Solid polymer electrolytes(SPEs)have become increasingly important in advanced lithium-ion batteries(LIBs)due to their improved safety and mechanical properties compared to organic liquid electrolytes.Cross-linked pol...Solid polymer electrolytes(SPEs)have become increasingly important in advanced lithium-ion batteries(LIBs)due to their improved safety and mechanical properties compared to organic liquid electrolytes.Cross-linked polymers have the potential to further improve the mechanical property without trading off Li-ion conductivity.In this study,focusing on a recently developed cross-linked SPE,i.e.,the one based on poly(vinylene carbonate)-poly(ethylene oxide)cross-linked network(PVCN),we used solid-state nuclear magnetic resonance(NMR)techniques to investigate the fundamental interaction between the chain segments and Li ions,as well as the lithium-ion motion.By utilizing homonuclear/heteronuclear correlation,CP(cross-polarization)kinetics,and spin-lattice relaxation experiments,etc.,we revealed the structural characteristics and their relations to lithium-ion mobilities.It is found that the network formation prevents poly(ethylene oxide)chains from crystallization,which could create sufficient space for segmental tumbling and Li-ion co nductio n.As such,the mechanical property is greatly improved with even higher Li-ion mobilities compared to the poly(vinylene carbonate)or poly(ethylene oxide)based SPE analogues.展开更多
Antimicrobial peptides(AMP)are small proteins that play critical roles in host defense against microbe invasion.Many AMPs disrupt the cellular membrane of microbe,while the mechanism of action of AMPs can be very soph...Antimicrobial peptides(AMP)are small proteins that play critical roles in host defense against microbe invasion.Many AMPs disrupt the cellular membrane of microbe,while the mechanism of action of AMPs can be very sophisticated.Solid-state NMR(SSNMR)technique is powerful in characterizing the mechanism of AMPs in vivo and in vitro.This review summarizes the recent advance of SSNMR technique in AMP mechanisms characterization.We highlight the sample preparation approaches,the SSNMR spectroscopic methods,and a number of outstanding examples of AMP mechanisms elucidated via SSNMR spectroscopy.展开更多
Layered rare earth hydroxides(LREHs)are a novel class of two-dimensional materials with potential applications in various fields.The exchange reactions with organic anions are typically the first step for the function...Layered rare earth hydroxides(LREHs)are a novel class of two-dimensional materials with potential applications in various fields.The exchange reactions with organic anions are typically the first step for the functionalization of LREHs.Although the laminar structures seem to be clear for anion-exchanged compounds,the state of intercalated organic anions and their interactions with cationic rare earth hydroxide layers remain unclear.Herein,we demonstrate that the use of 13C solid-state nuclear magnetic resonance(ssNMR)spectroscopy enables to extract key information on the state of intercalated organic anions such as their local chemical environment,stacking,and dynamics,which are often difficult or impossible to obtain previously.In combination with powder X-ray diffraction and ab initio density functional theory calculations,the intercalation chemistry of two representative layered yttrium hydroxides with selected monovalent organic anions was studied in detail.The products can undergo secondary exchange with a divalent organic anion,depending on the match between the basal spacing of two phases,i.e.,the replacement of benzenesulfonate(BS^(-)),2,4-dimethylbenzene sulfonate(DMBS^(-)),and 4-ethylbenzene sulfonate(EBS)with 2,6-naphthalene disulfonate(NDS^(2-))is allowed due to the insignificant change in basal spacing after exchange,while the replacement of very long dodecyl benzene sulfonate(DBS^(-))and dodecyl sulfate(DS)with NDS^(2-)is forbidden.The results therefore provide valuable insights into the structure-property relationships of LREH-based functional materials.展开更多
Solid electrolytes have received widespread attention due to their higher safety than liquid electrolytes in the past decades.In particular,organic-inorganic composite solid electro-lytes(CSEs)in which inorganic fller...Solid electrolytes have received widespread attention due to their higher safety than liquid electrolytes in the past decades.In particular,organic-inorganic composite solid electro-lytes(CSEs)in which inorganic fllers dispersed in polymer solid electrolytes are consid-ered to be one of the most promising candidate electrolytes for high-performance solid-state lithium batteries.Understanding the local environments and the conduction pathway/dynamics of Lit is essential for the design of high-performance CSEs.Nuclear magnetic resonance(NMR)is a non-invasive quantitative technique that has unique ca-pabilities in providing molecular structure information,morphological evolution,and measuring the movement of ions at different time scales.Therefore,for battery re-searchers,an accurate and comprehensive under standing of the basic principles and experimental design of solid-state NMR(SSNMR)is of great significance for investigating the abundant molecular structure and dynamics information in CSEs.The specific appli-cations of the SSNMR technique in CSEs are briefly introduced in this present review.展开更多
Bone is a hierarchical architecture that consists of both inorganic and organic components.The organic components,including collagen and numerous non-collagenous biomolecules,are crucial for maintaining the mechanical...Bone is a hierarchical architecture that consists of both inorganic and organic components.The organic components,including collagen and numerous non-collagenous biomolecules,are crucial for maintaining the mechanical strength and physiological functions of bone.The native structures of organic components and especially the mutual interactions between different components are important questions to be addressed.Among different analytical techniques,solid-state nuclear magnetic resonance(SSNMR)spectroscopy is a powerful tool to reveal the chemical and interactional information at an atomic level.Recent advancements of SSNMR technology and experimental protocols have brought great advances in understanding the molecular details in native bones.In this review,we summarize the progresses on the SSNMR studies of various organic components in the bone matrix.In the first part,we review the studies on collagen from four different aspects:(1)waterassociated molecular dynamics;(2)the intrahelical/interhelical interactions in collagen residues;(3)the interactions between collagen and citrate;and(4)the cross-linking between collagen and inorganic surface.In the second part,we review the studies on the non-protein biomolecules including sugar species,citrate,lipids,and nucleic acids.In the end,we propose an outlook of future directions for SSNMR investigations on bones.展开更多
基金financially supported by the National Natural Science Foundation of China(Grant No.22325405,22321002,22279153)Liaoning Revitalization Talents Program(XLYC1807207,XLYC2203134)DICP I202104。
文摘Solid polymer electrolytes(SPEs)have become increasingly important in advanced lithium-ion batteries(LIBs)due to their improved safety and mechanical properties compared to organic liquid electrolytes.Cross-linked polymers have the potential to further improve the mechanical property without trading off Li-ion conductivity.In this study,focusing on a recently developed cross-linked SPE,i.e.,the one based on poly(vinylene carbonate)-poly(ethylene oxide)cross-linked network(PVCN),we used solid-state nuclear magnetic resonance(NMR)techniques to investigate the fundamental interaction between the chain segments and Li ions,as well as the lithium-ion motion.By utilizing homonuclear/heteronuclear correlation,CP(cross-polarization)kinetics,and spin-lattice relaxation experiments,etc.,we revealed the structural characteristics and their relations to lithium-ion mobilities.It is found that the network formation prevents poly(ethylene oxide)chains from crystallization,which could create sufficient space for segmental tumbling and Li-ion co nductio n.As such,the mechanical property is greatly improved with even higher Li-ion mobilities compared to the poly(vinylene carbonate)or poly(ethylene oxide)based SPE analogues.
基金a research grant from the Natural Science and Engineering Research Council of Canadaan equipment grant from the Canada Foundation for Innovationfunding from the Canada Research Chair pro-gram
基金supported by the National Key Research and Development Program of the Ministry of Science and Technology,People's Republic of China(contract number 2016YFA0501203)the National Natural Science Foundation of China(21874004,31470727)the Interdisciplinary Medicine Seed Fund of Peking University,and the Fundamental Research Funds for the Central University.
文摘Antimicrobial peptides(AMP)are small proteins that play critical roles in host defense against microbe invasion.Many AMPs disrupt the cellular membrane of microbe,while the mechanism of action of AMPs can be very sophisticated.Solid-state NMR(SSNMR)technique is powerful in characterizing the mechanism of AMPs in vivo and in vitro.This review summarizes the recent advance of SSNMR technique in AMP mechanisms characterization.We highlight the sample preparation approaches,the SSNMR spectroscopic methods,and a number of outstanding examples of AMP mechanisms elucidated via SSNMR spectroscopy.
基金supported by the National Natural Science Foundation of China(grant no.21904071 and 22071115)the Open Funds(T151904)the State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics of China.
文摘Layered rare earth hydroxides(LREHs)are a novel class of two-dimensional materials with potential applications in various fields.The exchange reactions with organic anions are typically the first step for the functionalization of LREHs.Although the laminar structures seem to be clear for anion-exchanged compounds,the state of intercalated organic anions and their interactions with cationic rare earth hydroxide layers remain unclear.Herein,we demonstrate that the use of 13C solid-state nuclear magnetic resonance(ssNMR)spectroscopy enables to extract key information on the state of intercalated organic anions such as their local chemical environment,stacking,and dynamics,which are often difficult or impossible to obtain previously.In combination with powder X-ray diffraction and ab initio density functional theory calculations,the intercalation chemistry of two representative layered yttrium hydroxides with selected monovalent organic anions was studied in detail.The products can undergo secondary exchange with a divalent organic anion,depending on the match between the basal spacing of two phases,i.e.,the replacement of benzenesulfonate(BS^(-)),2,4-dimethylbenzene sulfonate(DMBS^(-)),and 4-ethylbenzene sulfonate(EBS)with 2,6-naphthalene disulfonate(NDS^(2-))is allowed due to the insignificant change in basal spacing after exchange,while the replacement of very long dodecyl benzene sulfonate(DBS^(-))and dodecyl sulfate(DS)with NDS^(2-)is forbidden.The results therefore provide valuable insights into the structure-property relationships of LREH-based functional materials.
基金This work was supported by the National Natural Science Foundation of China(Grant No.22075064,No.21673065,No.21611130177).
文摘Solid electrolytes have received widespread attention due to their higher safety than liquid electrolytes in the past decades.In particular,organic-inorganic composite solid electro-lytes(CSEs)in which inorganic fllers dispersed in polymer solid electrolytes are consid-ered to be one of the most promising candidate electrolytes for high-performance solid-state lithium batteries.Understanding the local environments and the conduction pathway/dynamics of Lit is essential for the design of high-performance CSEs.Nuclear magnetic resonance(NMR)is a non-invasive quantitative technique that has unique ca-pabilities in providing molecular structure information,morphological evolution,and measuring the movement of ions at different time scales.Therefore,for battery re-searchers,an accurate and comprehensive under standing of the basic principles and experimental design of solid-state NMR(SSNMR)is of great significance for investigating the abundant molecular structure and dynamics information in CSEs.The specific appli-cations of the SSNMR technique in CSEs are briefly introduced in this present review.
基金supported by the National Natural Science Foundation of China(Nos.21922410,22072133,and 22275159)Zhejiang Provincial Natural Science Foundation(No.LR19B050001)Zhejiang Provincial Natural Science Foundation(No.LQ20H170002).
文摘Bone is a hierarchical architecture that consists of both inorganic and organic components.The organic components,including collagen and numerous non-collagenous biomolecules,are crucial for maintaining the mechanical strength and physiological functions of bone.The native structures of organic components and especially the mutual interactions between different components are important questions to be addressed.Among different analytical techniques,solid-state nuclear magnetic resonance(SSNMR)spectroscopy is a powerful tool to reveal the chemical and interactional information at an atomic level.Recent advancements of SSNMR technology and experimental protocols have brought great advances in understanding the molecular details in native bones.In this review,we summarize the progresses on the SSNMR studies of various organic components in the bone matrix.In the first part,we review the studies on collagen from four different aspects:(1)waterassociated molecular dynamics;(2)the intrahelical/interhelical interactions in collagen residues;(3)the interactions between collagen and citrate;and(4)the cross-linking between collagen and inorganic surface.In the second part,we review the studies on the non-protein biomolecules including sugar species,citrate,lipids,and nucleic acids.In the end,we propose an outlook of future directions for SSNMR investigations on bones.
