Two-step conversion of methanol to aromatics via light hydrocarbons can significantly improve the conversion stability compared with direct aromatization of methanol,but it remains a challenge to achieve a high p-xyle...Two-step conversion of methanol to aromatics via light hydrocarbons can significantly improve the conversion stability compared with direct aromatization of methanol,but it remains a challenge to achieve a high p-xylene(PX)selectivity.Herein,silica coating was firstly used to passivate external acid sites of ZSM-5 catalyst for the aromatization of light hydrocarbons by the chemical liquid deposition method.With the increase of SiO_(2) deposition,the density of the external acid sites of the catalyst was decreased from 0.1 to 0.03 mmol·g^(-1),which inhibited the surface secondary reactions and increased the PX/X from 34.6% to 60.0%.In view of the fact that the aromatization process in the second step was partly inhibited as methanol was consumed in advance in the upper methanol-to-light hydrocarbons catalyst layer,part of methanol was directly introduced into the lower aromatization catalyst layer to promote the alkylation process during the aromatization,which decreased the toluene selectivity from 34.5% to 14.3% but increased the xylene selectivity from 40.0%to 55.3%.It was also found that an appropriate external acid density was needed for aromatization catalyst to strengthen the alkylation process and improve the selectivity of xylene under the conditions of methanol introduction.展开更多
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
Super-fine electrohydrodynamic inkjet(SIJ)printing of perovskite nanocrystal(PNC)colloid ink exhibits significant potential in the fabrication of high-resolution color conversion microstructures arrays for fullcolor m...Super-fine electrohydrodynamic inkjet(SIJ)printing of perovskite nanocrystal(PNC)colloid ink exhibits significant potential in the fabrication of high-resolution color conversion microstructures arrays for fullcolor micro-LED displays.However,the impact of solvent on both the printing process and the morphology of SIJ-printed PNC color conversion microstructures remains underexplored.In this study,we prepared samples of CsPbBr3PNC colloid inks in various solvents and investigated the solvent's impact on SIJ printed PNC microstructures.Our findings reveal that the boiling point of the solvent is crucial to the SIJ printing process of PNC colloid inks.Only does the boiling point of the solvent fall in the optimal range,the regular positioned,micron-scaled,conical PNC microstructures can be successfully printed.Below this optimal range,the ink is unable to be ejected from the nozzle;while above this range,irregular positioned microstructures with nanoscale height and coffee-ring-like morphology are produced.Based on these observations,high-resolution color conversion PNC microstructures were effectively prepared using SIJ printing of PNC colloid ink dispersed in dimethylbenzene solvent.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
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
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
Foreword It is our great privilege,as vip Editors of the International Journal of Minerals,Metallurgy and Materials(IJMMM),to present this special issue on“High-Entropy and Multicomponent-Doped Materials for Energy...Foreword It is our great privilege,as vip Editors of the International Journal of Minerals,Metallurgy and Materials(IJMMM),to present this special issue on“High-Entropy and Multicomponent-Doped Materials for Energy Applications:Innovations in Energy Conversion and Storage.”This collection highlights the latest research developments in the preparation,optimizing properties,and exploring potential applications of high-entropy materials(HEMs)and other com-pounds with increased configurational entropy.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
CO_(2)emissions are key contributors to global climate change,leading to temperature increases and sealevel rise.Converting CO_(2)into valuable products is beneficial for meeting'Carbon Peaking and Carbon Neutrali...CO_(2)emissions are key contributors to global climate change,leading to temperature increases and sealevel rise.Converting CO_(2)into valuable products is beneficial for meeting'Carbon Peaking and Carbon Neutrality'goals.Photocatalytic reduction of CO_(2)to produce liquid fuels is of great significance for both CO_(2)reduction and storage/transportation of high-value chemicals.However,so far,there is no relevant literature to summarize photocatalysts for CO_(2)conversion to obtain liquid products.Based on the thermodynamic examination of the catalytic process and basic principles guiding the design of the photocatalysts,this review summarized photocatalysts for the CO_(2)conversion into four liquid products:formic acid,methanol,acetic acid and ethanol.Based on this,strategic development goals are outlined,and innovative strategies are proposed to enhance the efficiency and product selectivity of photocatalysts in converting CO_(2)into liquid products.This review will serve as a valuable reference for CO_(2)photo conversion into liquid products.展开更多
Accurate prediction of the composition of pyrolysis products is the prerequisite for achieving directional regulation of organic-rich shale pyrolysis and conversion products.In this paper,the classical segmented pyrol...Accurate prediction of the composition of pyrolysis products is the prerequisite for achieving directional regulation of organic-rich shale pyrolysis and conversion products.In this paper,the classical segmented pyrolysis kinetics model and a new refined pyrolysis kinetics model were used to forecast the composition distribution of hydrocarbon generation products co-heated by supercritical water and medium and low maturity organic-rich shale.The prediction accuracy of the two reaction kinetics models for the composition of pyrolysis products of organic-rich shale was compared.The reaction path of hydrocarbon generation in centimeter sized organic-rich shale under the action of supercritical water was identified.The results show that the prediction accuracy of the classical segmented pyrolysis kinetics model was poor at the initial stage of the reaction,and gradually increased with increasing time.The prediction error can reach less than 25%when the reaction time was 12 h.The new refined model of reaction kinetics established is better than the classical reaction kinetics model in predicting the product distribution of pyrolysis oil and gas,and its prediction error is less than 14%in this paper.The reaction paths of hydrocarbon generation in centimeter sized organic-rich shale under supercritical water conversion mainly include organic-rich shale directly generates asphaltene and saturated hydrocarbon,asphaltene pyrolysis generates saturated hydrocarbon,aromatic hydrocarbon and resin,saturated hydrocarbon,aromatic hydrocarbon and resin polymerization generates asphaltene,and saturated hydrocarbon,resin and asphaltene generates gas.The reason for the difference of centimeter sized and millimeter sized medium and low maturity organic-rich shales hydrocarbon generation in supercritical water is that the increase of shale size promotes the reaction path of polymerization of saturated hydrocarbon and aromatic hydrocarbon to asphaltene.展开更多
Methane, an abundant one-carbon(C_(1)) resource, is extensively used in the industrial production of vital fuels and value-added chemicals. However, current industrial methane conversion technologies are energy-and ca...Methane, an abundant one-carbon(C_(1)) resource, is extensively used in the industrial production of vital fuels and value-added chemicals. However, current industrial methane conversion technologies are energy-and carbon-intensive, mainly due to the high activation energy required to break the inert C–H bond, low selectivity, and problematic side reactions, including CO_(2)emissions and coke deposition. Electrochemical conversion of methane(ECM) using intermittent renewable energy offers an attractive solution, due to its modular reactor design and operational flexibility across a broad spectrum of temperatures and pressures. This review emphasizes conversion pathways of methane in various reaction systems, highlighting the significance and advantages of ECM in facilitating a sustainable artificial carbon cycle. This work provides a comprehensive overview of conventional methane activation mechanisms and delineates the complete pathways of methane conversion in electrolysis contexts. Based on surface/interface chemistry, this work systematically analyzes proposed reaction pathways and corresponding strategies to enhance ECM efficiency towards various target products, including syngas, hydrocarbons, oxygenates, and advanced carbon materials. The discussion also encompasses opportunities and challenges for the ECM process, including insights into ECM pathways, rational electrocatalyst design, establishment of benchmarking protocols, electrolyte engineering, enhancement of CH4conversion rates, and minimization of CO_(2)emission.展开更多
基金financial support from the National Natural Science Foundation of China(21978191 and 22278292)Key Research and Development Project of Shanxi Province(International Science and Technology Cooperation Program)(201803D421011)。
文摘Two-step conversion of methanol to aromatics via light hydrocarbons can significantly improve the conversion stability compared with direct aromatization of methanol,but it remains a challenge to achieve a high p-xylene(PX)selectivity.Herein,silica coating was firstly used to passivate external acid sites of ZSM-5 catalyst for the aromatization of light hydrocarbons by the chemical liquid deposition method.With the increase of SiO_(2) deposition,the density of the external acid sites of the catalyst was decreased from 0.1 to 0.03 mmol·g^(-1),which inhibited the surface secondary reactions and increased the PX/X from 34.6% to 60.0%.In view of the fact that the aromatization process in the second step was partly inhibited as methanol was consumed in advance in the upper methanol-to-light hydrocarbons catalyst layer,part of methanol was directly introduced into the lower aromatization catalyst layer to promote the alkylation process during the aromatization,which decreased the toluene selectivity from 34.5% to 14.3% but increased the xylene selectivity from 40.0%to 55.3%.It was also found that an appropriate external acid density was needed for aromatization catalyst to strengthen the alkylation process and improve the selectivity of xylene under the conditions of methanol introduction.
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.
基金supported by the National Natural Science Foundation of China(No.62374142)Fundamental Research Funds for the Central Universities(Nos.20720220085 and 20720240064)+2 种基金External Cooperation Program of Fujian(No.2022I0004)Major Science and Technology Project of Xiamen in China(No.3502Z20191015)Xiamen Natural Science Foundation Youth Project(No.3502Z202471002)。
文摘Super-fine electrohydrodynamic inkjet(SIJ)printing of perovskite nanocrystal(PNC)colloid ink exhibits significant potential in the fabrication of high-resolution color conversion microstructures arrays for fullcolor micro-LED displays.However,the impact of solvent on both the printing process and the morphology of SIJ-printed PNC color conversion microstructures remains underexplored.In this study,we prepared samples of CsPbBr3PNC colloid inks in various solvents and investigated the solvent's impact on SIJ printed PNC microstructures.Our findings reveal that the boiling point of the solvent is crucial to the SIJ printing process of PNC colloid inks.Only does the boiling point of the solvent fall in the optimal range,the regular positioned,micron-scaled,conical PNC microstructures can be successfully printed.Below this optimal range,the ink is unable to be ejected from the nozzle;while above this range,irregular positioned microstructures with nanoscale height and coffee-ring-like morphology are produced.Based on these observations,high-resolution color conversion PNC microstructures were effectively prepared using SIJ printing of PNC colloid ink dispersed in dimethylbenzene solvent.
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.
文摘Foreword It is our great privilege,as vip Editors of the International Journal of Minerals,Metallurgy and Materials(IJMMM),to present this special issue on“High-Entropy and Multicomponent-Doped Materials for Energy Applications:Innovations in Energy Conversion and Storage.”This collection highlights the latest research developments in the preparation,optimizing properties,and exploring potential applications of high-entropy materials(HEMs)and other com-pounds with increased configurational entropy.
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.
基金financially supported by the National Natural Science Foundation of China(Nos.22279060 and 21975129)the Natural Science Foundation of Jiangsu Province(No.BK20211103)+1 种基金the Start-up Funds for Scientific Research of Nanjing Forestry University(No.163101160)the Science Fund for Distinguished Young Scholars(No.JC2019002)
文摘CO_(2)emissions are key contributors to global climate change,leading to temperature increases and sealevel rise.Converting CO_(2)into valuable products is beneficial for meeting'Carbon Peaking and Carbon Neutrality'goals.Photocatalytic reduction of CO_(2)to produce liquid fuels is of great significance for both CO_(2)reduction and storage/transportation of high-value chemicals.However,so far,there is no relevant literature to summarize photocatalysts for CO_(2)conversion to obtain liquid products.Based on the thermodynamic examination of the catalytic process and basic principles guiding the design of the photocatalysts,this review summarized photocatalysts for the CO_(2)conversion into four liquid products:formic acid,methanol,acetic acid and ethanol.Based on this,strategic development goals are outlined,and innovative strategies are proposed to enhance the efficiency and product selectivity of photocatalysts in converting CO_(2)into liquid products.This review will serve as a valuable reference for CO_(2)photo conversion into liquid products.
基金support by the Basic Science Center Program of the Ordered Energy Conversion of the National Nature Science Foundation of China(NO.52488201)is gratefully acknowledged.
文摘Accurate prediction of the composition of pyrolysis products is the prerequisite for achieving directional regulation of organic-rich shale pyrolysis and conversion products.In this paper,the classical segmented pyrolysis kinetics model and a new refined pyrolysis kinetics model were used to forecast the composition distribution of hydrocarbon generation products co-heated by supercritical water and medium and low maturity organic-rich shale.The prediction accuracy of the two reaction kinetics models for the composition of pyrolysis products of organic-rich shale was compared.The reaction path of hydrocarbon generation in centimeter sized organic-rich shale under the action of supercritical water was identified.The results show that the prediction accuracy of the classical segmented pyrolysis kinetics model was poor at the initial stage of the reaction,and gradually increased with increasing time.The prediction error can reach less than 25%when the reaction time was 12 h.The new refined model of reaction kinetics established is better than the classical reaction kinetics model in predicting the product distribution of pyrolysis oil and gas,and its prediction error is less than 14%in this paper.The reaction paths of hydrocarbon generation in centimeter sized organic-rich shale under supercritical water conversion mainly include organic-rich shale directly generates asphaltene and saturated hydrocarbon,asphaltene pyrolysis generates saturated hydrocarbon,aromatic hydrocarbon and resin,saturated hydrocarbon,aromatic hydrocarbon and resin polymerization generates asphaltene,and saturated hydrocarbon,resin and asphaltene generates gas.The reason for the difference of centimeter sized and millimeter sized medium and low maturity organic-rich shales hydrocarbon generation in supercritical water is that the increase of shale size promotes the reaction path of polymerization of saturated hydrocarbon and aromatic hydrocarbon to asphaltene.
基金National Key R&D Program of China (2023YFA1508001 and 2023YFA1508002)National Natural Science Foundation of China (22272120 and U2202251)+1 种基金Hainan Province Science and Technology Special Fund(ZDYF2023SHFZ120)Research Foundation of Marine Science and Technology Collaborative Innovation Center of Hainan University (XTCX2022HYB01)。
文摘Methane, an abundant one-carbon(C_(1)) resource, is extensively used in the industrial production of vital fuels and value-added chemicals. However, current industrial methane conversion technologies are energy-and carbon-intensive, mainly due to the high activation energy required to break the inert C–H bond, low selectivity, and problematic side reactions, including CO_(2)emissions and coke deposition. Electrochemical conversion of methane(ECM) using intermittent renewable energy offers an attractive solution, due to its modular reactor design and operational flexibility across a broad spectrum of temperatures and pressures. This review emphasizes conversion pathways of methane in various reaction systems, highlighting the significance and advantages of ECM in facilitating a sustainable artificial carbon cycle. This work provides a comprehensive overview of conventional methane activation mechanisms and delineates the complete pathways of methane conversion in electrolysis contexts. Based on surface/interface chemistry, this work systematically analyzes proposed reaction pathways and corresponding strategies to enhance ECM efficiency towards various target products, including syngas, hydrocarbons, oxygenates, and advanced carbon materials. The discussion also encompasses opportunities and challenges for the ECM process, including insights into ECM pathways, rational electrocatalyst design, establishment of benchmarking protocols, electrolyte engineering, enhancement of CH4conversion rates, and minimization of CO_(2)emission.
