目的研究正常成年人水平特异性CE-Chirp(level specific CE-Chirp,CE-Chirp LS)刺激声与Click刺激声诱发听性脑干反应(auditory brainstem response,ABR)反应阈与纯音听阈的关系及在不同声强下两种刺激声所诱发的ABR波形特点,探讨CE-Chi...目的研究正常成年人水平特异性CE-Chirp(level specific CE-Chirp,CE-Chirp LS)刺激声与Click刺激声诱发听性脑干反应(auditory brainstem response,ABR)反应阈与纯音听阈的关系及在不同声强下两种刺激声所诱发的ABR波形特点,探讨CE-Chirp LS声诱发的ABR在听觉功能客观评估中的应用价值。方法选择正常成年人21例(共42耳)分别在0.5、1.0、2.0、4.0 kHz进行纯音气导听阈测试,获取其双耳各频率的纯音听阈,分别采用CEChirp LS刺激声与Click刺激声诱发ABR,测量2种刺激声在80、60、40 dB nHL的Ⅴ波波幅,获得2种刺激声下受试者的Ⅴ波反应阈,获取其在80 dB nHL刺激强度时Ⅰ、Ⅲ、Ⅴ波潜伏期。按照自身对照的方法对相同刺激强度下2种刺激声诱发的ABR潜伏期及波幅差异性进行统计分析,比较2种刺激声下Ⅴ波反应阈与纯音听阈差值。结果正常成年人80、60、40 dB nHL刺激强度下,CE-Chirp LS刺激声诱发的ABR的Ⅴ波波幅均大于Click刺激声,差异有统计学意义(P<0.001);CE-Chirp LS刺激声诱发的ABR的V波反应阈与纯音平均听阈差值均低于Click刺激声,差异有统计学意义(P<0.05);80 dB nHL声强下CE-Chirp LS刺激声Ⅰ波潜伏期长于Click刺激声,差异有统计学意义(P<0.001),CE-Chirp LS刺激声Ⅲ、Ⅴ波潜伏期与Click刺激声比较,差异无统计学意义(P>0.05)。结论正常成年人CE-Chirp LS刺激声与Click刺激声比较,无论在高强度还是低强度刺激下波幅均明显增大,Ⅴ波反应阈更接近于纯音听阈,更有利于纯音听阈判定,但潜伏期个体差异更大。展开更多
Fatty acids(FAs),which were initially recognized as energy sources and essential building blocks of biomembranes,serve as the precursors of important signaling molecules.Tracing FA metabolism is essential to understan...Fatty acids(FAs),which were initially recognized as energy sources and essential building blocks of biomembranes,serve as the precursors of important signaling molecules.Tracing FA metabolism is essential to understanding the biochemical activity and role of FAs in physiological and pathological events.Inspired by the advances in click chemistry for protein enrichment,we herein established a click chemistry-based enrichment(CCBE)strategy for tracing the cellular metabolism of eicosapentaenoic acid(EPA,20:5 n-3)in neural cells.Terminal alkyne-labeled EPA(EPAA)used as a surrogate was incubated with N2a,mouse neuroblastoma cells,and alkyne-labeled metabolites(ALMs)were selectively captured by an azide-modified resin via a Cu(I)-catalyzed azide-alkyne cycloaddition reaction for enrichment.After removing unlabeled metabolites,ALMs containing a triazole moiety were cleaved from solid-phase resins and subjected to liquid chromatography mass spectrometry(LC-MS)analysis.The proposed CCBE strategy is highly selective for capturing and enriching alkyne-labeled metabolites from the complicated matrices.In addition,this method can overcome current detection limits by enhancing MS sensitivity of targets,improving the chromatographic separation of sn-position glycerophospholipid regioisomers,facilitating structural characterization of ALMs by a specific MS/MS fragmentation signature,and providing versatile fluorescence detection of ALMs for cellular distribution.This CCBE strategy might be expanded to trace the metabolism of other FAs,small molecules,or drugs.展开更多
As a new type of inorganic ductile semiconductor,silver sulfide(α-Ag_(2)S)has garnered a plethora of interests in recent years due to its promising applications in flexible electronics.However,the lack of detailed de...As a new type of inorganic ductile semiconductor,silver sulfide(α-Ag_(2)S)has garnered a plethora of interests in recent years due to its promising applications in flexible electronics.However,the lack of detailed defect calculations and chemical intuition has largely hindered the optimization of material's performance.In this study,we systematically investigate the defect chemistry of extrinsic doping inα-Ag_(2)S using first-principles calculations.We computationally examine a broad suite of 17 dopants and find that all aliovalent elements have extremely low doping limits(<0.002%)in α-Ag_(2)S,rendering them ineffective in tuning the electron concentrations.In contrast,the isovalent elements Se and Te have relatively high doping limits,being consistent with the experimental observations.While the dopant Se or Te itself does not provide additional electrons,its introduction has a significant impact on the band gap,the band-edge position,and especially the formation energy of Ag interstitials,which effectively improve the electron concentrations by 2–3 orders of magnitudes.The size effects of Se and Te doping are responsible for the more favorable Ag interstitials in Ag_(2)S_(0.875)Se_(0.125) and Ag_(2)S_(0.875)Te_(0.125) with respect to pristine Ag2S.This work serves as a theoretical foundation for the rational design of Ag_(2)S-based functional materials.展开更多
MXenes,the most recent addition to the 2D material family,have attracted significant attention owing to their distinctive characteristics,including high surface area,conductivity,surface characteristics,mechanical str...MXenes,the most recent addition to the 2D material family,have attracted significant attention owing to their distinctive characteristics,including high surface area,conductivity,surface characteristics,mechanical strength,etc.This review begins by presenting MXenes,providing insights into their structural characteristics,synthesis methods,and surface functional groups.The review covers a thorough analysis of MXene surface properties,including surface chemistry and termination group impacts.The properties of MXenes are influenced by their synthesis,which can be fluorine-based or fluorinedependent.Fluorine-based synthesis techniques involve etching with fluorine-based reagents,mainly including HF or LiF/HCl,while fluorine-free methods include electrochemical etching,chemical vapor deposition(CVD),alkaline etching,Lewis acid-based etching,etc.These techniques result in the emergence of functional groups such as-F,-O,-OH,-Cl,etc.on the MXenes surface,depending on the synthesis method used.Properties of MXenes,such as electrical conductivity,electronic properties,catalytic activity,magnetic properties,mechanical strength,and chemical and thermal stability,are examined,and the role of functional groups in determining these properties is explored.The review delves into the diverse applications of MXenes,encompassing supercapacitors,battery materials,hydrogen storage,fuel cells,electromagnetic interference(EMI) shielding,pollutant removal,water purification,flexible electronics,sensors,additive manufacturing,catalysis,biomedical and healthcare fields,etc.Finally,this article outlines the challenges and opportunities in the current and future development of MXenes research,addressing various aspects such as synthesis scalability,etching challenges,and multifunctionality,and exploring novel applications.The review concludes with future prospects and conclusions envisioning the impact of MXenes on future technologies and innovation.展开更多
Discharge plasmas, recognized as unique platforms for investigating the origins of chemical life, have garnered extensive interest for their potential to simulate prebiotic conditions. This paper embarks on a comprehe...Discharge plasmas, recognized as unique platforms for investigating the origins of chemical life, have garnered extensive interest for their potential to simulate prebiotic conditions. This paper embarks on a comprehensive overview of recent advancements in the plasma-enabled synthesis of life’s building blocks, charting the complex environmental parameters believed to have surrounded life’s inception. This discussion elaborates on the fundamental mechanisms of discharge plasmas and their likely role in fostering conditions necessary for the origin of life on early Earth. We consider a variety of chemical reactions facilitated by plasma, specifically the synthesis of vital organic molecules - amino acids, nucleobases, sugars, and lipids. Further, we delve into the impact of plasmas on prebiotic chemical evolution. We expect this review to open new horizons for future investigations in plasma-related prebiotic chemistry that could offer valuable insights for unraveling the mysteries of life's origin.展开更多
Water electrolysis poses a significant challenge for balancing catalytic activity and stability of oxygen evolution reaction(OER)electrocatalysts.In this study,we address this challenge by constructing asymmetric redo...Water electrolysis poses a significant challenge for balancing catalytic activity and stability of oxygen evolution reaction(OER)electrocatalysts.In this study,we address this challenge by constructing asymmetric redox chemistry through elaborate surface OO–Ru–OH and bulk Ru–O–Ni/Fe coordination moieties within single-atom Ru-decorated defective NiFe LDH nanosheets(Ru@d-NiFe LDH)in conjunction with strong metal-support interactions(SMSI).Rigorous spectroscopic characterization and theoretical calculations indicate that single-atom Ru can delocalize the O 2p electrons on the surface and optimize d-electron configurations of metal atoms in bulk through SMSI.The^(18)O isotope labeling experiment based on operando differential electrochemical mass spectrometry(DEMS),chemical probe experiments,and theoretical calculations confirm the encouraged surface lattice oxygen,stabilized bulk lattice oxygen,and enhanced adsorption of oxygen-containing intermediates for bulk metals in Ru@d-NiFe LDH,leading to asymmetric redox chemistry for OER.The Ru@d-NiFe LDH electrocatalyst exhibits exceptional performance with an overpotential of 230 mV to achieve 10 mA cm^(−2)and maintains high robustness under industrial current density.This approach for achieving asymmetric redox chemistry through SMSI presents a new avenue for developing high-performance electrocatalysts and instills confidence in its industrial applicability.展开更多
Since the D-band center theory was proposed,it has been widely used in the fields of surface chemistry by almost all researchers,due to its easy understanding,convenient operation and relative accuracy.However,with th...Since the D-band center theory was proposed,it has been widely used in the fields of surface chemistry by almost all researchers,due to its easy understanding,convenient operation and relative accuracy.However,with the continuous development of material systems and modification strategies,researchers have gradually found that D-band center theory is usually effective for large metal particle systems,but for small metal particle systems or semiconductors,such as single atom systems,the opposite conclusion to the D-band center theory is often obtained.To solve the issue above,here we propose a bonding and anti-bonding orbitals stable electron intensity difference(BASED)theory for surface chemistry.The newly-proposed BASED theory can not only successfully explain the abnormal phenomena of D-band center theory,but also exhibits a higher accuracy for prediction of adsorption energy and bond length of intermediates on active sites.Importantly,a new phenomenon of the spin transition state in the adsorption process is observed based on the BASED theory,where the active center atom usually yields an unstable high spin transition state to enhance its adsorption capability in the adsorption process of intermediates when their distance is about 2.5Å.In short,the BASED theory can be considered as a general principle to understand catalytic mechanism of intermediates on surfaces.展开更多
Physical chemistry experiments are an important branch of chemical experiments.In view of problems and shortcomings in physical chemistry experiment teaching of food quality and safety major in Chengdu University,the ...Physical chemistry experiments are an important branch of chemical experiments.In view of problems and shortcomings in physical chemistry experiment teaching of food quality and safety major in Chengdu University,the teaching methods of physical chemistry experiment course of food quality and safety major were explored and practiced,aiming to arouse students enthusiasm for experiments and cultivate their ability of independent learning,comprehensive thinking and independent problem solving.展开更多
Rechargeable magnesium batteries(RMBs),as a low-cost,high-safety and high-energy storage technology,have attracted tremendous attention in large-scale energy storage applications.However,the key anode/electrolyte inte...Rechargeable magnesium batteries(RMBs),as a low-cost,high-safety and high-energy storage technology,have attracted tremendous attention in large-scale energy storage applications.However,the key anode/electrolyte interfacial issues,including surface passivation,uneven Mg plating/stripping,and pulverization after cycling still result in a large overpotential,short cycling life,poor power density,and possible safety hazards of cells,severely impeding the commercial development of RMBs.In this review,a concise overview of recently advanced strategies to address these anode/electroyte interfacial issues is systematically classified and summarized.The design of magnesiophilic substrates,construction of artificial SEI layers,and modification of electrolyte are important and effective strategies to improve the uniformity/kinetics of Mg plating/stripping and achieve the stable anode/electrolyte interface.The key opportunities and challenges in this field are advisedly put forward,and the insights into future directions for stabilizing Mg metal anodes and the anode/electrolyte interface are highlighted.This review provides important references fordeveloping the high-performance and high-safety RMBs.展开更多
Integrating ideological and political theories teaching into the whole process of classroom teaching construction is a new requirement for implementing the fundamental task of cultivating people by virtue and playing ...Integrating ideological and political theories teaching into the whole process of classroom teaching construction is a new requirement for implementing the fundamental task of cultivating people by virtue and playing the role of collaborative education.In order to realize the seamless integration of inorganic and analytical chemistry courses and ideological and political education,this paper summarizes the current situation of ideological and political research on inorganic and analytical chemistry courses in three major databases in China(VIP,CNKI and Wanfang),and sorts out the knowledge points,ideological and political elements and educational goals according to the content of the course chapters,to provide a basic guarantee for the ideological and political education construction of the course.展开更多
P2/O3-type Ni/Mn-based layered oxides are promising cathode materials for sodium-ion batteries(SIBs)owing to their high energy density.However,exploring effective ways to enhance the synergy between the P2 and 03 phas...P2/O3-type Ni/Mn-based layered oxides are promising cathode materials for sodium-ion batteries(SIBs)owing to their high energy density.However,exploring effective ways to enhance the synergy between the P2 and 03 phases remains a necessity.Herein,we design a P2/O3-type Na_(0.76)Ni_(0.31)Zn_(0.07)Mn_(0.50)Ti_(0.12)0_(2)(NNZMT)with high chemical/electrochemical stability by enhancing the coupling between the two phases.For the first time,a unique Na*extraction is observed from a Na-rich O3 phase by a Na-poor P2 phase and systematically investigated.This process is facilitated by Zn^(2+)/Ti^(4+)dual doping and calcination condition regulation,allowing a higher Na*content in the P2 phase with larger Na^(+)transport channels and enhancing Na transport kinetics.Because of reduced Na^(+)in the O3 phase,which increases the difficulty of H^(+)/Na^(+) exchange,the hydrostability of the O3 phase in NNZMT is considerably improved.Furthermore,Zn^(2+)/Ti^(4+)presence in NNZMT synergistically regulates oxygen redox chemistry,which effectively suppresses O_(2)/CO_(2) gas release and electrolyte decomposition,and completely inhibits phase transitions above 4.0 V.As a result,NNZMT achieves a high discharge capacity of 144.8 mA h g^(-1) with a median voltage of 3.42 V at 20 mA g^(-1) and exhibits excellent cycling performance with a capacity retention of 77.3% for 1000 cycles at 2000 mA g^(-1).This study provides an effective strategy and new insights into the design of high-performance layered-oxide cathode materials with enhanced structure/interface stability forSIBs.展开更多
Groundwater serves as an important water source for residents in and around mining areas.To achieve scientific planning and efficient utilization of water resources in mining areas,it is essential to figure out the ch...Groundwater serves as an important water source for residents in and around mining areas.To achieve scientific planning and efficient utilization of water resources in mining areas,it is essential to figure out the chemical formation process and the ground water sulfur cycle that transpire after the coal mining activities.Based on studies of hydrochemistry and D,^(18)O-H_(2)O,^(34)S-SO_(4)isotopes,this study applied principal component analysis,ion ratio and other methods in its attempts to reveal the hydrogeochemical action and sulfur cycle in the subsidence area of Pingyu mining area.The study discovered that,in the studied area,precipitation provides the major supply of groundwater and the main water chemistry effects are dominated by oxidation dissolution of sulfide minerals as well as the dissolution of carbonate and silicate rocks.The sulfate in groundwater primarily originates from oxidation and dissolution of sulfide minerals in coal-bearing strata and human activities.The mixed sulfate formed by the oxidation of sulfide minerals and by human activities continuously recharges the groundwater,promoting the dissolution of carbonate rock and silicate rock in the process.展开更多
Ga-doped Li_(7)La_(3)Zr_(2)O_(12)(Ga-LLZO)has long been considered as a promising garnet-type electrolyte candidate for all-solid-state lithium metal batteries(ASSLBs)due to its high room temperature ionic conductivit...Ga-doped Li_(7)La_(3)Zr_(2)O_(12)(Ga-LLZO)has long been considered as a promising garnet-type electrolyte candidate for all-solid-state lithium metal batteries(ASSLBs)due to its high room temperature ionic conductivity.However,the typical synthesis of Ga-LLZO is usually accompanied by the formation of undesired LiGaO_(2) impurity phase that causes severe instability of the electrolyte in contact with molten Li metal during half/full cell assembly.In this study,we show that by simply engineering the defect chemistry of Ga-LLZO,namely,the lithium deficiency level,LiGaO_(2) impurity phase is effectively inhibited in the final synthetic product.Consequently,defect chemistry engineered Ga-LLZO exhibits excellent electrochemical stability against lithium metal,while its high room temperature ionic conductivity(~1.9×10^(-3)S·cm^(-1))is well reserved.The assembled Li/Ga-LLZO/Li symmetric cell has a superior critical current density of 0.9 mA·cm^(-2),and cycles stably for 500 hours at a current density of 0.3 mA·cm^(-2).This research facilitates the potential commercial applications of high performance Ga-LLZO solid electrolytes in ASSLBs.展开更多
A facile "click chemistry" approach to functionalize 2D macromolecules of graphene oxide nanosheets with poly(ethylene glycol) of different molecular weights,polystyrene,palmitic acid and various amino acids...A facile "click chemistry" approach to functionalize 2D macromolecules of graphene oxide nanosheets with poly(ethylene glycol) of different molecular weights,polystyrene,palmitic acid and various amino acids was presented.FTIR,TGA,Raman spectroscopy,XPS,XRD,TEM,AFM and SEM were utilized to characterize the products.High degree of functionalization was achieved on the flat surfaces of graphene oxide,affording polymer-grafted 2D brushes and amino acids-immobilized nanosheets,which show improved solubility in organic solvents.The click chemistry strategy reported herein provides a facile and general method for functionalization of graphene oxide with macromolecules and desired biomolecules.展开更多
文摘目的研究正常成年人水平特异性CE-Chirp(level specific CE-Chirp,CE-Chirp LS)刺激声与Click刺激声诱发听性脑干反应(auditory brainstem response,ABR)反应阈与纯音听阈的关系及在不同声强下两种刺激声所诱发的ABR波形特点,探讨CE-Chirp LS声诱发的ABR在听觉功能客观评估中的应用价值。方法选择正常成年人21例(共42耳)分别在0.5、1.0、2.0、4.0 kHz进行纯音气导听阈测试,获取其双耳各频率的纯音听阈,分别采用CEChirp LS刺激声与Click刺激声诱发ABR,测量2种刺激声在80、60、40 dB nHL的Ⅴ波波幅,获得2种刺激声下受试者的Ⅴ波反应阈,获取其在80 dB nHL刺激强度时Ⅰ、Ⅲ、Ⅴ波潜伏期。按照自身对照的方法对相同刺激强度下2种刺激声诱发的ABR潜伏期及波幅差异性进行统计分析,比较2种刺激声下Ⅴ波反应阈与纯音听阈差值。结果正常成年人80、60、40 dB nHL刺激强度下,CE-Chirp LS刺激声诱发的ABR的Ⅴ波波幅均大于Click刺激声,差异有统计学意义(P<0.001);CE-Chirp LS刺激声诱发的ABR的V波反应阈与纯音平均听阈差值均低于Click刺激声,差异有统计学意义(P<0.05);80 dB nHL声强下CE-Chirp LS刺激声Ⅰ波潜伏期长于Click刺激声,差异有统计学意义(P<0.001),CE-Chirp LS刺激声Ⅲ、Ⅴ波潜伏期与Click刺激声比较,差异无统计学意义(P>0.05)。结论正常成年人CE-Chirp LS刺激声与Click刺激声比较,无论在高强度还是低强度刺激下波幅均明显增大,Ⅴ波反应阈更接近于纯音听阈,更有利于纯音听阈判定,但潜伏期个体差异更大。
基金supported by grants from the Research Committee of the University of Macao,Macao SAR,China(Grant No.:MYRG2022-00020-ICMS)the Science and Technology Development Fund,Macao,China(File Nos.:0074/2021/AFJ and 0052/2022/A1).
文摘Fatty acids(FAs),which were initially recognized as energy sources and essential building blocks of biomembranes,serve as the precursors of important signaling molecules.Tracing FA metabolism is essential to understanding the biochemical activity and role of FAs in physiological and pathological events.Inspired by the advances in click chemistry for protein enrichment,we herein established a click chemistry-based enrichment(CCBE)strategy for tracing the cellular metabolism of eicosapentaenoic acid(EPA,20:5 n-3)in neural cells.Terminal alkyne-labeled EPA(EPAA)used as a surrogate was incubated with N2a,mouse neuroblastoma cells,and alkyne-labeled metabolites(ALMs)were selectively captured by an azide-modified resin via a Cu(I)-catalyzed azide-alkyne cycloaddition reaction for enrichment.After removing unlabeled metabolites,ALMs containing a triazole moiety were cleaved from solid-phase resins and subjected to liquid chromatography mass spectrometry(LC-MS)analysis.The proposed CCBE strategy is highly selective for capturing and enriching alkyne-labeled metabolites from the complicated matrices.In addition,this method can overcome current detection limits by enhancing MS sensitivity of targets,improving the chromatographic separation of sn-position glycerophospholipid regioisomers,facilitating structural characterization of ALMs by a specific MS/MS fragmentation signature,and providing versatile fluorescence detection of ALMs for cellular distribution.This CCBE strategy might be expanded to trace the metabolism of other FAs,small molecules,or drugs.
基金This work was supported by the National Natural Science Foundation of China(No.52372209 and 52232010)the Shanghai Pilot Program for Basic Research-Chinese Academy of Science,Shanghai Branch(JCYJ-SHFY-2022-002)。
文摘As a new type of inorganic ductile semiconductor,silver sulfide(α-Ag_(2)S)has garnered a plethora of interests in recent years due to its promising applications in flexible electronics.However,the lack of detailed defect calculations and chemical intuition has largely hindered the optimization of material's performance.In this study,we systematically investigate the defect chemistry of extrinsic doping inα-Ag_(2)S using first-principles calculations.We computationally examine a broad suite of 17 dopants and find that all aliovalent elements have extremely low doping limits(<0.002%)in α-Ag_(2)S,rendering them ineffective in tuning the electron concentrations.In contrast,the isovalent elements Se and Te have relatively high doping limits,being consistent with the experimental observations.While the dopant Se or Te itself does not provide additional electrons,its introduction has a significant impact on the band gap,the band-edge position,and especially the formation energy of Ag interstitials,which effectively improve the electron concentrations by 2–3 orders of magnitudes.The size effects of Se and Te doping are responsible for the more favorable Ag interstitials in Ag_(2)S_(0.875)Se_(0.125) and Ag_(2)S_(0.875)Te_(0.125) with respect to pristine Ag2S.This work serves as a theoretical foundation for the rational design of Ag_(2)S-based functional materials.
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korean government(MSIT)(NRF-2020R1A6A1A03043435 and 2020R1A2C1099862)supported by the Korea Institute for Advancement of Technology(KIAT)grant funded by the Korean Government(MOTIE)(P0012451,The Competency Development Program for Industry Specialist)。
文摘MXenes,the most recent addition to the 2D material family,have attracted significant attention owing to their distinctive characteristics,including high surface area,conductivity,surface characteristics,mechanical strength,etc.This review begins by presenting MXenes,providing insights into their structural characteristics,synthesis methods,and surface functional groups.The review covers a thorough analysis of MXene surface properties,including surface chemistry and termination group impacts.The properties of MXenes are influenced by their synthesis,which can be fluorine-based or fluorinedependent.Fluorine-based synthesis techniques involve etching with fluorine-based reagents,mainly including HF or LiF/HCl,while fluorine-free methods include electrochemical etching,chemical vapor deposition(CVD),alkaline etching,Lewis acid-based etching,etc.These techniques result in the emergence of functional groups such as-F,-O,-OH,-Cl,etc.on the MXenes surface,depending on the synthesis method used.Properties of MXenes,such as electrical conductivity,electronic properties,catalytic activity,magnetic properties,mechanical strength,and chemical and thermal stability,are examined,and the role of functional groups in determining these properties is explored.The review delves into the diverse applications of MXenes,encompassing supercapacitors,battery materials,hydrogen storage,fuel cells,electromagnetic interference(EMI) shielding,pollutant removal,water purification,flexible electronics,sensors,additive manufacturing,catalysis,biomedical and healthcare fields,etc.Finally,this article outlines the challenges and opportunities in the current and future development of MXenes research,addressing various aspects such as synthesis scalability,etching challenges,and multifunctionality,and exploring novel applications.The review concludes with future prospects and conclusions envisioning the impact of MXenes on future technologies and innovation.
基金National Natural Science Foundation of China General Project(52377160)National Natural Science Foundation of China National Young Talents Project(GYKP010)+1 种基金Shaanxi Provincial Natural Science Program(2023-JC-YB-425)Xi′an Jiaotong University Young Top Talents Program.
文摘Discharge plasmas, recognized as unique platforms for investigating the origins of chemical life, have garnered extensive interest for their potential to simulate prebiotic conditions. This paper embarks on a comprehensive overview of recent advancements in the plasma-enabled synthesis of life’s building blocks, charting the complex environmental parameters believed to have surrounded life’s inception. This discussion elaborates on the fundamental mechanisms of discharge plasmas and their likely role in fostering conditions necessary for the origin of life on early Earth. We consider a variety of chemical reactions facilitated by plasma, specifically the synthesis of vital organic molecules - amino acids, nucleobases, sugars, and lipids. Further, we delve into the impact of plasmas on prebiotic chemical evolution. We expect this review to open new horizons for future investigations in plasma-related prebiotic chemistry that could offer valuable insights for unraveling the mysteries of life's origin.
基金supported by the Guangdong Basic and Applied Basic Research Foundation(2021B1515120072)the Natural Science Foundation of China(22279096 and T2241003)the Fundamental Research Funds for the Central Universities(WUT:2023IVA094).
文摘Water electrolysis poses a significant challenge for balancing catalytic activity and stability of oxygen evolution reaction(OER)electrocatalysts.In this study,we address this challenge by constructing asymmetric redox chemistry through elaborate surface OO–Ru–OH and bulk Ru–O–Ni/Fe coordination moieties within single-atom Ru-decorated defective NiFe LDH nanosheets(Ru@d-NiFe LDH)in conjunction with strong metal-support interactions(SMSI).Rigorous spectroscopic characterization and theoretical calculations indicate that single-atom Ru can delocalize the O 2p electrons on the surface and optimize d-electron configurations of metal atoms in bulk through SMSI.The^(18)O isotope labeling experiment based on operando differential electrochemical mass spectrometry(DEMS),chemical probe experiments,and theoretical calculations confirm the encouraged surface lattice oxygen,stabilized bulk lattice oxygen,and enhanced adsorption of oxygen-containing intermediates for bulk metals in Ru@d-NiFe LDH,leading to asymmetric redox chemistry for OER.The Ru@d-NiFe LDH electrocatalyst exhibits exceptional performance with an overpotential of 230 mV to achieve 10 mA cm^(−2)and maintains high robustness under industrial current density.This approach for achieving asymmetric redox chemistry through SMSI presents a new avenue for developing high-performance electrocatalysts and instills confidence in its industrial applicability.
文摘Since the D-band center theory was proposed,it has been widely used in the fields of surface chemistry by almost all researchers,due to its easy understanding,convenient operation and relative accuracy.However,with the continuous development of material systems and modification strategies,researchers have gradually found that D-band center theory is usually effective for large metal particle systems,but for small metal particle systems or semiconductors,such as single atom systems,the opposite conclusion to the D-band center theory is often obtained.To solve the issue above,here we propose a bonding and anti-bonding orbitals stable electron intensity difference(BASED)theory for surface chemistry.The newly-proposed BASED theory can not only successfully explain the abnormal phenomena of D-band center theory,but also exhibits a higher accuracy for prediction of adsorption energy and bond length of intermediates on active sites.Importantly,a new phenomenon of the spin transition state in the adsorption process is observed based on the BASED theory,where the active center atom usually yields an unstable high spin transition state to enhance its adsorption capability in the adsorption process of intermediates when their distance is about 2.5Å.In short,the BASED theory can be considered as a general principle to understand catalytic mechanism of intermediates on surfaces.
文摘Physical chemistry experiments are an important branch of chemical experiments.In view of problems and shortcomings in physical chemistry experiment teaching of food quality and safety major in Chengdu University,the teaching methods of physical chemistry experiment course of food quality and safety major were explored and practiced,aiming to arouse students enthusiasm for experiments and cultivate their ability of independent learning,comprehensive thinking and independent problem solving.
基金supported by the National Key R&D Program of China(No.2023YFB3809500)the National Natural Science Foundation of China(No.U23A20555,52202211)+3 种基金the Ninth Young Elite Scientists Sponsorship Program by CAST(2023QNRC001)the Chongqing Technology Innovation and Application Development Project(No.CSTB2022TIAD-KPX0028)the Fundamental Research Funds for the Central Universities(2023CDJXY-018)the Venture&Innovation Support Program for Chongqing Overseas Returnees(cx2022119,cx2023087).
文摘Rechargeable magnesium batteries(RMBs),as a low-cost,high-safety and high-energy storage technology,have attracted tremendous attention in large-scale energy storage applications.However,the key anode/electrolyte interfacial issues,including surface passivation,uneven Mg plating/stripping,and pulverization after cycling still result in a large overpotential,short cycling life,poor power density,and possible safety hazards of cells,severely impeding the commercial development of RMBs.In this review,a concise overview of recently advanced strategies to address these anode/electroyte interfacial issues is systematically classified and summarized.The design of magnesiophilic substrates,construction of artificial SEI layers,and modification of electrolyte are important and effective strategies to improve the uniformity/kinetics of Mg plating/stripping and achieve the stable anode/electrolyte interface.The key opportunities and challenges in this field are advisedly put forward,and the insights into future directions for stabilizing Mg metal anodes and the anode/electrolyte interface are highlighted.This review provides important references fordeveloping the high-performance and high-safety RMBs.
基金Supported by 2020 Teaching Reform Research Project of Pingdingshan University(2020-JY05)School-level Ideological and Political Demonstration Course of Pingdingshan University in 2023-Ecological Engineering+1 种基金Science and Technology Research Project of Henan Provincial Department of Science and Technology(212102110189)High-level Talent Start-up Fund Project of Pingdingshan University(PXY-BSQD-202001).
文摘Integrating ideological and political theories teaching into the whole process of classroom teaching construction is a new requirement for implementing the fundamental task of cultivating people by virtue and playing the role of collaborative education.In order to realize the seamless integration of inorganic and analytical chemistry courses and ideological and political education,this paper summarizes the current situation of ideological and political research on inorganic and analytical chemistry courses in three major databases in China(VIP,CNKI and Wanfang),and sorts out the knowledge points,ideological and political elements and educational goals according to the content of the course chapters,to provide a basic guarantee for the ideological and political education construction of the course.
基金supported by the National Natural Science Foundation of China (22169002)the Chongzuo Key Research and Development Program of China (20220603)the Counterpart Aid Project for Discipline Construction from Guangxi University(2023M02)
文摘P2/O3-type Ni/Mn-based layered oxides are promising cathode materials for sodium-ion batteries(SIBs)owing to their high energy density.However,exploring effective ways to enhance the synergy between the P2 and 03 phases remains a necessity.Herein,we design a P2/O3-type Na_(0.76)Ni_(0.31)Zn_(0.07)Mn_(0.50)Ti_(0.12)0_(2)(NNZMT)with high chemical/electrochemical stability by enhancing the coupling between the two phases.For the first time,a unique Na*extraction is observed from a Na-rich O3 phase by a Na-poor P2 phase and systematically investigated.This process is facilitated by Zn^(2+)/Ti^(4+)dual doping and calcination condition regulation,allowing a higher Na*content in the P2 phase with larger Na^(+)transport channels and enhancing Na transport kinetics.Because of reduced Na^(+)in the O3 phase,which increases the difficulty of H^(+)/Na^(+) exchange,the hydrostability of the O3 phase in NNZMT is considerably improved.Furthermore,Zn^(2+)/Ti^(4+)presence in NNZMT synergistically regulates oxygen redox chemistry,which effectively suppresses O_(2)/CO_(2) gas release and electrolyte decomposition,and completely inhibits phase transitions above 4.0 V.As a result,NNZMT achieves a high discharge capacity of 144.8 mA h g^(-1) with a median voltage of 3.42 V at 20 mA g^(-1) and exhibits excellent cycling performance with a capacity retention of 77.3% for 1000 cycles at 2000 mA g^(-1).This study provides an effective strategy and new insights into the design of high-performance layered-oxide cathode materials with enhanced structure/interface stability forSIBs.
基金supported by Geological Research Project of the Construction Management Bureau of the Middle Route of the South to North Water Diversion Project(ZXJ/HN/YW/GC-2020037)。
文摘Groundwater serves as an important water source for residents in and around mining areas.To achieve scientific planning and efficient utilization of water resources in mining areas,it is essential to figure out the chemical formation process and the ground water sulfur cycle that transpire after the coal mining activities.Based on studies of hydrochemistry and D,^(18)O-H_(2)O,^(34)S-SO_(4)isotopes,this study applied principal component analysis,ion ratio and other methods in its attempts to reveal the hydrogeochemical action and sulfur cycle in the subsidence area of Pingyu mining area.The study discovered that,in the studied area,precipitation provides the major supply of groundwater and the main water chemistry effects are dominated by oxidation dissolution of sulfide minerals as well as the dissolution of carbonate and silicate rocks.The sulfate in groundwater primarily originates from oxidation and dissolution of sulfide minerals in coal-bearing strata and human activities.The mixed sulfate formed by the oxidation of sulfide minerals and by human activities continuously recharges the groundwater,promoting the dissolution of carbonate rock and silicate rock in the process.
基金financially supported by the National Natural Science Foundation of China (Grant No.52171221)the National Key Research and Development Program of China (Grant No.2019YFA0704900)。
文摘Ga-doped Li_(7)La_(3)Zr_(2)O_(12)(Ga-LLZO)has long been considered as a promising garnet-type electrolyte candidate for all-solid-state lithium metal batteries(ASSLBs)due to its high room temperature ionic conductivity.However,the typical synthesis of Ga-LLZO is usually accompanied by the formation of undesired LiGaO_(2) impurity phase that causes severe instability of the electrolyte in contact with molten Li metal during half/full cell assembly.In this study,we show that by simply engineering the defect chemistry of Ga-LLZO,namely,the lithium deficiency level,LiGaO_(2) impurity phase is effectively inhibited in the final synthetic product.Consequently,defect chemistry engineered Ga-LLZO exhibits excellent electrochemical stability against lithium metal,while its high room temperature ionic conductivity(~1.9×10^(-3)S·cm^(-1))is well reserved.The assembled Li/Ga-LLZO/Li symmetric cell has a superior critical current density of 0.9 mA·cm^(-2),and cycles stably for 500 hours at a current density of 0.3 mA·cm^(-2).This research facilitates the potential commercial applications of high performance Ga-LLZO solid electrolytes in ASSLBs.
基金financially supported by the National Natural Science Foundation of China (No.50773038,and No.20974093)National Basic Research Program of China (973 Program) (No.2007CB936000)+2 种基金Qianjiang Talent Foundation of Zhejiang Province (2010R10021)the Fundamental Research Funds for the Central Universities (2009QNA4040)the Foundation for the Author of National Excellent Doctoral Dissertation of China (No.200527)
文摘A facile "click chemistry" approach to functionalize 2D macromolecules of graphene oxide nanosheets with poly(ethylene glycol) of different molecular weights,polystyrene,palmitic acid and various amino acids was presented.FTIR,TGA,Raman spectroscopy,XPS,XRD,TEM,AFM and SEM were utilized to characterize the products.High degree of functionalization was achieved on the flat surfaces of graphene oxide,affording polymer-grafted 2D brushes and amino acids-immobilized nanosheets,which show improved solubility in organic solvents.The click chemistry strategy reported herein provides a facile and general method for functionalization of graphene oxide with macromolecules and desired biomolecules.