The electrochemical carbon dioxide reduction(eCO_(2)RR)to formate,driven by clean energy,is a promising approach for producing renewable chemicals and high-value fuels.Despite its potential,further development faces c...The electrochemical carbon dioxide reduction(eCO_(2)RR)to formate,driven by clean energy,is a promising approach for producing renewable chemicals and high-value fuels.Despite its potential,further development faces challenges due to limitations in electrocatalytic activity and durability,especially for nonnoble metal-based catalysts.Here,naturally abundant bismuth-based nanosheets that can effectively drive CO_(2)-to-formate electrocatalytic reduction are prepared using the plasma-activated Bi_(2)Se_(3) followed by a reduction process.Thus-obtained plasma-activated Bi nanosheets(P-BiNS)feature ultrathin structures and high surface areas.Such nanostructures ensure the P-BiNS with outstanding eCO_(2)RR catalytic performance,highlighted by the current density of over 80 mA cm^(-2) and a formate Faradic efficiency of>90%.Furthermore,P-BiNS catalysts demonstrate excellent durability and stability without deactivation following over 50h of operation.The selectivity for formate production is also studied by density functional theory(DFT)calculations,validating the importance and efficacy of the stabilization of intermediates(^(*)OCHO)on the P-BiNS surfaces.This study provides a facile plasma-assisted approach for developing high-performance and low-cost electrocatalysts.展开更多
Ever-increasing emissions of anthropogenic carbon dioxide(CO_(2))cause global environmental and climate challenges.Inspired by biological photosynthesis,developing effective strategies NeuNlto up-cycle CO_(2)into high...Ever-increasing emissions of anthropogenic carbon dioxide(CO_(2))cause global environmental and climate challenges.Inspired by biological photosynthesis,developing effective strategies NeuNlto up-cycle CO_(2)into high-value organics is crucial.Electrochemical CO_(2)reduction reaction(CO_(2)RR)is highly promising to convert CO_(2)into economically viable carbon-based chemicals or fuels under mild process conditions.Herein,mesoporous indium supported on multi-walled carbon nanotubes(mp-In@MWCNTs)is synthesized via a facile wet chemical method.The mp-In@MWCNTs electrocatalysts exhibit high CO_(2)RR performance in reducing CO_(2)into formate.An outstanding activity(current density-78.5 mA cm^(-2)),high conversion efficiency(Faradaic efficiency of formate over 90%),and persistent stability(∼30 h)for selective CO_(2)-to-formate conversion are observed.The outstanding CO_(2)RR process performance is attributed to the unique structures with mesoporous surfaces and a conductive network,which promote the adsorption and desorption of reactants and intermediates while improving electron transfer.These findings provide guiding principles for synthesizing conductive metal-based electrocatalysts for high-performance CO_(2)conversion.展开更多
Discharge plasmas, recognized as unique platforms for investigating the origins of chemical life, have garnered extensive interest for their potential to simulate prebiotic conditions. This paper embarks on a comprehe...Discharge plasmas, recognized as unique platforms for investigating the origins of chemical life, have garnered extensive interest for their potential to simulate prebiotic conditions. This paper embarks on a comprehensive overview of recent advancements in the plasma-enabled synthesis of life’s building blocks, charting the complex environmental parameters believed to have surrounded life’s inception. This discussion elaborates on the fundamental mechanisms of discharge plasmas and their likely role in fostering conditions necessary for the origin of life on early Earth. We consider a variety of chemical reactions facilitated by plasma, specifically the synthesis of vital organic molecules - amino acids, nucleobases, sugars, and lipids. Further, we delve into the impact of plasmas on prebiotic chemical evolution. We expect this review to open new horizons for future investigations in plasma-related prebiotic chemistry that could offer valuable insights for unraveling the mysteries of life's origin.展开更多
The prebiotic synthesis of peptides prior to ribosome-catalyzed processes remains an enigma.The synthesis of abiotic peptides from amino acids(AAs)is primarily constrained by high activation energies and unfavorable t...The prebiotic synthesis of peptides prior to ribosome-catalyzed processes remains an enigma.The synthesis of abiotic peptides from amino acids(AAs)is primarily constrained by high activation energies and unfavorable thermodynamics,necessitating the identification of plausible prebiotic alternatives for synthesizing prebiotic peptides.Here we present a plausible pathway to the formation of prebiotic peptides,wherein oligopeptides,oligopeptide amides,and cyclic oligopeptides can be directly synthesized from amino acid amides(AA-NH2)under wet–dry cycle conditions without the need for any enhancers.The subsequent investigation revealed that AA-NH2 demonstrated more favorable thermodynamic reaction effects than AAs in peptide formation.In contrast to the polymerization of AAs,the process of peptide formation through the polymerization of AA-NH2 was significantly simplified.Additionally,AA-NH2 was discovered to function as a“bridge”for the formation of peptides from AAs,thereby facilitating their participation in the synthesis of intricate peptide structures.On the basis of these findings,a plausible mechanism for the prebiotic origin network of peptides under primordial Earth conditions has been proposed.Overall,this research presents a plausible pathway for the generation of prebiotic peptides and peptide libraries within prebiotic environments.展开更多
Low-value,renewable,carbon-rich resources,with different biomass feedstocks and their derivatives as typical examples,represent virtually inexhaustive carbon sources and carbon-related energy on Earth.Upon conversion ...Low-value,renewable,carbon-rich resources,with different biomass feedstocks and their derivatives as typical examples,represent virtually inexhaustive carbon sources and carbon-related energy on Earth.Upon conversion to higher-value forms(referred to as“up-carbonization”here),these abundant feedstocks provide viable opportunities for energy-rich fuels and sustainable platform chemicals production.However,many of the current methods for such up-carbonization still lack sufficient energy,cost,and material efficiency,which affect their economics and carbon-emissions footprint.With external electricity precisely delivered,discharge plasmas enable many stubborn reactions to occur under mild conditions,by creating locally intensified and highly reactive environments.This technology emerges as a novel,versatile technology platform for integrated or stand-alone conversion of carbon-rich resources.The plasma-based processes are compatible for integration with increasingly abundant and cost-effective renewable electricity,making the whole conversion carbon-neutral and further paving the plasma-electrified upcarbonization to be performance-,environment-,and economics-viable.Despite the chief interest in this emerging area,no review article brings together the state-of-the-art results from diverse disciplines and underlies basic mechanisms and chemistry underpinned.As such,this review aims to fill this gap and provide basic guidelines for future research and transformation,by providing an overview of the application of plasma techniques for carbon-rich resource conversion,with particular focus on the perspective of discharge plasmas,the fundamentals of why plasmas are particularly suited for upcarbonization,and featured examples of plasma-enabled resource valorization.With parallels drawn and specificity highlighted,we also discuss the technique shortcomings,current challenges,and research needs for future work.展开更多
Sustainable ammonia synthesis at ambient conditions that relies on renewable sources of energy and feedstocks is globally sought to replace the Haber-Bosch process.Here,using nitrogen and water as raw materials,a nont...Sustainable ammonia synthesis at ambient conditions that relies on renewable sources of energy and feedstocks is globally sought to replace the Haber-Bosch process.Here,using nitrogen and water as raw materials,a nonthermal plasma catalysis approach is demonstrated as an effective powerto-chemicals conversion strategy for ammonia production.By sustaining a highly reactive environment,successful plasma-catalytic production of NH_(3) was achieved from the dissociation of N_(2) and H_(2)O under mild conditions.Plasma-induced vibrational excitation is found to decrease the N_(2) and H_(2)O dissociation barriers,with the presence of matched catalysts in the nonthermal plasma discharge reactor contributing significantly to molecular dissociation on the catalyst surface.Density functional theory calculations for the activation energy barrier for the dissociation suggest that ruthenium catalysts supported on magnesium oxide exhibit superior performance over other catalysts in NH_(3) production by lowering the activation energy for the dissociative adsorption of N_(2) down to 1.07 eV.The highest production rate,2.67 mmol gcat.^(-1) h^(-1),was obtained using ruthenium catalyst supported on magnesium oxide.This work highlights the potential of nonthermal plasma catalysis for the activation of renewable sources to serve as a new platform for sustainable ammonia production.展开更多
Atmospheric pressure low-temperature plasma is a promising tool in biomedicine applications including blood coagulation,bacterial inactivation,sterilization,and cancer treatment,due to its high chemical activity and l...Atmospheric pressure low-temperature plasma is a promising tool in biomedicine applications including blood coagulation,bacterial inactivation,sterilization,and cancer treatment,due to its high chemical activity and limited thermal damage.It is of great importance to develop portable plasma sources that are safe to human touch and suitable for outdoor and household operation.In this work,a portable and rechargeable low-temperature plasma spark discharge device(130 mm×80 mm×35 mm,300 g)was designed.The discharge frequency and plume length were optimized by the selection of resistance,capacitance,electrode gap,and ground electrode aperture.Results show that the spark plasma plume is generated with a length of 12 mm and a frequency of 10 Hz at a capacitance of 0.33μF.resistance of 1 MΩ,electrode gap of 2 mm,and ground electrode aperture of 1.5 mm.Biological tests indicate that the plasma produced by this device contains abundant reactive species,which can be applied in plasma biomedicine,including daily sterilization and wound healing.展开更多
In this work,a portable floating-electrode dielectric barrier discharge(FE-DBD)device is designed with a rechargeable battery as the power supply.The characteristics of the FE-DBD with a metal electrode and human hand...In this work,a portable floating-electrode dielectric barrier discharge(FE-DBD)device is designed with a rechargeable battery as the power supply.The characteristics of the FE-DBD with a metal electrode and human hand are studied and compared.The human contact safety is verified by calculating the current through the human body based on the equivalent circuit model.Escherichia coli inactivation experiments confirm the efficacy of the FE-DBD device in the envisaged applications.展开更多
Cellulose macrofibers (MFs) are gaining increasing interest as natural and biodegradable alternatives to fossil-derived polymers for both structural and functional applications. However, simultaneously achieving their...Cellulose macrofibers (MFs) are gaining increasing interest as natural and biodegradable alternatives to fossil-derived polymers for both structural and functional applications. However, simultaneously achieving their exceptional mechanical performance and desired functionality is challenging and requires complex processing. Here, we reported a one-step approach using a tension-assisted twisting (TAT) technique for MF fabrication from bacterial cellulose (BC). The TAT stretches and aligns BC nanofibers pre-arranged in hydrogel tubes to form MFs with compactly assembled structures and enhanced hydrogen bonding among neighboring nanofibers. The as-prepared BC MFs exhibited a very high tensile strength of 1 057 MPa and exceptional lifting capacity (over 340 000 when normalized by their own weight). Moreover, due to the volume expansion of BC nanofibers upon water exposure, BC MFs quickly harvested energy from environmental moisture to untwist the bundled networks, thus generating a torsional spinning with a peak rotation speed of 884 r/(min·m). The demonstrated rapid and intense actuation response makes the MFs ideal candidates for diverse humidity-response-based applications beyond advanced actuators, remote rain indicators, intelligent switches, and smart curtains.展开更多
The increasing amount of food waste from various industrial,agricultural,and household sources is an environmental burden if managed inappropriately.Numerous waste management approaches have been developed for the dis...The increasing amount of food waste from various industrial,agricultural,and household sources is an environmental burden if managed inappropriately.Numerous waste management approaches have been developed for the disposal of food waste,but still suffer from either high cost,production of toxic by-products,or secondary environmental pollutions.Herein,we report a new and sustainable plasma electrolysis biorefinery route for the rapid and efficient liquefaction of food waste.During the plasma electrolysis process,only the solvent is added to liquefy the waste,and anions in the waste can contribute to catalyzing the biowaste conversion.While liquefying the waste,the highly reactive species produced in the plasma electrolysis process can efficiently reduce the content of O,N,and Cl in the liquefied products and oxidize most of the metals into solid residues.Especially,the removal rate of Na and K elements was greater than 81%,which is significantly higher than using the traditional oil bath liquefaction,resulting in a relatively high-quality biocrude oil with a high heating value of 25.86 MJ·kg^(-1).Overall,this proposed strategy may provide a new sustainable and eco-friendly avenue for the power-to-chemicals valorization of food waste under benign conditions.展开更多
Continuous processes which allow for large amount of wastewater to be treated to meet drainage standards while reducing treatment time and energy consumption are urgently needed. In this study, a dielectric barrier di...Continuous processes which allow for large amount of wastewater to be treated to meet drainage standards while reducing treatment time and energy consumption are urgently needed. In this study, a dielectric barrier discharge plasma water bed system was designed and then coupled with granular activated carbon (GAC) adsorption to rapidly remove acid fuchsine (AF) with high efficiency. Effects of feeding gases, treatment time and initial concentration of AF on removal efficiency were investigated. Results showed that compared to the N2 and air plasmas treatments, O2 plasma processing was most effective for AF degradation due to the strong oxidation ability of generated activated species, especially the OH radicals. The addition of GAC significantly enhanced the removal efficiency of AF in aqueous solution and shorten the required time by 50%. The effect was attributed to the ability of porous carbon to trap and concentrate the dye, increasing the time dye molecules were exposed to the plasma discharge zone, and to enhance the production of OH radicals on/in GAC to boost the degradation of dyes by plasma as well as in situ regenerate the exhausted GAC. The study offers a new opportunity for continuous effective remediation of wastewater contaminated with organic dyes using plasma technologies.展开更多
Surface functionalization or modification to introduce more oxygen-containing functional groups to biochar is an effective strategy for tuning the physicochemical properties and promoting follow-up applications.In thi...Surface functionalization or modification to introduce more oxygen-containing functional groups to biochar is an effective strategy for tuning the physicochemical properties and promoting follow-up applications.In this study,non-thermal plasma was applied for biochar surface carving before being used in contaminant removal and energy storage applications.The results showed that even a low dose of plasma exposure could introduce a high number density of oxygen-functional groups and enhance the hydrophilicity and metal affinity of the pristine biochar.The plasma-treated biochar enabled a faster metal-adsorption rate and a 40%higher maximum adsorption capacity of heavy metal ion Pb^(2+).Moreover,to add more functionality to biochar surface,biochar with and without plasma pre-treatment was activated by KOH at a temperature of 800℃.Using the same amount of KOH,the plasma treatment resulted in an activated carbon product with the larger BET surface area and pore volume.The performance of the treated activated carbon as a supercapacitor electrode was also substantially improved by>30%.This study may provide guidelines for enhancing the surface functionality and application performances of biochar using non-thermal-based techniques.展开更多
Nano-zero-valent irons(nZVI)have shown great potential to function as universal a nd low-cost magnetic adsorbents.Yet,the rapid agglomeration and easy surface corrosion of nZVI in solution greatly hinders their overal...Nano-zero-valent irons(nZVI)have shown great potential to function as universal a nd low-cost magnetic adsorbents.Yet,the rapid agglomeration and easy surface corrosion of nZVI in solution greatly hinders their overall applicability.Here,carboxylated cellulose nanocrystals(CCNC),widely available from renewable biomass resources,wer e prepared and applied for the immobilization of nZVI.In doing so,carboxylated cellulose nanocrystals supporting nano-zero-valent irons(CCNC-nZVI)were obtained via an in-situ growth method.The CCNC-nZVI were characterized and then evaluated for their performances in wastewater treatment.The results obtained show that nZVI nanoparticles could attach to the carboxyl and hydroxyl groups of CCNC,and well disperse on the CCNC surface with a size of〜10nm.With the CCNC acting as corrosion inhibitors improving the reaction activity of nZVI,CCNC-nZVI exhibited an improved dispersion stability and electron utilization efficacy.The Pb(II)adsorption capacity of CCNC-nZVI reached 509.3 mg·g^-1(298.15 K,pH=4.0),significantly higher than that of CCNC.The adsorption was a spontaneous exothermic process and could be perfectly fitted by the pseudo-second-order kinetics model.This study may provide a novel and green method for immobilizing magnetic nanomaterials by using biomassbased resources to develop effective bio-adsorbents for wastewater decontamination.展开更多
Ternary nanocomposites of CuxZnySnzS(x+y+z)are considered as an emerging potential candidate as electrode materials for energy storage devices due to the considerable interlayer spaces and tunnels in its crystal struc...Ternary nanocomposites of CuxZnySnzS(x+y+z)are considered as an emerging potential candidate as electrode materials for energy storage devices due to the considerable interlayer spaces and tunnels in its crystal structures with excellent conducting ability.Recently,this nanocomposite used as anode material for Li-ion battery has been reported,but there is lim让ed research on让s application in supercapacitors which is considered a complementary energy storage device to battery.In this work,flower-like Cu5Sn2S7/ZnS and pristine Cu5Sn2S7 nanocomposite were prepared via a facile hydrothermal method.The electrochemical tests showed that the Cu5Sn2S7/ZnS nanocomposite exhibited better performance than pristine Cu5Zn2S7,suggesting that the existence of ZnS could significantly enhance the electrochemical performance of Cu5Sn2S7,with the good capacitance of 200 F/g at the current density of 1 A/g.Furthermore 170 F/g was obtained at the large current density of 10 A/g.Supercapacitors demonstrated energy density of 11.08 Wh/kg with power density 461 W/kg or 9.67 Wh/kg at power density of 4615 W/kg.展开更多
Non-thermal plasma exhibits unique advan-tages in biomass conversion for the sustainable production of higher-value energy carriers.Different homogeneous catalysts are usually required for plasma-enabled biomass lique...Non-thermal plasma exhibits unique advan-tages in biomass conversion for the sustainable production of higher-value energy carriers.Different homogeneous catalysts are usually required for plasma-enabled biomass liquefaction to achieve time-and energy-efficient conver-sions.However,the effects of such catalysts on the plasma-assisted liquefaction process and of the plasma on those catalysts have not been thoroughly studied.In this study,an electrical discharge plasma is employed to promote the direct liquefaction of sawdust in a mixture of polyethylene glycol 200 and glycerol.Three commonly used chemicals,sulfuric acid,nitric acid and sodium p-toluene sulfate,were selected as catalysts.The effects of the type of catalyst and concentration on the liquefaction yield were examined;further,the roles of the catalysts in the plasma liquefaction process have been discussed.The results showed that the liquefaction yield attains a value of 90%within 5 min when 1%sulfuric acid was employed as the catalyst.Compared with the other catalysts,sulfuric acid presents the highest efficiency for the liquefaction of sawdust.It was observed that hydrogen ions from the catalyst were primarily responsible for the significant thermal effects on the liquefaction system and the generation of large quantities of active species;these effects directly con-tributed to a higher efficacy of the plasma-enabled liquefaction process.展开更多
基金partial support from the Jiujiang Research Institute at Xiamen University.
文摘The electrochemical carbon dioxide reduction(eCO_(2)RR)to formate,driven by clean energy,is a promising approach for producing renewable chemicals and high-value fuels.Despite its potential,further development faces challenges due to limitations in electrocatalytic activity and durability,especially for nonnoble metal-based catalysts.Here,naturally abundant bismuth-based nanosheets that can effectively drive CO_(2)-to-formate electrocatalytic reduction are prepared using the plasma-activated Bi_(2)Se_(3) followed by a reduction process.Thus-obtained plasma-activated Bi nanosheets(P-BiNS)feature ultrathin structures and high surface areas.Such nanostructures ensure the P-BiNS with outstanding eCO_(2)RR catalytic performance,highlighted by the current density of over 80 mA cm^(-2) and a formate Faradic efficiency of>90%.Furthermore,P-BiNS catalysts demonstrate excellent durability and stability without deactivation following over 50h of operation.The selectivity for formate production is also studied by density functional theory(DFT)calculations,validating the importance and efficacy of the stabilization of intermediates(^(*)OCHO)on the P-BiNS surfaces.This study provides a facile plasma-assisted approach for developing high-performance and low-cost electrocatalysts.
基金Jiujiang Research Institute in Xiamen University for the partial supportthe support of QUT Faculty Centre Strategic Funding provided by the Faculty of Science and QUT Centre for a Waste-Free World+1 种基金the Australian Research Council(ARC)QUT Centre for Materials Science for partial support
文摘Ever-increasing emissions of anthropogenic carbon dioxide(CO_(2))cause global environmental and climate challenges.Inspired by biological photosynthesis,developing effective strategies NeuNlto up-cycle CO_(2)into high-value organics is crucial.Electrochemical CO_(2)reduction reaction(CO_(2)RR)is highly promising to convert CO_(2)into economically viable carbon-based chemicals or fuels under mild process conditions.Herein,mesoporous indium supported on multi-walled carbon nanotubes(mp-In@MWCNTs)is synthesized via a facile wet chemical method.The mp-In@MWCNTs electrocatalysts exhibit high CO_(2)RR performance in reducing CO_(2)into formate.An outstanding activity(current density-78.5 mA cm^(-2)),high conversion efficiency(Faradaic efficiency of formate over 90%),and persistent stability(∼30 h)for selective CO_(2)-to-formate conversion are observed.The outstanding CO_(2)RR process performance is attributed to the unique structures with mesoporous surfaces and a conductive network,which promote the adsorption and desorption of reactants and intermediates while improving electron transfer.These findings provide guiding principles for synthesizing conductive metal-based electrocatalysts for high-performance CO_(2)conversion.
基金National Natural Science Foundation of China General Project(52377160)National Natural Science Foundation of China National Young Talents Project(GYKP010)+1 种基金Shaanxi Provincial Natural Science Program(2023-JC-YB-425)Xi′an Jiaotong University Young Top Talents Program.
文摘Discharge plasmas, recognized as unique platforms for investigating the origins of chemical life, have garnered extensive interest for their potential to simulate prebiotic conditions. This paper embarks on a comprehensive overview of recent advancements in the plasma-enabled synthesis of life’s building blocks, charting the complex environmental parameters believed to have surrounded life’s inception. This discussion elaborates on the fundamental mechanisms of discharge plasmas and their likely role in fostering conditions necessary for the origin of life on early Earth. We consider a variety of chemical reactions facilitated by plasma, specifically the synthesis of vital organic molecules - amino acids, nucleobases, sugars, and lipids. Further, we delve into the impact of plasmas on prebiotic chemical evolution. We expect this review to open new horizons for future investigations in plasma-related prebiotic chemistry that could offer valuable insights for unraveling the mysteries of life's origin.
基金National Natural Science Foundation of China(Nos.42388101,92256203,and 42003062)Fundamental Research Funds for the Provincial Universities of Zhejiang(No.SJLY2023007)+1 种基金Technology and Engineering Center for Space Utilization,Chinese Academy of Sciences(No.YYWT-0901-EXP-16)Ningbo Top Talent Project(No.215-432094250).
文摘The prebiotic synthesis of peptides prior to ribosome-catalyzed processes remains an enigma.The synthesis of abiotic peptides from amino acids(AAs)is primarily constrained by high activation energies and unfavorable thermodynamics,necessitating the identification of plausible prebiotic alternatives for synthesizing prebiotic peptides.Here we present a plausible pathway to the formation of prebiotic peptides,wherein oligopeptides,oligopeptide amides,and cyclic oligopeptides can be directly synthesized from amino acid amides(AA-NH2)under wet–dry cycle conditions without the need for any enhancers.The subsequent investigation revealed that AA-NH2 demonstrated more favorable thermodynamic reaction effects than AAs in peptide formation.In contrast to the polymerization of AAs,the process of peptide formation through the polymerization of AA-NH2 was significantly simplified.Additionally,AA-NH2 was discovered to function as a“bridge”for the formation of peptides from AAs,thereby facilitating their participation in the synthesis of intricate peptide structures.On the basis of these findings,a plausible mechanism for the prebiotic origin network of peptides under primordial Earth conditions has been proposed.Overall,this research presents a plausible pathway for the generation of prebiotic peptides and peptide libraries within prebiotic environments.
基金support from the National Key R&D Program of China(2020YFD0900900)Science and Technology Planning Project of Zhoushan of China(2022C41001)Zhejiang Ocean University(11135091221)。
文摘Low-value,renewable,carbon-rich resources,with different biomass feedstocks and their derivatives as typical examples,represent virtually inexhaustive carbon sources and carbon-related energy on Earth.Upon conversion to higher-value forms(referred to as“up-carbonization”here),these abundant feedstocks provide viable opportunities for energy-rich fuels and sustainable platform chemicals production.However,many of the current methods for such up-carbonization still lack sufficient energy,cost,and material efficiency,which affect their economics and carbon-emissions footprint.With external electricity precisely delivered,discharge plasmas enable many stubborn reactions to occur under mild conditions,by creating locally intensified and highly reactive environments.This technology emerges as a novel,versatile technology platform for integrated or stand-alone conversion of carbon-rich resources.The plasma-based processes are compatible for integration with increasingly abundant and cost-effective renewable electricity,making the whole conversion carbon-neutral and further paving the plasma-electrified upcarbonization to be performance-,environment-,and economics-viable.Despite the chief interest in this emerging area,no review article brings together the state-of-the-art results from diverse disciplines and underlies basic mechanisms and chemistry underpinned.As such,this review aims to fill this gap and provide basic guidelines for future research and transformation,by providing an overview of the application of plasma techniques for carbon-rich resource conversion,with particular focus on the perspective of discharge plasmas,the fundamentals of why plasmas are particularly suited for upcarbonization,and featured examples of plasma-enabled resource valorization.With parallels drawn and specificity highlighted,we also discuss the technique shortcomings,current challenges,and research needs for future work.
基金partially supported by the Australian Research Council(ARC)the National Science Fund for Distinguished Young Scholars(grant number 51925703)。
文摘Sustainable ammonia synthesis at ambient conditions that relies on renewable sources of energy and feedstocks is globally sought to replace the Haber-Bosch process.Here,using nitrogen and water as raw materials,a nonthermal plasma catalysis approach is demonstrated as an effective powerto-chemicals conversion strategy for ammonia production.By sustaining a highly reactive environment,successful plasma-catalytic production of NH_(3) was achieved from the dissociation of N_(2) and H_(2)O under mild conditions.Plasma-induced vibrational excitation is found to decrease the N_(2) and H_(2)O dissociation barriers,with the presence of matched catalysts in the nonthermal plasma discharge reactor contributing significantly to molecular dissociation on the catalyst surface.Density functional theory calculations for the activation energy barrier for the dissociation suggest that ruthenium catalysts supported on magnesium oxide exhibit superior performance over other catalysts in NH_(3) production by lowering the activation energy for the dissociative adsorption of N_(2) down to 1.07 eV.The highest production rate,2.67 mmol gcat.^(-1) h^(-1),was obtained using ruthenium catalyst supported on magnesium oxide.This work highlights the potential of nonthermal plasma catalysis for the activation of renewable sources to serve as a new platform for sustainable ammonia production.
基金supported by National Natural Science Foundation of China(Nos.51677083 and 51377075)Postgraduate Research and Practice Innovation Program of Jiangsu Province(SJCX18_0340)
文摘Atmospheric pressure low-temperature plasma is a promising tool in biomedicine applications including blood coagulation,bacterial inactivation,sterilization,and cancer treatment,due to its high chemical activity and limited thermal damage.It is of great importance to develop portable plasma sources that are safe to human touch and suitable for outdoor and household operation.In this work,a portable and rechargeable low-temperature plasma spark discharge device(130 mm×80 mm×35 mm,300 g)was designed.The discharge frequency and plume length were optimized by the selection of resistance,capacitance,electrode gap,and ground electrode aperture.Results show that the spark plasma plume is generated with a length of 12 mm and a frequency of 10 Hz at a capacitance of 0.33μF.resistance of 1 MΩ,electrode gap of 2 mm,and ground electrode aperture of 1.5 mm.Biological tests indicate that the plasma produced by this device contains abundant reactive species,which can be applied in plasma biomedicine,including daily sterilization and wound healing.
基金supported by National Natural Science Foundation of China(Nos.51907088,51677019)。
文摘In this work,a portable floating-electrode dielectric barrier discharge(FE-DBD)device is designed with a rechargeable battery as the power supply.The characteristics of the FE-DBD with a metal electrode and human hand are studied and compared.The human contact safety is verified by calculating the current through the human body based on the equivalent circuit model.Escherichia coli inactivation experiments confirm the efficacy of the FE-DBD device in the envisaged applications.
基金support from the Zhejiang Provincial Natural Science Foundation of China(No.LR23C160001)the National Key Research and Development Program of China(No.2021YFD2100504).
文摘Cellulose macrofibers (MFs) are gaining increasing interest as natural and biodegradable alternatives to fossil-derived polymers for both structural and functional applications. However, simultaneously achieving their exceptional mechanical performance and desired functionality is challenging and requires complex processing. Here, we reported a one-step approach using a tension-assisted twisting (TAT) technique for MF fabrication from bacterial cellulose (BC). The TAT stretches and aligns BC nanofibers pre-arranged in hydrogel tubes to form MFs with compactly assembled structures and enhanced hydrogen bonding among neighboring nanofibers. The as-prepared BC MFs exhibited a very high tensile strength of 1 057 MPa and exceptional lifting capacity (over 340 000 when normalized by their own weight). Moreover, due to the volume expansion of BC nanofibers upon water exposure, BC MFs quickly harvested energy from environmental moisture to untwist the bundled networks, thus generating a torsional spinning with a peak rotation speed of 884 r/(min·m). The demonstrated rapid and intense actuation response makes the MFs ideal candidates for diverse humidity-response-based applications beyond advanced actuators, remote rain indicators, intelligent switches, and smart curtains.
基金supported by the National Natural Science Foundation of China(Grant No.51877184).
文摘The increasing amount of food waste from various industrial,agricultural,and household sources is an environmental burden if managed inappropriately.Numerous waste management approaches have been developed for the disposal of food waste,but still suffer from either high cost,production of toxic by-products,or secondary environmental pollutions.Herein,we report a new and sustainable plasma electrolysis biorefinery route for the rapid and efficient liquefaction of food waste.During the plasma electrolysis process,only the solvent is added to liquefy the waste,and anions in the waste can contribute to catalyzing the biowaste conversion.While liquefying the waste,the highly reactive species produced in the plasma electrolysis process can efficiently reduce the content of O,N,and Cl in the liquefied products and oxidize most of the metals into solid residues.Especially,the removal rate of Na and K elements was greater than 81%,which is significantly higher than using the traditional oil bath liquefaction,resulting in a relatively high-quality biocrude oil with a high heating value of 25.86 MJ·kg^(-1).Overall,this proposed strategy may provide a new sustainable and eco-friendly avenue for the power-to-chemicals valorization of food waste under benign conditions.
基金the National Natural Science Foundation of China (Grant No.51877184)the Central Analytical Research Facility operated by the Institute of Future Environment (QUT).
文摘Continuous processes which allow for large amount of wastewater to be treated to meet drainage standards while reducing treatment time and energy consumption are urgently needed. In this study, a dielectric barrier discharge plasma water bed system was designed and then coupled with granular activated carbon (GAC) adsorption to rapidly remove acid fuchsine (AF) with high efficiency. Effects of feeding gases, treatment time and initial concentration of AF on removal efficiency were investigated. Results showed that compared to the N2 and air plasmas treatments, O2 plasma processing was most effective for AF degradation due to the strong oxidation ability of generated activated species, especially the OH radicals. The addition of GAC significantly enhanced the removal efficiency of AF in aqueous solution and shorten the required time by 50%. The effect was attributed to the ability of porous carbon to trap and concentrate the dye, increasing the time dye molecules were exposed to the plasma discharge zone, and to enhance the production of OH radicals on/in GAC to boost the degradation of dyes by plasma as well as in situ regenerate the exhausted GAC. The study offers a new opportunity for continuous effective remediation of wastewater contaminated with organic dyes using plasma technologies.
基金supported by the National Natural Science Foundation of China(Grant No.52007023)the Natural Science Foundation of Liaoning Province,China(Grant Nos.2020-BS-073,2019-ZD-0160)+2 种基金the China Postdoctoral Science Foundation(Grant No.2019M661107)the Dalian Maritime University basic scientific research business expenses key scientific research cultivation project(Grant No.3132020371)the Fundamental Research Funds for the Central Universities(Grant No.3132021159).
文摘Surface functionalization or modification to introduce more oxygen-containing functional groups to biochar is an effective strategy for tuning the physicochemical properties and promoting follow-up applications.In this study,non-thermal plasma was applied for biochar surface carving before being used in contaminant removal and energy storage applications.The results showed that even a low dose of plasma exposure could introduce a high number density of oxygen-functional groups and enhance the hydrophilicity and metal affinity of the pristine biochar.The plasma-treated biochar enabled a faster metal-adsorption rate and a 40%higher maximum adsorption capacity of heavy metal ion Pb^(2+).Moreover,to add more functionality to biochar surface,biochar with and without plasma pre-treatment was activated by KOH at a temperature of 800℃.Using the same amount of KOH,the plasma treatment resulted in an activated carbon product with the larger BET surface area and pore volume.The performance of the treated activated carbon as a supercapacitor electrode was also substantially improved by>30%.This study may provide guidelines for enhancing the surface functionality and application performances of biochar using non-thermal-based techniques.
基金the Key Planning Project of Science and Technology of Fujian Province,China(Grant No.2018N0032).
文摘Nano-zero-valent irons(nZVI)have shown great potential to function as universal a nd low-cost magnetic adsorbents.Yet,the rapid agglomeration and easy surface corrosion of nZVI in solution greatly hinders their overall applicability.Here,carboxylated cellulose nanocrystals(CCNC),widely available from renewable biomass resources,wer e prepared and applied for the immobilization of nZVI.In doing so,carboxylated cellulose nanocrystals supporting nano-zero-valent irons(CCNC-nZVI)were obtained via an in-situ growth method.The CCNC-nZVI were characterized and then evaluated for their performances in wastewater treatment.The results obtained show that nZVI nanoparticles could attach to the carboxyl and hydroxyl groups of CCNC,and well disperse on the CCNC surface with a size of〜10nm.With the CCNC acting as corrosion inhibitors improving the reaction activity of nZVI,CCNC-nZVI exhibited an improved dispersion stability and electron utilization efficacy.The Pb(II)adsorption capacity of CCNC-nZVI reached 509.3 mg·g^-1(298.15 K,pH=4.0),significantly higher than that of CCNC.The adsorption was a spontaneous exothermic process and could be perfectly fitted by the pseudo-second-order kinetics model.This study may provide a novel and green method for immobilizing magnetic nanomaterials by using biomassbased resources to develop effective bio-adsorbents for wastewater decontamination.
基金the support via Postgraduate Research Award of Queensland University of Technology(QUTPRA)
文摘Ternary nanocomposites of CuxZnySnzS(x+y+z)are considered as an emerging potential candidate as electrode materials for energy storage devices due to the considerable interlayer spaces and tunnels in its crystal structures with excellent conducting ability.Recently,this nanocomposite used as anode material for Li-ion battery has been reported,but there is lim让ed research on让s application in supercapacitors which is considered a complementary energy storage device to battery.In this work,flower-like Cu5Sn2S7/ZnS and pristine Cu5Sn2S7 nanocomposite were prepared via a facile hydrothermal method.The electrochemical tests showed that the Cu5Sn2S7/ZnS nanocomposite exhibited better performance than pristine Cu5Zn2S7,suggesting that the existence of ZnS could significantly enhance the electrochemical performance of Cu5Sn2S7,with the good capacitance of 200 F/g at the current density of 1 A/g.Furthermore 170 F/g was obtained at the large current density of 10 A/g.Supercapacitors demonstrated energy density of 11.08 Wh/kg with power density 461 W/kg or 9.67 Wh/kg at power density of 4615 W/kg.
基金This work was supported by the Foundation of Key Laboratory of Biomass Chemical Engineering of Ministry of Education,China(Zhejiang University,No.2018BCE006)We are also grateful to the Australian Research Council for their partial support.
文摘Non-thermal plasma exhibits unique advan-tages in biomass conversion for the sustainable production of higher-value energy carriers.Different homogeneous catalysts are usually required for plasma-enabled biomass liquefaction to achieve time-and energy-efficient conver-sions.However,the effects of such catalysts on the plasma-assisted liquefaction process and of the plasma on those catalysts have not been thoroughly studied.In this study,an electrical discharge plasma is employed to promote the direct liquefaction of sawdust in a mixture of polyethylene glycol 200 and glycerol.Three commonly used chemicals,sulfuric acid,nitric acid and sodium p-toluene sulfate,were selected as catalysts.The effects of the type of catalyst and concentration on the liquefaction yield were examined;further,the roles of the catalysts in the plasma liquefaction process have been discussed.The results showed that the liquefaction yield attains a value of 90%within 5 min when 1%sulfuric acid was employed as the catalyst.Compared with the other catalysts,sulfuric acid presents the highest efficiency for the liquefaction of sawdust.It was observed that hydrogen ions from the catalyst were primarily responsible for the significant thermal effects on the liquefaction system and the generation of large quantities of active species;these effects directly con-tributed to a higher efficacy of the plasma-enabled liquefaction process.
