Prevention of mechanical and finally electrochemical failures of lithium batteries is a critical aspect to be considered during their design and performance, especially for those with high specific capacities. Interna...Prevention of mechanical and finally electrochemical failures of lithium batteries is a critical aspect to be considered during their design and performance, especially for those with high specific capacities. Internal failure is observed as one of the most serious factors, including loss of electrode materials, structure deformation and dendrite growth. It usually incubates from atomic/molecular level and progressively aggravates along with lithiation. Understanding the internal failure is of great importance for developing solutions of failure prevention and advanced anode materials. In this research, different internal failure processes of anode materials for lithium batteries are discussed. The progress on observation technologies of the anode failure is further summarized in order to understand their mechanisms of internal failure. On top of them, this review aims to summarize innovative methods to investigate the anode failure mechanisms and to gain new insights to develop advanced and stable anodes for lithium batteries.展开更多
In past decades,Ni-based catalytic materials and electrodes have been intensively explored as low-cost hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)catalysts for water splitting.With increasing de...In past decades,Ni-based catalytic materials and electrodes have been intensively explored as low-cost hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)catalysts for water splitting.With increasing demands for Ni worldwide,simplifying the fabrication process,increasing Ni recycling,and reducing waste are tangible sustainability goals.Here,binder-free,heteroatom-free,and recyclable Ni-based bifunctional catalytic electrodes were fabricated via a one-step quick electrodeposition method.Typically,active Ni nanodot(NiND)clusters are electrodeposited on Ni foam(NF)in Ni(NO3)2 acetonitrile solution.After drying in air,NiO/NiND composites are obtained,leading to a binder-free and heteroatom-free NiO/NiNDs@NF catalytic electrode.The electrode shows high efficiency and long-term stability for catalyzing hydrogen and oxygen evolution reactions at low overpotentials(10ηHER= 119 mV and 50ηOER=360 mV)and can promote water catalysis at 1.70 V@ 10mA cm-2.More importantly,the recovery of raw materials(NF and Ni(NO3)2)is quite easy because of the solubility of NiO/NiNDs composites in acid solution for recycling the electrodes.Additionally,a large-sized(S^70 cm2)NiO/NiNDs@NF catalytic electrode with high durability has also been constructed.This method provides a simple and fast technology to construct high-performance,low-cost,and environmentally friendly Ni-based bifunctional electrocatalytic electrodes for water splitting.展开更多
Photothermal conversion(PTC)nanostructures have great potential for applications in many fields,and therefore,they have attracted tremendous attention.However,the construction of a PTC nanoreactor with multi-compartme...Photothermal conversion(PTC)nanostructures have great potential for applications in many fields,and therefore,they have attracted tremendous attention.However,the construction of a PTC nanoreactor with multi-compartment structure to achieve the combination of unique chemical properties and structural feature is still challenging due to the synthetic difficulties.Herein,we designed and synthesized a catalytically active,PTC gold(Au)@polydopamine(PDA)nanoreactor driven by infrared irradiation using assembled PS-b-P2VP nanosphere as soft template.The particles exhibit multi-compartment structure which is revealed by 3D electron tomography characterization technique.They feature permeable shells with tunable shell thickness.Full kinetics for the reduction reaction of 4-nitrophenol has been investigated using these particles as nanoreactors and compared with other reported systems.Notably,a remarkable acceleration of the catalytic reaction upon near-infrared irradiation is demonstrated,which reveals for the first time the importance of the synergistic effect of photothermal conversion and complex inner structure to the kinetics of the catalytic reduction.The ease of synthesis and fresh insights into catalysis will promote a new platform for novel nanoreactor studies.展开更多
Synchrotron radiation based experimental techniques known as Anomalous Small-Angle X-ray Scattering (ASAXS) provide deep insight into the nanostructure of uncountable material systems in condensed matter research i.e....Synchrotron radiation based experimental techniques known as Anomalous Small-Angle X-ray Scattering (ASAXS) provide deep insight into the nanostructure of uncountable material systems in condensed matter research i.e. solid state physics, chemistry, engineering and life sciences thereby rendering the origin of the macroscopic functionalization of the various materials via correlation to its structural architecture on a nanometer length scale. The techniques constitute a system of linear equations, which can be treated by matrix theory. The study aims to analyze the significance of the solutions of the stated matrix equations by use of the so-called condition numbers first introduced by A. Turing, J. von Neumann and H. Goldstine. Special attention was given for the comparison with direct methods i.e. the Gaussian elimination method. The mathematical roots of ill-posed ASAXS equations preventing matrix inversion have been identified. In the framework of the theory of von Neumann and Goldstine the inversion of certain matrices constituted by ASAXS gradually becomes impossible caused by non-definiteness. In Turing’s theory which starts from more general prerequisites, the principal minors of the same matrices approach singularity thereby imposing large errors on inversion. In conclusion both theories recommend for extremely ill-posed ASAXS problems avoiding inversion and the use of direct methods for instance Gaussian elimination.展开更多
In the last three decades Synchrotron radiation became an indispensable experimental tool for chemical and structural analysis of nano-scaled properties in solid state physics, chemistry, materials science and life sc...In the last three decades Synchrotron radiation became an indispensable experimental tool for chemical and structural analysis of nano-scaled properties in solid state physics, chemistry, materials science and life science thereby rendering the explanation of the macroscopic behavior of the materials and systems under investigation. Especially the techniques known as Anomalous Small-Angle X-ray Scattering provide deep insight into the materials structural architecture according to the different chemical components on lengths scales starting just above the atomic scale (≈1 nm) up to several 100 nm. The techniques sensitivity to the different chemical components makes use of the energy dependence of the atomic scattering factors, which are different for all chemical elements, thereby disentangling the nanostructure of the different chemical components by the signature of the elemental X-ray absorption edges i.e. by employing synchrotron radiation. The paper wants to focus on the application of an algorithm from linear algebra in the field of synchrotron radiation. It provides a closer look to the algebraic prerequisites, which govern the system of linear equations established by these experimental techniques and its solution by solving the eigenvector problem. The pair correlation functions of the so-called basic scattering functions are expressed as a linear combination of eigenvectors.展开更多
Recently, we proposed a new strategy to construct artificial plant protein assemblies, which were induced by adding a small molecule, based on dual supramolecular interactions. In this paper, we further explored this ...Recently, we proposed a new strategy to construct artificial plant protein assemblies, which were induced by adding a small molecule, based on dual supramolecular interactions. In this paper, we further explored this method by employing Human Galectin-1 (Gal-1) as a building block to form self-assembled microribbons. Two non-covalent interactions, including lactose-lectin binding and dimerization of Rhodamine B (RhB), induced by the small molecule ligand addition, were involved in the crosslinking of the animal protein, resulting in the formation of assemblies. By using transmission electron microscopy (TEM), cryo-electron microscopy (cryo-EM), and three-dimensional (3D) tomographic analysis, we arrived at a possible mechanistic model for the microribbon formation. Furthermore, the morphology of protein assemblies could be fine-tuned by varying the incubation time, the protein/ligand ratio, and the chemical structures of ligands. Interestingly, the formation of protein microribbons successfully inhibited Gal-1 induced T-cell agglutination and apoptosis. This is because the multivalent and dynamic interactions in protein assemblies compete with the binding between Gal-1 and the glycans on cell surfaces, which suppresses the function of Gal-1 in promotion of tumor progression and metastasis.展开更多
Fresnel zone plates are the key optical elements for nanoscale focusing of X-ray beams with high spatial resolution. Conventional zone plates manufactured by planar nanotechnology processes are limited by the achievab...Fresnel zone plates are the key optical elements for nanoscale focusing of X-ray beams with high spatial resolution. Conventional zone plates manufactured by planar nanotechnology processes are limited by the achievable aspect ratios of their zone structures. Additionally, ultra-high resolution X-ray optics with high efficiency requires three-dimensional (3-D) shaped tilted zones. The combination of high spatial resolution and high diffraction efficiency is a fundamental problem in X-ray optics. Based on electrodynamical simulations, we find that the optimized zone plate profile for volume diffraction is given by zone structures with radially increasing tilt angles and decreasing zone heights. On-chip stacking permits the realization of such advanced 3-D profiles without significant loss of the maximum theoretical efficiency. We developed triple layer on-chip stacked zone plates with an overlay accuracy of sub-2 nm which fulfills the nanofabrication requirements. Efficiency measurements of on-chip stacked zone plates show significantly increased values compared to conventional zone plates.展开更多
基金the financial support on this research from National Key Research and Development Program of China (2017YFB0403300/2017YFB043305)National Natural Science Foundation of China under Grant No. 51425405+1 种基金Key Program of Chinese Academy of Sciences KFZD-SW-3151000 Talents Program of China (Z.S.)
文摘Prevention of mechanical and finally electrochemical failures of lithium batteries is a critical aspect to be considered during their design and performance, especially for those with high specific capacities. Internal failure is observed as one of the most serious factors, including loss of electrode materials, structure deformation and dendrite growth. It usually incubates from atomic/molecular level and progressively aggravates along with lithiation. Understanding the internal failure is of great importance for developing solutions of failure prevention and advanced anode materials. In this research, different internal failure processes of anode materials for lithium batteries are discussed. The progress on observation technologies of the anode failure is further summarized in order to understand their mechanisms of internal failure. On top of them, this review aims to summarize innovative methods to investigate the anode failure mechanisms and to gain new insights to develop advanced and stable anodes for lithium batteries.
基金the China and Germany Postdoctoral Exchange Program for this research in Helmholtz-Zentrum Berlin für Materialien und Energiethe Postdoctoral Science Foundation of China (2017M610324)NSFC (21704040)
文摘In past decades,Ni-based catalytic materials and electrodes have been intensively explored as low-cost hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)catalysts for water splitting.With increasing demands for Ni worldwide,simplifying the fabrication process,increasing Ni recycling,and reducing waste are tangible sustainability goals.Here,binder-free,heteroatom-free,and recyclable Ni-based bifunctional catalytic electrodes were fabricated via a one-step quick electrodeposition method.Typically,active Ni nanodot(NiND)clusters are electrodeposited on Ni foam(NF)in Ni(NO3)2 acetonitrile solution.After drying in air,NiO/NiND composites are obtained,leading to a binder-free and heteroatom-free NiO/NiNDs@NF catalytic electrode.The electrode shows high efficiency and long-term stability for catalyzing hydrogen and oxygen evolution reactions at low overpotentials(10ηHER= 119 mV and 50ηOER=360 mV)and can promote water catalysis at 1.70 V@ 10mA cm-2.More importantly,the recovery of raw materials(NF and Ni(NO3)2)is quite easy because of the solubility of NiO/NiNDs composites in acid solution for recycling the electrodes.Additionally,a large-sized(S^70 cm2)NiO/NiNDs@NF catalytic electrode with high durability has also been constructed.This method provides a simple and fast technology to construct high-performance,low-cost,and environmentally friendly Ni-based bifunctional electrocatalytic electrodes for water splitting.
基金support from the DFG through SFB 951 Hybrid Inorganic/Organic Systems for OptoElectronics(HIOS)funding by the European Research Council(ERC)Consolidator Grant with Project Number 646659-NANOREACTORthe Joint Lab for Structural Research at the Integrative Research Institute for the Sciences(IRIS Adlershof).
文摘Photothermal conversion(PTC)nanostructures have great potential for applications in many fields,and therefore,they have attracted tremendous attention.However,the construction of a PTC nanoreactor with multi-compartment structure to achieve the combination of unique chemical properties and structural feature is still challenging due to the synthetic difficulties.Herein,we designed and synthesized a catalytically active,PTC gold(Au)@polydopamine(PDA)nanoreactor driven by infrared irradiation using assembled PS-b-P2VP nanosphere as soft template.The particles exhibit multi-compartment structure which is revealed by 3D electron tomography characterization technique.They feature permeable shells with tunable shell thickness.Full kinetics for the reduction reaction of 4-nitrophenol has been investigated using these particles as nanoreactors and compared with other reported systems.Notably,a remarkable acceleration of the catalytic reaction upon near-infrared irradiation is demonstrated,which reveals for the first time the importance of the synergistic effect of photothermal conversion and complex inner structure to the kinetics of the catalytic reduction.The ease of synthesis and fresh insights into catalysis will promote a new platform for novel nanoreactor studies.
文摘Synchrotron radiation based experimental techniques known as Anomalous Small-Angle X-ray Scattering (ASAXS) provide deep insight into the nanostructure of uncountable material systems in condensed matter research i.e. solid state physics, chemistry, engineering and life sciences thereby rendering the origin of the macroscopic functionalization of the various materials via correlation to its structural architecture on a nanometer length scale. The techniques constitute a system of linear equations, which can be treated by matrix theory. The study aims to analyze the significance of the solutions of the stated matrix equations by use of the so-called condition numbers first introduced by A. Turing, J. von Neumann and H. Goldstine. Special attention was given for the comparison with direct methods i.e. the Gaussian elimination method. The mathematical roots of ill-posed ASAXS equations preventing matrix inversion have been identified. In the framework of the theory of von Neumann and Goldstine the inversion of certain matrices constituted by ASAXS gradually becomes impossible caused by non-definiteness. In Turing’s theory which starts from more general prerequisites, the principal minors of the same matrices approach singularity thereby imposing large errors on inversion. In conclusion both theories recommend for extremely ill-posed ASAXS problems avoiding inversion and the use of direct methods for instance Gaussian elimination.
文摘In the last three decades Synchrotron radiation became an indispensable experimental tool for chemical and structural analysis of nano-scaled properties in solid state physics, chemistry, materials science and life science thereby rendering the explanation of the macroscopic behavior of the materials and systems under investigation. Especially the techniques known as Anomalous Small-Angle X-ray Scattering provide deep insight into the materials structural architecture according to the different chemical components on lengths scales starting just above the atomic scale (≈1 nm) up to several 100 nm. The techniques sensitivity to the different chemical components makes use of the energy dependence of the atomic scattering factors, which are different for all chemical elements, thereby disentangling the nanostructure of the different chemical components by the signature of the elemental X-ray absorption edges i.e. by employing synchrotron radiation. The paper wants to focus on the application of an algorithm from linear algebra in the field of synchrotron radiation. It provides a closer look to the algebraic prerequisites, which govern the system of linear equations established by these experimental techniques and its solution by solving the eigenvector problem. The pair correlation functions of the so-called basic scattering functions are expressed as a linear combination of eigenvectors.
基金We acknowledge the financial support from the National Natural Science Foundation of China (Nos. 51721002, 21504016, and 91527305). We thank Joint Lab for Structural Research at the Integrative Research Institute for the Sciences (IRIS Adlershof, Berlin) for Cryo-TEM imaging.
文摘Recently, we proposed a new strategy to construct artificial plant protein assemblies, which were induced by adding a small molecule, based on dual supramolecular interactions. In this paper, we further explored this method by employing Human Galectin-1 (Gal-1) as a building block to form self-assembled microribbons. Two non-covalent interactions, including lactose-lectin binding and dimerization of Rhodamine B (RhB), induced by the small molecule ligand addition, were involved in the crosslinking of the animal protein, resulting in the formation of assemblies. By using transmission electron microscopy (TEM), cryo-electron microscopy (cryo-EM), and three-dimensional (3D) tomographic analysis, we arrived at a possible mechanistic model for the microribbon formation. Furthermore, the morphology of protein assemblies could be fine-tuned by varying the incubation time, the protein/ligand ratio, and the chemical structures of ligands. Interestingly, the formation of protein microribbons successfully inhibited Gal-1 induced T-cell agglutination and apoptosis. This is because the multivalent and dynamic interactions in protein assemblies compete with the binding between Gal-1 and the glycans on cell surfaces, which suppresses the function of Gal-1 in promotion of tumor progression and metastasis.
文摘Fresnel zone plates are the key optical elements for nanoscale focusing of X-ray beams with high spatial resolution. Conventional zone plates manufactured by planar nanotechnology processes are limited by the achievable aspect ratios of their zone structures. Additionally, ultra-high resolution X-ray optics with high efficiency requires three-dimensional (3-D) shaped tilted zones. The combination of high spatial resolution and high diffraction efficiency is a fundamental problem in X-ray optics. Based on electrodynamical simulations, we find that the optimized zone plate profile for volume diffraction is given by zone structures with radially increasing tilt angles and decreasing zone heights. On-chip stacking permits the realization of such advanced 3-D profiles without significant loss of the maximum theoretical efficiency. We developed triple layer on-chip stacked zone plates with an overlay accuracy of sub-2 nm which fulfills the nanofabrication requirements. Efficiency measurements of on-chip stacked zone plates show significantly increased values compared to conventional zone plates.