To meet the growing emission of water contaminants,the development of new materials that enhance the efficiency of the water treatment system is urgent.Ordered mesoporous materials provide opportunities in environment...To meet the growing emission of water contaminants,the development of new materials that enhance the efficiency of the water treatment system is urgent.Ordered mesoporous materials provide opportunities in environmental processing applications due to their exceptionally high surface areas,large pore sizes,and enough pore volumes.These properties might enhance the performance of materials concerning adsorption/catalysis capability,durability,and stability.In this review,we enumerate the ordered mesoporous materials as adsorbents/catalysts and their modifications in water pollution treatment from the past decade,including heavy metals(Hg^(2+),Pb^(2+),Cd^(2+),Cr^(6+),etc.),toxic anions(nitrate,phosphate,fluoride,etc.),and organic contaminants(organic dyes,antibiotics,etc.).These contributions demonstrate a deep understanding of the synergistic effect between the incorporated framework and homogeneous active centers.Besides,the challenges and perspectives of the future developments of ordered mesoporous materials in wastewater treatment are proposed.This work provides a theoretical basis and complete summary for the application of ordered mesoporous materials in the removal of contaminants from aqueous solutions.展开更多
Light-to-thermal conversion materials(LTCMs)have been of great interest to researchers due to their impressive energy conversion capacity and wide range of applications in biomedical,desalination,and synergistic catal...Light-to-thermal conversion materials(LTCMs)have been of great interest to researchers due to their impressive energy conversion capacity and wide range of applications in biomedical,desalination,and synergistic catalysis.Given the limited advances in existing materials(metals,semiconductors,π-conjugates),researchers generally adopt the method of constructing complex systems and hybrid structures to optimize performance and achieve multifunctional integration.However,the development of LTCMs is still in its infancy as the physical mechanism of light-to-thermal conversion is unclear.In this review,we proposed design strategies for efficient LTCMs by analyzing the physical process of light-tothermal conversion.First,we analyze the nature of light absorption and heat generation to reveal the physical processes of light-to-thermal conversion.Then,we explain the light-to-thermal conversion mechanisms of metallic,semiconducting andπ-conjugated LCTMs,and propose new material design strategies and performance improvement methods.Finally,we summarize the challenges and prospects of LTCMs in emerging applications such as solar water evaporation and photothermal catalysis.展开更多
Carbon peaking and carbon neutralization trigger a technical revolution in energy&environment related fields.Development of new technologies for green energy production and storage,industrial energy saving and eff...Carbon peaking and carbon neutralization trigger a technical revolution in energy&environment related fields.Development of new technologies for green energy production and storage,industrial energy saving and efficiency reinforcement,carbon capture,and pollutant gas treatment is in highly imperious demand.The emerging porous framework materials such as metal–organic frameworks(MOFs),covalent organic frameworks(COFs)and hydrogen-bonded organic frameworks(HOFs),owing to the permanent porosity,tremendous specific surface area,designable structure and customizable functionality,have shown great potential in major energy-consuming industrial processes,including sustainable energy gas catalytic conversion,energy-efficient industrial gas separation and storage.Herein,this manuscript presents a systematic review of porous framework materials for global and comprehensive energy&environment related applications,from a macroscopic and application perspective.展开更多
Single atom catalysts(SACs) possessing regulated electronic structure, high atom utilization, and superior catalytic efficiency have been studied in almost all fields in recent years. Carbon-based supporting SACs are ...Single atom catalysts(SACs) possessing regulated electronic structure, high atom utilization, and superior catalytic efficiency have been studied in almost all fields in recent years. Carbon-based supporting SACs are becoming popular materials because of their low cost, high electron conductivity, and controllable surface property. At the stage of catalysts preparation, the rational design of active sites is necessary for the substantial improvement of activity of catalysts. To date, the reported design strategies are mainly about synthesis mechanism and synthetic method. The level of understanding of design strategies of carbon-based single atom catalysts is requiring deep to be paved. The design strategies about manufacturing defects and coordination modulation of catalysts are presented. The design strategies are easy to carry out in the process of drawing up preparation routes. The components of carbon-based SACs can be divided into two parts: active site and carbon skeleton. In this review, the manufacture of defects and coordination modulation of two parts are introduced, respectively. The structure features and design strategies from the active sites and carbon skeletons to the overall catalysts are deeply discussed.Then, the structural design of different nano-carbon SACs is introduced systematically. The characterization of active site and carbon skeleton and the detailed mechanism of reaction process are summarized and analyzed. Next, the applications in the field of electrocatalysis for oxygen conversion and hydrogen conversion are illustrated. The relationships between the superior performance and the structure of active sites or carbon skeletons are discussed. Finally, the conclusion of this review and prospects on the abundant space for further promotion in broader fields are depicted. This review highlights the design and preparation thoughts from the parts to the whole. The detailed and systematic discussion will provide useful guidance for design of SACs for readers.展开更多
Closing the carbon loop,through CO_(2)capture and utilization,is a promising route to mitigate climate change.Solar energy is a sustainable energy source which can be exploited to drive catalytic reactions for utilizi...Closing the carbon loop,through CO_(2)capture and utilization,is a promising route to mitigate climate change.Solar energy is a sustainable energy source which can be exploited to drive catalytic reactions for utilizing CO_(2),including converting the CO_(2)into useful products.Solar energy can be harnessed through a range of different pathways to valorize CO_(2).Whilst using solar energy to drive CO_(2)reduction has vast potential to promote catalytic CO_(2)conversions,the progress is limited due to the lack of understanding of property-performance relations as well as feasible material engineering approaches.Herein,we outline the various driving forces involved in photothermal CO_(2)catalysis.The heat from solar energy can be utilized to induce CO_(2)catalytic reduction reactions via the photothermal effect.Further,solar energy can act to modify reaction pathways through light-matter interactions.Light-induced chemical functions have demonstrated the ability to regulate intermediary reaction steps,and thus control the reaction selectivity.Photothermal catalyst structures and specific catalyst design strategies are discussed in this context.This review provides a comprehensive understanding of the heat-light synergy and guidance for rational photothermal catalyst design for CO_(2)utilization.展开更多
^(129)Xe NMR has been proven to be a powerful tool to investigate the structure of porousmaterials. Xenon is a monatomic noble gas which could be used as a probe due to theextremely sensitive to its local environment....^(129)Xe NMR has been proven to be a powerful tool to investigate the structure of porousmaterials. Xenon is a monatomic noble gas which could be used as a probe due to theextremely sensitive to its local environment. Optical pumping techniques for production ofhyperpolarized (HP) xenon have led to an increase of sensitivity up to orders of magnitudecompared with traditional ^(129)Xe NMR. This review summarizes the application of thistechnique in porous materials and heterogeneous catalysis in recent ten years, involving ofzeolites, metal-organic frameworks (MOFs), catalytic process and kinetics.展开更多
Two-dimensional(2D)supports confined single-atom catalysts(2D SACs)with unique geometric and electronic structures have been attractive candidates in different catalytic applications,such as energy conversion and stor...Two-dimensional(2D)supports confined single-atom catalysts(2D SACs)with unique geometric and electronic structures have been attractive candidates in different catalytic applications,such as energy conversion and storage,value-added chemical synthesis and environmental remediation.However,their environmental appli-cations lack of a comprehensive summary and in-depth discussion.In this review,recent progresses in synthesis routes and advanced characterization techniques for 2D SACs are introduced,and a comprehensive discussion on their applications in environmental remediation is presented.Generally,2D SACs can be effective in catalytic elimination of aqueous and gaseous pollutants via radical or non-radical routes and transformation of toxic pollutants into less poisonous species or highly value-added products,opening a new horizon for the contami-nant treatment.In addition,in-depth reaction mechanisms and potential pathways are systematically discussed,and the relationship between the structure-performance is highlighted.Finally,several critical challenges within this field are presented,and possible directions for further explorations of 2D SACs in environmental remediation are suggested.Although the research of 2D SACs in the environmental application is still in its infancy,this review will provide a timely summary on the emerging field,and would stimulate tremendous interest for designing more attractive 2D SACs and promoting their wide applications.展开更多
Metal-containing crystalline porous materials(CPMs)are gaining popularity in heterogeneous catalysis because of their highly crystalline and porous systems,and their excellent chemical tunability.Modification of the m...Metal-containing crystalline porous materials(CPMs)are gaining popularity in heterogeneous catalysis because of their highly crystalline and porous systems,and their excellent chemical tunability.Modification of the metal species and framework structure permits them to have greater activity,selectivity,and stability over other materials.An in-depth understanding of the complex nature of metal active sites in CPMs is essential for revealing the structure-performance relationships and directing the rational design of such catalysts.Compared to conventional characterization techniques,the rapid development of X-ray absorption spectroscopy(XAS)has provided element-and site-specific deep insights into the electronic and structural information of metal species in CPMs.As such,this review begins by summarizing novel XAS techniques and analysis methods in accurately obtaining such data.Next,the combination of XAS with other high-level characterization methods into disclosing the configuration of active sites in metalcontaining CPMs is presented.Then,the utilization of theory-assisted XAS data analysis in examining complex metal-containing CPM catalysts is discussed.Afterwards,advanced in-situ/operando XAS studies into revealing the working sites in metal-containing CPMs under catalytic conditions are highlighted.We conclude by outlining the future challenges and prospects of XAS measurements,data analyses,and in-situ/operando setups in advancing the study of metal-in-CPM catalysts.展开更多
This paper reports the synthesis of host-guest nanocomposite material [Fe(bpy)(3)]Y2+ (where bpy=2,2'-bipyridine) using the flexible ligand method. X-ray diffraction analysis. adsorption technique, and cyclic volt...This paper reports the synthesis of host-guest nanocomposite material [Fe(bpy)(3)]Y2+ (where bpy=2,2'-bipyridine) using the flexible ligand method. X-ray diffraction analysis. adsorption technique, and cyclic voltammetry were used to characterize the material. The results show that [Fe(bpy)(3)](2+) has been entrapped in the supercage of zeolite, its electron transfer is realized by electron hopping of [Fe(bpy)(3)](2+) within the supercage of zeolite.展开更多
Quantitative oxygen detection,especially at low concentrations,holds significant importance in the realms of biology,complex environments,and chemical process engineering.Due to the high sensitivity and rapid response...Quantitative oxygen detection,especially at low concentrations,holds significant importance in the realms of biology,complex environments,and chemical process engineering.Due to the high sensitivity and rapid response of the triplet excitons of phosphorescence to oxygen,pure organic room-temperature phosphorescence(RTP)materials have garnered widespread attention in recent years for oxygen detection.However,simultaneously achieving ultralong phosphorescence at room temperature and quantitative oxygen detection from pure organic host-guest doped materials poses challenges.The d ensely packed materials may decrease non-radiative decay to increase the phosphorescence,but are unsuitable for oxygen diffusion in oxygen detection.Herein,the oxygen sensitivity of host-guest doped RTP materials using 4-bromo-N,N-bis(4-(tertbutyl)phenyl)aniline(TPABuBr)as the host and 6-bromo-2-butyl-1H-benzo[de]isoquinoline-1,3(2H)-dione(NIBr)as the guest was developed.The doped material exhibits fluorescence-phosphorescence dual-emission behavior at room temperature.The tert-butyl groups in TPABuBr facilitate appropriate intermolecular spacing in the crystal state,enhancing oxygen permeability.Therefore,oxygen penetration can quench the phosphorescence emission.The observed linear relationship between the phosphorescence intensity of the doped material and the oxygen volume fraction conforms to the Stern-Volmer equation,suggesting its potential for quantitative analysis of oxygen concentration.The calculated limit of detection is 0.015%(φ),enabling the analysis of oxygen with a volume fraction of less than 2.5%(φ).Moreover,the doped materials demonstrate rapid response and excellent photostability,indicating their potential utility as oxygen sensors.This study elucidates the design and characteristics of NIBr/TPABuBr doped materials,highlighting their potential application in oxygen concentration detection and offering insights for the design of oxygen sensors.展开更多
Hydrogen energy has been recognized as “Ultimate Power Source” in the 21st century, which could be the best solution to the looming energy crisis and climate degeneration in the near future. Due to its high safety, ...Hydrogen energy has been recognized as “Ultimate Power Source” in the 21st century, which could be the best solution to the looming energy crisis and climate degeneration in the near future. Due to its high safety, low price, abundant resources and decent hydrogen storage density, magnesium based solid-state hydrogen storage materials are becoming the leading candidate for onboard hydrogen storage. However,the high operation temperature and slow reaction rate of MgH_(2), as a result of the large formation enthalpy and high reaction activation energy,respectively, are the first and most difficult problems we need to face and overcome to realize its industrialization. Herein, a state-of-the-art review on tailoring the stable thermodynamics and sluggish kinetics of hydrogen storage in MgH_(2), particularly through nanoengnieering and catalysis is presented, aiming to provide references and solutions for its promotion and application. Promising methods to overcome the challenges faced by MgH_(2)/Mg, such as bidirectional catalysts and nanoconfinement with in-situ catalysis are compared and the required improvements are discussed to stimulate further discussions and ideas in the rational design of MgH_(2)/Mg systems with ability for hydrogen release/uptake at lower temperatures and cycle stability in the near future.展开更多
Prologue The rich scientific heritage of Dangsheng Su contains as substantial fraction his contributions to the field of catalysis with nanostructured carbon materials.Coming from microstructural analysis it became qu...Prologue The rich scientific heritage of Dangsheng Su contains as substantial fraction his contributions to the field of catalysis with nanostructured carbon materials.Coming from microstructural analysis it became quickly clear that the richness of morphological and hence surface electronic variations in this class of materials should be suitable for the development of a science base for heterogeneous catalysis.展开更多
Several types of solid acid catalysts were prepared based on oxides like (ZrO2, TiO2, HfO2, MCM-41 and SBA-15), using two main preparation methods: the precipitation and the sol-gel methods. Each catalyst was subjecte...Several types of solid acid catalysts were prepared based on oxides like (ZrO2, TiO2, HfO2, MCM-41 and SBA-15), using two main preparation methods: the precipitation and the sol-gel methods. Each catalyst was subjected to two types of impregnations: sulfate ions using sulfuric acid as precursor and niobium using niobium oxalate as precursor. These prepared catalysts were tested in the etherification reaction of 2-naphtol, where the catalysts showed both acidic and redox properties. The acidic character was manifested through the formation of 2-butoxynaphtalene (with moderate yields) when oxide is sulfated, and the redox character (when impregnated with niobium) manifested through the formation of the interesting product 2-ethylnaphtofuran (with low yields) and other products that were a result of oxidative coupling of two 2-naphtol molecules (binol and acetal of binol). However despite the effort, several attempts to increase the yield of 2-ethylnaphtofuran did not work. All products prepared were obtained in pure form and characterized by 1H and 13C NMR, GC and MS.展开更多
The nanotechnology is of great siguifieance to the country's future economic, social development and national security, and it will bring a revolutionary change to the medicine, manufacturing, materials and informati...The nanotechnology is of great siguifieance to the country's future economic, social development and national security, and it will bring a revolutionary change to the medicine, manufacturing, materials and information communication and other industries, therefore, in recent years, nano science and technology is greatly favored all over the world especially in developed countries. All the countries (areas) in the world have developed the nanotechnology as the main driver of the technical innovation in the twenty-first century, and have formulated development strategies and plans, to promote and guide their development in nanotechnology, which lead to fiercer and fiercer competition. In this paper, the author mainly introduces the application of nano materials in catalysis, filtration, separation, paint and new fine chemical industry and so on.展开更多
Catalysts can accelerate the chemical reaction rate and effectively promote the molecules transformation,which is of great significance in the research of chemical industry and material science.The extreme utilization...Catalysts can accelerate the chemical reaction rate and effectively promote the molecules transformation,which is of great significance in the research of chemical industry and material science.The extreme utilization of reactive sites has led to the emergence and development of atomically dispersed materials(ADMs).The highly active coordination unsaturated metal sites and fully utilized metal atoms make ADMs show great potential in catalytic reactions.The adjustment of coordination environment and electronic structure provides more possibilities for constructing reactive centers with different properties.This review summarized the application and research progress of ADMs in different fields.The design strategy and structure–activity relationship of ADMs for specific reactions were summarized and analyzed.Moreover,we also provided advices for the challenges and opportunities faced by ADMs in catalytic reactions.展开更多
Transition metal carbides and nitrides(MXenes)nanosheets are attractive two-dimensional(2D)materials,but they suffer from oxidation/degradation issues during storage and/or applications due to their sensitivity to wat...Transition metal carbides and nitrides(MXenes)nanosheets are attractive two-dimensional(2D)materials,but they suffer from oxidation/degradation issues during storage and/or applications due to their sensitivity to water and oxygen.Despite the great research progress,the exact oxidation kinetics of Ti_(3)C_(2)T_(x)(MXene)and their final products after oxidation are not fully understood.Herein,we systematically tracked the oxidation process of few-layer Ti_(3)C_(2)T_(x) nanosheets in an aqueous solution at room temperature over several weeks.We also studied the oxidation effects on the electrocatalytic properties of Ti_(3)C_(2)T_(x) for hydrogen evolution reaction and found that the overpotential to achieve a current density of 10 mA cm^(-2)increases from 0.435 to 0.877 V after three weeks of degradation,followed by improvement to stabilized values of around 0.40 V after eight weeks.These results suggest that severely oxidized MXene could be a promising candidate for designing efficient catalysts.According to our detailed experimental characterization and theoretical calculations,unlike previous studies,black titanium oxide is formed as the final product in addition to white Ti(IV)oxide and disordered carbons after the complete oxidation of Ti_(3)C_(2)T_(x).This work presents significant advancements in better understanding of 2D Ti_(3)C_(2)T_(x)(MXene)oxidation and enhances the prospects of this material for various applications.展开更多
基金supported by the National Natural Science Foundation of China(52370041)National Natural Science Foundation of China(21976134 and 21707104)State Key Laboratory of Pollution treatment and Resource Reuse Foundation(NO.PCRRK21001).
文摘To meet the growing emission of water contaminants,the development of new materials that enhance the efficiency of the water treatment system is urgent.Ordered mesoporous materials provide opportunities in environmental processing applications due to their exceptionally high surface areas,large pore sizes,and enough pore volumes.These properties might enhance the performance of materials concerning adsorption/catalysis capability,durability,and stability.In this review,we enumerate the ordered mesoporous materials as adsorbents/catalysts and their modifications in water pollution treatment from the past decade,including heavy metals(Hg^(2+),Pb^(2+),Cd^(2+),Cr^(6+),etc.),toxic anions(nitrate,phosphate,fluoride,etc.),and organic contaminants(organic dyes,antibiotics,etc.).These contributions demonstrate a deep understanding of the synergistic effect between the incorporated framework and homogeneous active centers.Besides,the challenges and perspectives of the future developments of ordered mesoporous materials in wastewater treatment are proposed.This work provides a theoretical basis and complete summary for the application of ordered mesoporous materials in the removal of contaminants from aqueous solutions.
基金the financial support from the National Natural Science Foundation of China(Grant Nos.52272153,52032004)the KLOMT Key Laboratory Open Project(2022KLOMT02-05)。
文摘Light-to-thermal conversion materials(LTCMs)have been of great interest to researchers due to their impressive energy conversion capacity and wide range of applications in biomedical,desalination,and synergistic catalysis.Given the limited advances in existing materials(metals,semiconductors,π-conjugates),researchers generally adopt the method of constructing complex systems and hybrid structures to optimize performance and achieve multifunctional integration.However,the development of LTCMs is still in its infancy as the physical mechanism of light-to-thermal conversion is unclear.In this review,we proposed design strategies for efficient LTCMs by analyzing the physical process of light-tothermal conversion.First,we analyze the nature of light absorption and heat generation to reveal the physical processes of light-to-thermal conversion.Then,we explain the light-to-thermal conversion mechanisms of metallic,semiconducting andπ-conjugated LCTMs,and propose new material design strategies and performance improvement methods.Finally,we summarize the challenges and prospects of LTCMs in emerging applications such as solar water evaporation and photothermal catalysis.
基金the financial support from the National Natural Science Foundation of China(22090062,21922810,21825802,22138003,22108083,and 21725603)the Guangdong Pearl River Talents Program(2021QN02C8)+3 种基金the Science and Technology Program of Guangzhou(202201010118)Zhejiang Provincial Natural Science Foundation of China(LR20B060001)National Science Fund for Excellent Young Scholars(22122811)China Postdoctoral Science Foundation(2022M710123)。
文摘Carbon peaking and carbon neutralization trigger a technical revolution in energy&environment related fields.Development of new technologies for green energy production and storage,industrial energy saving and efficiency reinforcement,carbon capture,and pollutant gas treatment is in highly imperious demand.The emerging porous framework materials such as metal–organic frameworks(MOFs),covalent organic frameworks(COFs)and hydrogen-bonded organic frameworks(HOFs),owing to the permanent porosity,tremendous specific surface area,designable structure and customizable functionality,have shown great potential in major energy-consuming industrial processes,including sustainable energy gas catalytic conversion,energy-efficient industrial gas separation and storage.Herein,this manuscript presents a systematic review of porous framework materials for global and comprehensive energy&environment related applications,from a macroscopic and application perspective.
基金funded by the National Natural Science Foundation of China (Nos. 22279118, 31901272, 21401168, U1204203)National Science Fund for Distinguished Young of China (No. 22225202)+1 种基金Young Top Talent Program of Zhongyuan-YingcaiJihua (No. 30602674)Top-Notch Talent Program of Henan Agricultural University (No. 30501034)。
文摘Single atom catalysts(SACs) possessing regulated electronic structure, high atom utilization, and superior catalytic efficiency have been studied in almost all fields in recent years. Carbon-based supporting SACs are becoming popular materials because of their low cost, high electron conductivity, and controllable surface property. At the stage of catalysts preparation, the rational design of active sites is necessary for the substantial improvement of activity of catalysts. To date, the reported design strategies are mainly about synthesis mechanism and synthetic method. The level of understanding of design strategies of carbon-based single atom catalysts is requiring deep to be paved. The design strategies about manufacturing defects and coordination modulation of catalysts are presented. The design strategies are easy to carry out in the process of drawing up preparation routes. The components of carbon-based SACs can be divided into two parts: active site and carbon skeleton. In this review, the manufacture of defects and coordination modulation of two parts are introduced, respectively. The structure features and design strategies from the active sites and carbon skeletons to the overall catalysts are deeply discussed.Then, the structural design of different nano-carbon SACs is introduced systematically. The characterization of active site and carbon skeleton and the detailed mechanism of reaction process are summarized and analyzed. Next, the applications in the field of electrocatalysis for oxygen conversion and hydrogen conversion are illustrated. The relationships between the superior performance and the structure of active sites or carbon skeletons are discussed. Finally, the conclusion of this review and prospects on the abundant space for further promotion in broader fields are depicted. This review highlights the design and preparation thoughts from the parts to the whole. The detailed and systematic discussion will provide useful guidance for design of SACs for readers.
基金supported by the Australian Research Council(ARC)under the Laureate Fellowship Scheme-FL140100081 and ARC Discovery Project DP170102410the support of Scientia Ph D Scholarship from UNSW Sydneythe support of Australia Government Research Training Program(RTP)Scholarship。
文摘Closing the carbon loop,through CO_(2)capture and utilization,is a promising route to mitigate climate change.Solar energy is a sustainable energy source which can be exploited to drive catalytic reactions for utilizing CO_(2),including converting the CO_(2)into useful products.Solar energy can be harnessed through a range of different pathways to valorize CO_(2).Whilst using solar energy to drive CO_(2)reduction has vast potential to promote catalytic CO_(2)conversions,the progress is limited due to the lack of understanding of property-performance relations as well as feasible material engineering approaches.Herein,we outline the various driving forces involved in photothermal CO_(2)catalysis.The heat from solar energy can be utilized to induce CO_(2)catalytic reduction reactions via the photothermal effect.Further,solar energy can act to modify reaction pathways through light-matter interactions.Light-induced chemical functions have demonstrated the ability to regulate intermediary reaction steps,and thus control the reaction selectivity.Photothermal catalyst structures and specific catalyst design strategies are discussed in this context.This review provides a comprehensive understanding of the heat-light synergy and guidance for rational photothermal catalyst design for CO_(2)utilization.
基金This work was supported by Natural Science Foundation of china(grant no.22022202,21972142,91745109,91545104)the LiaoNing Revitalization Talents Program(grant no.XLYC1807227)This work is dedicated to Professor Xiuwen Han on the occasion of her 80th birthday。
文摘^(129)Xe NMR has been proven to be a powerful tool to investigate the structure of porousmaterials. Xenon is a monatomic noble gas which could be used as a probe due to theextremely sensitive to its local environment. Optical pumping techniques for production ofhyperpolarized (HP) xenon have led to an increase of sensitivity up to orders of magnitudecompared with traditional ^(129)Xe NMR. This review summarizes the application of thistechnique in porous materials and heterogeneous catalysis in recent ten years, involving ofzeolites, metal-organic frameworks (MOFs), catalytic process and kinetics.
基金This work was financially supported by the National Natural Science Foundation of China(51602133,51876093)China MOST(2018YFE0183600).
文摘Two-dimensional(2D)supports confined single-atom catalysts(2D SACs)with unique geometric and electronic structures have been attractive candidates in different catalytic applications,such as energy conversion and storage,value-added chemical synthesis and environmental remediation.However,their environmental appli-cations lack of a comprehensive summary and in-depth discussion.In this review,recent progresses in synthesis routes and advanced characterization techniques for 2D SACs are introduced,and a comprehensive discussion on their applications in environmental remediation is presented.Generally,2D SACs can be effective in catalytic elimination of aqueous and gaseous pollutants via radical or non-radical routes and transformation of toxic pollutants into less poisonous species or highly value-added products,opening a new horizon for the contami-nant treatment.In addition,in-depth reaction mechanisms and potential pathways are systematically discussed,and the relationship between the structure-performance is highlighted.Finally,several critical challenges within this field are presented,and possible directions for further explorations of 2D SACs in environmental remediation are suggested.Although the research of 2D SACs in the environmental application is still in its infancy,this review will provide a timely summary on the emerging field,and would stimulate tremendous interest for designing more attractive 2D SACs and promoting their wide applications.
基金the National Natural Science Foundation of China(grant no.22301057)the financial support by the Natural Science Foundation of Hebei Province(grant no.B2023201065)+4 种基金Hebei University High-level Talent Research Program(grant no.521100223025)Y.L.thanks the funding from the National Natural Science Foundation of China(grant no.22305060)Hebei University High-level Talent Research Program(grant no.521100222060)P.Z.acknowledges the financial support from an Natural Sciences and Engineering Research Council of Canada(NSERC)Discovery GrantA.G.W.thanks financial support from an NSERC Canada Graduate Scholarships-Doctoral Program(CGS-D)scholarship.
文摘Metal-containing crystalline porous materials(CPMs)are gaining popularity in heterogeneous catalysis because of their highly crystalline and porous systems,and their excellent chemical tunability.Modification of the metal species and framework structure permits them to have greater activity,selectivity,and stability over other materials.An in-depth understanding of the complex nature of metal active sites in CPMs is essential for revealing the structure-performance relationships and directing the rational design of such catalysts.Compared to conventional characterization techniques,the rapid development of X-ray absorption spectroscopy(XAS)has provided element-and site-specific deep insights into the electronic and structural information of metal species in CPMs.As such,this review begins by summarizing novel XAS techniques and analysis methods in accurately obtaining such data.Next,the combination of XAS with other high-level characterization methods into disclosing the configuration of active sites in metalcontaining CPMs is presented.Then,the utilization of theory-assisted XAS data analysis in examining complex metal-containing CPM catalysts is discussed.Afterwards,advanced in-situ/operando XAS studies into revealing the working sites in metal-containing CPMs under catalytic conditions are highlighted.We conclude by outlining the future challenges and prospects of XAS measurements,data analyses,and in-situ/operando setups in advancing the study of metal-in-CPM catalysts.
文摘This paper reports the synthesis of host-guest nanocomposite material [Fe(bpy)(3)]Y2+ (where bpy=2,2'-bipyridine) using the flexible ligand method. X-ray diffraction analysis. adsorption technique, and cyclic voltammetry were used to characterize the material. The results show that [Fe(bpy)(3)](2+) has been entrapped in the supercage of zeolite, its electron transfer is realized by electron hopping of [Fe(bpy)(3)](2+) within the supercage of zeolite.
文摘Quantitative oxygen detection,especially at low concentrations,holds significant importance in the realms of biology,complex environments,and chemical process engineering.Due to the high sensitivity and rapid response of the triplet excitons of phosphorescence to oxygen,pure organic room-temperature phosphorescence(RTP)materials have garnered widespread attention in recent years for oxygen detection.However,simultaneously achieving ultralong phosphorescence at room temperature and quantitative oxygen detection from pure organic host-guest doped materials poses challenges.The d ensely packed materials may decrease non-radiative decay to increase the phosphorescence,but are unsuitable for oxygen diffusion in oxygen detection.Herein,the oxygen sensitivity of host-guest doped RTP materials using 4-bromo-N,N-bis(4-(tertbutyl)phenyl)aniline(TPABuBr)as the host and 6-bromo-2-butyl-1H-benzo[de]isoquinoline-1,3(2H)-dione(NIBr)as the guest was developed.The doped material exhibits fluorescence-phosphorescence dual-emission behavior at room temperature.The tert-butyl groups in TPABuBr facilitate appropriate intermolecular spacing in the crystal state,enhancing oxygen permeability.Therefore,oxygen penetration can quench the phosphorescence emission.The observed linear relationship between the phosphorescence intensity of the doped material and the oxygen volume fraction conforms to the Stern-Volmer equation,suggesting its potential for quantitative analysis of oxygen concentration.The calculated limit of detection is 0.015%(φ),enabling the analysis of oxygen with a volume fraction of less than 2.5%(φ).Moreover,the doped materials demonstrate rapid response and excellent photostability,indicating their potential utility as oxygen sensors.This study elucidates the design and characteristics of NIBr/TPABuBr doped materials,highlighting their potential application in oxygen concentration detection and offering insights for the design of oxygen sensors.
基金funded by Chongqing Special Key Project of Technology Innovation and Application Development(Grant No.cstc2019jscx-dxwt BX0016)Guiding Project of Scientific Research Program in Ministry of Education of Hubei Province (No. B2021025)Fundamental Research Funds for the Central Universities (2022CDJXY-010 and 2022CDJQY-013)。
文摘Hydrogen energy has been recognized as “Ultimate Power Source” in the 21st century, which could be the best solution to the looming energy crisis and climate degeneration in the near future. Due to its high safety, low price, abundant resources and decent hydrogen storage density, magnesium based solid-state hydrogen storage materials are becoming the leading candidate for onboard hydrogen storage. However,the high operation temperature and slow reaction rate of MgH_(2), as a result of the large formation enthalpy and high reaction activation energy,respectively, are the first and most difficult problems we need to face and overcome to realize its industrialization. Herein, a state-of-the-art review on tailoring the stable thermodynamics and sluggish kinetics of hydrogen storage in MgH_(2), particularly through nanoengnieering and catalysis is presented, aiming to provide references and solutions for its promotion and application. Promising methods to overcome the challenges faced by MgH_(2)/Mg, such as bidirectional catalysts and nanoconfinement with in-situ catalysis are compared and the required improvements are discussed to stimulate further discussions and ideas in the rational design of MgH_(2)/Mg systems with ability for hydrogen release/uptake at lower temperatures and cycle stability in the near future.
文摘Prologue The rich scientific heritage of Dangsheng Su contains as substantial fraction his contributions to the field of catalysis with nanostructured carbon materials.Coming from microstructural analysis it became quickly clear that the richness of morphological and hence surface electronic variations in this class of materials should be suitable for the development of a science base for heterogeneous catalysis.
文摘Several types of solid acid catalysts were prepared based on oxides like (ZrO2, TiO2, HfO2, MCM-41 and SBA-15), using two main preparation methods: the precipitation and the sol-gel methods. Each catalyst was subjected to two types of impregnations: sulfate ions using sulfuric acid as precursor and niobium using niobium oxalate as precursor. These prepared catalysts were tested in the etherification reaction of 2-naphtol, where the catalysts showed both acidic and redox properties. The acidic character was manifested through the formation of 2-butoxynaphtalene (with moderate yields) when oxide is sulfated, and the redox character (when impregnated with niobium) manifested through the formation of the interesting product 2-ethylnaphtofuran (with low yields) and other products that were a result of oxidative coupling of two 2-naphtol molecules (binol and acetal of binol). However despite the effort, several attempts to increase the yield of 2-ethylnaphtofuran did not work. All products prepared were obtained in pure form and characterized by 1H and 13C NMR, GC and MS.
文摘The nanotechnology is of great siguifieance to the country's future economic, social development and national security, and it will bring a revolutionary change to the medicine, manufacturing, materials and information communication and other industries, therefore, in recent years, nano science and technology is greatly favored all over the world especially in developed countries. All the countries (areas) in the world have developed the nanotechnology as the main driver of the technical innovation in the twenty-first century, and have formulated development strategies and plans, to promote and guide their development in nanotechnology, which lead to fiercer and fiercer competition. In this paper, the author mainly introduces the application of nano materials in catalysis, filtration, separation, paint and new fine chemical industry and so on.
基金supported by the National Key R&D Program of China(No.2018YFA0702003)the National Natural Science Foundation of China(Nos.21890383 and 21871159)+1 种基金the Science and Technology Key Project of Guangdong Province of China(No.2020B010188002)the China Postdoctoral Science Foundation(No.2022M721796).
文摘Catalysts can accelerate the chemical reaction rate and effectively promote the molecules transformation,which is of great significance in the research of chemical industry and material science.The extreme utilization of reactive sites has led to the emergence and development of atomically dispersed materials(ADMs).The highly active coordination unsaturated metal sites and fully utilized metal atoms make ADMs show great potential in catalytic reactions.The adjustment of coordination environment and electronic structure provides more possibilities for constructing reactive centers with different properties.This review summarized the application and research progress of ADMs in different fields.The design strategy and structure–activity relationship of ADMs for specific reactions were summarized and analyzed.Moreover,we also provided advices for the challenges and opportunities faced by ADMs in catalytic reactions.
基金supported by the Australian Research Council (DE220100521 and DP200101217)supported by Fellow research grant of National University of Mongolia (No.P2021-4197)+2 种基金the support of Griffith University internal grantssupport from King Abdullah University of Science and Technology (KAUST)through the Ibn Rushd Postdoctoral Fellowship Awardsupport from the US Office of Naval Research (ONR),Office of Naval Research Global (ONRG)under the grant N62909-23-1-2035。
文摘Transition metal carbides and nitrides(MXenes)nanosheets are attractive two-dimensional(2D)materials,but they suffer from oxidation/degradation issues during storage and/or applications due to their sensitivity to water and oxygen.Despite the great research progress,the exact oxidation kinetics of Ti_(3)C_(2)T_(x)(MXene)and their final products after oxidation are not fully understood.Herein,we systematically tracked the oxidation process of few-layer Ti_(3)C_(2)T_(x) nanosheets in an aqueous solution at room temperature over several weeks.We also studied the oxidation effects on the electrocatalytic properties of Ti_(3)C_(2)T_(x) for hydrogen evolution reaction and found that the overpotential to achieve a current density of 10 mA cm^(-2)increases from 0.435 to 0.877 V after three weeks of degradation,followed by improvement to stabilized values of around 0.40 V after eight weeks.These results suggest that severely oxidized MXene could be a promising candidate for designing efficient catalysts.According to our detailed experimental characterization and theoretical calculations,unlike previous studies,black titanium oxide is formed as the final product in addition to white Ti(IV)oxide and disordered carbons after the complete oxidation of Ti_(3)C_(2)T_(x).This work presents significant advancements in better understanding of 2D Ti_(3)C_(2)T_(x)(MXene)oxidation and enhances the prospects of this material for various applications.