Direct in vivo conversion of astrocytes into functional new neurons induced by neural transcription factors has been recognized as a potential new therapeutic intervention for neural injury and degenerative disorders....Direct in vivo conversion of astrocytes into functional new neurons induced by neural transcription factors has been recognized as a potential new therapeutic intervention for neural injury and degenerative disorders. However, a few recent studies have claimed that neural transcription factors cannot convert astrocytes into neurons, attributing the converted neurons to pre-existing neurons mis-expressing transgenes. In this study, we overexpressed three distinct neural transcription factors––NeuroD1, Ascl1, and Dlx2––in reactive astrocytes in mouse cortices subjected to stab injury, resulting in a series of significant changes in astrocyte properties. Initially, the three neural transcription factors were exclusively expressed in the nuclei of astrocytes. Over time, however, these astrocytes gradually adopted neuronal morphology, and the neural transcription factors was gradually observed in the nuclei of neuron-like cells instead of astrocytes. Furthermore,we noted that transcription factor-infected astrocytes showed a progressive decrease in the expression of astrocytic markers AQP4(astrocyte endfeet signal), CX43(gap junction signal), and S100β. Importantly, none of these changes could be attributed to transgene leakage into preexisting neurons. Therefore, our findings suggest that neural transcription factors such as NeuroD1, Ascl1, and Dlx2 can effectively convert reactive astrocytes into neurons in the adult mammalian brain.展开更多
The prevalence of intrahepatic cholangiocarcinoma(ICC)is increasing globally.Despite advancements in comprehending this intricate malignancy and formulating novel therapeutic approaches over the past few decades,the p...The prevalence of intrahepatic cholangiocarcinoma(ICC)is increasing globally.Despite advancements in comprehending this intricate malignancy and formulating novel therapeutic approaches over the past few decades,the prognosis for ICC remains poor.Owing to the high degree of malignancy and insidious onset of ICC,numerous cases are detected at intermediate or advanced stages of the disease,hence eliminating the chance for surgical intervention.Moreover,because of the highly invasive characteristics of ICC,recurrence and metastasis postresection are prevalent,leading to a 5-year survival rate of only 20%-35%following surgery.In the past decade,different methods of treatment have been investigated,including transarterial chemoembolization,transarterial radioembolization,radiotherapy,systemic therapy,and combination therapies.For certain patients with advanced ICC,conversion treatment may be utilized to facilitate surgical resection and manage disease progression.This review summarizes the definition of downstaging conversion treatment and presents the clinical experience and evidence concerning conversion treatment for advanced ICC.展开更多
Lithium-sulfur (Li-S) batteries have gained great attention due to the high theoretical energy density and low cost,yet their further commercialization has been obstructed by the notorious shuttle effect and sluggish ...Lithium-sulfur (Li-S) batteries have gained great attention due to the high theoretical energy density and low cost,yet their further commercialization has been obstructed by the notorious shuttle effect and sluggish redox dynamics.Herein,we supply a strategy to optimize the electron structure of Ni_(2)P by concurrently introducing B-doped atoms and P vacancies in Ni_(2)P (Vp-B-Ni_(2)P),thereby enhancing the bidirectional sulfur conversion.The study indicates that the simultaneous introduction of B-doped atoms and P vacancies in Ni_(2)P causes the redistribution of electron around Ni atoms,bringing about the upward shift of d-band center of Ni atoms and effective d-p orbital hybridization between Ni atoms and sulfur species,thus strengthening the chemical anchoring for lithium polysulfides (LiPSs) as well as expediting the bidirectional conversion kinetics of sulfur species.Meanwhile,theoretical calculations reveal that the incorporation of B-doped atoms and P vacancies in Ni_(2)P selectively promotes Li2S dissolution and nucleation processes.Thus,the Li-S batteries with Vp-B-Ni_(2)P-separators present outstanding rate ability of 777 m A h g^(-1)at 5 C and high areal capacity of 8.03 mA h cm^(-2)under E/S of 5μL mg^(-1)and sulfur loading of 7.20 mg cm^(-2).This work elucidates that introducing heteroatom and vacancy in metal phosphide collaboratively regulates the electron structure to accelerate bidirectional sulfur conversion.展开更多
V_(2)O_(5)·nH_(2)O has been widely studied for aqueous zinc-ion batteries.The intercalation of inorganic ions has been used as a feasible method to improve the capacity of vanadium pentoxide.To further improve th...V_(2)O_(5)·nH_(2)O has been widely studied for aqueous zinc-ion batteries.The intercalation of inorganic ions has been used as a feasible method to improve the capacity of vanadium pentoxide.To further improve the stability,organic small molecule choline chloride intercalation is used to expand the spacing of the vanadium pentoxide layers and increase the cycling stability.Therefore,we consider the introduction of Sr^(2+)to cointercalate with choline chloride.Here,we synthes-ized vanadium pentoxide cointercalated with Sr^(2+)and choline ions(Ch^(+))via a simple hydrothermal method.The electro-chemical performance shows an enhanced cathode capacitance contribution of Sr&Ch-V_(2)O_(5),with a discharge capacity of 526 mAh·g^(-1)at 0.1 A·g^(-1)and a retention rate of 78.9%after 2000 cycles at 5 A·g^(-1).This work offers a novel strategy for the design of organic‒inorganic hybrid materials for use as cathodes in aqueous zinc-ion batteries.展开更多
Diamond combines many unique properties,including high stability,strong optical dispersion,excellent mechanical strength,and outstanding thermal conductivity.Its structure,surface groups,and electrical conductivity ar...Diamond combines many unique properties,including high stability,strong optical dispersion,excellent mechanical strength,and outstanding thermal conductivity.Its structure,surface groups,and electrical conductivity are also tunable,increasing its functional versatility.These make diamond and its related materials,such as its composites,highly promising for various applications in energy fields.This review summarizes recent advances and key achievements in energy storage and conversion,covering electrochemical energy storage(e.g.,batteries and supercapacitors),electrocatalytic energy conversion(e.g.,CO_(2)and nitrogen reduction reactions),and solar energy conversion(e.g.,photo-(electro)chemical CO_(2)and nitrogen reduction reactions,and solar cells).Current challenges and prospects related to the synthesis of diamond materials and the technologies for their energy applications are outlined and discussed.展开更多
Methane(CH4),the predominant component of natural gas and shale gas,is regarded as a promising carbon feedstock for chemical synthesis[1].However,considering the extreme stability of CH4 molecules,it's quite chall...Methane(CH4),the predominant component of natural gas and shale gas,is regarded as a promising carbon feedstock for chemical synthesis[1].However,considering the extreme stability of CH4 molecules,it's quite challenging in simultaneously achieving high activity and selectivity for target products under mild conditions,especially when synthesizing high-value C2t chemicals such as ethanol[2].The conversion of methane to ethanol by photocatalysis is promising for achieving transformation under ambient temperature and pressure conditions.Currently,the apparent quantum efficiency(AQE)of solar-driven methane-to-ethanol conversion is generally below 0.5%[3,4].Furthermore,the stability of photocatalysts remains inadequate,offering substantial potential for further improvement.展开更多
Three-dimensional(3D)graphene monoliths are a new carbon material,that has tremendous potential in the fields of energy conversion and storage.They can solve the limitations of two-dimensional(2D)graphene sheets,inclu...Three-dimensional(3D)graphene monoliths are a new carbon material,that has tremendous potential in the fields of energy conversion and storage.They can solve the limitations of two-dimensional(2D)graphene sheets,including interlayer restacking,high contact resistance,and insufficient pore accessibility.By constructing interconnected porous networks,3D graphenes not only retain the intrinsic advantages of 2D graphene sheets,such as high specific surface area,excellent electrical and thermal conductivities,good mechanical properties,and outstanding chemical stability,but also enable efficient mass transport of external fluid species.We summarize the fabrication methods for 3D graphenes,with a particular focus on their applications in energy-related systems.Techniques including chemical reduction assembly,chemical vapor deposition,3D printing,chemical blowing,and zinc-tiered pyrolysis have been developed to change their pore structure and elemental composition,and ways in which they can be integrated with functional components.In terms of energy conversion and storage,they have found broad use in buffering mechanical impacts,suppressing noise,photothermal conversion,electromagnetic shielding and absorption.They have also been used in electrochemical energy systems such as supercapacitors,secondary batteries,and electrocatalysis.By reviewing recent progress in structural design and new applications,we also discuss the problems these materials face,including scalable fabrication and precise pore structure control,and possible new applications.展开更多
Metal nanoparticles with high surface area and high electrochemical activity exhibit excellent catalytic performance in the photocatalytic reduction of carbon dioxide(CO_(2)).However,poor stability,small specific surf...Metal nanoparticles with high surface area and high electrochemical activity exhibit excellent catalytic performance in the photocatalytic reduction of carbon dioxide(CO_(2)).However,poor stability,small specific surface area,and less active sites limits its solar energy utilization.Hydrothermal method was utilized to synthesize the bimetallic material of Cu_(x)Co_(1-x)in this work.Co was loaded onto the Cu surface due to the electrons generated by the surface plasmon resonance(SPR)effect occurring on the Cu surface.Cu_(x)Co_(1-x)exhibits high photocatalytic conversion of CO_(2)efficiency under irradiation,which mainly because the Co nanoparticles on the surface of Cu can be used as cocatalysts to enhance the photocharge transfer.Cu_(0.6)Co_(0.4)exhibits the comparatively best photocatalytic conversion efficiency of CO_(2)in the first 6 h light irradiation.The yields of CO and CH_(4)reached 35.26 and 2.71μmol/(g·h),respectively.Upon illumination,electrons were produced,with the majority of them moving towards the interface.This movement contributes to the increased lifetime of photogenerated electron-hole pairs,which in turn boosts the photocatalytic efficiency.The findings of this research provide significant insights for creating photocatalysts that are both highly effective and stable in CO_(2)reduction processes.展开更多
Carbon materials are a key component in energy storage and conversion devices and their microstructure plays a crucial role in determining device performance.However,traditional carbon materials are unable to meet the...Carbon materials are a key component in energy storage and conversion devices and their microstructure plays a crucial role in determining device performance.However,traditional carbon materials are unable to meet the requirements for applications in emerging fields such as renewable energy and electric vehicles due to limitations including a disordered structure and uncontrolled defects.With an aim of realizing devisable structures,adjustable functions,and performance breakthroughs,superstructured carbons is proposed and represent a category of carbon-based materials,characterized by precisely-built pores,networks,and interfaces.Superstructured carbons can overcome the limitations of traditional carbon materials and improve the performance of energy storage and conversion devices.We review the structure-activity relationships of superstructured carbons and recent research advances from three aspects including a precisely customized pore structure,a dense carbon network framework,and a multi-component highly coupled interface between the different components.Finally,we provide an outlook on the future development of and practical challenges in energy storage and conversion devices.展开更多
Intercalation catalysis research involves inserting metal ions,molecules,or ionic liquids into the layered structure of catalysts to adjust their electronic structure and surface properties,thereby optimizing catalyti...Intercalation catalysis research involves inserting metal ions,molecules,or ionic liquids into the layered structure of catalysts to adjust their electronic structure and surface properties,thereby optimizing catalytic reaction efficiency and selectivity[1–3].This technique has achieved significant progress in areas such as electrocatalysis,catalytic cracking,and energy conversion,especially in reactions like hydrogen generation,oxygen reduction,nitrogen reduction,and carbon dioxide reduction[4–6].Intercalation catalysis can enhance catalyst activity and selectivity,but challenges remain regarding stability,reusability,and industrial application.Future research will focus on developing new intercalation materials,optimizing catalyst design,and exploring their potential applications in complex environments[7].展开更多
The quest for sustainable energy solutions has intensified the search for alternative feedstocks that can supplement or replace fossil fuels. Obtaining fuels or chemicals through the conversion of renewable biomass is...The quest for sustainable energy solutions has intensified the search for alternative feedstocks that can supplement or replace fossil fuels. Obtaining fuels or chemicals through the conversion of renewable biomass is a promising candidate [1,2]. Some noblemetal-based (e.g., Pt, Pd and Rh) catalysts exhibit significant catalytic activity to the conversion reaction of these biomass.展开更多
Direct electrolysis of seawater offers a transformative technology for sustainable hydrogen production,circumventing the constraint of freshwater scarcity.However,the serious electrode corrosion and competitive chlori...Direct electrolysis of seawater offers a transformative technology for sustainable hydrogen production,circumventing the constraint of freshwater scarcity.However,the serious electrode corrosion and competitive chloride oxidation reactions make oxygen evolution reaction(OER)in seawater extremely challenging.Herein,the low-cost and scalable CoFe layered double hydroxides with Cl^(-)intercalation and decorated with Ce(OH)_(3)(named as CoFe-Cl^(-)/Ce(OH)_(3))catalyst is synthesized via rapid electrodeposition under ambient conditions,which is quickly reconstructed into a CeO_(2)decorated and Cl^(-)intercalated CoFeOOH(CoFeOOH-Cl^(-)/CeO_(2))during OER.Theoretical investigation reveals that Cl^(-)intercalation weakens the adsorption ability of Cl^(-)on Co/Fe atoms and hinders unfavorable coupling with chloride,thereby preventing the chlorine corrosion process and enhancing catalytic stability and activity.The CeO_(2)with hard Lewis acidity preferentially binds to OH-with harder Lewis base to ensure the OH-rich microenvironment around catalyst even under high current operating conditions,thus further enhancing stability and improving OER activity.The functionalized CoFe-Cl^(-)/Ce(OH)_(3)delivers 1000 mA cm^(-2)current density at only 329 mV overpotential with excellent stability for 1000 h under alkaline seawater.Electrochemical experiments elucidate the OER catalytic mechanism in which CeO_(2)serves as a co-catalyst for enriching OH-and CoFeOOH-Cl^(-)is the active species.Our work is a substantial step towards achieving massive and sustainable production of hydrogen fuel from immense seawater.展开更多
Two-dimensional(2D)organic-inorganic hybrid perovskites(OIHPs)have been developed as promising candidates for photodetection,owing to their excellent semiconducting features and structural tunability.However,as an imp...Two-dimensional(2D)organic-inorganic hybrid perovskites(OIHPs)have been developed as promising candidates for photodetection,owing to their excellent semiconducting features and structural tunability.However,as an important parameter for photodetection,the photoresponsive range of 2D OIHPs is usually modulated by finite metal-halide combinations,constraining their further development.The emerging aromatic amine-based alternating-cations-interlayered(A-ACI)hybrid perovskites that exhibit excellent charge transport and additional interlayered structural designability,provide an extra solution for achieving ideal photoresponsive range.Herein,for the first time,the photoresponsive range is successfully broadened in A-ACI hybrid perovskites(NMA)_(4)(FA)_(2)Pb_(3)Br_(12)(2)remolding from(NMA)_(4)(MA)_(2)Pb_(3)Br_(12)(1)(NMA=N-methylbenzylaminium,FA=formamidinium and MA=methylammonium).Particularly,1 and 2adopt an unprecedented configuration that NMA and MA/FA are alternately arranged in the interlayer in a 4:2 manner.Importantly,2 exhibits a narrower bandgap than 1,which can be ascribed to the lowlying conduct band composed of intercalation FAπ*orbitals.Meanwhile,2 possesses a shorter interlayer distance and flatter inorganic skeleton,synergistically facilitating the wider photo-absorption range and further endowing a broadening photoresponsive range(70 nm).This research not only enriches the perovskite family but also provides insights into structure-property relationships.展开更多
Quantum dots(QDs)can modulate the solar spectrum through the down-conversion mechanism to better match the spectral response of solar cells.Following previous work,this paper first tested the response of QD solar cell...Quantum dots(QDs)can modulate the solar spectrum through the down-conversion mechanism to better match the spectral response of solar cells.Following previous work,this paper first tested the response of QD solar cells to specific monochromatic light,and found that QDs can effectively improve the photoelectric conversion efficiency(PCE)in the ultraviolet(UV)band by comparison.Then the photoelectric properties of the QD solar cells are tested under the air-mass 1.5(AM1.5)and air-mass 0(AM0)spectra.The experimental results show that because the absorption band of QDs is in the UV region,the space solar cells in the AM0 spectrum can obtain better PCE after coating QDs.The research results show the technical route of space solar cells with down-conversion mechanism,and put forward an important direction for the application of space solar photovoltaic(PV)technology,and have a good application prospect.展开更多
Toluene is widely used as a raw material for many chemical products/pharmaceutical intermediates and as a solvent in many chemical and manufacturing industries.The conversion of toluene into higher value chemicals(ben...Toluene is widely used as a raw material for many chemical products/pharmaceutical intermediates and as a solvent in many chemical and manufacturing industries.The conversion of toluene into higher value chemicals(benzyl alcohol,benzaldehyde,and benzoic acid,etc.)using sunlight is a very promising means.To achieve the full conversion and utilization of toluene,it is necessary to construct photocatalysts with high conversion and selectivity while synergistically optimizing the optimal reaction environment to significantly affect the photo-conversion of toluene.High-performance photocatalysts not only widely absorb sunlight,but also have abundant active sites and generation of free radicals,which can promote the chemical bonds cleavage of toluene,thus greatly increasing the yield of higher-valued products.In addition,the type of photocatalyst and the modification strategy would influence the selectivity of toluene photo-conversion.Therefore,it makes sense that this review presents the reaction mechanism and the influence of reaction factors for the(mainly)photo-oxidation of toluene,a thorough analysis and prediction of the reaction mechanism by theoretical calculations,and the toluene oxidation by different photocatalysts(in particular halogen-containing perovskite materials)to yield specific products,as well as photocatalysts’modifications.Finally,the challenges and prospects for designing efficient photocatalysts and optimizing the toluene oxidation reaction process are summarized.展开更多
Magnesium-ion batteries hold promise as future energy storage solutions,yet current Mg cathodes are challenged by low voltage and specific capacity.Herein,we present an AI-driven workflow for discovering high-performa...Magnesium-ion batteries hold promise as future energy storage solutions,yet current Mg cathodes are challenged by low voltage and specific capacity.Herein,we present an AI-driven workflow for discovering high-performance Mg cathode materials.Utilizing the common characteristics of various ionic intercalation-type electrodes,we design and train a Crystal Graph Convolutional Neural Network model that can accurately predict electrode voltages for various ions with mean absolute errors(MAE)between0.25 and 0.33 V.By deploying the trained model to stable Mg compounds from Materials Project and GNoME AI dataset,we identify 160 high voltage structures out of 15,308 candidates with voltages above3.0 V and volumetric capacity over 800 mA h/cm^(3).We further train a precise NequIP model to facilitate accurate and rapid simulations of Mg ionic conductivity.From the 160 high voltage structures,the machine learning molecular dynamics simulations have selected 23 cathode materials with both high energy density and high ionic conductivity.This Al-driven workflow dramatically boosts the efficiency and precision of material discovery for multivalent ion batteries,paving the way for advanced Mg battery development.展开更多
MnBi_(2)Te_(4),which is emerging as an intrinsic antiferromagnetic(AFM)topological insulator,provides a unique platform to investigate the interplay between magnetism and topology.Modulating its magnetic properties en...MnBi_(2)Te_(4),which is emerging as an intrinsic antiferromagnetic(AFM)topological insulator,provides a unique platform to investigate the interplay between magnetism and topology.Modulating its magnetic properties enables the observation of exotic quantum phenomena such as the quantum anomalous Hall effect,axion insulator states,and Majorana fermions.While the intercalation of Bi_(2)Te_(3)can tune its magnetism,synthesizing pure-phase MnBi_(2)Te_(4)with uniform Bi_(2)Te_(3)intercalation remains challenging,and the fixed interlayer spacing of Bi_(2)Te_(3)limits magnetic coupling tunability.Here,we utilize electrochemical organic molecule intercalation to expand the van der Waals gap of MnBi_(2)Te_(4)and modulate its magnetic properties.Through x-ray diffraction(XRD)characterizations,we confirm that the interlayer spacing of MnBi_(2)Te_(4)is expanded from 13.6°A to 30.5°A and 61.0°A by intercalating quaternary ammonium cations(THA^(+)and CTA^(+)),respectively.The THA-MnBi_(2)Te_(4)exhibits dual complex magnetic behavior,combining AFM ordering with a Neel temperature(T_(N))of 12 K and a small ferromagnetic hysteresis loop at 2 K.The CTA-MnBi_(2)Te_(4)shows robust ferromagnetism,with a Curie point(T_(C))of 15 K,similar to that of the MnBi_(2)Te_(4)monolayer.These results demonstrate that remarkable changes in the magnetic properties of MnBi_(2)Te_(4)can be achieved via electrochemical intercalation,providing new insights into manipulating magnetism in layered magnetic materials.展开更多
The conversion of the greenhouse gas methane to value-added chemicals such as alcohols is a promising technology to mitigate environmental issue and the energy crisis.Especially,the sustainable photocatalytic,electroc...The conversion of the greenhouse gas methane to value-added chemicals such as alcohols is a promising technology to mitigate environmental issue and the energy crisis.Especially,the sustainable photocatalytic,electrocatalytic and photoelectrocatalytic conversion of methane at ambient conditions is regarded as an alternative technology to replace with thermocatalysis.In this review,we summarize recent advances in photocatalytic,electrocatalytic and photoelectrocatalytic conversion of methane into alcohols.We firstly introduce the general principles of photocatalysis,electrocatalysis and photoelectrocatalysis.Then,we discuss the mechanism for selective activation of C-H bond and following oxygenation over metal,inorganic semiconductor,organic semiconductor,and heterojunction composite systems in the photocatalytic,electrocatalytic and photoelectrocatalytic methane oxidation in detail.Later,we present insights into the construction of effective photocatalyst,electrocatalyst and photoelectrocatalyst for methane conversion into alcohols from the perspective of band structures and active sites.Finally,the challenges and outlook for future designs of photocatalytic,electrocatalytic and photoelectrocatalytic methane oxidation systems are also proposed.展开更多
The hydrothermal stability of zeolites is essential for their potential applications in biomass conversion,especially in processes involving elevated temperatures alongside the use or generation of H_(2)O.In this stud...The hydrothermal stability of zeolites is essential for their potential applications in biomass conversion,especially in processes involving elevated temperatures alongside the use or generation of H_(2)O.In this study,we employed F-ions as mineralizers to synthesize hydrothermally stable ZSM-5 zeolites under acidic conditions.The acidic synthesis system promotes zeolites with fewer silanol-terminated lattice defects(ZSM-5(A))compared to the traditional basic conditions(ZSM-5(B)),endowing materials with substantially higher structural integrity and hydrophobicity.After 10 days of autoclave treatment at 200℃ in aqueous phase,H-ZSM-5(A)demonstrated nearly unchanged reaction rates in the dehydration of cyclohexanol,while H-ZSM-5(B)lost>50%of the dehydration activity.Additionally,H-ZSM-5(A)delivered higher initial dehydration rates compared to H-ZSM-5(B).The different measured activation energies further revealed variations in reaction pathways during cyclohexanol dehydration,i.e.,the monomer-or dimer-mediated routes depending on the concentration of alcohol molecule within zeolite pores,providing additional evidence for the strengthened hydrophobic nature of H-ZSM-5(A).Beyond this,the zeolite surface properties and the strength of cyclohexanol-zeolite interactions may impose additional transport/adsorption barriers attributed to multi-phase phenomena on the more polar H-ZSM-5(B)zeolite surfaces.More importantly,the hydrothermal treatment did not induce significant desilication and dealumination in H-ZSM-5(A),thereby preserving its active acid sites and ensuring exceptional hydrothermal stability.The present work fundamentally studies the synthesis of hydrothermally stable zeolites in an acidic medium using fluorides and expands the understanding of polar interactions in catalysis,characterized by the dehydration of cyclohexanol,for future application in biomass conversion.展开更多
Plasma,the fourth state of matter,is characterized by the presence of charged particles,including ions and electrons.It has been shown to induce unique physical and chemical reactions.Recently,there have been increase...Plasma,the fourth state of matter,is characterized by the presence of charged particles,including ions and electrons.It has been shown to induce unique physical and chemical reactions.Recently,there have been increased applications of plasma technology in the field of multiscale functional materials'preparation,with a number of interesting results.This review will begin by introducing the basic knowledge of plasma,including the definition,typical parameters,and classification of plasma setups.Following this,we will provide a comprehensive review and summary of the applications(phase conversion,doping,deposition,etching,exfoliation,and surface treatment)of plasma in common energy conversion and storage systems,such as electrocatalytic conversion of small molecules,batteries,fuel cells,and supercapacitors.This article summarizes the structure-performance relationships of electrochemical energy conversion and storage materials(ECSMs)that have been prepared or modified by plasma.It also provides an overview of the challenges and perspectives of plasma technology,which could lead to a new approach for designing and modifying electrode materials in ECSMs.展开更多
基金supported by the Key Project of Guangzhou City,No.202206060002Science and Technology Project of Guangdong Province,No.2018B030332001Guangdong Provincial Pearl River Project,No.2021ZT09Y552 (all to GC)。
文摘Direct in vivo conversion of astrocytes into functional new neurons induced by neural transcription factors has been recognized as a potential new therapeutic intervention for neural injury and degenerative disorders. However, a few recent studies have claimed that neural transcription factors cannot convert astrocytes into neurons, attributing the converted neurons to pre-existing neurons mis-expressing transgenes. In this study, we overexpressed three distinct neural transcription factors––NeuroD1, Ascl1, and Dlx2––in reactive astrocytes in mouse cortices subjected to stab injury, resulting in a series of significant changes in astrocyte properties. Initially, the three neural transcription factors were exclusively expressed in the nuclei of astrocytes. Over time, however, these astrocytes gradually adopted neuronal morphology, and the neural transcription factors was gradually observed in the nuclei of neuron-like cells instead of astrocytes. Furthermore,we noted that transcription factor-infected astrocytes showed a progressive decrease in the expression of astrocytic markers AQP4(astrocyte endfeet signal), CX43(gap junction signal), and S100β. Importantly, none of these changes could be attributed to transgene leakage into preexisting neurons. Therefore, our findings suggest that neural transcription factors such as NeuroD1, Ascl1, and Dlx2 can effectively convert reactive astrocytes into neurons in the adult mammalian brain.
文摘The prevalence of intrahepatic cholangiocarcinoma(ICC)is increasing globally.Despite advancements in comprehending this intricate malignancy and formulating novel therapeutic approaches over the past few decades,the prognosis for ICC remains poor.Owing to the high degree of malignancy and insidious onset of ICC,numerous cases are detected at intermediate or advanced stages of the disease,hence eliminating the chance for surgical intervention.Moreover,because of the highly invasive characteristics of ICC,recurrence and metastasis postresection are prevalent,leading to a 5-year survival rate of only 20%-35%following surgery.In the past decade,different methods of treatment have been investigated,including transarterial chemoembolization,transarterial radioembolization,radiotherapy,systemic therapy,and combination therapies.For certain patients with advanced ICC,conversion treatment may be utilized to facilitate surgical resection and manage disease progression.This review summarizes the definition of downstaging conversion treatment and presents the clinical experience and evidence concerning conversion treatment for advanced ICC.
基金Institute of Technology Research Fund Program for Young Scholars21C Innovation Laboratory Contemporary Amperex Technology Co.,Limited,Ninde, 352100, China (21C–OP-202314)。
文摘Lithium-sulfur (Li-S) batteries have gained great attention due to the high theoretical energy density and low cost,yet their further commercialization has been obstructed by the notorious shuttle effect and sluggish redox dynamics.Herein,we supply a strategy to optimize the electron structure of Ni_(2)P by concurrently introducing B-doped atoms and P vacancies in Ni_(2)P (Vp-B-Ni_(2)P),thereby enhancing the bidirectional sulfur conversion.The study indicates that the simultaneous introduction of B-doped atoms and P vacancies in Ni_(2)P causes the redistribution of electron around Ni atoms,bringing about the upward shift of d-band center of Ni atoms and effective d-p orbital hybridization between Ni atoms and sulfur species,thus strengthening the chemical anchoring for lithium polysulfides (LiPSs) as well as expediting the bidirectional conversion kinetics of sulfur species.Meanwhile,theoretical calculations reveal that the incorporation of B-doped atoms and P vacancies in Ni_(2)P selectively promotes Li2S dissolution and nucleation processes.Thus,the Li-S batteries with Vp-B-Ni_(2)P-separators present outstanding rate ability of 777 m A h g^(-1)at 5 C and high areal capacity of 8.03 mA h cm^(-2)under E/S of 5μL mg^(-1)and sulfur loading of 7.20 mg cm^(-2).This work elucidates that introducing heteroatom and vacancy in metal phosphide collaboratively regulates the electron structure to accelerate bidirectional sulfur conversion.
文摘V_(2)O_(5)·nH_(2)O has been widely studied for aqueous zinc-ion batteries.The intercalation of inorganic ions has been used as a feasible method to improve the capacity of vanadium pentoxide.To further improve the stability,organic small molecule choline chloride intercalation is used to expand the spacing of the vanadium pentoxide layers and increase the cycling stability.Therefore,we consider the introduction of Sr^(2+)to cointercalate with choline chloride.Here,we synthes-ized vanadium pentoxide cointercalated with Sr^(2+)and choline ions(Ch^(+))via a simple hydrothermal method.The electro-chemical performance shows an enhanced cathode capacitance contribution of Sr&Ch-V_(2)O_(5),with a discharge capacity of 526 mAh·g^(-1)at 0.1 A·g^(-1)and a retention rate of 78.9%after 2000 cycles at 5 A·g^(-1).This work offers a novel strategy for the design of organic‒inorganic hybrid materials for use as cathodes in aqueous zinc-ion batteries.
基金西南大学中央高校基本科研业务费项目(SWU-KT22030)重庆市教育委员会科学技术研究项目(KJQN202300205)Deutsche Forschungsgemeinschaft(DFG,German Research Foundation,457444676).
文摘Diamond combines many unique properties,including high stability,strong optical dispersion,excellent mechanical strength,and outstanding thermal conductivity.Its structure,surface groups,and electrical conductivity are also tunable,increasing its functional versatility.These make diamond and its related materials,such as its composites,highly promising for various applications in energy fields.This review summarizes recent advances and key achievements in energy storage and conversion,covering electrochemical energy storage(e.g.,batteries and supercapacitors),electrocatalytic energy conversion(e.g.,CO_(2)and nitrogen reduction reactions),and solar energy conversion(e.g.,photo-(electro)chemical CO_(2)and nitrogen reduction reactions,and solar cells).Current challenges and prospects related to the synthesis of diamond materials and the technologies for their energy applications are outlined and discussed.
基金the support from the National Natural Science Foundation of China(52202306)Program from Guangdong Introducing Innovative and Entrepreneurial Teams(2019ZT08L101 and RCTDPT-2020-001)+1 种基金Shenzhen Key Laboratory of Eco-materials and Renewable Energy(ZDSYS20200922160400001)the Provincial Talent Plan of Guangdong(2023TB0012).
文摘Methane(CH4),the predominant component of natural gas and shale gas,is regarded as a promising carbon feedstock for chemical synthesis[1].However,considering the extreme stability of CH4 molecules,it's quite challenging in simultaneously achieving high activity and selectivity for target products under mild conditions,especially when synthesizing high-value C2t chemicals such as ethanol[2].The conversion of methane to ethanol by photocatalysis is promising for achieving transformation under ambient temperature and pressure conditions.Currently,the apparent quantum efficiency(AQE)of solar-driven methane-to-ethanol conversion is generally below 0.5%[3,4].Furthermore,the stability of photocatalysts remains inadequate,offering substantial potential for further improvement.
基金supported by National Natural Science Foundation of China(52272039,U23B2075,51972168)Key Research and Development Program in Jiangsu Province(BE2023085)Natural Science Foundation of Jiangsu Province of China(BK20231406)。
文摘Three-dimensional(3D)graphene monoliths are a new carbon material,that has tremendous potential in the fields of energy conversion and storage.They can solve the limitations of two-dimensional(2D)graphene sheets,including interlayer restacking,high contact resistance,and insufficient pore accessibility.By constructing interconnected porous networks,3D graphenes not only retain the intrinsic advantages of 2D graphene sheets,such as high specific surface area,excellent electrical and thermal conductivities,good mechanical properties,and outstanding chemical stability,but also enable efficient mass transport of external fluid species.We summarize the fabrication methods for 3D graphenes,with a particular focus on their applications in energy-related systems.Techniques including chemical reduction assembly,chemical vapor deposition,3D printing,chemical blowing,and zinc-tiered pyrolysis have been developed to change their pore structure and elemental composition,and ways in which they can be integrated with functional components.In terms of energy conversion and storage,they have found broad use in buffering mechanical impacts,suppressing noise,photothermal conversion,electromagnetic shielding and absorption.They have also been used in electrochemical energy systems such as supercapacitors,secondary batteries,and electrocatalysis.By reviewing recent progress in structural design and new applications,we also discuss the problems these materials face,including scalable fabrication and precise pore structure control,and possible new applications.
基金supported by the Doctoral Research Start-up Project of Yuncheng University(YQ-2023067)Project of Shanxi Natural Science Foundation(202303021211189)+2 种基金Fund Program for the Scientific Activities of Selected Returned Overseas Professionals in Shanxi Provinces(20220036)Shanxi Province Intelligent Optoelectronic Sensing Application Technology Innovation CenterShanxi Province Optoelectronic Information Science and Technology Laboratory,Yuncheng University。
文摘Metal nanoparticles with high surface area and high electrochemical activity exhibit excellent catalytic performance in the photocatalytic reduction of carbon dioxide(CO_(2)).However,poor stability,small specific surface area,and less active sites limits its solar energy utilization.Hydrothermal method was utilized to synthesize the bimetallic material of Cu_(x)Co_(1-x)in this work.Co was loaded onto the Cu surface due to the electrons generated by the surface plasmon resonance(SPR)effect occurring on the Cu surface.Cu_(x)Co_(1-x)exhibits high photocatalytic conversion of CO_(2)efficiency under irradiation,which mainly because the Co nanoparticles on the surface of Cu can be used as cocatalysts to enhance the photocharge transfer.Cu_(0.6)Co_(0.4)exhibits the comparatively best photocatalytic conversion efficiency of CO_(2)in the first 6 h light irradiation.The yields of CO and CH_(4)reached 35.26 and 2.71μmol/(g·h),respectively.Upon illumination,electrons were produced,with the majority of them moving towards the interface.This movement contributes to the increased lifetime of photogenerated electron-hole pairs,which in turn boosts the photocatalytic efficiency.The findings of this research provide significant insights for creating photocatalysts that are both highly effective and stable in CO_(2)reduction processes.
文摘Carbon materials are a key component in energy storage and conversion devices and their microstructure plays a crucial role in determining device performance.However,traditional carbon materials are unable to meet the requirements for applications in emerging fields such as renewable energy and electric vehicles due to limitations including a disordered structure and uncontrolled defects.With an aim of realizing devisable structures,adjustable functions,and performance breakthroughs,superstructured carbons is proposed and represent a category of carbon-based materials,characterized by precisely-built pores,networks,and interfaces.Superstructured carbons can overcome the limitations of traditional carbon materials and improve the performance of energy storage and conversion devices.We review the structure-activity relationships of superstructured carbons and recent research advances from three aspects including a precisely customized pore structure,a dense carbon network framework,and a multi-component highly coupled interface between the different components.Finally,we provide an outlook on the future development of and practical challenges in energy storage and conversion devices.
文摘Intercalation catalysis research involves inserting metal ions,molecules,or ionic liquids into the layered structure of catalysts to adjust their electronic structure and surface properties,thereby optimizing catalytic reaction efficiency and selectivity[1–3].This technique has achieved significant progress in areas such as electrocatalysis,catalytic cracking,and energy conversion,especially in reactions like hydrogen generation,oxygen reduction,nitrogen reduction,and carbon dioxide reduction[4–6].Intercalation catalysis can enhance catalyst activity and selectivity,but challenges remain regarding stability,reusability,and industrial application.Future research will focus on developing new intercalation materials,optimizing catalyst design,and exploring their potential applications in complex environments[7].
文摘The quest for sustainable energy solutions has intensified the search for alternative feedstocks that can supplement or replace fossil fuels. Obtaining fuels or chemicals through the conversion of renewable biomass is a promising candidate [1,2]. Some noblemetal-based (e.g., Pt, Pd and Rh) catalysts exhibit significant catalytic activity to the conversion reaction of these biomass.
基金financial support from the National Natural Science Foundation of China(52372173,52072034)。
文摘Direct electrolysis of seawater offers a transformative technology for sustainable hydrogen production,circumventing the constraint of freshwater scarcity.However,the serious electrode corrosion and competitive chloride oxidation reactions make oxygen evolution reaction(OER)in seawater extremely challenging.Herein,the low-cost and scalable CoFe layered double hydroxides with Cl^(-)intercalation and decorated with Ce(OH)_(3)(named as CoFe-Cl^(-)/Ce(OH)_(3))catalyst is synthesized via rapid electrodeposition under ambient conditions,which is quickly reconstructed into a CeO_(2)decorated and Cl^(-)intercalated CoFeOOH(CoFeOOH-Cl^(-)/CeO_(2))during OER.Theoretical investigation reveals that Cl^(-)intercalation weakens the adsorption ability of Cl^(-)on Co/Fe atoms and hinders unfavorable coupling with chloride,thereby preventing the chlorine corrosion process and enhancing catalytic stability and activity.The CeO_(2)with hard Lewis acidity preferentially binds to OH-with harder Lewis base to ensure the OH-rich microenvironment around catalyst even under high current operating conditions,thus further enhancing stability and improving OER activity.The functionalized CoFe-Cl^(-)/Ce(OH)_(3)delivers 1000 mA cm^(-2)current density at only 329 mV overpotential with excellent stability for 1000 h under alkaline seawater.Electrochemical experiments elucidate the OER catalytic mechanism in which CeO_(2)serves as a co-catalyst for enriching OH-and CoFeOOH-Cl^(-)is the active species.Our work is a substantial step towards achieving massive and sustainable production of hydrogen fuel from immense seawater.
基金financially supported by the National Natural Science Foundation of China(Nos.22435005,22193042,21921001,52202194,22305105,22201284)the Key Research Program of Frontier Sciences of the Chinese Academy of Sciences(No.ZDBSLY-SLH024)。
文摘Two-dimensional(2D)organic-inorganic hybrid perovskites(OIHPs)have been developed as promising candidates for photodetection,owing to their excellent semiconducting features and structural tunability.However,as an important parameter for photodetection,the photoresponsive range of 2D OIHPs is usually modulated by finite metal-halide combinations,constraining their further development.The emerging aromatic amine-based alternating-cations-interlayered(A-ACI)hybrid perovskites that exhibit excellent charge transport and additional interlayered structural designability,provide an extra solution for achieving ideal photoresponsive range.Herein,for the first time,the photoresponsive range is successfully broadened in A-ACI hybrid perovskites(NMA)_(4)(FA)_(2)Pb_(3)Br_(12)(2)remolding from(NMA)_(4)(MA)_(2)Pb_(3)Br_(12)(1)(NMA=N-methylbenzylaminium,FA=formamidinium and MA=methylammonium).Particularly,1 and 2adopt an unprecedented configuration that NMA and MA/FA are alternately arranged in the interlayer in a 4:2 manner.Importantly,2 exhibits a narrower bandgap than 1,which can be ascribed to the lowlying conduct band composed of intercalation FAπ*orbitals.Meanwhile,2 possesses a shorter interlayer distance and flatter inorganic skeleton,synergistically facilitating the wider photo-absorption range and further endowing a broadening photoresponsive range(70 nm).This research not only enriches the perovskite family but also provides insights into structure-property relationships.
基金supported by the Science&Technology Development Fund of Tianjin Education Commission for Higher Education(No.2022KJ133).
文摘Quantum dots(QDs)can modulate the solar spectrum through the down-conversion mechanism to better match the spectral response of solar cells.Following previous work,this paper first tested the response of QD solar cells to specific monochromatic light,and found that QDs can effectively improve the photoelectric conversion efficiency(PCE)in the ultraviolet(UV)band by comparison.Then the photoelectric properties of the QD solar cells are tested under the air-mass 1.5(AM1.5)and air-mass 0(AM0)spectra.The experimental results show that because the absorption band of QDs is in the UV region,the space solar cells in the AM0 spectrum can obtain better PCE after coating QDs.The research results show the technical route of space solar cells with down-conversion mechanism,and put forward an important direction for the application of space solar photovoltaic(PV)technology,and have a good application prospect.
基金supported by the Natural Sciences and Engineering Research Council of Canada-Discovery Grant(Canada).
文摘Toluene is widely used as a raw material for many chemical products/pharmaceutical intermediates and as a solvent in many chemical and manufacturing industries.The conversion of toluene into higher value chemicals(benzyl alcohol,benzaldehyde,and benzoic acid,etc.)using sunlight is a very promising means.To achieve the full conversion and utilization of toluene,it is necessary to construct photocatalysts with high conversion and selectivity while synergistically optimizing the optimal reaction environment to significantly affect the photo-conversion of toluene.High-performance photocatalysts not only widely absorb sunlight,but also have abundant active sites and generation of free radicals,which can promote the chemical bonds cleavage of toluene,thus greatly increasing the yield of higher-valued products.In addition,the type of photocatalyst and the modification strategy would influence the selectivity of toluene photo-conversion.Therefore,it makes sense that this review presents the reaction mechanism and the influence of reaction factors for the(mainly)photo-oxidation of toluene,a thorough analysis and prediction of the reaction mechanism by theoretical calculations,and the toluene oxidation by different photocatalysts(in particular halogen-containing perovskite materials)to yield specific products,as well as photocatalysts’modifications.Finally,the challenges and prospects for designing efficient photocatalysts and optimizing the toluene oxidation reaction process are summarized.
基金supported by the National Key R&D Program of China(2022YFA1203400)the National Natural Science Foundation of China(W2441009)。
文摘Magnesium-ion batteries hold promise as future energy storage solutions,yet current Mg cathodes are challenged by low voltage and specific capacity.Herein,we present an AI-driven workflow for discovering high-performance Mg cathode materials.Utilizing the common characteristics of various ionic intercalation-type electrodes,we design and train a Crystal Graph Convolutional Neural Network model that can accurately predict electrode voltages for various ions with mean absolute errors(MAE)between0.25 and 0.33 V.By deploying the trained model to stable Mg compounds from Materials Project and GNoME AI dataset,we identify 160 high voltage structures out of 15,308 candidates with voltages above3.0 V and volumetric capacity over 800 mA h/cm^(3).We further train a precise NequIP model to facilitate accurate and rapid simulations of Mg ionic conductivity.From the 160 high voltage structures,the machine learning molecular dynamics simulations have selected 23 cathode materials with both high energy density and high ionic conductivity.This Al-driven workflow dramatically boosts the efficiency and precision of material discovery for multivalent ion batteries,paving the way for advanced Mg battery development.
基金supported by the National Key Research and Development Program of China(Grant Nos.2022YFA1402404 and 2023YFA1406304)the National Natural Science Foundation of China(Grant Nos.92161201,T2221003,12104221,12104220,12274208,12025404,12004174,91961101,T2394473,62274085,12374043,and U2032208)+1 种基金the Natural Science Foundation of Jiangsu Province(Grant Nos.BK20230079,BK20243013,and BK20233001)the Fundamental Research Funds for the Central Universities(Grant Nos.020414380192 and 2024300432).
文摘MnBi_(2)Te_(4),which is emerging as an intrinsic antiferromagnetic(AFM)topological insulator,provides a unique platform to investigate the interplay between magnetism and topology.Modulating its magnetic properties enables the observation of exotic quantum phenomena such as the quantum anomalous Hall effect,axion insulator states,and Majorana fermions.While the intercalation of Bi_(2)Te_(3)can tune its magnetism,synthesizing pure-phase MnBi_(2)Te_(4)with uniform Bi_(2)Te_(3)intercalation remains challenging,and the fixed interlayer spacing of Bi_(2)Te_(3)limits magnetic coupling tunability.Here,we utilize electrochemical organic molecule intercalation to expand the van der Waals gap of MnBi_(2)Te_(4)and modulate its magnetic properties.Through x-ray diffraction(XRD)characterizations,we confirm that the interlayer spacing of MnBi_(2)Te_(4)is expanded from 13.6°A to 30.5°A and 61.0°A by intercalating quaternary ammonium cations(THA^(+)and CTA^(+)),respectively.The THA-MnBi_(2)Te_(4)exhibits dual complex magnetic behavior,combining AFM ordering with a Neel temperature(T_(N))of 12 K and a small ferromagnetic hysteresis loop at 2 K.The CTA-MnBi_(2)Te_(4)shows robust ferromagnetism,with a Curie point(T_(C))of 15 K,similar to that of the MnBi_(2)Te_(4)monolayer.These results demonstrate that remarkable changes in the magnetic properties of MnBi_(2)Te_(4)can be achieved via electrochemical intercalation,providing new insights into manipulating magnetism in layered magnetic materials.
文摘The conversion of the greenhouse gas methane to value-added chemicals such as alcohols is a promising technology to mitigate environmental issue and the energy crisis.Especially,the sustainable photocatalytic,electrocatalytic and photoelectrocatalytic conversion of methane at ambient conditions is regarded as an alternative technology to replace with thermocatalysis.In this review,we summarize recent advances in photocatalytic,electrocatalytic and photoelectrocatalytic conversion of methane into alcohols.We firstly introduce the general principles of photocatalysis,electrocatalysis and photoelectrocatalysis.Then,we discuss the mechanism for selective activation of C-H bond and following oxygenation over metal,inorganic semiconductor,organic semiconductor,and heterojunction composite systems in the photocatalytic,electrocatalytic and photoelectrocatalytic methane oxidation in detail.Later,we present insights into the construction of effective photocatalyst,electrocatalyst and photoelectrocatalyst for methane conversion into alcohols from the perspective of band structures and active sites.Finally,the challenges and outlook for future designs of photocatalytic,electrocatalytic and photoelectrocatalytic methane oxidation systems are also proposed.
文摘The hydrothermal stability of zeolites is essential for their potential applications in biomass conversion,especially in processes involving elevated temperatures alongside the use or generation of H_(2)O.In this study,we employed F-ions as mineralizers to synthesize hydrothermally stable ZSM-5 zeolites under acidic conditions.The acidic synthesis system promotes zeolites with fewer silanol-terminated lattice defects(ZSM-5(A))compared to the traditional basic conditions(ZSM-5(B)),endowing materials with substantially higher structural integrity and hydrophobicity.After 10 days of autoclave treatment at 200℃ in aqueous phase,H-ZSM-5(A)demonstrated nearly unchanged reaction rates in the dehydration of cyclohexanol,while H-ZSM-5(B)lost>50%of the dehydration activity.Additionally,H-ZSM-5(A)delivered higher initial dehydration rates compared to H-ZSM-5(B).The different measured activation energies further revealed variations in reaction pathways during cyclohexanol dehydration,i.e.,the monomer-or dimer-mediated routes depending on the concentration of alcohol molecule within zeolite pores,providing additional evidence for the strengthened hydrophobic nature of H-ZSM-5(A).Beyond this,the zeolite surface properties and the strength of cyclohexanol-zeolite interactions may impose additional transport/adsorption barriers attributed to multi-phase phenomena on the more polar H-ZSM-5(B)zeolite surfaces.More importantly,the hydrothermal treatment did not induce significant desilication and dealumination in H-ZSM-5(A),thereby preserving its active acid sites and ensuring exceptional hydrothermal stability.The present work fundamentally studies the synthesis of hydrothermally stable zeolites in an acidic medium using fluorides and expands the understanding of polar interactions in catalysis,characterized by the dehydration of cyclohexanol,for future application in biomass conversion.
基金National Natural Science Foundation of China,Grant/Award Numbers:52002052,52073252,52372235Science and Technology Department of Zhejiang Province,Grant/Award Number:2023C01231+2 种基金Key Research and Development Project of Science and Technology Department of Sichuan Province,Grant/Award Number:2022YFSY0004the Open Project Program of the State Key Laboratory of New textile Materials and Advanced Processing Technologies,Grant/Award Number:FZ2021009Key Laboratory of Engineering Dielectrics and Its Application(Harbin University of Science and Technology),the Ministry of Education,Grant/Award Numbers:KFM202202,KFM202302,KFM202303。
文摘Plasma,the fourth state of matter,is characterized by the presence of charged particles,including ions and electrons.It has been shown to induce unique physical and chemical reactions.Recently,there have been increased applications of plasma technology in the field of multiscale functional materials'preparation,with a number of interesting results.This review will begin by introducing the basic knowledge of plasma,including the definition,typical parameters,and classification of plasma setups.Following this,we will provide a comprehensive review and summary of the applications(phase conversion,doping,deposition,etching,exfoliation,and surface treatment)of plasma in common energy conversion and storage systems,such as electrocatalytic conversion of small molecules,batteries,fuel cells,and supercapacitors.This article summarizes the structure-performance relationships of electrochemical energy conversion and storage materials(ECSMs)that have been prepared or modified by plasma.It also provides an overview of the challenges and perspectives of plasma technology,which could lead to a new approach for designing and modifying electrode materials in ECSMs.
