1.Introduction The development of human society has caused global energy demand and consumption to grow rapidly.The extensive consump-tion of fossil fuels(e.g.,oil and coal)has dramatically increased environmental pol...1.Introduction The development of human society has caused global energy demand and consumption to grow rapidly.The extensive consump-tion of fossil fuels(e.g.,oil and coal)has dramatically increased environmental pollution and greenhouse gas emissions,seriously threatening the ecological system and human health.Developing green and sustainable technologies should be investigated and pur-sued to benefit human society.In addition,designing efficient and multifunctional materials is vital in new energy and environmental development.The metal-organic framework(MOF)is a kind of functional and highly porous nanomaterial composed of metal-based nodes and organic ligands,providing reactive sites for energy and environmental fields.展开更多
The introduction of the heterogeneous catalysts with high activity can significantly improve hydrogen storage performance of MgH_(2),therefore,in this paper,we synthesize a carbon-supported transition metal compound,F...The introduction of the heterogeneous catalysts with high activity can significantly improve hydrogen storage performance of MgH_(2),therefore,in this paper,we synthesize a carbon-supported transition metal compound,FeCoS@C derivative from ZIF-67,by utilizing the in situ formed C dispersive multiphase Mg_(2)Co,α-Fe,Co_(3)Fe_(7),and MgS to implement catalysis to MgH_(2).Noteworthily,MgH_(2)-FeCoS@C rapidly ab-sorbs 6.78 wt%H_(2)within 60 s at 573 K and can also absorb 4.56 wt%H_(2)in 900 s at 473 K.Besides,the addition of FeCoS@C results in decreasing of the initial dehydrogenation temperatures of MgH_(2)from 620 to 550 K.The dehydrogenation activation energy of MgH_(2)decreases from 160.7 to 91.9 kJ mol^(-1).Studies show that the Mg_(2)Co,α-Fe,and Co_(3)Fe_(7)act as“hydrogen channels”to accelerate hydrogen transfer due to the presence of transition metals,and MgS with excellent catalytic effect formed from MgH_(2)-FeCoS@C provides a strong and stable catalytic effect.Besides,the carbon skeleton obtained by the carbonization of ZIF-67 not only serves as a dispersion for the multiphase catalytic system,but also provides more active sites for the catalysts.Our study shows that the multiphase and multiscale catalytic system provides an effective strategy for improving the hydrogen storage performance of MgH_(2).展开更多
Implant-associated infections caused by biomedical catheters severely threaten patients'health.The use of electrochemical control on NO release from benign nitrite equipped in the catheter can potentially resolve ...Implant-associated infections caused by biomedical catheters severely threaten patients'health.The use of electrochemical control on NO release from benign nitrite equipped in the catheter can potentially resolve this issue with excellent biocompatibility.Inspired by nitrite reductase,a Cu-BDC(BDC:benzene-1,4-dicarboxylic acid)catalyst with coordinated Cu(Ⅱ)sites was constructed as a heterogeneous electrocatalyst to control nitrite reduction to nitric oxide for catheter antibacteria.The combined results of in situ and ex situ tests unveil the key function of interconversion between Cu(Ⅱ)and Cu(Ⅰ)species in NO_(2)^(-)reduction to NO.After being incorporated into the actual catheter,the Cu-BDC catalyst exhibits high electrocatalytic activity toward NO_(2)^(-)reduction to NO and excellent antibacteria efficacy with a sterilizing rate of 99.9%,paving the way for the development of advanced metal-organic frameworks(MOFs)electrocatalysts for catheter antibacteria.展开更多
Bi is a promising anode material for potassium-ion batteries(PIBs)due to its high theoretical capacity.However,severe pulverization upon cycling limits its practical applications.In this work,we propose a new approach...Bi is a promising anode material for potassium-ion batteries(PIBs)due to its high theoretical capacity.However,severe pulverization upon cycling limits its practical applications.In this work,we propose a new approach of using metastable alloys with Bi elements.Metastable Bi:Co and Bi:Fe alloys nanodots@carbon anode materials(Bi:Co and Bi:Fe@C)are synthesized for the first time via simple annealing of their metal-organic frameworks(MOF)precursors.These prepared materials are demonstrated as ideal hosts for high-rate K-ion storage.Bi_(0.85)Co_(0.15)@C and Bi_(0.83)Fe_(0.17)@C electrodes respectively deliver superior 178 and 253 mAh·g^(−1)at 20 A·g^(−1),as well as stable cycling performance at 2 A·g^(−1).Ex situ scanning electron microscopy(SEM),X-ray photoelectron spectroscopy(XPS),X-ray diffraction(XRD),and transmission electron microscopy(TEM)studies on Bi:Co@C indicate that the elemental Co separates out during the initial potassiation and stands during the following discharge/charge cycles.In situ formed Co precipitates can act as(1)“conductive binders”as well as(2)“separators”to prevent the severe aggregation of adjacent active elemental Bi nanoparticles and(3)accelerate the potassiation/de-potassiation kinetics in elemental Bi precipitates after initial discharge/charge cycles.This work could inspire the development of metal-type anodes.展开更多
This review provides a recompilation of the most important and recent strategies employed to increase the efficiency of metal-organic framework(MOF)-based systems toward the photocatalytic hydrogen evolution(PHE)react...This review provides a recompilation of the most important and recent strategies employed to increase the efficiency of metal-organic framework(MOF)-based systems toward the photocatalytic hydrogen evolution(PHE)reaction through specific strategies:tailoring the photocatalytic activity of bare MOFs and vip@MOF composites,formation of heterojunctions based on MOFs and various photocatalysts,and inorganic photocatalysts derived from MOFs.According to the data reported in this mini-review,the most effective strategy to improve the PHE of MOFs relies on modifying the linkers with new secondary building units(SBUs).Although several reviews have investigated the photocatalytic activity of MOFs from a general point of view,many of these studies relate this activity to the physicochemical and catalytic properties of MOFs.However,they did not consider the interactions between the components of the photocatalytic material.This study highlights the effects of strength of the supramolecular interactions on the photocatalytic performance of bare and MOF-based materials during PHE.A thorough review and comparison of the results established that metal-nanoparticle@MOF composites have weak van der Waals forces between components,whereas heterostructures only interact with MOFs at the surface of bare materials.Regarding material derivatives from MOFs,we found that pyrolysis destroyed some beneficial properties of MOFs for PHE.Thus,we conclude that adding SBUs to organic linkers is the most efficient strategy to perform the PHE because the SBUs added to the MOFs promote synergy between the two materials through strong coordination bonds.展开更多
文摘1.Introduction The development of human society has caused global energy demand and consumption to grow rapidly.The extensive consump-tion of fossil fuels(e.g.,oil and coal)has dramatically increased environmental pollution and greenhouse gas emissions,seriously threatening the ecological system and human health.Developing green and sustainable technologies should be investigated and pur-sued to benefit human society.In addition,designing efficient and multifunctional materials is vital in new energy and environmental development.The metal-organic framework(MOF)is a kind of functional and highly porous nanomaterial composed of metal-based nodes and organic ligands,providing reactive sites for energy and environmental fields.
基金This work was financially supported by the National Natural Science Foundation of China(Nos.52071281 and 51971197)the Natural Science Foundation of Hebei Province(Nos.C2022203003 and E2020203081)+1 种基金the Science and Technology Project of Hebei Education Department(No.BJK2022033)the Hebei Province Foundation for Returned Talent(No.C20210322).
文摘The introduction of the heterogeneous catalysts with high activity can significantly improve hydrogen storage performance of MgH_(2),therefore,in this paper,we synthesize a carbon-supported transition metal compound,FeCoS@C derivative from ZIF-67,by utilizing the in situ formed C dispersive multiphase Mg_(2)Co,α-Fe,Co_(3)Fe_(7),and MgS to implement catalysis to MgH_(2).Noteworthily,MgH_(2)-FeCoS@C rapidly ab-sorbs 6.78 wt%H_(2)within 60 s at 573 K and can also absorb 4.56 wt%H_(2)in 900 s at 473 K.Besides,the addition of FeCoS@C results in decreasing of the initial dehydrogenation temperatures of MgH_(2)from 620 to 550 K.The dehydrogenation activation energy of MgH_(2)decreases from 160.7 to 91.9 kJ mol^(-1).Studies show that the Mg_(2)Co,α-Fe,and Co_(3)Fe_(7)act as“hydrogen channels”to accelerate hydrogen transfer due to the presence of transition metals,and MgS with excellent catalytic effect formed from MgH_(2)-FeCoS@C provides a strong and stable catalytic effect.Besides,the carbon skeleton obtained by the carbonization of ZIF-67 not only serves as a dispersion for the multiphase catalytic system,but also provides more active sites for the catalysts.Our study shows that the multiphase and multiscale catalytic system provides an effective strategy for improving the hydrogen storage performance of MgH_(2).
基金the financial support from National Postdoctoral Science Foundation of China(Nos.2021M702436 and BX2021211)Haihe Laboratory of Sustainable Chemical Transformations+1 种基金National Natural Science Foundation of China(Nos.22101202 and 22071173)Tianjin Science and Technology Programme(Nos.20JCJQJC00050 and 22ZYJDSS00060)。
文摘Implant-associated infections caused by biomedical catheters severely threaten patients'health.The use of electrochemical control on NO release from benign nitrite equipped in the catheter can potentially resolve this issue with excellent biocompatibility.Inspired by nitrite reductase,a Cu-BDC(BDC:benzene-1,4-dicarboxylic acid)catalyst with coordinated Cu(Ⅱ)sites was constructed as a heterogeneous electrocatalyst to control nitrite reduction to nitric oxide for catheter antibacteria.The combined results of in situ and ex situ tests unveil the key function of interconversion between Cu(Ⅱ)and Cu(Ⅰ)species in NO_(2)^(-)reduction to NO.After being incorporated into the actual catheter,the Cu-BDC catalyst exhibits high electrocatalytic activity toward NO_(2)^(-)reduction to NO and excellent antibacteria efficacy with a sterilizing rate of 99.9%,paving the way for the development of advanced metal-organic frameworks(MOFs)electrocatalysts for catheter antibacteria.
基金the NSFC/RGC Joint Research Scheme 2020/21(No.N_CityU104/20).
文摘Bi is a promising anode material for potassium-ion batteries(PIBs)due to its high theoretical capacity.However,severe pulverization upon cycling limits its practical applications.In this work,we propose a new approach of using metastable alloys with Bi elements.Metastable Bi:Co and Bi:Fe alloys nanodots@carbon anode materials(Bi:Co and Bi:Fe@C)are synthesized for the first time via simple annealing of their metal-organic frameworks(MOF)precursors.These prepared materials are demonstrated as ideal hosts for high-rate K-ion storage.Bi_(0.85)Co_(0.15)@C and Bi_(0.83)Fe_(0.17)@C electrodes respectively deliver superior 178 and 253 mAh·g^(−1)at 20 A·g^(−1),as well as stable cycling performance at 2 A·g^(−1).Ex situ scanning electron microscopy(SEM),X-ray photoelectron spectroscopy(XPS),X-ray diffraction(XRD),and transmission electron microscopy(TEM)studies on Bi:Co@C indicate that the elemental Co separates out during the initial potassiation and stands during the following discharge/charge cycles.In situ formed Co precipitates can act as(1)“conductive binders”as well as(2)“separators”to prevent the severe aggregation of adjacent active elemental Bi nanoparticles and(3)accelerate the potassiation/de-potassiation kinetics in elemental Bi precipitates after initial discharge/charge cycles.This work could inspire the development of metal-type anodes.
基金supported by CONACYT through the following projects:Cátedras CONACYT-ID7708,CONACYT-FC-1725Luis.A.Alfonso-Herrera thanks CONACYT for the M.C.scholarship 844207UANL also supported this research through projects PAICYT CE1352-20 and PAICYT 601-CE-2022.
文摘This review provides a recompilation of the most important and recent strategies employed to increase the efficiency of metal-organic framework(MOF)-based systems toward the photocatalytic hydrogen evolution(PHE)reaction through specific strategies:tailoring the photocatalytic activity of bare MOFs and vip@MOF composites,formation of heterojunctions based on MOFs and various photocatalysts,and inorganic photocatalysts derived from MOFs.According to the data reported in this mini-review,the most effective strategy to improve the PHE of MOFs relies on modifying the linkers with new secondary building units(SBUs).Although several reviews have investigated the photocatalytic activity of MOFs from a general point of view,many of these studies relate this activity to the physicochemical and catalytic properties of MOFs.However,they did not consider the interactions between the components of the photocatalytic material.This study highlights the effects of strength of the supramolecular interactions on the photocatalytic performance of bare and MOF-based materials during PHE.A thorough review and comparison of the results established that metal-nanoparticle@MOF composites have weak van der Waals forces between components,whereas heterostructures only interact with MOFs at the surface of bare materials.Regarding material derivatives from MOFs,we found that pyrolysis destroyed some beneficial properties of MOFs for PHE.Thus,we conclude that adding SBUs to organic linkers is the most efficient strategy to perform the PHE because the SBUs added to the MOFs promote synergy between the two materials through strong coordination bonds.
