduction reaction(CO_(2)RR)provides an attractive approach to carbon capture and utilization for the production high-value-added products.However,CO_(2)RR still suffers from poor selectivity and low current density due to its sluggish kinetics and multitudinous reaction pathways.Single-atom catalysts(SACs)demonstrate outstanding activity,excellent selectivity,and remarkable atom utilization efficiency,which give impetus to the search for electrocatalytic processes aiming at high selectivity.There appears significant activity in the development of efficient SACs for CO_(2)RR,while the density of the atomic sites remains a considerable barrier to be overcome.To construct high-metal-loading SACs,aggregation must be prevented,and thus novel strategies are required.The key to creating high-density atomically dispersed sites is designing enough anchoring sites,normally defects,to stabilize the highly mobile separated metal atoms.In this review,we summarized the advances in developing high-loading SACs through defect engineering,with a focus on the synthesis strategies to achieve high atomic site loading.Finally,the future opportunities and challenges for CO_(2)RR in the area of high-loading single-atom electrocatalysts are also discussed.展开更多
By using HDI and TMP as the main raw materials,polyethylene glycol 400(PEG400)is used as a non-ionic hydrophilic modifier,and sodium hydroxyethyl sulfonate is used as an ionic hydrophilic modifier to synthesize a dual...By using HDI and TMP as the main raw materials,polyethylene glycol 400(PEG400)is used as a non-ionic hydrophilic modifier,and sodium hydroxyethyl sulfonate is used as an ionic hydrophilic modifier to synthesize a dual hydrophilic modified polyurethane curing agent.Research revealed that introducing PEG400 for hydrophilic chain segments and sodium hydroxyethyl sulfonate for hydrophilic ionic groups in the polyurethane curing agent component leads to a uniform distribution of hydrophilic components,significantly enhancing compatibility with the aqueous polyol component,and results in excellent film performance.The synthesis process and film were characterized using Fourier transform infrared spectroscopy and high-resolution scanning electron microscopy in the study.展开更多
The rational design of a novel catalytic center with a sound basis remains both challenging and rewarding for the electrochemical reduction of N2(e NRR),which has provided a feasible route for achieving clean and sust...The rational design of a novel catalytic center with a sound basis remains both challenging and rewarding for the electrochemical reduction of N2(e NRR),which has provided a feasible route for achieving clean and sustainable NH3production under ambient conditions.Herein,using density functional theory calculations,we demonstrate that hybrid metal(M)-boron(B)double-atom catalysts(DACs)embedded in gC_(2)N substrate(M-B@C_(2)N,M=3d,4d and 5d transition metals)can achieve both high catalytic activity and high selectivity in e NRR.The proposed M-B@C_(2)N DACs have exhibited impressive feasibility and stability thanks to the resilient and robust C_(2)N substrate with abundant pyridinic N atoms distributed among right-sized pore structures.Our results reveal that like the metal center,the embedded B atom can actively involve in N≡N bond activation viaπ*-backdonation mechanism concomitant with the substantial charge transfer to adsorbed*N2,leading to sizable NAN bond elongation.Accordingly,both adsorption energy and NAN bond length of*N2can be employed as catalytic descriptors for predicting e NRR activity in terms of the limiting potentials(UL).Using high-throughput screening method,we found that six M-B@C_(2)N candidates have stood out as the outstanding electrocatalysts for driving e NRR,namely,M=Ti(UL=0 V),Mo(UL=0 V),Nb(UL=-0.04 V),W(UL=-0.23 V),Zr(UL=-0.26 V),V(UL=-0.28 V).The underlying origin is attributed to the balanced and constrained N-affinity of M-B dual site working in synergy,which can thus be used as one important guide of catalyst design.展开更多
The electrochemical performances of cathode play a key role in the marine sediment microbial fuel cells(MSMFCs)as a long lasting power source to drive instruments,especially when the dissolved oxygen concentration is ...The electrochemical performances of cathode play a key role in the marine sediment microbial fuel cells(MSMFCs)as a long lasting power source to drive instruments,especially when the dissolved oxygen concentration is very low in seawater.A CTS-Fe^(3+)modified cathode is prepared here by grafting chitosan(CTS)on a carbon fiber surface and then chelating Fe^(3+)through the coordination process.The electrochemical performance in seawater and the output power of the assembled MSMFCs are both studied.The results show that the exchange current densities of CTS and the CTS-Fe^(3+)group are 5.5 and 6.2 times higher than that of the blank group,respectively.The potential of the CTS-Fe^(3+)modified cathode increases by 138 mV.The output power of the fuel cell(613.0 mW m^(-2))assembled with CTS-Fe^(3+)is 54 times larger than that of the blank group(11.4 mW m^(-2))and the current output corresponding with the maximum power output also increases by 56 times.Due to the valence conversion between Fe^(3+)and Fe^(2+)on the modified cathode,the kinetic activity of the dissolved oxygen reduction is accelerated and the depolarization capability of the cathode is enhanced,resulting higher cell power.On the basis of this study,the new cathode materials will be encouraged to design with the complex of iron ion in natural seawater as the catalysis for oxygen reduction to improve the cell power in deep sea.展开更多
Bio-photoelectrochemical cells(BPECs)can further expand the use of conventional biofuel cells for renewable energy,but the poor stability of the photoelectrode still hinders their practical application.Herein,a BPEC c...Bio-photoelectrochemical cells(BPECs)can further expand the use of conventional biofuel cells for renewable energy,but the poor stability of the photoelectrode still hinders their practical application.Herein,a BPEC capable of long-term operating in a fuel-free model is fabricated by WO3-xphotoanode with oxygen vacancy(Ov)and bilirubin oxidase catalyzed biocathode.The construction of Ov on the WO3surface significantly suppresses the dissolution of W species into the electrolyte,and improves the charge separation efficiency and the reaction kinetics during the photoelectrochemical oxygen evolution process,thus enhancing the stability and power output performance of the BPEC.As a result,the assembled BPEC can output an open circuit voltage of 0.81 V and deliver a maximum output power of up to 283μW cm^(-2).Impressively,the BPECs maintain 97%of their original power after 36000 s of consecutive discharge under an enclosed environment.This fuel-free BPEC based on a robust WO3-xphotoanode shows excellent promise for accurate application.展开更多
The SRI analysis tool was used to comprehensively analyze the seven sets of chemistry questions in the 2021 college entrance examination paper from multiple dimensions such as exploratory test questions,various inquir...The SRI analysis tool was used to comprehensively analyze the seven sets of chemistry questions in the 2021 college entrance examination paper from multiple dimensions such as exploratory test questions,various inquiry standards and exploratory levels.The study found that all test papers involve the examination of scientific inquiry literacy;from the perspective of examination objectives,the 2021 college entrance examination questions as a whole focus on the examination of a single inquiry objective;the questions of each examination paper mainly examine three standards:design scheme,evidence processing and obtaining.The conclusion is drawn;the exploratory level of the chemistry questions in several sets of test papers is mostly a high level.展开更多
Although multifunctional aerogels are expected to be used in applications such as portable electronic devices,it is still a great challenge to confer multifunctionality to aerogels while maintaining their inherent mic...Although multifunctional aerogels are expected to be used in applications such as portable electronic devices,it is still a great challenge to confer multifunctionality to aerogels while maintaining their inherent microstructure.Herein,a simple method is proposed to prepare multifunctional NiCo/C aerogels with excellent electromagnetic wave absorption properties,superhydrophobicity,and self-cleaning by water-induced NiCo-MOF self-assembly.Specifically,the impedance matching of the three-dimensional(3D)structure and the interfacial polarization provided by CoNi/C as well as the defect-induced dipole polarization are the primary contributors to the broadband absorption.As a result,the prepared NiCo/C aerogels have a broadband width of 6.22 GHz at 1.9 mm.Due to the presence of hydrophobic functional groups,CoNi/C aerogels improve the stability in humid environments and obtain hydrophobicity with large contact angles>140°.This multifunctional aerogel has promising applications in electromagnetic wave absorption,resistance to water or humid environments.展开更多
基金the National Natural Science Foundation of China(No.52374279)the Natural Science Foundation of Shaanxi Province(No.2023-YBGY-055).
文摘Coal gasification fine slag(FS)is a typical solid waste generated in coal gasification.Its current disposal methods of stockpil-ing and landfilling have caused serious soil and ecological hazards.Separation recovery and the high-value utilization of residual carbon(RC)in FS are the keys to realizing the win-win situation of the coal chemical industry in terms of economic and environmental benefits.The structural properties,such as pore,surface functional group,and microcrystalline structures,of RC in FS(FS-RC)not only affect the flotation recovery efficiency of FS-RC but also form the basis for the high-value utilization of FS-RC.In this paper,the characteristics of FS-RC in terms of pore structure,surface functional groups,and microcrystalline structure are sorted out in accordance with gasification type and FS particle size.The reasons for the formation of the special structural properties of FS-RC are analyzed,and their influence on the flotation separation and high-value utilization of FS-RC is summarized.Separation methods based on the pore structural characterist-ics of FS-RC,such as ultrasonic pretreatment-pore-blocking flotation and pore breaking-flocculation flotation,are proposed to be the key development technologies for improving FS-RC recovery in the future.The design of low-cost,low-dose collectors containing polar bonds based on the surface and microcrystalline structures of FS-RC is proposed to be an important breakthrough point for strengthening the flotation efficiency of FS-RC in the future.The high-value utilization of FS should be based on the physicochemical structural proper-ties of FS-RC and should focus on the environmental impact of hazardous elements and the recyclability of chemical waste liquid to es-tablish an environmentally friendly utilization method.This review is of great theoretical importance for the comprehensive understand-ing of the unique structural properties of FS-RC,the breakthrough of the technological bottleneck in the efficient flotation separation of FS,and the expansion of the field of the high value-added utilization of FS-RC.
基金supported by the National Natural Science Foundation of China(No.21776264).
文摘Studying the relationship between ionic interactions and salt solubility in seawater has implications for seawater desalination and mineral extraction.In this paper,a new method of expressing ion-to-ion interaction is proposed by using molecular dynamics simulation,and the relationship between ion-to-ion interaction and salt solubility in a simulated seawater water-salt system is investigated.By analyzing the variation of distance and contact time between ions in an electrolyte solution,from both spatial and temporal perspectives,new parameters were proposed to describe the interaction between ions:interaction distance(ID),and interaction time ratio(ITR).The best correlation between characteristic time ratio and solubility was found for a molar ratio of salt-to-water of 10:100 with a correlation coefficient of 0.96.For the same salt,a positive correlation was found between CTR and the molar ratio of salt and water.For type 1-1,type 2-1,type 1-2,and type 2-2 salts,the correlation coefficients between CTR and solubility were 0.93,0.96,0.92,and 0.98 for a salt-to-water molar ratio of 10:100,respectively.The solubility of multiple salts was predicted by simulations and compared with experimental values,yielding an average relative deviation of 12.4%.The new ion-interaction parameters offer significant advantages in describing strongly correlated and strongly hydrated electrolyte solutions.
基金The authors acknowledge the financial supports from the National Science Foundation of China(U1908204,91845201,and 22002093)the funds that Central Government Guides Local Science and Technology Development(2022JH6/100100052)Scientific Research Project of Education Department of Liaoning Province(LQN202006).
文摘Yolk-shell SiO2 particles(YP)with center-radial meso-channels were fabricated through a simple and effective method.Al-containing YP-supported NiMo catalysts with different Al amounts(NiMo/AYP-x,x=Si/Al molar proportion)were prepared and dibenzothiophene(DBT)and 4,6-dimethyl-dibenzothiophene(4,6-DMDBT)were employed as the probes to evaluate the hydrodesulfurization(HDS)catalytic performance.The as-prepared AYP-x carriers and corresponding catalysts were characterized by some advanced characterizations to obtain deeper correlations between physicochemical properties and the HDS performance.The average pore sizes of series AYP-x supports are above 6.0 nm,which favors the mass transfer of organic sulfides.The cavity between the yolk and the shell is beneficial for the enrichment of S-containing compounds and the accessibility between reactants and active metals.Aluminum embedded into the silica framework could facilitate the formation of Lewis(L)and Brønsted(B)acid sites and adjust the metal-support interaction(MSI).Among all the as-synthesized catalysts,NiMo/AYP-20 catalyst shows the highest HDS activities.The improved HDS activity of NiMo/AYP-20 catalyst is attributed to the perfect combination of excellent structural properties of the yolk-shell mesoporous silica,enhanced acidity,moderate MSI,and good accessibility/dispersion of active components.
文摘To simplify the composite propellant formulation and address the current issue of the single-functionality present in existing additives,the multi-cyano,amine-based polybutadiene(AEHTPB-CN)was prepared based on AEHTPB by adopting appropriate synthesis strategies.By replacing 10% of HTPB binder in the propellant formulation,it can effectively enhance the interfacial bond strength between the propellant binder matrix and solid fillers(AP(ammonium perchlorate)and RDX(cyclotrimethylene-trinitramine)),the mechanical properties of the HTPB/AP/RDX/Al propellant were superior to blank control propellant with an improvement of 35.4% in tensile strength,62.0% enhancement in elongation at break,and reduce the propellant burn rate by 10.7% with any energy loss.The function mechanism of AEHTPB-CN was systematically elucidated through experiments and computer simulation techniques.The results show that the tertiary amine group in AEHTPB-CN can react with AP to form ammonium ionic bonds,and the hydroxyl and cyano groups can form hydrogen bonding interactions with AP,which enables AEHTPB-CN to be firmly adsorbed on the AP surface through chemical and physical interactions.For RDX,the interfacial bonding effect of AEHTPB-CN is attributed to their ability to form C-H···N≡C weak hydrogen bonding interaction between the cyano group and RDX methylene group.
基金supported by the National Natural Science Foundation of China(21872040,22162004)the Excellent Scholars and Innovation Team of Guangxi Universities,the Innovation Project of Guangxi Graduate Education(YCBZ2022038)the High-performance Computing Platform of Guangxi University.
文摘Exploitation of oxygen evolution reaction(OER)and urea oxidation reaction(UOR)catalysts with high activity and stability at large current density is a major challenge for energy-saving H_(2) production in water electrolysis.Herein,we use the pyridinic-N doping carbon layers coupled with tensile strain of FeNi alloy activated by NiFe_(2)O_(4)(FeNi/NiFe_(2)O_(4)@NC)for efficiently increasing the performance of water and urea oxidation.Due to the tensile strain effect on FeNi/NiFe_(2)O_(4)@NC,it provides a favorable modulation on the electronic properties of the active center,thus enabling amazing OER(η_(100)=196 mV)and UOR(E_(10)=1.32 V)intrinsic activity.Besides,the carbon-coated layers can be used as armor to prevent FeNi alloy from being corroded by the electrolyte for enhancing the OER/UOR stability at large current density,showing high industrial practicability.This work thus provides a simple way to prepare high-efficiency catalyst for activating water and urea oxidation.
基金supported by the top talent program of Henan Agricultural University[grant numbers 30501029].
文摘The pursuit of high-performance is worth considerable effort in catalysis for energy efficiency and environmental sustainability. To develop redox catalysts with superior performance for soot combustion, a series of Mn_(x)Co_(y) oxides were synthesized using MgO template substitution.This method greatly improves the preparation and catalytic efficiency and is more in line with the current theme of green catalysts and sustainable development. The resulting Mn_(1)Co_(2.3) has a strong activation capability of gaseous oxygen due to a high concentration of Co^(3+) and Mn^(3+). The Mn doping enhanced the intrinsic activity by prompting oxygen vacancy formation and gaseous oxygen adsorption. The nanosheet morphology with abundant mesoporous significantly increased the solid–solid contact efficiency and improved the adsorption capability of gaseous reactants. The novel design of Mn_(1)Co_(2.3)oxide enhanced its catalytic performance through a synergistic effect of Mn doping and the porous nanosheet morphology, showing significant potential for the preparation of high-performance soot combustion catalysts.
基金This study is supported by the National Key Research and Development Program of China(2017YFB0307500).
文摘Implementing a new energy-saving electrochemical synthesis system with high commercial value is a strategy of the sustainable development for upgrading the bulk chemicals preparation technology in the future.Here,we report a multiple redox-mediated linear paired electrolysis system,combining the hydrogen peroxide mediated cathode process with the I2 mediated anode process,and realize the conversion of furfural to furoic acid in both side of the dividedflow cell simultaneously.By reasonably controlling the cathode potential,the undesired water splitting reaction and furfural reduction side reactions are avoided.Under the galvanostatic electrolysis,the two-mediated electrode processes have good compatibility,which reduce the energy consumption by about 22%while improving the electronic efficiency by about 125%.This system provides a green electrochemical synthesis route with commercial prospects.
基金supported by the National Natural Science Foundation of China(Grant Nos.22175060 and 21975067)the Natural Science Foundation of Hunan Province of China(Grant Nos.2021JJ10014 and 2021JJ30092).
文摘Two-dimensional(2D)magnetic materials have been demonstrated to have excellent chemical,optical,electrical,and magnetic properties,particularly in the development of multifunctional electronic and spin electronic devices,showcasing tremendous potential.Therefore,corresponding synthesis techniques for 2D magnetic materials that offer high quality,high yield,low cost,time-saving,and simplicity are highly desired.This review provides a comprehensive overview of recent research advances in preparation of magnetic 2D materials,with a particular focus on the preparation methods employed.Moreover,the characteristics and applications of these magnetic materials are also discussed.Finally,the challenges and prospects of synthesis methods for magnetic 2D materials are briefly addressed.This review serves as a guiding reference for the controlled synthesis of 2D magnetic materials.
基金supported by the National Natural Science Foundation of China (32172972,U19A2040)Science and Technology Innovation Program of Hunan Province (2021RC4028)+4 种基金Earmarked Fund for China Agriculture Research System (CARS-45)Hunan Provincial Science and Technology Department (2019RS5001)Special Funds for Construction of Innovative Provinces in Hunan Province (2021NK1010)Special Science Found of Nansha-South China Agricultural University Fishery Research Institute,Guangzhou (NSYYKY202305,NSYYKY202306)Aid Program for Science and Technology Innovative Research Team in Higher Educational Institutions of Hunan Province。
文摘The autotetraploid Carassius auratus(4nRR,4n=200,RRRR)is derived from whole-genome duplication of Carassius auratus red var.(RCC,2n=100,RR).In the current study,we demonstrated that chromatophores and pigment changes directly caused the coloration and variation of 4nRR skin(red in RCC,brownish-yellow in4nRR).To further explore the molecular mechanisms underlying coloration formation and variation in 4nRR,we performed transcriptome profiling and molecular functional verification in RCC and 4nRR.Results revealed that scarb1,associated with carotenoid metabolism,underwent significant down-regulation in 4nRR.Efficient editing of this candidate pigment gene provided clear evidence of its significant role in RCC coloration.Subsequently,we identified four divergent scarb1 homeologs in 4nRR:two original scarb1 homeologs from RCC and two duplicated ones.Notably,three of these homeologs possessed two highly conserved alleles,exhibiting biased and allelespecific expression in the skin.Remarkably,after precise editing of both the original and duplicated scarb1homeologs and/or alleles,4nRR individuals,whether singly or multiply mutated,displayed a transition from brownishyellow skin to a cyan-gray phenotype.Concurrently,the proportional areas of the cyan-gray regions displayed a gene-dose correlation.These findings illustrate the subfunctionalization of duplicated scarb1,with all scarb1genes synergistically and equally contributing to the pigmentation of 4nRR.This is the first report concerning the functional differentiation of duplicated homeologs in an autopolyploidfish,substantiallyenrichingour understanding of coloration formation and change within this group of organisms.
基金funded by Qingyang Science and Technology Support Project(KT2019-03)。
文摘A silylated melamine sponge(SMS)was prepared by two simple steps,namely,immersion and dehydration of a melamine sponge coated with methyltrichlorosilane.The silylated structure of SMS was characterized by FT-IR(Fourier-transform infrared)spectroscopy,SEM(Scanning electron microscopy)and in terms of water contact angles.Its oil-water absorption and separation capacities were measured by FT-IR and UV-visible spectrophoto-metry.The experimental results have shown that oligomeric silanol covalently bonds by Si-N onto the surface of melamine sponge skeletons.SMS has shown superhydrophobicity with a water contact angle exceeding 150°±1°,a better separation efficiency with regard to diesel oil(by 99.31%(wt/wt%)in oil-water mixture and even up to 99.99%(wt/wt%)for diesel oil in its saturated aqueous solution.Moreover,SMS inherited the intrinsicflame retardancy of the melamine sponge.In general,SMS has shown superhydrophobicity,high porosity,excellent selectivity,remarkable recyclability,and better absorption capacity for various oils and organic solvents,and a high separation efficiency for oil in saturated aqueous solutions.
基金the financial funding of the Guangdong Province Applied Science and Technology R&D Special Fund Project:Key Technologies for Industrialization of Sulfur-Resistant and High Refractive-Index LED Packaging Silicone Materials(2016B090930010).
文摘In this article,a series of high refractive indices(1.50-1.53)thiol phenyl polysiloxane(TPS)were synthesized via hydrolytic sol-gel reaction.The Fourier transform infrared spectra(FT-IR)and nuclear magnetic resonance spectra(NMR)results showed that TPS conformed to the predicted structures.Natural terpene linalool was exploited as photocrosslinker to fabricate UV-curing linalool-polysiloxane hybrid films(LPH)with TPS via photoinitiated thiol-ene reaction.LPH rapidly cured under UV irradiation at the intensity of 80 mW/cm2 in 30 s,exhibiting good UV-curing properties.The optical transmittance of LPH in the wavelength of 300-800 nm was over 90%,exhibiting good optical transparency.The water contact angle and water vapor permeability results showed that the introduction of phenyl groups enhance the hydrophobicity and water vapor barrier properties of LPH.The results indicated the potential of LPHs in the applications of optical functional coatings.
基金funded by the Scarce and Quality Economic Forest Engineering Technology Research Center(2022GCZX002)the Key Lab.of Biomass Energy and Material,Jiangsu Province(Grant No.JSBEM-S-202305).
文摘Plasticizers are essential additives in the processing of polyvinyl chloride(PVC),with phthalate plasticizers being widely used.However,these conventional plasticizers have been shown to be harmful to human health and environmentally unfriendly,necessitating the exploration of eco-friendly bio-based alternatives.In this study,Camellia oleifera seed oil,a specialty resource in China,was utilized as a raw material and reacted with 4,4′-Methylenebis(N,N-diglycidylaniline)(AG-80)to synthesize Phenyl Camellia seed Oil Ester(PCSOE).PCSOE was employed as a plasticizer to prepare modified PVC films with varying concentrations,with the conventional plasticizer dioctyl phthalate(DOP)serving as a control.Experimental results demonstrate that PSCOE-plasticized PVC films exhibit enhanced hydrophilicity,tensile strength,and thermal stability compared to DOP-modified PVC films.The contact angle of PSCOE-plasticized PVC films ranges from 66.26°to 78.48°,which is generally lower than the contact angle of DOP-modified PVC films at 78.40°,indicating improved hydrophilicity due to the modification with PCSOE.The tensile strength of PSCOE-plasticized PVC films ranges from 17.73 to 20.17 MPa,all surpassing the value of 16.41 MPa for DOP-modified PVC films.Moreover,the temperatures corresponding to 5%,10%,and 50%weight loss for PVC samples modified with PCSOE are higher than those for DOP.Hence,PCSOE presents a viable alternative to DOP as a plasticizer for PVC materials.
文摘In the search of alternative resources to make commodity chemicals and transportation fuels for a low carbon future,lignocellulosic biomass with over 180-billion-ton annual production rate has been identified as a promising feedstock.This review focuses on the state-of-the-art catalytic transformation of lignocellulosic biomass into value-added chemicals and fuels.Following a brief introduction on the structure,major resources and pretreatment methods of lignocellulosic biomass,the catalytic conversion of three main components,i.e.,cellulose,hemicellulose and lignin,into various compounds are comprehensively discussed.Either in separate steps or in one-pot,cellulose and hemicellulose are hydrolyzed into sugars and upgraded into oxygen-containing chemicals such as 5-HMF,furfural,polyols,and organic acids,or even nitrogen-containing chemicals such as amino acids.On the other hand,lignin is first depolymerized into phenols,catechols,guaiacols,aldehydes and ketones,and then further transformed into hydrocarbon fuels,bioplastic precursors and bioactive compounds.The review then introduces the transformations of whole biomass via catalytic gasification,catalytic pyrolysis,as well as emerging strategies.Finally,opportunities,challenges and prospective of woody biomass valorization are highlighted.
基金This project was supported by the National Natural Science Foundation of China(U19A2017,22272206,51976143)Natural Science Foundation of Hunan Province(S2021JJMSXM3153).
文摘Electrochemical carbon dioxide reduction reaction(CO_(2)RR)provides an attractive approach to carbon capture and utilization for the production high-value-added products.However,CO_(2)RR still suffers from poor selectivity and low current density due to its sluggish kinetics and multitudinous reaction pathways.Single-atom catalysts(SACs)demonstrate outstanding activity,excellent selectivity,and remarkable atom utilization efficiency,which give impetus to the search for electrocatalytic processes aiming at high selectivity.There appears significant activity in the development of efficient SACs for CO_(2)RR,while the density of the atomic sites remains a considerable barrier to be overcome.To construct high-metal-loading SACs,aggregation must be prevented,and thus novel strategies are required.The key to creating high-density atomically dispersed sites is designing enough anchoring sites,normally defects,to stabilize the highly mobile separated metal atoms.In this review,we summarized the advances in developing high-loading SACs through defect engineering,with a focus on the synthesis strategies to achieve high atomic site loading.Finally,the future opportunities and challenges for CO_(2)RR in the area of high-loading single-atom electrocatalysts are also discussed.
文摘By using HDI and TMP as the main raw materials,polyethylene glycol 400(PEG400)is used as a non-ionic hydrophilic modifier,and sodium hydroxyethyl sulfonate is used as an ionic hydrophilic modifier to synthesize a dual hydrophilic modified polyurethane curing agent.Research revealed that introducing PEG400 for hydrophilic chain segments and sodium hydroxyethyl sulfonate for hydrophilic ionic groups in the polyurethane curing agent component leads to a uniform distribution of hydrophilic components,significantly enhancing compatibility with the aqueous polyol component,and results in excellent film performance.The synthesis process and film were characterized using Fourier transform infrared spectroscopy and high-resolution scanning electron microscopy in the study.
基金supported by the National Natural Science Foundation of China(21673137)the support from the Program for Top Talents in Songjiang District of Shanghai。
文摘The rational design of a novel catalytic center with a sound basis remains both challenging and rewarding for the electrochemical reduction of N2(e NRR),which has provided a feasible route for achieving clean and sustainable NH3production under ambient conditions.Herein,using density functional theory calculations,we demonstrate that hybrid metal(M)-boron(B)double-atom catalysts(DACs)embedded in gC_(2)N substrate(M-B@C_(2)N,M=3d,4d and 5d transition metals)can achieve both high catalytic activity and high selectivity in e NRR.The proposed M-B@C_(2)N DACs have exhibited impressive feasibility and stability thanks to the resilient and robust C_(2)N substrate with abundant pyridinic N atoms distributed among right-sized pore structures.Our results reveal that like the metal center,the embedded B atom can actively involve in N≡N bond activation viaπ*-backdonation mechanism concomitant with the substantial charge transfer to adsorbed*N2,leading to sizable NAN bond elongation.Accordingly,both adsorption energy and NAN bond length of*N2can be employed as catalytic descriptors for predicting e NRR activity in terms of the limiting potentials(UL).Using high-throughput screening method,we found that six M-B@C_(2)N candidates have stood out as the outstanding electrocatalysts for driving e NRR,namely,M=Ti(UL=0 V),Mo(UL=0 V),Nb(UL=-0.04 V),W(UL=-0.23 V),Zr(UL=-0.26 V),V(UL=-0.28 V).The underlying origin is attributed to the balanced and constrained N-affinity of M-B dual site working in synergy,which can thus be used as one important guide of catalyst design.
基金supported by the National Natural Science Foundation of China(No.22075262)。
文摘The electrochemical performances of cathode play a key role in the marine sediment microbial fuel cells(MSMFCs)as a long lasting power source to drive instruments,especially when the dissolved oxygen concentration is very low in seawater.A CTS-Fe^(3+)modified cathode is prepared here by grafting chitosan(CTS)on a carbon fiber surface and then chelating Fe^(3+)through the coordination process.The electrochemical performance in seawater and the output power of the assembled MSMFCs are both studied.The results show that the exchange current densities of CTS and the CTS-Fe^(3+)group are 5.5 and 6.2 times higher than that of the blank group,respectively.The potential of the CTS-Fe^(3+)modified cathode increases by 138 mV.The output power of the fuel cell(613.0 mW m^(-2))assembled with CTS-Fe^(3+)is 54 times larger than that of the blank group(11.4 mW m^(-2))and the current output corresponding with the maximum power output also increases by 56 times.Due to the valence conversion between Fe^(3+)and Fe^(2+)on the modified cathode,the kinetic activity of the dissolved oxygen reduction is accelerated and the depolarization capability of the cathode is enhanced,resulting higher cell power.On the basis of this study,the new cathode materials will be encouraged to design with the complex of iron ion in natural seawater as the catalysis for oxygen reduction to improve the cell power in deep sea.
基金supported by the National Natural Science Foundation of China(81871506 and 81301345)。
文摘Bio-photoelectrochemical cells(BPECs)can further expand the use of conventional biofuel cells for renewable energy,but the poor stability of the photoelectrode still hinders their practical application.Herein,a BPEC capable of long-term operating in a fuel-free model is fabricated by WO3-xphotoanode with oxygen vacancy(Ov)and bilirubin oxidase catalyzed biocathode.The construction of Ov on the WO3surface significantly suppresses the dissolution of W species into the electrolyte,and improves the charge separation efficiency and the reaction kinetics during the photoelectrochemical oxygen evolution process,thus enhancing the stability and power output performance of the BPEC.As a result,the assembled BPEC can output an open circuit voltage of 0.81 V and deliver a maximum output power of up to 283μW cm^(-2).Impressively,the BPECs maintain 97%of their original power after 36000 s of consecutive discharge under an enclosed environment.This fuel-free BPEC based on a robust WO3-xphotoanode shows excellent promise for accurate application.
文摘The SRI analysis tool was used to comprehensively analyze the seven sets of chemistry questions in the 2021 college entrance examination paper from multiple dimensions such as exploratory test questions,various inquiry standards and exploratory levels.The study found that all test papers involve the examination of scientific inquiry literacy;from the perspective of examination objectives,the 2021 college entrance examination questions as a whole focus on the examination of a single inquiry objective;the questions of each examination paper mainly examine three standards:design scheme,evidence processing and obtaining.The conclusion is drawn;the exploratory level of the chemistry questions in several sets of test papers is mostly a high level.
基金financially supported by the National Natural Science Foundation of China (No.51407134, No.52002196)Natural Science Foundation of Shandong Province (No.ZR2019YQ24, No.ZR2020QF084)+2 种基金Taishan Scholars and Young Experts Program of Shandong Province (No.tsqn202103057)the Qingchuang Talents Induction Program of Shandong Higher Education Institution (Research and Innovation Team of Structural-Functional Polymer Composites)Special Financial of Shandong Province (Structural Design of Highefficiency Electromagnetic Wave-absorbing Composite Materials and Construction of Shandong Provincial Talent Teams (No. 37000022P990304116449))
文摘Although multifunctional aerogels are expected to be used in applications such as portable electronic devices,it is still a great challenge to confer multifunctionality to aerogels while maintaining their inherent microstructure.Herein,a simple method is proposed to prepare multifunctional NiCo/C aerogels with excellent electromagnetic wave absorption properties,superhydrophobicity,and self-cleaning by water-induced NiCo-MOF self-assembly.Specifically,the impedance matching of the three-dimensional(3D)structure and the interfacial polarization provided by CoNi/C as well as the defect-induced dipole polarization are the primary contributors to the broadband absorption.As a result,the prepared NiCo/C aerogels have a broadband width of 6.22 GHz at 1.9 mm.Due to the presence of hydrophobic functional groups,CoNi/C aerogels improve the stability in humid environments and obtain hydrophobicity with large contact angles>140°.This multifunctional aerogel has promising applications in electromagnetic wave absorption,resistance to water or humid environments.
