Heavy metals usually exist stably as the species of organic complexes in high-salinity wastewater.Therefore,their effective removal is challenging,especially when the initial p H is neutral.Herein,a novel nitrogen dop...Heavy metals usually exist stably as the species of organic complexes in high-salinity wastewater.Therefore,their effective removal is challenging,especially when the initial p H is neutral.Herein,a novel nitrogen doped biomass-based composite(N-CMCS)was synthesized to remove the complexed heavy metal of Cr(Ⅲ)-carboxyl.The maximum adsorption capacity of Cr(Ⅲ)-Citrate(Cr-Cit)by N-CMCS under neutral p H(7.0)and high-salinity(200 mmol/L NaCl)condition was up to 2.50 mmol/g.And the removal performance remained stable after 6 times of regeneration.Combined with species and characterizations analysis,electrostatic attraction and hydrogen bonding were the main mechanisms for N-CMCS to remove Cr(Ⅲ)-carboxyl complexes.Dynamic adsorption indicated N-CMCS column could treat about 1300BV simulated wastewater and 350 BV actual wastewater with the concentration of effluent lower than1.0 mg/L.Furthermore,N-CMCS could remove a variety of complexed heavy metal ions under neutral p H,indicating the great potential in practical application.展开更多
CO_(2) utilization becomes a promising solution for reducing anthropogenic greenhouse gas (GHG) emissions. Biomass-based CO_(2) utilization (BCU) even has the potential to generate negative emissions, but the correspo...CO_(2) utilization becomes a promising solution for reducing anthropogenic greenhouse gas (GHG) emissions. Biomass-based CO_(2) utilization (BCU) even has the potential to generate negative emissions, but the corresponding quantitative evaluation is limited. Herein, the biomass-based CO_(2) utilization with an iron cycle (BCU-Fe) system, which converts CO_(2) into formate by Fe under hydrothermal conditions and recovers Fe with biomass-derived glycerin, was investigated. The GHG reduction potential under various process designs was quantified by a multidisciplinary method, including experiments, simulations, and an ex-ante life-cycle assessment. The results reveal that the BCU-Fe system could bring considerable GHG emission reduction. Significantly, the lowest value is −34.03 kg CO_(2)-eq/kg absorbed CO_(2) (−2.44 kg CO_(2)-eq/kg circulated Fe) with the optimal yield of formate (66%) and Fe (80%). The proposed ex-ante evaluation approach not only reveals the benefits of mitigating climate change by applying the BCU-Fe system, but also serves as a generic tool to guide the industrialization of emerging carbon-neutral technologies.展开更多
Interfacial solar steam generation(ISSG),involving the use of solar energy to evaporate water at the water-to-vapor interface,has presented prospects for the desalination and purification of water due to high energy c...Interfacial solar steam generation(ISSG),involving the use of solar energy to evaporate water at the water-to-vapor interface,has presented prospects for the desalination and purification of water due to high energy conversion efficiency and low-cost freshwater generation.Herein,inspired by the aligned nanostructure of plants for efficiently transporting nutrient ions,we optimally design and construct a biomass-based Janus architecture evaporator with an oriented nanostructure for ISSG,using the ice template method,followed by biomimetic mineralization with the resource-abundant and low-cost biomass of the carboxymethyl cellulose and sodium alginate as the raw materials.Taking advantage of the oriented nanostructure allowing efficient transportation of water and coordination capacity of sodium alginate for effective enrichment of heavy-metal ions,the biomass-based Janus architecture shows much lower thermal conductivity and an ultrahigh steam regeneration rate of 2.3 kg m−2 h−1,considerably surpassing those of previously reported oriented biomass-based evaporators.Moreover,the biomass precursor materials are used for this Janus evaporator,guaranteeing minimum impact on the water ecology and environment during the regeneration process of clean drinking water.This study presents an efficient,green,and sustainable pathway for ISSG to effectively achieve heavy-metal-free drinking water.展开更多
Developing an energy supply-chain based on renewable biomass holds great potential to build a low carbon society.High-energy-density(HED)jet fuel,featuring unique fused/strained cycloalkanes,is of great significance f...Developing an energy supply-chain based on renewable biomass holds great potential to build a low carbon society.High-energy-density(HED)jet fuel,featuring unique fused/strained cycloalkanes,is of great significance for volume-limited military aircrafts,as their high density and combustion heat can extend flight duration and increase the payload.Therefore,the exploration of biomass-based routes towards HED fuel has drawn much attention over the past decade.Cycloaddition reaction features rapid construction of various carbocycles in an atom-and step-economical fashion.This elegant strategy has been widely applied in the manufacture of sustainable HED fuel.Here we carefully summarize the progress achieved in this fascinating area and the review is categorized by the cycloaddition patterns including[4+2],[2+2],[4+4],and[2+1]cycloadditions.Besides,the energy densities of the as-prepared biofuels and petroleumbased fuels(conventional Jet-A and advanced JP-10)are also compared.This review will provide important insights into rational design of new HED fuel with different ring-types/sizes and inspire the chemists to turn those literature studies into practical applications in military field.展开更多
Noble metal-based-bimetallic catalysts have been highly investigated and applied in wide applications including biomass transformation via regioselective C−O hydrogenolysis while further modification especially with n...Noble metal-based-bimetallic catalysts have been highly investigated and applied in wide applications including biomass transformation via regioselective C−O hydrogenolysis while further modification especially with noble metal is highly promising yet still under investigation.Herein,Ru was found as an effective modifier among the screened noble metals(Ru,Pt,Rh,Pd,Au,and Ag)for Ir-Fe/BN(Ir=5 wt%,Fe/Ir=0.25)catalyst in terminal C−O hydrogenolysis of 1,2-butanediol(1,2-BuD)to 2-butanol(2-BuOH).Only trace amount of Ru(up to 0.5 wt%)was effective in terms of high 2-BuOH selectivity(>60%)and activity(about twice).Larger amount of Ru species(3 wt%)highly enhanced the activity but gave low selectivity to 2-BuOH with by-products of terminal C−C bond scission.Optimized catalyst(Ru(0.5)-Ir-Fe/BN)was reusable at least 4 times and gave moderate 2-BuOH yield(47%)in hydrogenolysis of 1,2-BuD.The promoting effect of Ru addition(0.5 wt%)to Ir-Fe/BN on hydrogenolysis of various alcohols was also confirmed.Combining catalytic tests with various characterizations,the promotion mechanism of Ru species in trimetallic catalysts was clarified.The Ru species in Ru(0.5)-Ir-Fe/BN form alloy with Ir and are enriched at the interface with BN surface,and direct interaction between Ru and Fe was not necessary in Ru-Ir-Fe alloy.The interface of Ir and Fe on the surface of Ir-Fe alloy may work as active sites for 1,2-diols to secondary alcohols via direct C−O hydrogenolysis,in which Ru-modified Ir activates H_(2) to form hydride-like species.The activity of Ru species in C−C bond cleavage was highly suppressed due to the direct interaction with Ir species and less exposed to substrate.Larger loading amount of Ru species(3 wt%)led to the formation Ru-rich trimetallic alloy,which further works as active sites for C−C bond scission.展开更多
Rechargeable Zn-air batteries(ZAB)have drawn extensive attention due to their eco-friendliness and safety.However,the lack of high-performance and low-cost oxygen redox reactions(OER and ORR)catalysts has become one o...Rechargeable Zn-air batteries(ZAB)have drawn extensive attention due to their eco-friendliness and safety.However,the lack of high-performance and low-cost oxygen redox reactions(OER and ORR)catalysts has become one of the main stumbling blocks in their development.Herein,we successfully fabricate a CoFe nanobubble encapsulated in nitrogen-doped carbon nanocage on wood carbon support(CoFe@NC/WC)via pyrolysis of a novel Prussian blue analog(PBA)/spruce precursor.The hierarchical CoFe@NC/WC catalyst exhibits an excellent potential difference of 0.74 V between the OER potential at 10 mA cm^(-2)and half-wave potential of ORR in 0.1 M KOH,comparable to recently reported preeminent electrocatalysts.Further,CoFe@NC/WC shows outstanding electrochemical performance in liquid ZAB,with a peak power density of 138.9 mW cm^(-2)and a specific capacity of 763.5 mAh g^(-1).More importantly,a bacterial cellulose nanofiber reinforced polyacrylic acid(BC-PAA)hydrogel electrolyte shows ultrahigh tensile-breaking stress of 1.58 MPa.In conjunction with the as-prepared CoFe@NC/WC catalyst,BC-PAA-based wearable ZAB displays impressive rechargeability and foldability,and can power portable electronics,such as electronic timer and mobile phone,in bent states.This work provides a new approach toward high-activity and low-cost catalysts for ZAB.展开更多
基金the support provided by the National Natural Science Foundation of China(No.51522805)。
文摘Heavy metals usually exist stably as the species of organic complexes in high-salinity wastewater.Therefore,their effective removal is challenging,especially when the initial p H is neutral.Herein,a novel nitrogen doped biomass-based composite(N-CMCS)was synthesized to remove the complexed heavy metal of Cr(Ⅲ)-carboxyl.The maximum adsorption capacity of Cr(Ⅲ)-Citrate(Cr-Cit)by N-CMCS under neutral p H(7.0)and high-salinity(200 mmol/L NaCl)condition was up to 2.50 mmol/g.And the removal performance remained stable after 6 times of regeneration.Combined with species and characterizations analysis,electrostatic attraction and hydrogen bonding were the main mechanisms for N-CMCS to remove Cr(Ⅲ)-carboxyl complexes.Dynamic adsorption indicated N-CMCS column could treat about 1300BV simulated wastewater and 350 BV actual wastewater with the concentration of effluent lower than1.0 mg/L.Furthermore,N-CMCS could remove a variety of complexed heavy metal ions under neutral p H,indicating the great potential in practical application.
基金support of the National Natural Science Foundation of China(No.21978170)the Natural Science Foundation of Shanghai(No.19ZR1424800)the Center of Hydrogen Science,Shanghai Jiao Tong University,China.
文摘CO_(2) utilization becomes a promising solution for reducing anthropogenic greenhouse gas (GHG) emissions. Biomass-based CO_(2) utilization (BCU) even has the potential to generate negative emissions, but the corresponding quantitative evaluation is limited. Herein, the biomass-based CO_(2) utilization with an iron cycle (BCU-Fe) system, which converts CO_(2) into formate by Fe under hydrothermal conditions and recovers Fe with biomass-derived glycerin, was investigated. The GHG reduction potential under various process designs was quantified by a multidisciplinary method, including experiments, simulations, and an ex-ante life-cycle assessment. The results reveal that the BCU-Fe system could bring considerable GHG emission reduction. Significantly, the lowest value is −34.03 kg CO_(2)-eq/kg absorbed CO_(2) (−2.44 kg CO_(2)-eq/kg circulated Fe) with the optimal yield of formate (66%) and Fe (80%). The proposed ex-ante evaluation approach not only reveals the benefits of mitigating climate change by applying the BCU-Fe system, but also serves as a generic tool to guide the industrialization of emerging carbon-neutral technologies.
基金Fundamental Research Funds for the Central Universities,Grant/Award Numbers:WK2060000034,WK2060000036,WK2480000007Science and Technology Major Project of Anhui Province,Grant/Award Number:201903a05020003+6 种基金Key Research Program of Frontier Sciences,Chinese Academy of Sciences,Grant/Award Number:QYZDJ-SSW-SLH036Foundation for Innovative Research Groups of the National Natural Science Foundation of China,Grant/Award Number:21521001Hefei Innovative Program for Overseas Excellent Scholars,Grant/Award Number:BJ2090007002National Natural Science Foundation of China,Grant/Award Numbers:22075269,22105196,51732011,U1932213National Key Research and Development Program of China,Grant/Award Numbers:2018YFE0202201,2020YFA0710100,2021YFA0715700University Synergy Innovation Program of Anhui Province,Grant/Award Number:GXXT-2019-028National Natural Science Fund for Excellent Young Scientists Fund Program(Overseas)。
文摘Interfacial solar steam generation(ISSG),involving the use of solar energy to evaporate water at the water-to-vapor interface,has presented prospects for the desalination and purification of water due to high energy conversion efficiency and low-cost freshwater generation.Herein,inspired by the aligned nanostructure of plants for efficiently transporting nutrient ions,we optimally design and construct a biomass-based Janus architecture evaporator with an oriented nanostructure for ISSG,using the ice template method,followed by biomimetic mineralization with the resource-abundant and low-cost biomass of the carboxymethyl cellulose and sodium alginate as the raw materials.Taking advantage of the oriented nanostructure allowing efficient transportation of water and coordination capacity of sodium alginate for effective enrichment of heavy-metal ions,the biomass-based Janus architecture shows much lower thermal conductivity and an ultrahigh steam regeneration rate of 2.3 kg m−2 h−1,considerably surpassing those of previously reported oriented biomass-based evaporators.Moreover,the biomass precursor materials are used for this Janus evaporator,guaranteeing minimum impact on the water ecology and environment during the regeneration process of clean drinking water.This study presents an efficient,green,and sustainable pathway for ISSG to effectively achieve heavy-metal-free drinking water.
基金supported by the National Key R&D Program of China(2022YFB4201802)the Xuzhou Basic Research Project(KC23018)+1 种基金the Fundamental Research Funds for the Central Universities(2023-00104)the Priority Academic Program Development of Jiangsu Higher Education Institutions。
文摘Developing an energy supply-chain based on renewable biomass holds great potential to build a low carbon society.High-energy-density(HED)jet fuel,featuring unique fused/strained cycloalkanes,is of great significance for volume-limited military aircrafts,as their high density and combustion heat can extend flight duration and increase the payload.Therefore,the exploration of biomass-based routes towards HED fuel has drawn much attention over the past decade.Cycloaddition reaction features rapid construction of various carbocycles in an atom-and step-economical fashion.This elegant strategy has been widely applied in the manufacture of sustainable HED fuel.Here we carefully summarize the progress achieved in this fascinating area and the review is categorized by the cycloaddition patterns including[4+2],[2+2],[4+4],and[2+1]cycloadditions.Besides,the energy densities of the as-prepared biofuels and petroleumbased fuels(conventional Jet-A and advanced JP-10)are also compared.This review will provide important insights into rational design of new HED fuel with different ring-types/sizes and inspire the chemists to turn those literature studies into practical applications in military field.
文摘Noble metal-based-bimetallic catalysts have been highly investigated and applied in wide applications including biomass transformation via regioselective C−O hydrogenolysis while further modification especially with noble metal is highly promising yet still under investigation.Herein,Ru was found as an effective modifier among the screened noble metals(Ru,Pt,Rh,Pd,Au,and Ag)for Ir-Fe/BN(Ir=5 wt%,Fe/Ir=0.25)catalyst in terminal C−O hydrogenolysis of 1,2-butanediol(1,2-BuD)to 2-butanol(2-BuOH).Only trace amount of Ru(up to 0.5 wt%)was effective in terms of high 2-BuOH selectivity(>60%)and activity(about twice).Larger amount of Ru species(3 wt%)highly enhanced the activity but gave low selectivity to 2-BuOH with by-products of terminal C−C bond scission.Optimized catalyst(Ru(0.5)-Ir-Fe/BN)was reusable at least 4 times and gave moderate 2-BuOH yield(47%)in hydrogenolysis of 1,2-BuD.The promoting effect of Ru addition(0.5 wt%)to Ir-Fe/BN on hydrogenolysis of various alcohols was also confirmed.Combining catalytic tests with various characterizations,the promotion mechanism of Ru species in trimetallic catalysts was clarified.The Ru species in Ru(0.5)-Ir-Fe/BN form alloy with Ir and are enriched at the interface with BN surface,and direct interaction between Ru and Fe was not necessary in Ru-Ir-Fe alloy.The interface of Ir and Fe on the surface of Ir-Fe alloy may work as active sites for 1,2-diols to secondary alcohols via direct C−O hydrogenolysis,in which Ru-modified Ir activates H_(2) to form hydride-like species.The activity of Ru species in C−C bond cleavage was highly suppressed due to the direct interaction with Ir species and less exposed to substrate.Larger loading amount of Ru species(3 wt%)led to the formation Ru-rich trimetallic alloy,which further works as active sites for C−C bond scission.
基金supported by the Innovation and Technology Commission(Grant no.PRP/032/20FX)the RFBR(Grant no.20-03-00772)
文摘Rechargeable Zn-air batteries(ZAB)have drawn extensive attention due to their eco-friendliness and safety.However,the lack of high-performance and low-cost oxygen redox reactions(OER and ORR)catalysts has become one of the main stumbling blocks in their development.Herein,we successfully fabricate a CoFe nanobubble encapsulated in nitrogen-doped carbon nanocage on wood carbon support(CoFe@NC/WC)via pyrolysis of a novel Prussian blue analog(PBA)/spruce precursor.The hierarchical CoFe@NC/WC catalyst exhibits an excellent potential difference of 0.74 V between the OER potential at 10 mA cm^(-2)and half-wave potential of ORR in 0.1 M KOH,comparable to recently reported preeminent electrocatalysts.Further,CoFe@NC/WC shows outstanding electrochemical performance in liquid ZAB,with a peak power density of 138.9 mW cm^(-2)and a specific capacity of 763.5 mAh g^(-1).More importantly,a bacterial cellulose nanofiber reinforced polyacrylic acid(BC-PAA)hydrogel electrolyte shows ultrahigh tensile-breaking stress of 1.58 MPa.In conjunction with the as-prepared CoFe@NC/WC catalyst,BC-PAA-based wearable ZAB displays impressive rechargeability and foldability,and can power portable electronics,such as electronic timer and mobile phone,in bent states.This work provides a new approach toward high-activity and low-cost catalysts for ZAB.