The solid-state lithium battery is considered as an ideal next-generation energy storage device owing to its high safety,high energy density and low cost.However,the poor ionic conductivity of solid electrolyte and lo...The solid-state lithium battery is considered as an ideal next-generation energy storage device owing to its high safety,high energy density and low cost.However,the poor ionic conductivity of solid electrolyte and low interfacial stability has hindered the application of solid-state lithium battery.Here,a flexible polymer/garnet solid electrolyte is prepared with poly(ethylene oxide),poly(vinylidene fluoride),Li6.75La3 Zr1.75Ta0.25O12,lithium bis(trifluoromethanesulfonyl)imide and oxalate,which exhibits an ionic conductivity of 2.0 ×10^(-4) S cm^(-1) at 55℃,improved mechanical property,wide electrochemical window(4.8 V vs.Li/Li+),enhanced thermal stabilities.Tiny acidic OX was introduced to inhibit the alkalinity reactions between Li6.75La3 Zr1.75Ta0.25O12 and poly(vinylidene fluoride).In order to improve the interfacial stability between cathode and electrolyte,an Al2 O3@LiNi0.5Co0.2Mn0.3O2 based composite cathode framework is also fabricated with poly(ethylene oxide) polymer and lithium salt as additives.The solid-state lithium battery assembled with polymer/garnet solid electrolyte and composite cathode framework demonstrates a high initial discharge capacity of 150.6 mAh g^(-1) and good capacity retention of 86.7% after 80 cycles at 0.2 C and 55℃,which provides a promising choice for achieving the stable electrode/electrolyte interfacial contact in solid-state lithium batteries.展开更多
Photocatalytic dual-functional reaction under visible light irradiation represents a sustainable development strategy.In detail,H2production coupled with benzylamine oxidation can remarkably lower the cost by replacin...Photocatalytic dual-functional reaction under visible light irradiation represents a sustainable development strategy.In detail,H2production coupled with benzylamine oxidation can remarkably lower the cost by replacing sacrificial agents.In this work,Cd S quantum dots(Cd S QDs)were successfully loaded onto the surface of a porphyrinic metal-organic framework(Pd-PCN-222)by the electrostatic selfassembly at room temperature.The consequent Pd-PCN-222/CdS heterojunction composites displayed superb photocatalytic activity under visible light irradiation,achieving a H2production and benzylamine oxidation rate of 5069 and 3717μmol g^(-1)h^(-1)with>99%selectivity in 3 h.There is no noticeable loss of catalytic capability during three successive runs.Mechanistic studies by in situ electron spin resonance and X-ray photoelectron spectroscopy disclosed that CdS QDs injected photoexcited electrons to Pd-PCN-222 and then Zr6clusters under visible-light irradiation,and thus Cd S QDs and Zr6clusters behave as the photocatalytic oxidation and reduction centers,respectively.展开更多
Reliable technologies for CO_(2) capture and conversion(C3) are of vital importance for the establishment of a sustainable society.Metal-organic framework(MOF) composites have shown their compelling potentials for C3 ...Reliable technologies for CO_(2) capture and conversion(C3) are of vital importance for the establishment of a sustainable society.Metal-organic framework(MOF) composites have shown their compelling potentials for C3 due to the plentiful reticular chemistry of MOF structures and the synergistic catalysis between MOFs and the functional vips.This review focuses on the syntheses and catalytic applications towards C3 of MOF composites,which is divided into three sections.The first section gives a brief introduction about synthetic strategies of MOF composites.The second section discusses the recent progress of MOF composites in C3,including CO_(2) chemical fixation,hydrogenation,photoreduction,electro reduction and photoelectro reduction.The third section summarizes the challenges and future prospects of MOF composites for C3.We hope that this review cannot only provide an inspiration for the rational design of MOF composites for C3,but also stimulate more and more research works in this emerging area.展开更多
A computational study was firstly performed in this work to examine the applicability of an acid-functionalized metal-organic framework(MOF), Ui O-66(Zr)-(COOH)2, in membrane-based H2S/CH4 separation. The results show...A computational study was firstly performed in this work to examine the applicability of an acid-functionalized metal-organic framework(MOF), Ui O-66(Zr)-(COOH)2, in membrane-based H2S/CH4 separation. The results show that this MOF could be potentially interesting when being used as the pure membrane material for the separation of the mixture with low H2 S concentration. Further, the performance of 10 different mixed matrix membranes(MMMs) on the basis of the MOF was predicted by combing the molecular simulation data and the Maxwell permeation model. The results indicate that using this MOF as filler particles in MMMs can signi ficantly enhance the permeation performance of pure polymers. The findings obtained in this work may be helpful in facilitating the application of this promising MOF for practical desulfurization process of fuel gas.展开更多
Uncontrollable dendrite growth and side reactions resulting in short operating life and low Coulombic efficiency have severely hindered the further development of aqueous zinc-ion batteries(AZIBs).In this work,we desi...Uncontrollable dendrite growth and side reactions resulting in short operating life and low Coulombic efficiency have severely hindered the further development of aqueous zinc-ion batteries(AZIBs).In this work,we designed to grow zeolitic imidazolate framework-8(ZIF-8)uniformly on CuO nanosheets(NSs)and prepared carbon-coated CuZn alloy NSs(CuZn@C NSs)by calcination under H_(2)/Ar atmosphere.As reflected by extended X-ray absorption fine structure(EXAFS),density functional theory(DFT),in-situ Raman,the Cu–Zn and Zn–N bonds present in CuZn@C NSs act as zincophilic sites to uniformly absorb Zn ions and inhibit the formation of Zn dendrites.At the same time,CuZn@C NSs hinder the direct contact between zinc anode and electrolyte,preventing the occurrence of side reactions.More impressively,the symmetric cells constructed with CuZn@C NSs anodes exhibited excellent zinc plating/exfoliation performance and long life cycle at different current densities with low voltage hysteresis.In addition,low polarization,high capacity retention,long cycle life over 1000 cycles at 5 A∙g^(−1) were achieved when CuZn@C NSs were used as anodes for CuZn@C/V_(2)O_(5)full cells.展开更多
Composites composed of a carbon matrix decorated with a metal or metal oxide derived from zeolitic imidazolate frameworks(ZIFs)have been widely applied as suitable electromagnetic wave absorbers due to their high poro...Composites composed of a carbon matrix decorated with a metal or metal oxide derived from zeolitic imidazolate frameworks(ZIFs)have been widely applied as suitable electromagnetic wave absorbers due to their high porosity and controllable morphology.However,achieving ideal absorption performance remains a challenge owing to the inadequate conductivity and high density of the metal components.Therefore,a temperature-controlling treatment was employed for the bimetal ZIFs,and the corresponding derivatives exhibited an excellent dissipation ability with a minimum reflection loss value of−54.3 dB and an effective bandwidth of 7.0 GHz at a thickness of 2.4 mm,which resulted from the strong dipole polarization behavior.Furthermore,after successfully controlling the Zn/Co ratio,the attenuation capability was greatly enhanced at a thickness of 1.4 mm,with bandwidths of 13.0–18.0 GHz.Overall,this work provides an ameliorated strategy for microwave absorption performance of carbon-based materials.展开更多
基金Financial supports from the National Natural Science Foundation of China (51575030, 51532002 and 51872027)Beijing Natural Science Foundation (L172023)National Basic Research Program of China (2017YFE0113500)。
文摘The solid-state lithium battery is considered as an ideal next-generation energy storage device owing to its high safety,high energy density and low cost.However,the poor ionic conductivity of solid electrolyte and low interfacial stability has hindered the application of solid-state lithium battery.Here,a flexible polymer/garnet solid electrolyte is prepared with poly(ethylene oxide),poly(vinylidene fluoride),Li6.75La3 Zr1.75Ta0.25O12,lithium bis(trifluoromethanesulfonyl)imide and oxalate,which exhibits an ionic conductivity of 2.0 ×10^(-4) S cm^(-1) at 55℃,improved mechanical property,wide electrochemical window(4.8 V vs.Li/Li+),enhanced thermal stabilities.Tiny acidic OX was introduced to inhibit the alkalinity reactions between Li6.75La3 Zr1.75Ta0.25O12 and poly(vinylidene fluoride).In order to improve the interfacial stability between cathode and electrolyte,an Al2 O3@LiNi0.5Co0.2Mn0.3O2 based composite cathode framework is also fabricated with poly(ethylene oxide) polymer and lithium salt as additives.The solid-state lithium battery assembled with polymer/garnet solid electrolyte and composite cathode framework demonstrates a high initial discharge capacity of 150.6 mAh g^(-1) and good capacity retention of 86.7% after 80 cycles at 0.2 C and 55℃,which provides a promising choice for achieving the stable electrode/electrolyte interfacial contact in solid-state lithium batteries.
基金support from the National Natural Science Foundation of China(Nos.21773314,21821003 and 21890382)the Guangdong Natural Science Funds for Distinguished Young Scholar(No.2019B151502017)。
文摘Photocatalytic dual-functional reaction under visible light irradiation represents a sustainable development strategy.In detail,H2production coupled with benzylamine oxidation can remarkably lower the cost by replacing sacrificial agents.In this work,Cd S quantum dots(Cd S QDs)were successfully loaded onto the surface of a porphyrinic metal-organic framework(Pd-PCN-222)by the electrostatic selfassembly at room temperature.The consequent Pd-PCN-222/CdS heterojunction composites displayed superb photocatalytic activity under visible light irradiation,achieving a H2production and benzylamine oxidation rate of 5069 and 3717μmol g^(-1)h^(-1)with>99%selectivity in 3 h.There is no noticeable loss of catalytic capability during three successive runs.Mechanistic studies by in situ electron spin resonance and X-ray photoelectron spectroscopy disclosed that CdS QDs injected photoexcited electrons to Pd-PCN-222 and then Zr6clusters under visible-light irradiation,and thus Cd S QDs and Zr6clusters behave as the photocatalytic oxidation and reduction centers,respectively.
基金the support from the National Natural Science Foundation of China (Nos.21773314, 21720102007,21821003 and 21890382)the Guangdong Natural Science Funds for Distinguished Young Scholar (No. 2019B151502017)+3 种基金the Tip-top Youth Talents of Guangdong special support program (No.20173100042150021)Science and Technology Planning Project of Guangzhou (No.201707010168)the General Financial Grant from the China Postdoctoral Science Foundation (No.2019M662809)Local Innovative and Research Teams Project of Guangdong Peal River Talents Program (No.2017BT01C161)。
文摘Reliable technologies for CO_(2) capture and conversion(C3) are of vital importance for the establishment of a sustainable society.Metal-organic framework(MOF) composites have shown their compelling potentials for C3 due to the plentiful reticular chemistry of MOF structures and the synergistic catalysis between MOFs and the functional vips.This review focuses on the syntheses and catalytic applications towards C3 of MOF composites,which is divided into three sections.The first section gives a brief introduction about synthetic strategies of MOF composites.The second section discusses the recent progress of MOF composites in C3,including CO_(2) chemical fixation,hydrogenation,photoreduction,electro reduction and photoelectro reduction.The third section summarizes the challenges and future prospects of MOF composites for C3.We hope that this review cannot only provide an inspiration for the rational design of MOF composites for C3,but also stimulate more and more research works in this emerging area.
基金Supported by the National Key Basic Research Program of China(2013CB733503)the National Natural Science Foundation of China(21136001,21276009 and 21322603)the Program for New Century Excellent Talents in University(NCET-12-0755)
文摘A computational study was firstly performed in this work to examine the applicability of an acid-functionalized metal-organic framework(MOF), Ui O-66(Zr)-(COOH)2, in membrane-based H2S/CH4 separation. The results show that this MOF could be potentially interesting when being used as the pure membrane material for the separation of the mixture with low H2 S concentration. Further, the performance of 10 different mixed matrix membranes(MMMs) on the basis of the MOF was predicted by combing the molecular simulation data and the Maxwell permeation model. The results indicate that using this MOF as filler particles in MMMs can signi ficantly enhance the permeation performance of pure polymers. The findings obtained in this work may be helpful in facilitating the application of this promising MOF for practical desulfurization process of fuel gas.
基金the National Natural Science Foundation of China(Nos.NSFC-U1904215,21805192,and 12102422)the Natural Science Foundation of Jiangsu Province(No.BK20200044)+2 种基金the Top-notch Academic Programs Project(TAPP)of Jiangsu Higher Education Institutions,and the Program for Young Changjiang Scholars of the Ministry of Education,China(No.Q2018270)We also acknowledge the Priority Academic Program Development of Jiangsu Higher Education Institutions.Y.Y.L.acknowledges the Guangdong Basic and Applied Basic Research Foundation(No.2019A1515110735)the Natural Science Research Project of Anhui Educational Committee for Excellent Young Scholars(No.2022AH030152).
文摘Uncontrollable dendrite growth and side reactions resulting in short operating life and low Coulombic efficiency have severely hindered the further development of aqueous zinc-ion batteries(AZIBs).In this work,we designed to grow zeolitic imidazolate framework-8(ZIF-8)uniformly on CuO nanosheets(NSs)and prepared carbon-coated CuZn alloy NSs(CuZn@C NSs)by calcination under H_(2)/Ar atmosphere.As reflected by extended X-ray absorption fine structure(EXAFS),density functional theory(DFT),in-situ Raman,the Cu–Zn and Zn–N bonds present in CuZn@C NSs act as zincophilic sites to uniformly absorb Zn ions and inhibit the formation of Zn dendrites.At the same time,CuZn@C NSs hinder the direct contact between zinc anode and electrolyte,preventing the occurrence of side reactions.More impressively,the symmetric cells constructed with CuZn@C NSs anodes exhibited excellent zinc plating/exfoliation performance and long life cycle at different current densities with low voltage hysteresis.In addition,low polarization,high capacity retention,long cycle life over 1000 cycles at 5 A∙g^(−1) were achieved when CuZn@C NSs were used as anodes for CuZn@C/V_(2)O_(5)full cells.
基金The authors are thankful for the financial supports of the Science Foundation for The Excellent Youth Scholars of Henan Province(No.212300410089)the Foundation for University Youth Key Teachers of Henan Province(No.2020GGJS170)the Support Program for Scientific and Technological Innovation Talents of Higher Education in Henan Province(No.21HASTIT004).
文摘Composites composed of a carbon matrix decorated with a metal or metal oxide derived from zeolitic imidazolate frameworks(ZIFs)have been widely applied as suitable electromagnetic wave absorbers due to their high porosity and controllable morphology.However,achieving ideal absorption performance remains a challenge owing to the inadequate conductivity and high density of the metal components.Therefore,a temperature-controlling treatment was employed for the bimetal ZIFs,and the corresponding derivatives exhibited an excellent dissipation ability with a minimum reflection loss value of−54.3 dB and an effective bandwidth of 7.0 GHz at a thickness of 2.4 mm,which resulted from the strong dipole polarization behavior.Furthermore,after successfully controlling the Zn/Co ratio,the attenuation capability was greatly enhanced at a thickness of 1.4 mm,with bandwidths of 13.0–18.0 GHz.Overall,this work provides an ameliorated strategy for microwave absorption performance of carbon-based materials.
