Li–CO_(2)/O_(2)batteries,a promising energy storage technology,not only provide ultrahigh discharge capacity but also capture CO_(2)and turn it into renewable energy.Their electrochemical reaction pathways'ambigu...Li–CO_(2)/O_(2)batteries,a promising energy storage technology,not only provide ultrahigh discharge capacity but also capture CO_(2)and turn it into renewable energy.Their electrochemical reaction pathways'ambiguity,however,creates a hurdle for their practical application.This study used copper selenide(CuSe)nanosheets as the air cathode medium in an environmental transmission electron microscope to in situ study Li–CO_(2)/O_(2)(mix CO_(2)as well as O_(2)at a volume ratio of 1:1)and Li–O_(2)batteries as well as Li–CO_(2)batteries.Primary discharge reactions take place successively in the Li–CO_(2)/O_(2)–CuSe nanobattery:(I)4Li^(+)+O_(2)+4e^(−)→2Li_(2)O;(II)Li_(2)O+CO_(2)→Li_(2)CO_(3).The charge reaction proceeded via(III)2Li_(2)CO_(3)→4Li^(+)+2CO_(2)+O_(2)+4e^(−).However,Li–O_(2)and Li–CO_(2)nanobatteries showed poor cycling stability,suggesting the difficulty in the direct decomposition of the discharge product.The fluctuations of the Li–CO_(2)/O_(2)battery's electrochemistry were also shown to depend heavily on O_(2).The CuSe‐based Li–CO_(2)/O_(2)battery showed exceptional electrochemical performance.The Li^–CO_(2)/O_(2)battery offered a discharge capacity apex of 15,492 mAh g^(−1) and stable cycling 60 times at 100 mA g^(−1).Our research offers crucial insight into the electrochemical behavior of Li–CO_(2)/O_(2),Li–O_(2),and Li–CO_(2)nanobatteries,which may help the creation of high‐performance Li–CO_(2)/O_(2)batteries for energy storage applications.展开更多
Detection of sulfur-oxidizing bacteria has largely been dependent on targeted gene sequencing technology or traditional cell cultivation, which usually takes from days to months to carry out. This clearly does not mee...Detection of sulfur-oxidizing bacteria has largely been dependent on targeted gene sequencing technology or traditional cell cultivation, which usually takes from days to months to carry out. This clearly does not meet the requirements of analysis for time-sensitive samples and/or complicated environmental samples. Since energy-dispersive X-ray spectrometry(EDS) can be used to simultaneously detect multiple elements in a sample, including sulfur, with minimal sample treatment, this technology was applied to detect sulfur-oxidizing bacteria using their high sulfur content within the cell. This article describes the application of scanning electron microscopy imaging coupled with EDS mapping for quick detection of sulfur oxidizers in contaminated environmental water samples, with minimal sample handling. Scanning electron microscopy imaging revealed the existence of dense granules within the bacterial cells, while EDS identified large amounts of sulfur within them. EDS mapping localized the sulfur to these granules. Subsequent 16S rRNA gene sequencing showed that the bacteria detected in our samples belonged to the genus Chromatium, which are sulfur oxidizers. Thus, EDS mapping made it possible to identify sulfur oxidizers in environmental samples based on localized sulfur within their cells, within a short time(within 24 h of sampling). This technique has wide ranging applications for detection of sulfur bacteria in environmental water samples.展开更多
Reaction dynamics in gases at operating temperatures at the atomic level are the basis of heterogeneous gas-solid catalyst reactions and are crucial to the catalyst function.Supported noble metal nanocatalysts such as...Reaction dynamics in gases at operating temperatures at the atomic level are the basis of heterogeneous gas-solid catalyst reactions and are crucial to the catalyst function.Supported noble metal nanocatalysts such as platinum are of interest in fuel cells and as diesel oxidation catalysts for pollution control,and practical ruthenium nanocatalysts are explored for ammonia synthesis.Graphite and graphitic carbons are of interest as supports for the nanocatalysts.Despite considerable literature on the catalytic processes on graphite and graphitic supports,reaction dynamics of the nanocatalysts on the supports in different reactive gas environments and operating temperatures at the single atom level are not well understood.Here we present real time in-situ observations and analyses of reaction dynamics of Pt in oxidation,and practical Ru nanocatalysts in ammonia synthesis,on graphite and related supports under controlled reaction environments using a novel in-situ environmental(scanning) transmission electron microscope with single atom resolution.By recording snapshots of the reaction dynamics,the behaviour of the catalysts is imaged.The images reveal single metal atoms,clusters of a few atoms on the graphitic supports and the support function.These all play key roles in the mobility,sintering and growth of the catalysts.The experimental findings provide new structural insights into atomic scale reaction dynamics,morphology and stability of the nanocatalysts.展开更多
The oxidation chemistry of two-dimensional transition metal carbide MXenes has brought new research significance to their protection and application.However,the oxidation behavior and degradation mechanism of MXenes,i...The oxidation chemistry of two-dimensional transition metal carbide MXenes has brought new research significance to their protection and application.However,the oxidation behavior and degradation mechanism of MXenes,in particular with time under oxygen conditions at room tem-perature,remain largely unexplored.Here,several experimental and theo-retical techniques are used to determine a very early stage of the oxidation mechanism of HF-etched Ti3C2Tx(a major member of MXenes and Tx=surface functional groups)in an oxygen environment at room temper-ature.Aberration-corrected environmental transmission electron micros-copy coupled with reactive molecular dynamics simulations show that the crystal plane-dependent oxidation rate of Ti3C2Tx and oxide expansion are attributed to differences in the coordination and charge of superficial Ti atoms,and the existence of the channels between neighboring MXene layers on the different crystal planes.The complementary x-ray photoelec-tron spectroscopy and Raman spectroscopy analyses indicate that the ana-tase and a tiny fraction of brookite TiO2 successively precipitate from the amorphous region of oxidized Ti3C2Tx,grow irregularly and transform to rutile TiO2.Our study reveals the early-stage structural evolution of MXenes in the presence of oxygen and facilitates further tailoring of the MXene per-formance employing oxidation strategy.展开更多
Cerebral ischemia activates an endogenous repair program that induces plastic changes in neurons. In this study, we investigated the effects of environmental enrichment on spatial learning and memory as well as on syn...Cerebral ischemia activates an endogenous repair program that induces plastic changes in neurons. In this study, we investigated the effects of environmental enrichment on spatial learning and memory as well as on synaptic remodeling in a mouse model of chronic cerebral ischemia, produced by subjecting adult male C57 BL/6 mice to permanent left middle cerebral artery occlusion. Three days postoperatively, mice were randomly assigned to the environmental enrichment and standard housing groups. Mice in the standard housing group were housed and fed a standard diet. Mice in the environmental enrichment group were housed in a cage with various toys and fed a standard diet. Then, 28 days postoperatively, spatial learning and memory were tested using the Morris water maze. The expression levels of growth-associated protein 43, synaptophysin and postsynaptic density protein 95 in the hippocampus were analyzed by western blot assay. The number of synapses was evaluated by electron microscopy. In the water maze test, mice in the environmental enrichment group had a shorter escape latency, traveled markedly longer distances, spent more time in the correct quadrant(northeast zone), and had a higher frequency of crossings compared with the standard housing group. The expression levels of growth-associated protein 43, synaptophysin and postsynaptic density protein 95 were substantially upregulated in the hippocampus in the environmental enrichment group compared with the standard housing group. Furthermore, electron microscopy revealed that environmental enrichment increased the number of synapses in the hippocampal CA1 region. Collectively, these findings suggest that environmental enrichment ameliorates the spatial learning and memory impairment induced by permanent middle cerebral artery occlusion. Environmental enrichment in mice with cerebral ischemia likely promotes cognitive recovery by inducing plastic changes in synapses.展开更多
The dynamics of oxidation of cobalt nanoparticles were directly revealed by in situ environmental transmission electron microscopy.Firstly,cobalt nanoparticles were oxidized to polycrystalline cobalt monoxide,then to ...The dynamics of oxidation of cobalt nanoparticles were directly revealed by in situ environmental transmission electron microscopy.Firstly,cobalt nanoparticles were oxidized to polycrystalline cobalt monoxide,then to polycrystalline tricobalt tetroxide,in the presence of oxygen with a low partial pressure.Numerous cavities(or voids) were formed during the oxidation,owing to the Kirkendall effect.Analysis of the oxides growth suggested that the oxidation of cobalt nanoparticles followed a parabolic rate law,which was consistent with diffusion-limited kinetics.In situ transmission electron microscopy allowed potential atomic oxidation pathways to be considered.The outward diffusion of cobalt atoms inside the oxide layer controlled the oxidation,and formed the hollow structure.Irradiation by the electron beam,which destroyed the sealing effect of graphite layer coated on the cobalt surface and resulted in fast oxidation rate,played an important role in activating and promoting the oxidations.These findings further our understanding on the microscopic kinetics of metal nanocrystal oxidation and knowledge of energetic electrons promoting oxidation reaction.展开更多
By using environmental scanning electron microscopy, the morphological changes of Vero cells attached to and grown on the microcarrier Cytodex-3 were observed, and their behavior of adhesion, spreading and proliferati...By using environmental scanning electron microscopy, the morphological changes of Vero cells attached to and grown on the microcarrier Cytodex-3 were observed, and their behavior of adhesion, spreading and proliferation was analyzed. The effect of exogenous fibronectin/ laminin on adhesion and spreading of MCC/Vero cell was studied. The images of ESEM showed that expansion of cell growth was directed toward vacancy space. The growth curve and cell concentration change during the whole culture process were obtained from the statistical counting method based on ESEM images and the crystal violet method. The growth rate of Vero cells increases with increasing the concentration of cell inoculation, that is, the specific growth rate increases quickly with increasing the concentration of cell inoculation. When serum concentration in medium #199 ranged from 5% to 10%, experimental results indicated that serum concentration is one of the important factors influencing cell growth, particularly in the cell adhesion and spreading stage.展开更多
Thermal treatment is a general and efficient way to synthesize intermetallic catalysts and may involve complicated physical processes.So far,the mechanisms leading to the size and composition heterogeneity,as well as ...Thermal treatment is a general and efficient way to synthesize intermetallic catalysts and may involve complicated physical processes.So far,the mechanisms leading to the size and composition heterogeneity,as well as the phase segregation behavior in Pt-Co nanoparticles(NPs)are still not well understood.Via in-situ environmental transmission electron microscopy,the formation dynamics and segregation behaviors of Pt-Co alloyed NPs during the thermal treatment were investigated.It is found that Pt-Co NPs on zeolitic imidazolate frameworks-67-derived nanocarbon(NC)are formed consecutively through both particle migration coalescence and the Ostwald ripening process.The existence of Pt NPs is found to affect the movement of Co NPs during their migration.With the help of theoretical calculations,the correlations between the composition and migration of the Pt and Co during the ripening process were uncovered.These complex alloying processes are revealed as key factors leading to the heterogeneity of the synthesized Pt-Co alloyed NPs.Under oxidation environment,the Pt-Co NPs become surface faceted gradually,which can be attributed to the oxygen facilitated relatively higher segregation rate of Co from the(111)surface.This work advances the fundamental understanding of design,synthesis,and durability of the Pt-based nanocatalysts.展开更多
The deep-learning protein structure prediction method AlphaFold2 has garnered enormous attention beyond the realm of structural biology,for its groundbreaking contribution to solving the"protein foiding problem&q...The deep-learning protein structure prediction method AlphaFold2 has garnered enormous attention beyond the realm of structural biology,for its groundbreaking contribution to solving the"protein foiding problem"In this perspective,we explore the connection between protein structure studies and environmental research,delving into the potential for addressing specific environmental challenges.Proteins are promising for environmental applications because of the functional diversity endowed by their structural complexity.However,structural studies on proteins with environmental significance remain scarce.Here,we present the opportunity to study proteins by advancing experimental determination and deep-learning prediction methods.Specifically,the latest progress in environmental research via cryogenic electron microscopy is highlighted.It allows us to determine the structure of protein complexes in their native state within cells at molecular resolution,revealing environmentally-associated structural dynamics.With the remarkable advancements in computational power and experimental resolution,the study of protein structure and dynamics has reached unprecedented depth and accuracy.These advancements will undoubtedly accelerate the establishment of comprehensive environmental protein structural and functional databases.Tremendous opportunities for protein engineering exist to enable innovative solutions for environmental applications,such as the degradation of persistent contaminants,and the recovery of valuable metals as well as rare earth elements.展开更多
Rechargeable lithium-carbon dioxide(Li-CO_(2))batteries have attracted much attention due to their high theoretical energy densities and capture of C0_(2).However,the electrochemical reaction mechanisms of rechargeabl...Rechargeable lithium-carbon dioxide(Li-CO_(2))batteries have attracted much attention due to their high theoretical energy densities and capture of C0_(2).However,the electrochemical reaction mechanisms of rechargeable Lo-CO_(2) batteries,particularly the decomposition mechanisms of the discharge product Li_(2)CO_(3) are still unclear,impeding their practical applications.Exploring electrochemistry of Li_(2)CO_(3) is critical for improving the performance of Li-C0_(2) batteries.Herein,in-situ environmental transmission electron microscopy(ETEM)technique was used to study electrochemistry of Li_(2)CO_(3) in Li-C0_(2) batteries during discharge and charge processes.During discharge,Li_(2)CO_(3) was nucleated and accumulated on the surface of the cathode media such as carbon nanotubes(CNTs)and Ag nanowires(Ag NWs),but it was hard to decompose during charging at room temperature.To promote the decomposition of Li2C03,the charge reactions were conducted at high temperatures,during which Li_(2)CO_(3) was decomposed to lithium with release of gases.Density functional theory(DFT)calculations revealed that the synergistic effect of temperature and biasing facilitates the decomposition of Li_(2)CO_(3).This study not only provides a fundamental understanding to the high temperature Li-C0_(2) nanobatteries,but also offers a valid technique,i.e.,discharging/charging at high temperatures,to improve the cyclability of Li-CO_(2) batteries for energy storage applications.展开更多
Our research introduces a groundbreaking chemical reduction method for synthesizing silver nanoparticles, marking a significant advancement in the field. The nanoparticles were meticulously characterized using various...Our research introduces a groundbreaking chemical reduction method for synthesizing silver nanoparticles, marking a significant advancement in the field. The nanoparticles were meticulously characterized using various techniques, including optical analysis, structural analysis, transmission electron microscopy (TEM), and field-emission scanning electron microscope (FESEM). This thorough process instills confidence in the accuracy of our findings. The results unveiled that the silver nanoparticles had a diameter of less than 20 nm, a finding of great importance. The absorption spectrum decreased in the peak wavelength range (405 - 394 mm) with increasing concentrations of Ag nanoparticles in the range (1 - 5%). The XRD results indicated a cubic crystal structure for silver nanoparticles with the lattice constant (a = 4.0855 Å), and Miller indices were (111), (002), (002), and (113). The simulation on the XRD pattern showed a face center cubic phase with space group Fm-3m, providing valuable insights into the structure of the nanoparticles.展开更多
基金Natural Science Foundation of Hebei Province,Grant/Award Number:F2021203097China Postdoctoral Science Foundation,Grant/Award Numbers:2021M702756,2023T160551National Natural Science Foundation of China,Grant/Award Numbers:51971245,52022088。
文摘Li–CO_(2)/O_(2)batteries,a promising energy storage technology,not only provide ultrahigh discharge capacity but also capture CO_(2)and turn it into renewable energy.Their electrochemical reaction pathways'ambiguity,however,creates a hurdle for their practical application.This study used copper selenide(CuSe)nanosheets as the air cathode medium in an environmental transmission electron microscope to in situ study Li–CO_(2)/O_(2)(mix CO_(2)as well as O_(2)at a volume ratio of 1:1)and Li–O_(2)batteries as well as Li–CO_(2)batteries.Primary discharge reactions take place successively in the Li–CO_(2)/O_(2)–CuSe nanobattery:(I)4Li^(+)+O_(2)+4e^(−)→2Li_(2)O;(II)Li_(2)O+CO_(2)→Li_(2)CO_(3).The charge reaction proceeded via(III)2Li_(2)CO_(3)→4Li^(+)+2CO_(2)+O_(2)+4e^(−).However,Li–O_(2)and Li–CO_(2)nanobatteries showed poor cycling stability,suggesting the difficulty in the direct decomposition of the discharge product.The fluctuations of the Li–CO_(2)/O_(2)battery's electrochemistry were also shown to depend heavily on O_(2).The CuSe‐based Li–CO_(2)/O_(2)battery showed exceptional electrochemical performance.The Li^–CO_(2)/O_(2)battery offered a discharge capacity apex of 15,492 mAh g^(−1) and stable cycling 60 times at 100 mA g^(−1).Our research offers crucial insight into the electrochemical behavior of Li–CO_(2)/O_(2),Li–O_(2),and Li–CO_(2)nanobatteries,which may help the creation of high‐performance Li–CO_(2)/O_(2)batteries for energy storage applications.
基金Supported by the Basic Scientific Fund for National Public Research Institutes of China(Nos.GY02-2011T10,2015P07)the Qingdao Talent Program(No.13-CX-20)+1 种基金the National Natural Science Foundation of China(Nos.31100567,41176061)the National Natural Science Foundation for Creative Groups(No.41521064)
文摘Detection of sulfur-oxidizing bacteria has largely been dependent on targeted gene sequencing technology or traditional cell cultivation, which usually takes from days to months to carry out. This clearly does not meet the requirements of analysis for time-sensitive samples and/or complicated environmental samples. Since energy-dispersive X-ray spectrometry(EDS) can be used to simultaneously detect multiple elements in a sample, including sulfur, with minimal sample treatment, this technology was applied to detect sulfur-oxidizing bacteria using their high sulfur content within the cell. This article describes the application of scanning electron microscopy imaging coupled with EDS mapping for quick detection of sulfur oxidizers in contaminated environmental water samples, with minimal sample handling. Scanning electron microscopy imaging revealed the existence of dense granules within the bacterial cells, while EDS identified large amounts of sulfur within them. EDS mapping localized the sulfur to these granules. Subsequent 16S rRNA gene sequencing showed that the bacteria detected in our samples belonged to the genus Chromatium, which are sulfur oxidizers. Thus, EDS mapping made it possible to identify sulfur oxidizers in environmental samples based on localized sulfur within their cells, within a short time(within 24 h of sampling). This technique has wide ranging applications for detection of sulfur bacteria in environmental water samples.
基金the Engineering and Physical Science Research Council(EPSRC),U.K.for the award of a research grant EP/J0118058/1 and postdoctoral research assistantships(PDRAs) to M.R.W.and R.W.M.from the grant。
文摘Reaction dynamics in gases at operating temperatures at the atomic level are the basis of heterogeneous gas-solid catalyst reactions and are crucial to the catalyst function.Supported noble metal nanocatalysts such as platinum are of interest in fuel cells and as diesel oxidation catalysts for pollution control,and practical ruthenium nanocatalysts are explored for ammonia synthesis.Graphite and graphitic carbons are of interest as supports for the nanocatalysts.Despite considerable literature on the catalytic processes on graphite and graphitic supports,reaction dynamics of the nanocatalysts on the supports in different reactive gas environments and operating temperatures at the single atom level are not well understood.Here we present real time in-situ observations and analyses of reaction dynamics of Pt in oxidation,and practical Ru nanocatalysts in ammonia synthesis,on graphite and related supports under controlled reaction environments using a novel in-situ environmental(scanning) transmission electron microscope with single atom resolution.By recording snapshots of the reaction dynamics,the behaviour of the catalysts is imaged.The images reveal single metal atoms,clusters of a few atoms on the graphitic supports and the support function.These all play key roles in the mobility,sintering and growth of the catalysts.The experimental findings provide new structural insights into atomic scale reaction dynamics,morphology and stability of the nanocatalysts.
基金appreciate the support from the National Natural Science Foundation of China(Grant Nos.52061003,52174368,U20A20274)the Natural Science Foundation of Yunnan Province(Grant No.202301AT070209).
文摘The oxidation chemistry of two-dimensional transition metal carbide MXenes has brought new research significance to their protection and application.However,the oxidation behavior and degradation mechanism of MXenes,in particular with time under oxygen conditions at room tem-perature,remain largely unexplored.Here,several experimental and theo-retical techniques are used to determine a very early stage of the oxidation mechanism of HF-etched Ti3C2Tx(a major member of MXenes and Tx=surface functional groups)in an oxygen environment at room temper-ature.Aberration-corrected environmental transmission electron micros-copy coupled with reactive molecular dynamics simulations show that the crystal plane-dependent oxidation rate of Ti3C2Tx and oxide expansion are attributed to differences in the coordination and charge of superficial Ti atoms,and the existence of the channels between neighboring MXene layers on the different crystal planes.The complementary x-ray photoelec-tron spectroscopy and Raman spectroscopy analyses indicate that the ana-tase and a tiny fraction of brookite TiO2 successively precipitate from the amorphous region of oxidized Ti3C2Tx,grow irregularly and transform to rutile TiO2.Our study reveals the early-stage structural evolution of MXenes in the presence of oxygen and facilitates further tailoring of the MXene per-formance employing oxidation strategy.
基金supported by the National Natural Science Foundation of China,No.81672242(to YW)the Key Construction Projects of Shanghai Health and Family Planning on Weak Discipline,China,No.2015ZB0401(to YW)
文摘Cerebral ischemia activates an endogenous repair program that induces plastic changes in neurons. In this study, we investigated the effects of environmental enrichment on spatial learning and memory as well as on synaptic remodeling in a mouse model of chronic cerebral ischemia, produced by subjecting adult male C57 BL/6 mice to permanent left middle cerebral artery occlusion. Three days postoperatively, mice were randomly assigned to the environmental enrichment and standard housing groups. Mice in the standard housing group were housed and fed a standard diet. Mice in the environmental enrichment group were housed in a cage with various toys and fed a standard diet. Then, 28 days postoperatively, spatial learning and memory were tested using the Morris water maze. The expression levels of growth-associated protein 43, synaptophysin and postsynaptic density protein 95 in the hippocampus were analyzed by western blot assay. The number of synapses was evaluated by electron microscopy. In the water maze test, mice in the environmental enrichment group had a shorter escape latency, traveled markedly longer distances, spent more time in the correct quadrant(northeast zone), and had a higher frequency of crossings compared with the standard housing group. The expression levels of growth-associated protein 43, synaptophysin and postsynaptic density protein 95 were substantially upregulated in the hippocampus in the environmental enrichment group compared with the standard housing group. Furthermore, electron microscopy revealed that environmental enrichment increased the number of synapses in the hippocampal CA1 region. Collectively, these findings suggest that environmental enrichment ameliorates the spatial learning and memory impairment induced by permanent middle cerebral artery occlusion. Environmental enrichment in mice with cerebral ischemia likely promotes cognitive recovery by inducing plastic changes in synapses.
基金supported by the National Natural Science Foundation of China(11227403,11327901,51472215,51222202)the National Basic Research Program of China(2014CB932500,2015CB921004)+1 种基金Cyrus Tang Center for Sensor Materials and Applicationsthe resources of the Center of Electron Microscopy of Zhejiang University(ZJU)
文摘The dynamics of oxidation of cobalt nanoparticles were directly revealed by in situ environmental transmission electron microscopy.Firstly,cobalt nanoparticles were oxidized to polycrystalline cobalt monoxide,then to polycrystalline tricobalt tetroxide,in the presence of oxygen with a low partial pressure.Numerous cavities(or voids) were formed during the oxidation,owing to the Kirkendall effect.Analysis of the oxides growth suggested that the oxidation of cobalt nanoparticles followed a parabolic rate law,which was consistent with diffusion-limited kinetics.In situ transmission electron microscopy allowed potential atomic oxidation pathways to be considered.The outward diffusion of cobalt atoms inside the oxide layer controlled the oxidation,and formed the hollow structure.Irradiation by the electron beam,which destroyed the sealing effect of graphite layer coated on the cobalt surface and resulted in fast oxidation rate,played an important role in activating and promoting the oxidations.These findings further our understanding on the microscopic kinetics of metal nanocrystal oxidation and knowledge of energetic electrons promoting oxidation reaction.
文摘By using environmental scanning electron microscopy, the morphological changes of Vero cells attached to and grown on the microcarrier Cytodex-3 were observed, and their behavior of adhesion, spreading and proliferation was analyzed. The effect of exogenous fibronectin/ laminin on adhesion and spreading of MCC/Vero cell was studied. The images of ESEM showed that expansion of cell growth was directed toward vacancy space. The growth curve and cell concentration change during the whole culture process were obtained from the statistical counting method based on ESEM images and the crystal violet method. The growth rate of Vero cells increases with increasing the concentration of cell inoculation, that is, the specific growth rate increases quickly with increasing the concentration of cell inoculation. When serum concentration in medium #199 ranged from 5% to 10%, experimental results indicated that serum concentration is one of the important factors influencing cell growth, particularly in the cell adhesion and spreading stage.
基金the National Natural Science Foundation of China(Nos.52072345,U21A20328,22103047,and 12174348)the China Postdoctoral Science Foundation(No.2021T140621)+3 种基金the Natural Science Foundation of Henan Province(No.222300420077)Henan Center for Outstanding Overseas Scientists(No.GZS201903)support from Strategic Priority Research Program(B)(No.XDB33030200)of Chinese Academy of Sciencesperformed at the Center for Functional Nanomaterials,which is a US DOE Office of Science Facility,at Brookhaven National Laboratory under Contract No.DESC0012704.
文摘Thermal treatment is a general and efficient way to synthesize intermetallic catalysts and may involve complicated physical processes.So far,the mechanisms leading to the size and composition heterogeneity,as well as the phase segregation behavior in Pt-Co nanoparticles(NPs)are still not well understood.Via in-situ environmental transmission electron microscopy,the formation dynamics and segregation behaviors of Pt-Co alloyed NPs during the thermal treatment were investigated.It is found that Pt-Co NPs on zeolitic imidazolate frameworks-67-derived nanocarbon(NC)are formed consecutively through both particle migration coalescence and the Ostwald ripening process.The existence of Pt NPs is found to affect the movement of Co NPs during their migration.With the help of theoretical calculations,the correlations between the composition and migration of the Pt and Co during the ripening process were uncovered.These complex alloying processes are revealed as key factors leading to the heterogeneity of the synthesized Pt-Co alloyed NPs.Under oxidation environment,the Pt-Co NPs become surface faceted gradually,which can be attributed to the oxygen facilitated relatively higher segregation rate of Co from the(111)surface.This work advances the fundamental understanding of design,synthesis,and durability of the Pt-based nanocatalysts.
基金Financial support from the National Natural Science Foundation of China(Grant Nos.52225001 and 51978485)the State Key Laboratory for Pollution Control(China)is acknowledged.
文摘The deep-learning protein structure prediction method AlphaFold2 has garnered enormous attention beyond the realm of structural biology,for its groundbreaking contribution to solving the"protein foiding problem"In this perspective,we explore the connection between protein structure studies and environmental research,delving into the potential for addressing specific environmental challenges.Proteins are promising for environmental applications because of the functional diversity endowed by their structural complexity.However,structural studies on proteins with environmental significance remain scarce.Here,we present the opportunity to study proteins by advancing experimental determination and deep-learning prediction methods.Specifically,the latest progress in environmental research via cryogenic electron microscopy is highlighted.It allows us to determine the structure of protein complexes in their native state within cells at molecular resolution,revealing environmentally-associated structural dynamics.With the remarkable advancements in computational power and experimental resolution,the study of protein structure and dynamics has reached unprecedented depth and accuracy.These advancements will undoubtedly accelerate the establishment of comprehensive environmental protein structural and functional databases.Tremendous opportunities for protein engineering exist to enable innovative solutions for environmental applications,such as the degradation of persistent contaminants,and the recovery of valuable metals as well as rare earth elements.
基金supported by the the National Natural Science Foundation of China(Nos.52022088,51971245,51772262,21406191,U20A20336,and 21935009)Beijing Natural Science Foundation(No.2202046)+3 种基金Selective funding for provincial postdoctoral research projects(No.B2019003018)Fok Ying-Tong Education Foundation of China(No.171064)Natural Science Foundation of Hebei Province(Nos.B2020203037,and B2018203297)Hunan Innovation Team(No.2018RS3091).
文摘Rechargeable lithium-carbon dioxide(Li-CO_(2))batteries have attracted much attention due to their high theoretical energy densities and capture of C0_(2).However,the electrochemical reaction mechanisms of rechargeable Lo-CO_(2) batteries,particularly the decomposition mechanisms of the discharge product Li_(2)CO_(3) are still unclear,impeding their practical applications.Exploring electrochemistry of Li_(2)CO_(3) is critical for improving the performance of Li-C0_(2) batteries.Herein,in-situ environmental transmission electron microscopy(ETEM)technique was used to study electrochemistry of Li_(2)CO_(3) in Li-C0_(2) batteries during discharge and charge processes.During discharge,Li_(2)CO_(3) was nucleated and accumulated on the surface of the cathode media such as carbon nanotubes(CNTs)and Ag nanowires(Ag NWs),but it was hard to decompose during charging at room temperature.To promote the decomposition of Li2C03,the charge reactions were conducted at high temperatures,during which Li_(2)CO_(3) was decomposed to lithium with release of gases.Density functional theory(DFT)calculations revealed that the synergistic effect of temperature and biasing facilitates the decomposition of Li_(2)CO_(3).This study not only provides a fundamental understanding to the high temperature Li-C0_(2) nanobatteries,but also offers a valid technique,i.e.,discharging/charging at high temperatures,to improve the cyclability of Li-CO_(2) batteries for energy storage applications.
文摘Our research introduces a groundbreaking chemical reduction method for synthesizing silver nanoparticles, marking a significant advancement in the field. The nanoparticles were meticulously characterized using various techniques, including optical analysis, structural analysis, transmission electron microscopy (TEM), and field-emission scanning electron microscope (FESEM). This thorough process instills confidence in the accuracy of our findings. The results unveiled that the silver nanoparticles had a diameter of less than 20 nm, a finding of great importance. The absorption spectrum decreased in the peak wavelength range (405 - 394 mm) with increasing concentrations of Ag nanoparticles in the range (1 - 5%). The XRD results indicated a cubic crystal structure for silver nanoparticles with the lattice constant (a = 4.0855 Å), and Miller indices were (111), (002), (002), and (113). The simulation on the XRD pattern showed a face center cubic phase with space group Fm-3m, providing valuable insights into the structure of the nanoparticles.