Constructing heterojunctions have received significant attention in photocatalysis because of their effi-cient separation of photogenerated carriers and improving light utilization efficiency.Bimetallic sulfides(e.g.N...Constructing heterojunctions have received significant attention in photocatalysis because of their effi-cient separation of photogenerated carriers and improving light utilization efficiency.Bimetallic sulfides(e.g.NiCo_(2)S_(4))are applied in electrocatalysis and supercapacitors that can be coupled with TiO_(2)to form a heterojunction.Owing to the staggered energy band arrangement between TiO_(2)and NiCo_(2)S_(4),the es-tablishing of a Z-scheme heterojunction between them is expected to enhance the carrier separation effi-ciency and reduce the sulfide photo-corrosion.However,the application of NiCo_(2)S_(4)in photocatalysis and studies on the mechanism of the TiO_(2)/NiCo_(2)S_(4)Z-scheme heterojunction have seldom been reported.In this work,we obtained a hollow core-shell TiO_(2)/NiCo_(2)S_(4)Z-scheme photocatalyst through a solvothermal method for photocatalytic hydrogen evolution(PHE).The PHE rate of the optimized TiO_(2)/NiCo_(2)S_(4)-0.3 is 8.55 mmol g^(−1)h^(−1),approximately 34 times higher than pure TiO_(2),94 times higher than pure NiCo_(2)S_(4).The remarkable photocatalytic activity can be ascribed to the hollow structure and the in-situ constructed Z-scheme heterojunction.The photogenerated charge transfer mechanism is revealed by hydroxyl radical trapping experiments and electron paramagnetic resonance(EPR)characterization.The in-situ construc-tion of the Z-scheme heterojunction not only enhances the efficiency of separating the photogenerated carriers but also reduces the photo-corrosion of NiCo_(2)S_(4).This study proposes an effective strategy for the design of TiO_(2)-based Z-scheme heterojunctions and the application of NiCo_(2)S_(4)in photocatalysis.展开更多
The trends and characteristics of global CH_(4)emissions were analyzed using greenhouse gas data reported by both Annex I and non-Annex I countries under the United Nations Framework Convention on Climate Change(UNFCC...The trends and characteristics of global CH_(4)emissions were analyzed using greenhouse gas data reported by both Annex I and non-Annex I countries under the United Nations Framework Convention on Climate Change(UNFCCC)from 1990 to 2021.The results show the following:(1)In 2021,the cumulative CH_(4)emissions from the 42 nations listed in Annex I of the UNFCCC amounted to 1871521.79 kt CO_(2)eq.The top 10 countries account for 82.0%of the total CH_(4)emissions.(2)Most Annex I countries showed a gradual decline in CH_(4)emissions over the period.In contrast,emissions from non-Annex I countries have increased year by year.Notably,CH_(4)emissions in the United States,the European Union,the Russian Federation,and Ukraine decreased by 14.0%,37.4%,24.0%,and 60.9%,respectively.(3)In 2020,the CH_(4)emissions of the agriculture,energy,waste treatment and LULUCF(land use,land-use change and forestry)sectors in Annex I countries were 72240.43,63863.51,41573.08,and 889019 million tons of CO_(2)eq,accounting for 38.6%,34.1%,22.2%,and 4.8%,respectively.Among non-Annex I countries,the main CH_(4)sources vary by country.In China and Mexico,energy and agriculture were the largest contributors,accounting for 44.8%and 40.2%in China,and 34.4%and 43.3%in Mexico,respectively.In India,Brazil,Nigeria,Argentina,and Vietnam,agriculture dominated,contributing 73.8%,75.8%,59.7%,60.3%,and 58.5%of total emissions,respectively.Indonesia was an exception,with waste treatment being the primary source,accounting for 64.8%of its total CH_(4)emissions.展开更多
Plasma-based CO_(2)conversion is promising for carbon capture and utilization.However,inconsistent reporting of the performance metrics makes it difficult to compare plasma processes systematically,complicates elucida...Plasma-based CO_(2)conversion is promising for carbon capture and utilization.However,inconsistent reporting of the performance metrics makes it difficult to compare plasma processes systematically,complicates elucidating the underlying mechanisms and compromises further development of this technology.Therefore,this critical review summarizes the correct definitions for gas conversion in plasma reactors and highlights common errors and inconsistencies observed throughout literature.This is done for pure CO_(2)splitting,dry reforming of methane and CO_(2)hydrogenation.We demonstrate that the change in volumetric flow rate is a critical aspect,inherent to these reactions,that is often not correctly taken into account.For dry reforming of methane and CO_(2)hydrogenation,we also demonstrate inconsistent reporting of energy efficiency,and through numerical examples,we show the significance of these deviations.Furthermore,we discuss how to measure changes in volumetric flow rate,supported by data from two experimental examples,showing that the sensitivity inherent to a standard component and a flow meter is essential to consider when deriving the performance metrics.Finally,some general recommendations and good practices are provided.This paper aims to be a comprehensive guideline for authors,to encourage more consistent calculations and stimulate the further development of this technology.展开更多
MXenes,a new family of functional two-dimensional(2 D) materials,have shown great potential for an extensive variety of applications within the last decade.Atomic defects and functional groups in MXenes are known to h...MXenes,a new family of functional two-dimensional(2 D) materials,have shown great potential for an extensive variety of applications within the last decade.Atomic defects and functional groups in MXenes are known to have a tremendous influence on the functional properties.In this review,we focus on recent progress in the characterization of atomic defects and functional group chemistry in MXenes,and how to control them to directly influence various properties(e.g.,electron transport,Li^(+) adsorption,hydrogen evolution reaction(HER) activity,and magnetism) of 2 D MXenes materials.Dynamic structural transformations such as oxidation and growth induced by atomic defects in MXenes are also discussed.The review thus provides perspectives on property optimization through atomic defect engineering,and bottom-up synthesis methods based on defect-assisted homoepitaxial growth of MXenes.展开更多
The effect of Cu on the evolution of the Al_(3)Zr phase in an Al-Cu-Zr cast alloy during solution treatment at 500℃has been thoroughly studied by combining atomic resolution high-angle annular dark-field scanning tra...The effect of Cu on the evolution of the Al_(3)Zr phase in an Al-Cu-Zr cast alloy during solution treatment at 500℃has been thoroughly studied by combining atomic resolution high-angle annular dark-field scanning transmission electron microscopy,energy-dispersive X-ray spectroscopy and first-principles cal-culations.The heat treatment initially produces a pure L1_(2)-Al_(3)Zr microstructure,allowing for about 13%Cu to be incorporated in the dispersoid.Cu incorporation increases the energy barrier for anti-phase boundary(APB)activation,thus stabilizing the L1_(2)structure.Additional heating leads to a Cu-induced“branched”path for the L1_(2)structural transformation,with the latter process accelerated once the first APB has been created.Cu atoms may either(i)be repelled by the APBs,promoting the transformation to a Cu-poor D0_(23) phase,or(ii)they may segregate at one Al-Zr layer adjacent to the APB,promoting a transformation to a new thermodynamically favored phase,Al4 CuZr,formed when these segregation layers are periodically arranged.Theoretical studies suggest that the branching of the L1_(2)transformation path is linked to the speed at which an APB is created,with Cu attraction triggered by a comparatively slow process.This unexpected transformation behavior of the L1_(2)-Al_(3)Zr phase opens a new path to un-derstanding,and potentially regulating the Al_(3)Zr dispersoid evolution for high temperature applications.展开更多
Malachite green (MG) dye is a common industrial dye and organic contaminant that can be found in (waste)water. Textile and food industries make use of MG as dyeing and food coloring agents, respectively. However, MG i...Malachite green (MG) dye is a common industrial dye and organic contaminant that can be found in (waste)water. Textile and food industries make use of MG as dyeing and food coloring agents, respectively. However, MG is both genotoxic and mutagenic. Hence, the elimination of MG from MG-laden-wastewater is germane. This review summarizes up-to-date researches that have been reported in literature as regards the decontamination of toxic MG wastewater. Various removal methods (adsorption, membrane, Fenton system, and heterogenous and homogeneous photodegradation) were discussed. Of the two basic technologies that are comprehensively explored and reviewed, chemical treatment methods are not as viable as physical removal methods, such as the adsorption technology, due to the lack of secondary pollutant production, simple design, low operation costs, and resource availability. This review also presents various practical knowledge gaps needed for large-scale applications of adsorptive removal methods for MG. It concludes by recommending further research on the techniques of cheap and simple decontamination of MG to get clean water.展开更多
Pine wilt is a dramatic disease that kills infected trees within a few weeks to a few months.The cause is the pathogen Pinewood Nematode.Most plant-parasitic nematodes are attached to plant roots,but pinewood nematode...Pine wilt is a dramatic disease that kills infected trees within a few weeks to a few months.The cause is the pathogen Pinewood Nematode.Most plant-parasitic nematodes are attached to plant roots,but pinewood nematodes are found in the tops of trees.Nematodes kill the tree by feeding the cells around the resin ducts.The modeling of a pine wilt disease is based on six compartments,including three for plants(susceptible trees,exposed trees,and infected trees)and the other for the beetles(susceptible beetles,exposed beetles,and infected beetles).The deterministic modeling,along with subpopulations,is based on Law of mass action.The stability of the model along with equilibria is studied rigorously.The authentication of analytical results is examined through well-known computer methods like Non-standard finite difference(NSFD)and the model’s feasible properties(positivity,boundedness,and dynamical consistency).In the end,comparison analysis shows the effectiveness of the NSFD algorithm.展开更多
Steve Pennycook is a pioneer in the application of high-resolution scanning transmission electron microscopy(STEM)and in particular the use of annular dark-field(ADF)imaging.Here we show how a general framework for 4D...Steve Pennycook is a pioneer in the application of high-resolution scanning transmission electron microscopy(STEM)and in particular the use of annular dark-field(ADF)imaging.Here we show how a general framework for 4D STEM allows clear links to be made between ADF imaging and the emerging methods for reconstructing images from 4D STEM data sets.We show that both ADF imaging and ptychographical reconstruction can be thought of in terms of integrating over the overlap regions of diffracted discs in the detector plane.This approach allows the similarities in parts of their transfer functions to be understood,though we note that the transfer functions for ptychographic imaging cannot be used as a measure of information transfer.We also show that conditions of partial spatial and temporal coherence affect ADF imaging and ptychography similarly,showing that achromatic interference can always contribute to the image in both cases,leading to a robustness to partial temporal coherence that has enabled high-resolution imaging.展开更多
Metal halide perovskite(MHP)quantum dots(QDs)offer immense potentialfor several areas of photonics research due to their easy and low-costfabrication and excellent optoelectronic properties.However,practicalapplicatio...Metal halide perovskite(MHP)quantum dots(QDs)offer immense potentialfor several areas of photonics research due to their easy and low-costfabrication and excellent optoelectronic properties.However,practicalapplications of MHP QDs are limited by their poor stability and,in particular,their tendency to aggregate.Here,we develop a two-step double-solventstrategy to grow and confine CsPbBr_(3)QDs within the three-dimensional(3D)cavities of a mesoporous SBA-16 silica scaffold(CsPbBr_(3)@SBA-16).Strongconfinement and separation of the MHP QDs lead to a relatively uniform sizedistribution,narrow luminescence,and good ambient stability over 2 months.In addition,the CsPbBr_(3)@SBA-16 presents a high activity and stability forvisible-light-driven photocatalytic toluene C(sp^(3))-H bond activation toproduce benzaldehyde with~730 umolg^(-1)h^(-l) yield rate and near-unityselectivity.Similarly,the structural stability of CsPbBr_(3)@SBA-16QDs issuperior to that of both pure CsPbBr3 QDs and those confined in MCM-41with 1D channels.展开更多
基金supported by the National Key R&D Program of China(Nos.2022YFB3504000,2021YFE0115800)the National Natural Science Foundation of China(Nos.52103285,22275142,22293022,U22B6011)+2 种基金the Program of Introducing Talents of Dis-cipline to Universities-Plan 111 from the Ministry of Science and Technology and the Ministry of Education of China(Grant No.B20002)the Natural Science Foundation of Hubei Province(No.2023AFB605)the Dawning Program from Bureau of Science and Technology of Wuhan(No.2023020201020306).
文摘Constructing heterojunctions have received significant attention in photocatalysis because of their effi-cient separation of photogenerated carriers and improving light utilization efficiency.Bimetallic sulfides(e.g.NiCo_(2)S_(4))are applied in electrocatalysis and supercapacitors that can be coupled with TiO_(2)to form a heterojunction.Owing to the staggered energy band arrangement between TiO_(2)and NiCo_(2)S_(4),the es-tablishing of a Z-scheme heterojunction between them is expected to enhance the carrier separation effi-ciency and reduce the sulfide photo-corrosion.However,the application of NiCo_(2)S_(4)in photocatalysis and studies on the mechanism of the TiO_(2)/NiCo_(2)S_(4)Z-scheme heterojunction have seldom been reported.In this work,we obtained a hollow core-shell TiO_(2)/NiCo_(2)S_(4)Z-scheme photocatalyst through a solvothermal method for photocatalytic hydrogen evolution(PHE).The PHE rate of the optimized TiO_(2)/NiCo_(2)S_(4)-0.3 is 8.55 mmol g^(−1)h^(−1),approximately 34 times higher than pure TiO_(2),94 times higher than pure NiCo_(2)S_(4).The remarkable photocatalytic activity can be ascribed to the hollow structure and the in-situ constructed Z-scheme heterojunction.The photogenerated charge transfer mechanism is revealed by hydroxyl radical trapping experiments and electron paramagnetic resonance(EPR)characterization.The in-situ construc-tion of the Z-scheme heterojunction not only enhances the efficiency of separating the photogenerated carriers but also reduces the photo-corrosion of NiCo_(2)S_(4).This study proposes an effective strategy for the design of TiO_(2)-based Z-scheme heterojunctions and the application of NiCo_(2)S_(4)in photocatalysis.
基金supported by the National Key Research and Development Program of China[grant number 2022YFC3703003]the Energy Foundation Project[grant number G-2309-35044]the SinoNorwegian Project on Methane from Livestock Production and Waste Management(ChiNorCH4)[grant number CHN-2148,22/0011].
文摘The trends and characteristics of global CH_(4)emissions were analyzed using greenhouse gas data reported by both Annex I and non-Annex I countries under the United Nations Framework Convention on Climate Change(UNFCCC)from 1990 to 2021.The results show the following:(1)In 2021,the cumulative CH_(4)emissions from the 42 nations listed in Annex I of the UNFCCC amounted to 1871521.79 kt CO_(2)eq.The top 10 countries account for 82.0%of the total CH_(4)emissions.(2)Most Annex I countries showed a gradual decline in CH_(4)emissions over the period.In contrast,emissions from non-Annex I countries have increased year by year.Notably,CH_(4)emissions in the United States,the European Union,the Russian Federation,and Ukraine decreased by 14.0%,37.4%,24.0%,and 60.9%,respectively.(3)In 2020,the CH_(4)emissions of the agriculture,energy,waste treatment and LULUCF(land use,land-use change and forestry)sectors in Annex I countries were 72240.43,63863.51,41573.08,and 889019 million tons of CO_(2)eq,accounting for 38.6%,34.1%,22.2%,and 4.8%,respectively.Among non-Annex I countries,the main CH_(4)sources vary by country.In China and Mexico,energy and agriculture were the largest contributors,accounting for 44.8%and 40.2%in China,and 34.4%and 43.3%in Mexico,respectively.In India,Brazil,Nigeria,Argentina,and Vietnam,agriculture dominated,contributing 73.8%,75.8%,59.7%,60.3%,and 58.5%of total emissions,respectively.Indonesia was an exception,with waste treatment being the primary source,accounting for 64.8%of its total CH_(4)emissions.
基金Supported by NSFC(No.11201107,No.11271283,No.11501435)the Natural Science Basic Research Plan in Shaanxi Province of China(No.2016JM1013)the Starting Research Fund for Doctors of Xi'an Polytechnic University(No.BS1508)
基金financial support from the Fund for Scientific Research(FWO)Flanders(Grant ID 110221N)the European Research Council(ERC)under the European Union’s Horizon 2020 Research and Innovation Program(grant agreement No 810182-SCOPE ERC Synergy project)the Methusalem funding of the University of Antwerp。
文摘Plasma-based CO_(2)conversion is promising for carbon capture and utilization.However,inconsistent reporting of the performance metrics makes it difficult to compare plasma processes systematically,complicates elucidating the underlying mechanisms and compromises further development of this technology.Therefore,this critical review summarizes the correct definitions for gas conversion in plasma reactors and highlights common errors and inconsistencies observed throughout literature.This is done for pure CO_(2)splitting,dry reforming of methane and CO_(2)hydrogenation.We demonstrate that the change in volumetric flow rate is a critical aspect,inherent to these reactions,that is often not correctly taken into account.For dry reforming of methane and CO_(2)hydrogenation,we also demonstrate inconsistent reporting of energy efficiency,and through numerical examples,we show the significance of these deviations.Furthermore,we discuss how to measure changes in volumetric flow rate,supported by data from two experimental examples,showing that the sensitivity inherent to a standard component and a flow meter is essential to consider when deriving the performance metrics.Finally,some general recommendations and good practices are provided.This paper aims to be a comprehensive guideline for authors,to encourage more consistent calculations and stimulate the further development of this technology.
基金supported by the National Natural Science Foundation of China(No.51902237)the Fundamental Research Funds for the Central Universities of China(No.WUT:2019III012GX)+1 种基金Nanostructure Research Center(NRC),and Center for Materials Analysis and Testing at Wuhan University of TechnologyA portion of this work was supported by the Fluid Interface Reactions,Structures and Transport(FIRST)Center,an Energy Frontier Research Center funded by the U.S.Department of Energy,Office of Science,Office of Basic Energy Sciences(RRU)。
文摘MXenes,a new family of functional two-dimensional(2 D) materials,have shown great potential for an extensive variety of applications within the last decade.Atomic defects and functional groups in MXenes are known to have a tremendous influence on the functional properties.In this review,we focus on recent progress in the characterization of atomic defects and functional group chemistry in MXenes,and how to control them to directly influence various properties(e.g.,electron transport,Li^(+) adsorption,hydrogen evolution reaction(HER) activity,and magnetism) of 2 D MXenes materials.Dynamic structural transformations such as oxidation and growth induced by atomic defects in MXenes are also discussed.The review thus provides perspectives on property optimization through atomic defect engineering,and bottom-up synthesis methods based on defect-assisted homoepitaxial growth of MXenes.
基金supported by the National Key Research and Development Program(No.2020YFA0405900)the National Natural Science Foundation of China(Grant No.52371111 and U2141215)the Natural Science Foundation of Jiangsu Province(No.BE2022159).
文摘The effect of Cu on the evolution of the Al_(3)Zr phase in an Al-Cu-Zr cast alloy during solution treatment at 500℃has been thoroughly studied by combining atomic resolution high-angle annular dark-field scanning transmission electron microscopy,energy-dispersive X-ray spectroscopy and first-principles cal-culations.The heat treatment initially produces a pure L1_(2)-Al_(3)Zr microstructure,allowing for about 13%Cu to be incorporated in the dispersoid.Cu incorporation increases the energy barrier for anti-phase boundary(APB)activation,thus stabilizing the L1_(2)structure.Additional heating leads to a Cu-induced“branched”path for the L1_(2)structural transformation,with the latter process accelerated once the first APB has been created.Cu atoms may either(i)be repelled by the APBs,promoting the transformation to a Cu-poor D0_(23) phase,or(ii)they may segregate at one Al-Zr layer adjacent to the APB,promoting a transformation to a new thermodynamically favored phase,Al4 CuZr,formed when these segregation layers are periodically arranged.Theoretical studies suggest that the branching of the L1_(2)transformation path is linked to the speed at which an APB is created,with Cu attraction triggered by a comparatively slow process.This unexpected transformation behavior of the L1_(2)-Al_(3)Zr phase opens a new path to un-derstanding,and potentially regulating the Al_(3)Zr dispersoid evolution for high temperature applications.
文摘Malachite green (MG) dye is a common industrial dye and organic contaminant that can be found in (waste)water. Textile and food industries make use of MG as dyeing and food coloring agents, respectively. However, MG is both genotoxic and mutagenic. Hence, the elimination of MG from MG-laden-wastewater is germane. This review summarizes up-to-date researches that have been reported in literature as regards the decontamination of toxic MG wastewater. Various removal methods (adsorption, membrane, Fenton system, and heterogenous and homogeneous photodegradation) were discussed. Of the two basic technologies that are comprehensively explored and reviewed, chemical treatment methods are not as viable as physical removal methods, such as the adsorption technology, due to the lack of secondary pollutant production, simple design, low operation costs, and resource availability. This review also presents various practical knowledge gaps needed for large-scale applications of adsorptive removal methods for MG. It concludes by recommending further research on the techniques of cheap and simple decontamination of MG to get clean water.
文摘Pine wilt is a dramatic disease that kills infected trees within a few weeks to a few months.The cause is the pathogen Pinewood Nematode.Most plant-parasitic nematodes are attached to plant roots,but pinewood nematodes are found in the tops of trees.Nematodes kill the tree by feeding the cells around the resin ducts.The modeling of a pine wilt disease is based on six compartments,including three for plants(susceptible trees,exposed trees,and infected trees)and the other for the beetles(susceptible beetles,exposed beetles,and infected beetles).The deterministic modeling,along with subpopulations,is based on Law of mass action.The stability of the model along with equilibria is studied rigorously.The authentication of analytical results is examined through well-known computer methods like Non-standard finite difference(NSFD)and the model’s feasible properties(positivity,boundedness,and dynamical consistency).In the end,comparison analysis shows the effectiveness of the NSFD algorithm.
基金funding from the European Research Council(ERC)under the European Union’s Horizon 2020 Research and Innovation Programme via Grant Agreement No.802123-HDEM(TJP)from the UK Engineering and Physical Sciences Research Council(EPSRC)via grant EP/M010708/1(PDN).
文摘Steve Pennycook is a pioneer in the application of high-resolution scanning transmission electron microscopy(STEM)and in particular the use of annular dark-field(ADF)imaging.Here we show how a general framework for 4D STEM allows clear links to be made between ADF imaging and the emerging methods for reconstructing images from 4D STEM data sets.We show that both ADF imaging and ptychographical reconstruction can be thought of in terms of integrating over the overlap regions of diffracted discs in the detector plane.This approach allows the similarities in parts of their transfer functions to be understood,though we note that the transfer functions for ptychographic imaging cannot be used as a measure of information transfer.We also show that conditions of partial spatial and temporal coherence affect ADF imaging and ptychography similarly,showing that achromatic interference can always contribute to the image in both cases,leading to a robustness to partial temporal coherence that has enabled high-resolution imaging.
基金Research Foundation—Flanders,Grant/Award Numbers:1242922N,1280021N,12Y7221N,V400622NFlemishgovernment for iBOF funding,Grant/Award Number:PERsist:iBOF-21-085+2 种基金KU Leuven Research Fund,Grant/A ward Number:C14/23/090China Scholarship Council(CSC),Grant/Award Number:201806650002Australian Research Council,Grant/Award Number:DE230100173。
文摘Metal halide perovskite(MHP)quantum dots(QDs)offer immense potentialfor several areas of photonics research due to their easy and low-costfabrication and excellent optoelectronic properties.However,practicalapplications of MHP QDs are limited by their poor stability and,in particular,their tendency to aggregate.Here,we develop a two-step double-solventstrategy to grow and confine CsPbBr_(3)QDs within the three-dimensional(3D)cavities of a mesoporous SBA-16 silica scaffold(CsPbBr_(3)@SBA-16).Strongconfinement and separation of the MHP QDs lead to a relatively uniform sizedistribution,narrow luminescence,and good ambient stability over 2 months.In addition,the CsPbBr_(3)@SBA-16 presents a high activity and stability forvisible-light-driven photocatalytic toluene C(sp^(3))-H bond activation toproduce benzaldehyde with~730 umolg^(-1)h^(-l) yield rate and near-unityselectivity.Similarly,the structural stability of CsPbBr_(3)@SBA-16QDs issuperior to that of both pure CsPbBr3 QDs and those confined in MCM-41with 1D channels.
