1.Introduction Water pollution is the major cause of ecological degradation on our planet;it directly affects human water supplies,often with serious consequences to public health.A wide range of contaminants—includi...1.Introduction Water pollution is the major cause of ecological degradation on our planet;it directly affects human water supplies,often with serious consequences to public health.A wide range of contaminants—including chemicals,pathogens,and nutrients—has been and is currently being introduced into the natural environment.Household and industrial effluents,as well as urban and agricultural runoffs,are damaging aquatic ecosystems on a scale never seen before.展开更多
The oxygen evolution reaction(OER) plays a crucial role in many electrochemical energy technologies,and creating multiple beneficial factors for OER catalysis is desirable for achieving high catalytic efficiency.Here,...The oxygen evolution reaction(OER) plays a crucial role in many electrochemical energy technologies,and creating multiple beneficial factors for OER catalysis is desirable for achieving high catalytic efficiency.Here,we highlight a new halogen-chlorine(Cl)-anion doping strategy to boost the OER activity of perovskite oxides.As a proof-of-concept,proper Cl doping at the oxygen site of LaFeO3(LFO) perovskite can induce multiple favorable characteristics for catalyzing the OER,including rich oxygen vacancies,increased electrical conductivity and enhanced Fe-O covalency.Benefiting from these factors,the LaFeO2.9-δCl0.1(LFOCl) perovskite displays significant intrinsic activity enhancement by a factor of around three relative to its parent LFO.This work uncovers the effect of Cl-anion doping in perovskites on promoting OER performance and paves a new way to design highly efficient electrocatalysts.展开更多
Dimethoxymethane(DMM),a diesel blend fuel,is being researched with high interest recently due to its unique fuel properties.It is commercially produced via a two step-process of methanol oxidation to make formaldehyde...Dimethoxymethane(DMM),a diesel blend fuel,is being researched with high interest recently due to its unique fuel properties.It is commercially produced via a two step-process of methanol oxidation to make formaldehyde,followed by its condensation with methanol.This study presents a one-pot method of DMM synthesis from methanol mediated carbon dioxide hydrogenation over novel heterogeneous catalysts.The effect of catalyst pore structure was investigated by synthesizing 3 wt%Ru over novel hierarchical zeolite beta(HBEASX)and comparing against Ru doped commercial zeolite beta(CBEA)and desilicated hierarchical zeolite beta(HBZDS).The results showed that 3%Ru/HBEASX provided the best activity for DMM production due to its large average pore size.It also showed the decisive role of SiO_(2)/Al_(2)O_(3)molar ratio,with SiO_(2)/Al_(2)O_(3)=75 providing the highest DMM yield of 13.2 mmol/gcat.LMeOH with ca.100%selectivity.The activity of 3%Ru/HBEAS3 after 5 recycle steps demonstrated the reusability of this catalyst.展开更多
Metal-air batteries face a great challenge in developing efficient and durable low-cost oxygen reduction reaction(ORR)electrocatalysts.Single-atom iron catalysts embedded into nitrogen doped carbon(Fe-N-C)have emerged...Metal-air batteries face a great challenge in developing efficient and durable low-cost oxygen reduction reaction(ORR)electrocatalysts.Single-atom iron catalysts embedded into nitrogen doped carbon(Fe-N-C)have emerged as attractive materials for potential replacement of Pt in ORR,but their catalytic performance was limited by the symmetrical electronic structure distribution around the single-atom Fe site.Here,we report our findings in significantly enhancing the ORR performance of Fe-N-C by moderate Fe_(2)O_(3) integration via the strong electronic interaction.Remarkably,the optimized catalyst(M-Fe_(2)O_(3)/Fe_(SA)@NC)exhibits excellent activity,durability and good tolerance to methanol,outperforming the benchmark Pt/C catalyst.When M-Fe_(2)O_(3)/Fe_(SA)@NC catalyst was used in a practical zinc-air battery assembly,peak power density of 155 mW cm^(-2)and specific capacity of 762 mA h g_(Zn)^(-1)were achieved and the battery assembly has shown superior cycling stability over a period of 200 h.More importantly,theoretical studies suggest that the introduction of Fe_(2)O_(3) can evoke the crystal field alteration and electron redistribution on single Fe atoms,which can break the symmetric charge distribution of Fe-N_(4) and thereby optimize the corresponding adsorption energy of intermediates to promote the O_(2)reduction.This study provides a new pathway to promote the catalytic performance of single-atom catalysts.展开更多
Solid oxide cells(SOCs)are pivotal for renewable energy storage and conversion.They operate in two key modes:solid oxide electrolysis cells(SOECs)efficiently transform electrical power into fuel,while solid oxide fuel...Solid oxide cells(SOCs)are pivotal for renewable energy storage and conversion.They operate in two key modes:solid oxide electrolysis cells(SOECs)efficiently transform electrical power into fuel,while solid oxide fuel cells(SOFCs)convert fuel back into power.Conventional SOC fabrication relies on high-temperature sintering,leading to microstructured components that limit performance at reduced operating temperatures.Nanostructured electrodes and electrolytes are essential to enhance electrochemical activity(e.g.,oxygen reduction and hydrogen evolution reactions)and ion transport rates at low temperatures,thereby addressing challenges such as material degradation and sealing reliability under high-temperature operation.This review systematically examines advanced nanofabrication techniques for SOCs,including infiltration,exsolution,electrospinning,template-assisted synthesis,selfassembly,vapor deposition,high-pressure compaction,and sintering-free direct assembly.For each method,we analyze the process-microstructure-performance relationships,alongside comparative assessments of cost,scalability,complexity,and technological maturity.Furthermore,we critically evaluate the current limitations and future prospects of SOC nanofabrication,providing insights for next-generation energy technologies.展开更多
Excessive fluoride anions in drinking water are toxic to the health of human beings.In this article,an effective fluoride removal adsorbent on the basis of amino-functionalized porous polydivinylbenzene(PDVB)was prepa...Excessive fluoride anions in drinking water are toxic to the health of human beings.In this article,an effective fluoride removal adsorbent on the basis of amino-functionalized porous polydivinylbenzene(PDVB)was prepared through low cost processes,which included solvothermal preparation of porous PDVB and subsequent surface amino-functionalization.The obtained amino-functionalized porous PDVB(A-PDVB)has high surface area of 443 m2 g1 and high adsorption capacity towards fluoride anion up to 105.9 mg g1.Considering adsorbents surface area,the adsorption capacity per unit surface area of A-PDVB is 0.24 mg m2 which is more than 4 times of porous PDVB(0.058 mg m2).The enhanced adsorption performance of A-PDVB was due to amino groups electrostatic interaction coupled with hydrogen bond binding with fluoride anions.In addition,the aminofunctionalized porous PDVB could be regenerated in high efficiency under alkaline conditions.This work not only exhibits the possibility of A-PDVB for application as an environment-friendly adsorbent for fluoride removal but also gives an insight into understanding mechanism of the fluoride anions adsorption onto aminofunctionalized porous PDVB.展开更多
Graphene based nanosheets have been widely used as building blocks for fabrication of superior separation membrane for water processing.In particular,membranes made of reduced graphene oxide(rGO)show better stability ...Graphene based nanosheets have been widely used as building blocks for fabrication of superior separation membrane for water processing.In particular,membranes made of reduced graphene oxide(rGO)show better stability compared with graphene oxide(GO).However,densely stacked of rGO often results in low water flux.In this study,cellulose nanofibers(CNFs)were incorporated into the rGO laminates by vacuum filtration of dilute GO/CNF solution and thermal reduction at 150C for 1.5 h.The resulting rGO/CNF membrane was treated with oxygen plasma for 1–4 min to create nanopores on the membrane surface for the purpose of enhancing nano-filtration performance.The results showed that the optimum membrane performance was obtained by using the equal amount of GO(31.83 mg m^(-2))and CNFs accompanied by 3 min of plasma treatment,exhibiting a pure water permeance of 37.23.9 L m^(-2)h^(-1)bar^(-1)maintaining a rejection above 90%for Acid Fuchsin(1.2×1.1 nm),Rose Bengal(1.5×1.2 nm)and Brilliant Blue(2.2×1.7 nm).展开更多
CONSPECTUS:Selective ion transport in nanoporous membranes has become a research hot spot in the fields of both nanofluidics and membrane separation because of its wide potential applications,such as ion separation,en...CONSPECTUS:Selective ion transport in nanoporous membranes has become a research hot spot in the fields of both nanofluidics and membrane separation because of its wide potential applications,such as ion separation,energy harvesting and conversion,and ion sensing.Developing nanofluidic devices or membranes with nanoconfined to subnanoconfined space is the core part of nanofluidic studies because the materials used to construct nanofluidic devices determine the exploration potential of the ion-transport performance.展开更多
Membrane-based separation technologies have been widely used in extracting fresh water from various water sources,including seawater,brackish water,and wastewater,to address the shortage of clean and safe water worldw...Membrane-based separation technologies have been widely used in extracting fresh water from various water sources,including seawater,brackish water,and wastewater,to address the shortage of clean and safe water worldwide[1].These technologies can produce high-quality water and are highly scalable.展开更多
Membrane technologies are broadly used in many industrial separation processes owing to their distinct advantages in low energy consumption,high separation efficiency and low environmental impact.The membrane science ...Membrane technologies are broadly used in many industrial separation processes owing to their distinct advantages in low energy consumption,high separation efficiency and low environmental impact.The membrane science has become one of the core drivers for green chemical engineering.In the membrane field,tremendous research efforts are being devoted to develop novel membranes and advance fundamental membrane science for improving existing membrane separations and addressing pendent separation challenges for a greener future.展开更多
Membranes are widely used in separation processes due to their low energy requirement,small footprint and simplicity.New membranes have been developed based on novel materials and fabrication techniques to address sep...Membranes are widely used in separation processes due to their low energy requirement,small footprint and simplicity.New membranes have been developed based on novel materials and fabrication techniques to address separation challenges in the field of membrane science.In the case of liquid phase separations,ion-ion separation and chiral resolution using membranes have attracted growing interest for their applications such as in high-value mineral extraction and pharmaceutical manufacturing.Furthermore,reverse osmosis operation favors ultra-high-pressure range for treating feed with higher salinity with higher water recovery.Herein we highlight the latest development and design approaches of single species-selective membranes and pressure-resistant membranes and discuss the current limitations of membrane separation in the liquid phase.We subsequently review recent advancement in the fabrication techniques that enable the making of these membranes from emerging materials.展开更多
文摘1.Introduction Water pollution is the major cause of ecological degradation on our planet;it directly affects human water supplies,often with serious consequences to public health.A wide range of contaminants—including chemicals,pathogens,and nutrients—has been and is currently being introduced into the natural environment.Household and industrial effluents,as well as urban and agricultural runoffs,are damaging aquatic ecosystems on a scale never seen before.
基金financially supported by the Australian Research Council (Discovery Early Career Researcher Award No. DE190100005)the support of the Australian Research Council (Grant No. FT160100207)the ontinued support from the Queensland University of Technology (QUT) through the centre for Materials Science。
文摘The oxygen evolution reaction(OER) plays a crucial role in many electrochemical energy technologies,and creating multiple beneficial factors for OER catalysis is desirable for achieving high catalytic efficiency.Here,we highlight a new halogen-chlorine(Cl)-anion doping strategy to boost the OER activity of perovskite oxides.As a proof-of-concept,proper Cl doping at the oxygen site of LaFeO3(LFO) perovskite can induce multiple favorable characteristics for catalyzing the OER,including rich oxygen vacancies,increased electrical conductivity and enhanced Fe-O covalency.Benefiting from these factors,the LaFeO2.9-δCl0.1(LFOCl) perovskite displays significant intrinsic activity enhancement by a factor of around three relative to its parent LFO.This work uncovers the effect of Cl-anion doping in perovskites on promoting OER performance and paves a new way to design highly efficient electrocatalysts.
基金Australian Research Council(Grant No.DP170104017)for the financial support of this projectAT and AS received financial support from the Institute for Catalysis,Hokkaido University as part of their Strategic Research Fellowship grant schemesupported by the Cooperative Research Program of Institute for Catalysis,Hokkaido University(Proposal No.19A1005)。
文摘Dimethoxymethane(DMM),a diesel blend fuel,is being researched with high interest recently due to its unique fuel properties.It is commercially produced via a two step-process of methanol oxidation to make formaldehyde,followed by its condensation with methanol.This study presents a one-pot method of DMM synthesis from methanol mediated carbon dioxide hydrogenation over novel heterogeneous catalysts.The effect of catalyst pore structure was investigated by synthesizing 3 wt%Ru over novel hierarchical zeolite beta(HBEASX)and comparing against Ru doped commercial zeolite beta(CBEA)and desilicated hierarchical zeolite beta(HBZDS).The results showed that 3%Ru/HBEASX provided the best activity for DMM production due to its large average pore size.It also showed the decisive role of SiO_(2)/Al_(2)O_(3)molar ratio,with SiO_(2)/Al_(2)O_(3)=75 providing the highest DMM yield of 13.2 mmol/gcat.LMeOH with ca.100%selectivity.The activity of 3%Ru/HBEAS3 after 5 recycle steps demonstrated the reusability of this catalyst.
基金supported by the Australian Research Council Australian Laureate Fellowship(No.FL200100049)the support of Natural Science Foundation for Young Scholars of Jiangsu Province(No.BK20220879)+1 种基金National Natural Science Foundation for Young Scholars of China(No.22209072)Monash University for a PhD scholarship as part of the university support for establishment of the ARC Research Hub for Energy-efficient Separation(H170100009)。
文摘Metal-air batteries face a great challenge in developing efficient and durable low-cost oxygen reduction reaction(ORR)electrocatalysts.Single-atom iron catalysts embedded into nitrogen doped carbon(Fe-N-C)have emerged as attractive materials for potential replacement of Pt in ORR,but their catalytic performance was limited by the symmetrical electronic structure distribution around the single-atom Fe site.Here,we report our findings in significantly enhancing the ORR performance of Fe-N-C by moderate Fe_(2)O_(3) integration via the strong electronic interaction.Remarkably,the optimized catalyst(M-Fe_(2)O_(3)/Fe_(SA)@NC)exhibits excellent activity,durability and good tolerance to methanol,outperforming the benchmark Pt/C catalyst.When M-Fe_(2)O_(3)/Fe_(SA)@NC catalyst was used in a practical zinc-air battery assembly,peak power density of 155 mW cm^(-2)and specific capacity of 762 mA h g_(Zn)^(-1)were achieved and the battery assembly has shown superior cycling stability over a period of 200 h.More importantly,theoretical studies suggest that the introduction of Fe_(2)O_(3) can evoke the crystal field alteration and electron redistribution on single Fe atoms,which can break the symmetric charge distribution of Fe-N_(4) and thereby optimize the corresponding adsorption energy of intermediates to promote the O_(2)reduction.This study provides a new pathway to promote the catalytic performance of single-atom catalysts.
基金financially supported by Moganshan Institute ZJUT,Deqing,Zhejiang,China,and the Australian Research Council through Huanting Wang's Australian Laureate Fellowship(project no.FL200100049).
文摘Solid oxide cells(SOCs)are pivotal for renewable energy storage and conversion.They operate in two key modes:solid oxide electrolysis cells(SOECs)efficiently transform electrical power into fuel,while solid oxide fuel cells(SOFCs)convert fuel back into power.Conventional SOC fabrication relies on high-temperature sintering,leading to microstructured components that limit performance at reduced operating temperatures.Nanostructured electrodes and electrolytes are essential to enhance electrochemical activity(e.g.,oxygen reduction and hydrogen evolution reactions)and ion transport rates at low temperatures,thereby addressing challenges such as material degradation and sealing reliability under high-temperature operation.This review systematically examines advanced nanofabrication techniques for SOCs,including infiltration,exsolution,electrospinning,template-assisted synthesis,selfassembly,vapor deposition,high-pressure compaction,and sintering-free direct assembly.For each method,we analyze the process-microstructure-performance relationships,alongside comparative assessments of cost,scalability,complexity,and technological maturity.Furthermore,we critically evaluate the current limitations and future prospects of SOC nanofabrication,providing insights for next-generation energy technologies.
基金supported by the National Natural Science Foundation of China(Grant No.21976003)the Major Project of Natural Science Research in Colleges and Universities of Anhui Province(Grant No.KJ2019ZD51)+1 种基金the Key Research and Development Projects in Anhui Province(Grant No.201904b11020041,1708085QE120)the Academic Funding Project for Top Talents in Colleges and Universities of Anhui Province(Grant No.gxbjZD2020077).
文摘Excessive fluoride anions in drinking water are toxic to the health of human beings.In this article,an effective fluoride removal adsorbent on the basis of amino-functionalized porous polydivinylbenzene(PDVB)was prepared through low cost processes,which included solvothermal preparation of porous PDVB and subsequent surface amino-functionalization.The obtained amino-functionalized porous PDVB(A-PDVB)has high surface area of 443 m2 g1 and high adsorption capacity towards fluoride anion up to 105.9 mg g1.Considering adsorbents surface area,the adsorption capacity per unit surface area of A-PDVB is 0.24 mg m2 which is more than 4 times of porous PDVB(0.058 mg m2).The enhanced adsorption performance of A-PDVB was due to amino groups electrostatic interaction coupled with hydrogen bond binding with fluoride anions.In addition,the aminofunctionalized porous PDVB could be regenerated in high efficiency under alkaline conditions.This work not only exhibits the possibility of A-PDVB for application as an environment-friendly adsorbent for fluoride removal but also gives an insight into understanding mechanism of the fluoride anions adsorption onto aminofunctionalized porous PDVB.
基金the Australian Research Council(Project No.IH170100009)。
文摘Graphene based nanosheets have been widely used as building blocks for fabrication of superior separation membrane for water processing.In particular,membranes made of reduced graphene oxide(rGO)show better stability compared with graphene oxide(GO).However,densely stacked of rGO often results in low water flux.In this study,cellulose nanofibers(CNFs)were incorporated into the rGO laminates by vacuum filtration of dilute GO/CNF solution and thermal reduction at 150C for 1.5 h.The resulting rGO/CNF membrane was treated with oxygen plasma for 1–4 min to create nanopores on the membrane surface for the purpose of enhancing nano-filtration performance.The results showed that the optimum membrane performance was obtained by using the equal amount of GO(31.83 mg m^(-2))and CNFs accompanied by 3 min of plasma treatment,exhibiting a pure water permeance of 37.23.9 L m^(-2)h^(-1)bar^(-1)maintaining a rejection above 90%for Acid Fuchsin(1.2×1.1 nm),Rose Bengal(1.5×1.2 nm)and Brilliant Blue(2.2×1.7 nm).
基金Australian Research Council Australian Laureate Fellowship funded by the Australian Government(FL200100049).
文摘CONSPECTUS:Selective ion transport in nanoporous membranes has become a research hot spot in the fields of both nanofluidics and membrane separation because of its wide potential applications,such as ion separation,energy harvesting and conversion,and ion sensing.Developing nanofluidic devices or membranes with nanoconfined to subnanoconfined space is the core part of nanofluidic studies because the materials used to construct nanofluidic devices determine the exploration potential of the ion-transport performance.
文摘Membrane-based separation technologies have been widely used in extracting fresh water from various water sources,including seawater,brackish water,and wastewater,to address the shortage of clean and safe water worldwide[1].These technologies can produce high-quality water and are highly scalable.
文摘Membrane technologies are broadly used in many industrial separation processes owing to their distinct advantages in low energy consumption,high separation efficiency and low environmental impact.The membrane science has become one of the core drivers for green chemical engineering.In the membrane field,tremendous research efforts are being devoted to develop novel membranes and advance fundamental membrane science for improving existing membrane separations and addressing pendent separation challenges for a greener future.
基金Professor Huanting Wang is the recipient of an Australian Research Council Australian Laureate Fellowship(project number FL200100049)funded by the Australian Government.
文摘Membranes are widely used in separation processes due to their low energy requirement,small footprint and simplicity.New membranes have been developed based on novel materials and fabrication techniques to address separation challenges in the field of membrane science.In the case of liquid phase separations,ion-ion separation and chiral resolution using membranes have attracted growing interest for their applications such as in high-value mineral extraction and pharmaceutical manufacturing.Furthermore,reverse osmosis operation favors ultra-high-pressure range for treating feed with higher salinity with higher water recovery.Herein we highlight the latest development and design approaches of single species-selective membranes and pressure-resistant membranes and discuss the current limitations of membrane separation in the liquid phase.We subsequently review recent advancement in the fabrication techniques that enable the making of these membranes from emerging materials.
