It is significant for the rational construction of the high–efficient bifunctional electrocatalysts for in–depth understandings of how to improve the electron transfer and ion/oxygen transport in catalyzing oxygen r...It is significant for the rational construction of the high–efficient bifunctional electrocatalysts for in–depth understandings of how to improve the electron transfer and ion/oxygen transport in catalyzing oxygen reduction reaction and oxygen evolution reaction(ORR and OER),but still full of vital challenges.Herein,we synthesize the novel“three–in–one”catalyst that engineers core–shell Mott–Schottky Co_(9)S_(8)/Co heterostructure on the defective reduced graphene oxide(Co_(9)S_(8)/Co–rGO).The Co_(9)S_(8)/Co–rGO catalyst exhibits abundant Mott–Schottky heterogeneous–interfaces,the well–defined core–shell nanostructure as well as the defective carbon architecture,which provide the multiple guarantees for enhancing the electron transfer and ion/oxygen transport,thus boosting the catalytic ORR and OER activities in neutral electrolyte.As expected,the integrated core–shell Mott–Schottky Co_(9)S_(8)/Co–rGO catalyst delivers the most robust and efficient rechargeable ZABs performance in neutral solution electrolytes accompanied with a power density of 59.5 mW cm^(-2) and superior cycling stability at 5 mA cm^(-2) over 200 h.This work not only emphasizes the rational designing of the high–efficient bifunctional oxygen catalysts from the fundamental understanding of accelerating the electron transfer and ion/oxygen transport,but also sheds light on the practical application prospects in more friendly environmentally neutral rechargeable ZABs.展开更多
Ethane conversion to ethylene and aromatics over Zn/zeolite catalysts is a promising technology for efficient exploitation of light alkanes. However, the reaction faces two major hurdles including the limited ethane c...Ethane conversion to ethylene and aromatics over Zn/zeolite catalysts is a promising technology for efficient exploitation of light alkanes. However, the reaction faces two major hurdles including the limited ethane conversion due to thermodynamics and the drastic catalyst deactivation by kinetical coke accumulation. Here we present a route to improve ethane conversion using a composite catalyst, involving Zn/HZSM-5 for ethane dehydroaromatization and CaMnO3-δperovskite for in situ selective hydrogen oxidation. The in situ H2 consumption shifts ethane dehydrogenation equilibrium to the desired side and can obviously increase the yield of target product. Furthermore, it is found that the in situ generated H2 O through H2 combustion can significantly suppress the coke formation and consequently enhance the stability of the composite catalyst. After 400 min reaction, a product yield of 23% was retained over the composite catalyst, almost a threefold increase with respect to the Zn/HZSM-5 reference(8%). It is anticipated that this novel composite catalyst combined with an efficient reactor technology may improve the viability of ethane aromatization in utilization.展开更多
Employing the alkaline water electrolysis system to generate hydrogen holds great prospects but still poses significant challenges,particularly for the construction of hydrogen evolution reaction(HER)catalysts operati...Employing the alkaline water electrolysis system to generate hydrogen holds great prospects but still poses significant challenges,particularly for the construction of hydrogen evolution reaction(HER)catalysts operating at ampere-level current density.Herein,the unique Ru and RuP_(2)dual nano-islands are deliberately implanted on N-doped carbon substrate(denoted as Ru-RuP_(2)/NC),in which a built-in electric field(BEF)is spontaneously generated between Ru-RuP_(2)dual nano-islands driven by their work function difference.Experimental and theoretical results unveil that such constructed BEF could serve as the driving force for triggering fast hydrogen spillover process on bridged Ru-RuP_(2)dual nano-islands,which could invalidate the inhibitory effect of high hydrogen coverage at ampere-level current density,and synchronously speed up the water dissociation on Ru nano-islands and hydrogen adsorption/desorption on RuP_(2)nano-islands through hydrogen spillover process.As a result,the Ru-RuP_(2)/NC affords an ultra-low overpotential of 218 mV to achieve 1.0 A·cm^(−2)along with the superior stability over 1000 h,holding the great promising prospect in practical applications at ampere-level current density.More importantly,this work is the first to advance the scientific understanding of the relationship between the constructed BEF and hydrogen spillover process,which could be enlightening for the rational design of the cost-effective alkaline HER catalysts at ampere-level current density.展开更多
Cathode interfacial materials(CIMs)stand as critical elemental in organic solar cells(OSCs),which can align energy levels,and foster ohmic contacts between the cathode and active layer of the OSCs.Nevertheless,the lag...Cathode interfacial materials(CIMs)stand as critical elemental in organic solar cells(OSCs),which can align energy levels,and foster ohmic contacts between the cathode and active layer of the OSCs.Nevertheless,the lagging advancement in CIMs has concurrently engendered the oversight of theoretical inquiries pertaining to the impact of molecular structure on their performance.Delving into this realm,we present two propeller-shaped isomers,4,4',4''-(benzo[1,2-b:3,4-b':5,6-b'']trithiophene-2,5,8-triyl)tris(2-(3-(dimethylamino)propyl)-1H-benzo[de]isoquinoline-1,3(2H)-dione)(3ONIN)and 6,6',6''-(benzo[1,2-b:3,4-b':5,6-b'']trithiophene-2,5,8-triyl)tris(2-(3-(dimethylamino)propyl)-1H-benzo[de]isoquinoline-1,3(2H)-dione)(3PNIN),distinguished by their molecular planarity,as a promising foundation for crafting highly efficient OSCs.This study illuminates the superiority of 3PNIN with more plane structure,exemplified by its enhanced molar extinction coefficient,deeper lowest unoccupied molecular orbital(LUMO)and highest occupied molecular orbital(HOMO)energy levels,intensified self-doping effect,heightened electron mobility,and elevated conductivity,in comparison to its counterpart,3ONIN.As a result,3PNIN and 3ONIN-treated OSC devices yield efficiencies of 17.73%and 16.82%,respectively.This finding serves as a compelling validation of the critical role played by molecular planarity in influencing CIM performance.展开更多
Renewable-energy-driven nitrate(NO_(3)^(−))electroreduction to ammonia(NH_(3))(NERA)has been an attractive technology for decarbonizing NH_(3)production and wastewater treatment.Improving NERA efficiency requires elec...Renewable-energy-driven nitrate(NO_(3)^(−))electroreduction to ammonia(NH_(3))(NERA)has been an attractive technology for decarbonizing NH_(3)production and wastewater treatment.Improving NERA efficiency requires electrocatalysts that are earth-abundant and show fantastic performance.Here we report a semiempirical activity descriptor of eg occupancy(of surface B-site cations)for identifying inexpensive perovskite oxides with extremely high efficacy toward NERA.We establish the descriptor by systematic investigations of more than 10 perovskite oxides.These investigations demonstrate that their intrinsic NERA activities display a volcano-shaped dependence on eg occupancy and the optimized intrinsic activities are accessible at near-1 eg occupancies.This could plausibly be attributed to the favorable overlaps between surface adsorbates and vertically-oriented eg orbitals.More importantly,utilizing this descriptor,we predict a highly active,selective,and durable NERA electrocatalyst with a composition of Ba_(0.5)Sr_(0.5)Co_(0.8)Fe_(0.2)O_(3−δ)(BSCF).Because of its close-to-1 e_(g)occupancy(i.e.~1.2),the BSCF features a superior NH_(3)production rate of 0.12 g·h^(−1)·mg_(cat.)^(−1)(Faradaic efficiency of 97.8%)that is at top of the volcano plot,and substantially outperforms most NERA electrocatalysts reported in literature.展开更多
Indoor heating results in high energy consumption and severe atmospheric pollution.Although the development of solar air heaters provides a sustainable route for indoor thermal comfort,such heaters still face challeng...Indoor heating results in high energy consumption and severe atmospheric pollution.Although the development of solar air heaters provides a sustainable route for indoor thermal comfort,such heaters still face challenges in terms of adequate heat exchange and filtering of atmospheric pollutants.Inspired by solar-driven interfacial evaporation,we propose a multifunctional carbon nanotube-based photothermal membrane for efficient cold air heating and purification via ventilation.Carbon nanotubes endow the membrane with high light absorption and thermal conversion capabilities,thereby sufficiently heating the approaching cold air.With the hierarchical structure formed by phase inversion,the thin upper skin of the composite membrane intercepts micropollutants via the size-sieving effect,whereas the finger-like pores and interpenetrating macrovoids inside the membrane ensure that the heated clear air passes through quickly.A proof-of-principle experiment indicated a cold airflow of 1 L/min across the membrane,yielding a temperature increase of ca.37℃ as well as a PM 2.5 rejection always higher than 93%.Further antibacterial experiments demonstrated that the membrane effectively removed airborne bacteria.This multifunctional carbon nanotube-based photothermal membrane with specific microstructures not only improves the indoor living quality but also provides a sustainable development scheme to coordinate the relationship among energy utilization,building heating,and air purification.展开更多
The excessive consumption of fossil fuels increases carbon dioxide(CO_(2))emissions,and the consequent greenhouse effect resulting from higher levels of this gas in the atmosphere has a significant impact on the envir...The excessive consumption of fossil fuels increases carbon dioxide(CO_(2))emissions,and the consequent greenhouse effect resulting from higher levels of this gas in the atmosphere has a significant impact on the environment and climate.This has necessitated the development of environmentally friendly and efficient methods for CO_(2)conversion.The carbon dioxide electroreduction reaction(CO_(2)RR),which is driven by electricity generated by renewable energy sources(e.g.,wind and solar)to convert CO_(2)into value-added fuels or chemicals,is regarded as a promising prospective path toward carbon cycling.Among the various products,formate,with its relatively simple preparation process,has broad application prospects,and can be used as fuel,hydrogen storage material,and raw material for downstream chemicals.Sn-based oxide electrocatalysts have the advantages of being inexpensive and nontoxic.In addition,these catalysts offer high product selectivity and are regarded as promising catalysts for the electrochemical reduction of CO_(2)to formate.In this review,we first clarify the reaction mechanisms and factors that influence the reduction of CO_(2)to formate,and then provide some examples of technologies that could be used to study the evolution of catalysts during the reaction.In particular,we focus on traditional Sn-based oxides(SnO_(2))and novel Sn-based perovskite oxides that have been developed for use in the field of CO_(2)RR in recent years by considering their synthesis,catalytic performance,optimization strategies,and intrinsic principles.Finally,the current challenges and opportunities for Sn-based oxide electrocatalysts are discussed.The perspectives and latest trends presented in this review are expected to inspire researchers to contribute more efforts toward comprehensively optimizing the performance of the CO_(2)RR to produce formate.展开更多
Nanoscale thin-film composite(TFC)polyamide membranes are highly desirable for desalination owing to their excellent separation performance.It is a permanent pursuit to further improve the water flux of membrane witho...Nanoscale thin-film composite(TFC)polyamide membranes are highly desirable for desalination owing to their excellent separation performance.It is a permanent pursuit to further improve the water flux of membrane without deteriorating the salt rejection.Herein,we fabricated a high-performance polyamide membrane with nanoscale structures through introducing multifunctional crown ether interlayer on the porous substrate impregnated with m-phenylenediamine.The crown ether interlayer can reduce the diffusion of amine monomers to reaction interface influenced by its interaction with m-phenylenediamine and the spatial shielding effect,leading to a controlled interfacial polymerization(IP)reaction.Besides,crown ether with intrinsic cavity is also favorable to adjust the IP process and the microstructure of polyamide layer.Since the outer surface of the nanocavity is lipophilic,crown ether has good solvency with the organic phase,thus attracting more trimesoyl chloride molecules to the interlayer and promoting the IP reaction in the confined space.As a result,a nanoscale polyamide membrane with an ultrathin selective layer of around 50 nm is obtained.The optimal TFC polyamide membrane at crown ether concentration of 0.25 wt.%exhibits a water flux of 61.2 L·m^(−2)·h^(−1),which is 364%of the pristine TFC membrane,while maintaining a rejection of above 97%to NaCl.The development of the tailor-made nanoscale polyamide membrane via constructing multifunctional crown ether interlayer provides a straightforward route to fabricate competitive membranes for highly efficient desalination.展开更多
Ordered mesoporous Cu-Mg-A1 composite oxides were synthesized via the one-pot evaporation-in- duced self-assembly strategy. Using this method, copper was first homogeneously incorporated into the ordered mesoporous sp...Ordered mesoporous Cu-Mg-A1 composite oxides were synthesized via the one-pot evaporation-in- duced self-assembly strategy. Using this method, copper was first homogeneously incorporated into the ordered mesoporous spinel matrix. After H2 reduction treatment, according to X-ray diffraction (XRD) and transmission electron microscopy (TEM) results, copper existed as metallic nanoparticles with the size of 6-10 nm that well decorated the parent mesoporous skeleton. The metallic nanoparticles were then re-oxidized to copper oxide when exposed to air or during CO oxidation reaction at low temperatures. Thus, copper migrated from bulk spinel phase to the surface after the reduction-oxidation treat- ment. Moreover, the copper on the surface was re-incor- porated into the bulk spinel phase by further thermal treatment at much higher temperature in the presence of air. The correlation between the state of copper in the mesoporous composite oxides and the catalytic perfor- mance toward CO oxidation was studied. It was found that copper existed as oxide nanoparticles on the surface of mesoporous Mg-Al skeleton is much more active than that existed as lattice Cu ions in spinel phase.展开更多
基金financially supported by the National Natural Science Foundation of China (21775142)the Sino–German Center for Research Promotion (Grants GZ 1351)+1 种基金the Natural Science Foundation of Shandong Province (ZR2020ZD10)the Research Funds for the Central Universities (202061031)。
文摘It is significant for the rational construction of the high–efficient bifunctional electrocatalysts for in–depth understandings of how to improve the electron transfer and ion/oxygen transport in catalyzing oxygen reduction reaction and oxygen evolution reaction(ORR and OER),but still full of vital challenges.Herein,we synthesize the novel“three–in–one”catalyst that engineers core–shell Mott–Schottky Co_(9)S_(8)/Co heterostructure on the defective reduced graphene oxide(Co_(9)S_(8)/Co–rGO).The Co_(9)S_(8)/Co–rGO catalyst exhibits abundant Mott–Schottky heterogeneous–interfaces,the well–defined core–shell nanostructure as well as the defective carbon architecture,which provide the multiple guarantees for enhancing the electron transfer and ion/oxygen transport,thus boosting the catalytic ORR and OER activities in neutral electrolyte.As expected,the integrated core–shell Mott–Schottky Co_(9)S_(8)/Co–rGO catalyst delivers the most robust and efficient rechargeable ZABs performance in neutral solution electrolytes accompanied with a power density of 59.5 mW cm^(-2) and superior cycling stability at 5 mA cm^(-2) over 200 h.This work not only emphasizes the rational designing of the high–efficient bifunctional oxygen catalysts from the fundamental understanding of accelerating the electron transfer and ion/oxygen transport,but also sheds light on the practical application prospects in more friendly environmentally neutral rechargeable ZABs.
基金Financial support from the National Natural Science Foundation of China (grant 21606249, 21536005)the Director Innovation Fund of Key Laboratory of Biofuels, Chinese Academy of Sciences (grant Y57201190V)QIBEBT and Dalian National Laboratory For Clean Energy (DNL), CAS (Grant QIBEBT I201924)。
文摘Ethane conversion to ethylene and aromatics over Zn/zeolite catalysts is a promising technology for efficient exploitation of light alkanes. However, the reaction faces two major hurdles including the limited ethane conversion due to thermodynamics and the drastic catalyst deactivation by kinetical coke accumulation. Here we present a route to improve ethane conversion using a composite catalyst, involving Zn/HZSM-5 for ethane dehydroaromatization and CaMnO3-δperovskite for in situ selective hydrogen oxidation. The in situ H2 consumption shifts ethane dehydrogenation equilibrium to the desired side and can obviously increase the yield of target product. Furthermore, it is found that the in situ generated H2 O through H2 combustion can significantly suppress the coke formation and consequently enhance the stability of the composite catalyst. After 400 min reaction, a product yield of 23% was retained over the composite catalyst, almost a threefold increase with respect to the Zn/HZSM-5 reference(8%). It is anticipated that this novel composite catalyst combined with an efficient reactor technology may improve the viability of ethane aromatization in utilization.
基金the National Natural Science Foundation of China(Nos.22279124 and 52261145700)Shandong Province Natural Science Foundation(No.ZR2022ZD30)National Research Foundation of Korea(NRF)grant funded by the Korea government(MSIT)(Nos.NRF-2020R1A2C3004146 and RS-2023-00235596).
文摘Employing the alkaline water electrolysis system to generate hydrogen holds great prospects but still poses significant challenges,particularly for the construction of hydrogen evolution reaction(HER)catalysts operating at ampere-level current density.Herein,the unique Ru and RuP_(2)dual nano-islands are deliberately implanted on N-doped carbon substrate(denoted as Ru-RuP_(2)/NC),in which a built-in electric field(BEF)is spontaneously generated between Ru-RuP_(2)dual nano-islands driven by their work function difference.Experimental and theoretical results unveil that such constructed BEF could serve as the driving force for triggering fast hydrogen spillover process on bridged Ru-RuP_(2)dual nano-islands,which could invalidate the inhibitory effect of high hydrogen coverage at ampere-level current density,and synchronously speed up the water dissociation on Ru nano-islands and hydrogen adsorption/desorption on RuP_(2)nano-islands through hydrogen spillover process.As a result,the Ru-RuP_(2)/NC affords an ultra-low overpotential of 218 mV to achieve 1.0 A·cm^(−2)along with the superior stability over 1000 h,holding the great promising prospect in practical applications at ampere-level current density.More importantly,this work is the first to advance the scientific understanding of the relationship between the constructed BEF and hydrogen spillover process,which could be enlightening for the rational design of the cost-effective alkaline HER catalysts at ampere-level current density.
基金supported by the National Natural Science Foundation of China(No.22105189).
文摘Cathode interfacial materials(CIMs)stand as critical elemental in organic solar cells(OSCs),which can align energy levels,and foster ohmic contacts between the cathode and active layer of the OSCs.Nevertheless,the lagging advancement in CIMs has concurrently engendered the oversight of theoretical inquiries pertaining to the impact of molecular structure on their performance.Delving into this realm,we present two propeller-shaped isomers,4,4',4''-(benzo[1,2-b:3,4-b':5,6-b'']trithiophene-2,5,8-triyl)tris(2-(3-(dimethylamino)propyl)-1H-benzo[de]isoquinoline-1,3(2H)-dione)(3ONIN)and 6,6',6''-(benzo[1,2-b:3,4-b':5,6-b'']trithiophene-2,5,8-triyl)tris(2-(3-(dimethylamino)propyl)-1H-benzo[de]isoquinoline-1,3(2H)-dione)(3PNIN),distinguished by their molecular planarity,as a promising foundation for crafting highly efficient OSCs.This study illuminates the superiority of 3PNIN with more plane structure,exemplified by its enhanced molar extinction coefficient,deeper lowest unoccupied molecular orbital(LUMO)and highest occupied molecular orbital(HOMO)energy levels,intensified self-doping effect,heightened electron mobility,and elevated conductivity,in comparison to its counterpart,3ONIN.As a result,3PNIN and 3ONIN-treated OSC devices yield efficiencies of 17.73%and 16.82%,respectively.This finding serves as a compelling validation of the critical role played by molecular planarity in influencing CIM performance.
基金the National Natural Science Foundation of China(No.52102258)the Taishan Scholars Program(No.tsqn202306309)+2 种基金Natural Science Foundation of Shandong Province(No.ZR2023YQ012)Natural Science Foundation of Jiangsu Province(No.BK20210447)the Special Fund Project of Jiangsu Province for Scientific and Technological Innovation in Carbon Peaking and Carbon Neutrality(No.BK20220023).
文摘Renewable-energy-driven nitrate(NO_(3)^(−))electroreduction to ammonia(NH_(3))(NERA)has been an attractive technology for decarbonizing NH_(3)production and wastewater treatment.Improving NERA efficiency requires electrocatalysts that are earth-abundant and show fantastic performance.Here we report a semiempirical activity descriptor of eg occupancy(of surface B-site cations)for identifying inexpensive perovskite oxides with extremely high efficacy toward NERA.We establish the descriptor by systematic investigations of more than 10 perovskite oxides.These investigations demonstrate that their intrinsic NERA activities display a volcano-shaped dependence on eg occupancy and the optimized intrinsic activities are accessible at near-1 eg occupancies.This could plausibly be attributed to the favorable overlaps between surface adsorbates and vertically-oriented eg orbitals.More importantly,utilizing this descriptor,we predict a highly active,selective,and durable NERA electrocatalyst with a composition of Ba_(0.5)Sr_(0.5)Co_(0.8)Fe_(0.2)O_(3−δ)(BSCF).Because of its close-to-1 e_(g)occupancy(i.e.~1.2),the BSCF features a superior NH_(3)production rate of 0.12 g·h^(−1)·mg_(cat.)^(−1)(Faradaic efficiency of 97.8%)that is at top of the volcano plot,and substantially outperforms most NERA electrocatalysts reported in literature.
基金supported by the National Natural Science Foundation of China(No.22205252)the Natural Science Foundation of Shandong Province(No.ZR2021QB111)+1 种基金the Taishan Scholars Program of Shandong Province(No.tstq20221151)the Innovation Funds of Shandong Energy Institute(SEI I202140).
文摘Indoor heating results in high energy consumption and severe atmospheric pollution.Although the development of solar air heaters provides a sustainable route for indoor thermal comfort,such heaters still face challenges in terms of adequate heat exchange and filtering of atmospheric pollutants.Inspired by solar-driven interfacial evaporation,we propose a multifunctional carbon nanotube-based photothermal membrane for efficient cold air heating and purification via ventilation.Carbon nanotubes endow the membrane with high light absorption and thermal conversion capabilities,thereby sufficiently heating the approaching cold air.With the hierarchical structure formed by phase inversion,the thin upper skin of the composite membrane intercepts micropollutants via the size-sieving effect,whereas the finger-like pores and interpenetrating macrovoids inside the membrane ensure that the heated clear air passes through quickly.A proof-of-principle experiment indicated a cold airflow of 1 L/min across the membrane,yielding a temperature increase of ca.37℃ as well as a PM 2.5 rejection always higher than 93%.Further antibacterial experiments demonstrated that the membrane effectively removed airborne bacteria.This multifunctional carbon nanotube-based photothermal membrane with specific microstructures not only improves the indoor living quality but also provides a sustainable development scheme to coordinate the relationship among energy utilization,building heating,and air purification.
基金supported by the National Natural Science Foundation of China(52102258)Taishan Scholars Program(tsqn202306309)+1 种基金Natural Science Foundation of Shandong Province(ZR2023YQ012)Natural Science Foundation of Jiangsu Province(BK20210447).
文摘The excessive consumption of fossil fuels increases carbon dioxide(CO_(2))emissions,and the consequent greenhouse effect resulting from higher levels of this gas in the atmosphere has a significant impact on the environment and climate.This has necessitated the development of environmentally friendly and efficient methods for CO_(2)conversion.The carbon dioxide electroreduction reaction(CO_(2)RR),which is driven by electricity generated by renewable energy sources(e.g.,wind and solar)to convert CO_(2)into value-added fuels or chemicals,is regarded as a promising prospective path toward carbon cycling.Among the various products,formate,with its relatively simple preparation process,has broad application prospects,and can be used as fuel,hydrogen storage material,and raw material for downstream chemicals.Sn-based oxide electrocatalysts have the advantages of being inexpensive and nontoxic.In addition,these catalysts offer high product selectivity and are regarded as promising catalysts for the electrochemical reduction of CO_(2)to formate.In this review,we first clarify the reaction mechanisms and factors that influence the reduction of CO_(2)to formate,and then provide some examples of technologies that could be used to study the evolution of catalysts during the reaction.In particular,we focus on traditional Sn-based oxides(SnO_(2))and novel Sn-based perovskite oxides that have been developed for use in the field of CO_(2)RR in recent years by considering their synthesis,catalytic performance,optimization strategies,and intrinsic principles.Finally,the current challenges and opportunities for Sn-based oxide electrocatalysts are discussed.The perspectives and latest trends presented in this review are expected to inspire researchers to contribute more efforts toward comprehensively optimizing the performance of the CO_(2)RR to produce formate.
基金the Deanship of Scientific Research at Imam Mohammad Ibn Saud Islamic University(IMSIU)for funding and supporting this work through Research Partnership Program(No.RP-21-09-75)。
文摘Nanoscale thin-film composite(TFC)polyamide membranes are highly desirable for desalination owing to their excellent separation performance.It is a permanent pursuit to further improve the water flux of membrane without deteriorating the salt rejection.Herein,we fabricated a high-performance polyamide membrane with nanoscale structures through introducing multifunctional crown ether interlayer on the porous substrate impregnated with m-phenylenediamine.The crown ether interlayer can reduce the diffusion of amine monomers to reaction interface influenced by its interaction with m-phenylenediamine and the spatial shielding effect,leading to a controlled interfacial polymerization(IP)reaction.Besides,crown ether with intrinsic cavity is also favorable to adjust the IP process and the microstructure of polyamide layer.Since the outer surface of the nanocavity is lipophilic,crown ether has good solvency with the organic phase,thus attracting more trimesoyl chloride molecules to the interlayer and promoting the IP reaction in the confined space.As a result,a nanoscale polyamide membrane with an ultrathin selective layer of around 50 nm is obtained.The optimal TFC polyamide membrane at crown ether concentration of 0.25 wt.%exhibits a water flux of 61.2 L·m^(−2)·h^(−1),which is 364%of the pristine TFC membrane,while maintaining a rejection of above 97%to NaCl.The development of the tailor-made nanoscale polyamide membrane via constructing multifunctional crown ether interlayer provides a straightforward route to fabricate competitive membranes for highly efficient desalination.
基金supported by the Natural Science Foundation of Shandong Province(ZR2020ZD10)the National Natural Science Foundation of China(21775142)Shenzhen Natural Science Fund(20200925154115001 and JCYJ20210324115809026).
基金This work was supported by the Recruitment Program of Global Youth Experts of China, the National Natural Science Foundation of China (21403267, 21450110410), and Shandong Postdoctoral Innovation Program (201303065).
文摘Ordered mesoporous Cu-Mg-A1 composite oxides were synthesized via the one-pot evaporation-in- duced self-assembly strategy. Using this method, copper was first homogeneously incorporated into the ordered mesoporous spinel matrix. After H2 reduction treatment, according to X-ray diffraction (XRD) and transmission electron microscopy (TEM) results, copper existed as metallic nanoparticles with the size of 6-10 nm that well decorated the parent mesoporous skeleton. The metallic nanoparticles were then re-oxidized to copper oxide when exposed to air or during CO oxidation reaction at low temperatures. Thus, copper migrated from bulk spinel phase to the surface after the reduction-oxidation treat- ment. Moreover, the copper on the surface was re-incor- porated into the bulk spinel phase by further thermal treatment at much higher temperature in the presence of air. The correlation between the state of copper in the mesoporous composite oxides and the catalytic perfor- mance toward CO oxidation was studied. It was found that copper existed as oxide nanoparticles on the surface of mesoporous Mg-Al skeleton is much more active than that existed as lattice Cu ions in spinel phase.