Polar surfaces are prevalent in metal oxides,the interactions between surface species with polar surfaces are different from those with non-polar surfaces,a thorough understanding of the interactions is key to regulat...Polar surfaces are prevalent in metal oxides,the interactions between surface species with polar surfaces are different from those with non-polar surfaces,a thorough understanding of the interactions is key to regulate the performance of heterogeneous catalysts.In this work,we delve into the interaction of Pt_(n)(n=1-4)with polar ZnO(0001)-Zn and ZnO(0001)-O,and the influence of the surface polarity on the electronic structures and reactivity of Pt_(n)by using density functional theory calculations.The results suggest distinct differences in electronic structures of two exposed terminations,leading to different interactions with Pt_(n).The interaction between Pt_(n)and two terminations not only stabilizes the surface and clusters through polar compensation,but also induces opposite charges on the cluster at two terminations.Remarkably,the Pearson correlation coefficient reveals the interdependency between the electronic states of Pt_(n)and its performance in terms of small molecule adsorption/activation.These observations demonstrate the crucial role of surface polarity in regulating the electronic states and catalytic performance of active sites,and offer a possible design principle for supported catalysts.展开更多
The direct synthesis of dimethyl carbonate(DMC)from CO_(2)and methanol has attracted much attention as an environmentally benign and alternative route for conventional routes.Herein,a series of cerium oxide catalysts ...The direct synthesis of dimethyl carbonate(DMC)from CO_(2)and methanol has attracted much attention as an environmentally benign and alternative route for conventional routes.Herein,a series of cerium oxide catalysts with various textural features and surface properties were prepared by the one-pot synthesis method for the direct DMC synthesis from CO_(2)and methanol,and the structure-performance relationship was investigated in detail.Characterization results revealed that both of surface acid-base properties and the oxygen vacancies contents decreased with the rising crystallinity at increasingly higher calcination temperature accompanied by an unexpectedly volcano-shaped trend of DMC yield observed on the catalysts.In situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS)studies indicated that the adsorption rate of methanol is slower than that of CO_(2)and the methanol activation state largely influences the formation of key intermediate.Although the enhanced surface acidity-basicity and oxygen vacancies brought by low-temperature calcination could facilitate the activation of CO_(2),the presence of excess strongly basic sites on low-crystallinity sample was detrimental to DMC synthesis due to the preferred formation of unreactive mono/polydentate carbonates as well as the further impediment of methanol activation.Moreover,with the use of 2-cyanopyridine as a dehydration reagent,the DMC synthesis was found to be both influenced by the promotion from the rapid in situ removal of water and the inhibition from the competitive adsorption of hydration products on the same active sites.展开更多
A peculiar sawfly genus from middle Asia,Cacosyndya Kirby,1883 and the type species Cacosyndya dimorpha(Freymuth,1870)are redescribed and illustrated.The systematic position of this genus in Tenthredinidae is discusse...A peculiar sawfly genus from middle Asia,Cacosyndya Kirby,1883 and the type species Cacosyndya dimorpha(Freymuth,1870)are redescribed and illustrated.The systematic position of this genus in Tenthredinidae is discussed.The females in the genus are apterous,the only known apterous Symphytan,but the male is normally winged.Cacosyndya is not a member of Fenusinae or Heterarthrinae,but a member of Phymatocerini of Blennocampinae,Tenthredinidae as shown by the structure of the antenna,wing venation and body structure.The relationship between Cacosyndya and members of Phymatocerini is briefly discussed.展开更多
Dynamical behaviors of a class of second order Hopfield neural networks with time delays is investigated.The existence of a unique equilibrium point is proved by using Brouwer's fixed point theorem and the counter...Dynamical behaviors of a class of second order Hopfield neural networks with time delays is investigated.The existence of a unique equilibrium point is proved by using Brouwer's fixed point theorem and the counter proof method,and some sufficient conditions for the global asymptotic stability of the equilibrium point are obtained through the combination of a suitable Lyapunov function and an algebraic inequality technique.展开更多
Species of Pamphiliidae in the Himalaya region are quite rare.Only seven species belonging to three genera of this family have been recorded.Two new species of Pamphiliidae from Linzhi,Xizang of China are described:Ce...Species of Pamphiliidae in the Himalaya region are quite rare.Only seven species belonging to three genera of this family have been recorded.Two new species of Pamphiliidae from Linzhi,Xizang of China are described:Cephalcia xizangica Wei sp.nov.and Onycholyda nigrothorax Wei sp.nov.Cephalcia is recorded from the Himalaya region for the first time.A key to currently known species of Pamphiliidae from Himalayas is provided.展开更多
Background,aim,and scope Solar radiation is the main source of energy for terrestrial ecosystems.Small changes in the absorption of solar radiation at the ground surface can have a significant impact on the climatic e...Background,aim,and scope Solar radiation is the main source of energy for terrestrial ecosystems.Small changes in the absorption of solar radiation at the ground surface can have a significant impact on the climatic environment.Natural and anthropogenic changes in ground cover are important factors affecting the absorption of solar radiation at the ground surface.This phenomenon is particularly pronounced in the mid and high latitudes.In order to quantify the inf luence of surface cover change on the absorption of solar radiation at the surface and to provide a scientific basis for changes in the climatic environment,this paper analyzed ground cover change,ground absorbed solar radiation change and the effect of ground cover change on ground absorbed solar radiation in the Three Northeastern Provinces of China from 2001 to 2018.Materials and methods In this study,the Three Northeastern Provinces of China were used as the study area.Firstly,satellite remote sensing data were used to obtain land cover data and albedo data for Aug.1st of each year in 2001,2005,2010,2015 and 2018.The albedo data were further used to calculate the absorbed solar radiation data at the ground surface.Next,the land cover data were used to count the area changes and shifts of different land classes over the five-year period.The land cover data were overlaid with the surface absorbed solar radiation data to obtain the mean and standard deviation of radiation absorption for different ground classes.The surface absorbed solar radiation data were subtracted to obtain the changes in surface absorbed solar radiation for 2001-2005,2005-2010,2010-2015 and 2015-2018.Ultimately,we used a combination of shifted changes in ground classes and changes in surface absorbed solar radiation data,with unchanged ground classes as a baseline and data such as slope orientation as an aid.We analyzed the effect of ground cover change on surface absorbed solar radiation at regional and pixel point scales.Results(1)The area of woodland and waters in the Three Northeastern Provinces of China increased and then decreased from 2001 to 2018,with an overall increase of 3.96%and 10.51%respectively.Cropland decreased and then increased,with a total decrease of 1.22%.Grassland continued to decrease,with an overall decrease of 19.36%.Building sites increased all the time,with a total increase of 11.08%.The main types of ground cover shifted were woodland,cropland and grassland.The main factors for the change in ground cover were China’s woodland protection policy and the saturation of the total woodland stock.(2)The five ground types absorb solar radiation in the order of waters>building sites>woodland>grassland>cropland.The surface absorption of solar radiation in the Songnen Plain,the Sanjiang Plain and the Songhua River Basin flowing through the Songnen Plain and the Sanjiang Plain varies significantly,by more than 25 W·m^(-2).(3)Changes in the ground cover type affected the absorption of solar radiation energy by the ground surface.There was a clear trend of interconversion between waters and cropland/grassland,cropland and woodland/grassland.In particular,the conversion of waters to both cropland and grassland radiation absorption values decreased significantly,while the opposite increased.The absolute difference between waters and cropland was a maximum of -156.66 W·m^(-2)in 2010-2015,and between waters and grassland was a maximum of 102.36 W·m^(-2) in 2005-2010.The radiative absorption values of woodland and grassland reclamation declined and conversely increased.The absolute difference between woodland and cropland was a maximum of-13.94 W·m^(-2) in 2010-2015 when woodland converted to cropland,and between grassland and cropland was a maximum of 22.36 W·m^(-2) in 2001-2005 when cropland converted to grassland,respectively.Discussion Ground cover changes in the Three Northeastern Provinces of China from 2001-2018 were inextricably linked to natural factors and the inf luence of Chinese national policies.The main inf luencing factors were China’s woodland protection policy,restoration of woodland fire sites,saturation of total woodland,optimization of cropland patterns,sanding of grassland,expansion of water conservancy projects,and urbanization expansion.There were differences in the radiation absorption characteristics of different ground cover types.This was due to the nature of the ground type itself and the regional environment.When ground cover types changed,their ability to absorb solar radiation also changed.The degree of change could be inf luenced by different ground types and different environmental factors.Different spatial scales can also produce variability.We need to consider the effects of ground cover change on the absorption of solar radiation at the surface in an integrated and comprehensive way.Conclusions The Three Northeastern Provinces of China had frequent changes in ground cover from 2001-2018,with the area of grassland decreased by almost 20%.These changes were due to natural environmental change and policies issued by China since the 21st century.The extent to which solar radiation was absorbed by different ground cover types was different,with grassland being the strongest and cropland the least.In the past few years,the Songnen Plain and Sanjiang Plain regions were the most significant changes in the absorption of solar radiation by the ground cover.The change in ground cover type led to a change in solar radiation absorption at the ground surface,with the conversion of waters to cropland or grassland and the conversion of cropland to woodland or grassland showing the greatest change in radiation absorption values,and vice versa.Of these,the absolute difference in the conversion of waters to cropland amounts to-156.66 W·m^(-2) in 2010-2015.The variation in the absorption of solar radiation at the ground surface was related to the characteristics of the ground class itself,but was also limited by the regional environment.Recommendations and perspectives This study showed that surface cover change can affect the absorption of solar radiation at the surface to varying degrees.The unchanged land classes were used as a comparative analysis in this paper,and it was clear from the paper that some of the unchanged land classes showed significant changes in radiation absorption that should be of interest in future studies.展开更多
A series of Co–Cr–O mixed oxides with different Co/Cr molar ratios are synthesized and tested for the total oxidation of propane.The reaction behaviors are closely related to the structural features of the mixed oxi...A series of Co–Cr–O mixed oxides with different Co/Cr molar ratios are synthesized and tested for the total oxidation of propane.The reaction behaviors are closely related to the structural features of the mixed oxides.The catalyst with a Co/Cr molar ratio of 1:2(1 Co2 Cr)and a spinel structure has the best activity(with a reaction rate of 1.38μmol g^–1 s^–1 at 250℃),which is attributed to the synergistic roles of its high surface acidity and good low-temperature reducibility,as evidenced by the temperature-programmed desorption of ammonia,reduction of hydrogen,and surface reaction of propane.Kinetic study shows that the reaction orders of propane and oxygen on the 1 Co2 Cr catalyst(0.58±0.03 and 0.34±0.05,respectively)are lower than those on the 2 Co1 Cr catalyst(0.77±0.02 and 0.98±0.16,respectively)and 1 Co5 Cr(0.66±0.05 and 1.30±0.11,respectively),indicating that the coverages of propane and oxygen on 1 Co2 Cr are higher than those on the other catalysts due to its higher surface acidity and higher reducibility.In addition,in-situ diffuse reflectance infrared spectroscopic investigation reveals that the main surface species on 1 Co2 Cr during the reaction are polydentate carbonate species,which accumulate on the surface at low temperatures(<250℃)but decompose at relatively high temperatures.展开更多
The photocatalytic activity of a semiconductor‐based photocatalyst largely depends on the semiconductor’s intrinsic crystal and electronic properties.We have prepared two types of La and Cr co‐doped SrTiO3photocata...The photocatalytic activity of a semiconductor‐based photocatalyst largely depends on the semiconductor’s intrinsic crystal and electronic properties.We have prepared two types of La and Cr co‐doped SrTiO3photocatalysts(SrTiO3(La,Cr))using the polymerized complex method(PCM)and sol‐gel hydrothermal method(SHM).Under?>420‐nm visible light irradiation,only the Pt‐loaded SrTiO3(La,Cr)prepared by the SHM showed efficient photocatalytic activities for both H2evolution in the presence of an I?sacrificial reagent and for Z‐scheme overall water splitting when it was coupled with the Pt‐loaded WO3in the presence of I?and IO3?as the shuttle redox mediator.The superior photocatalytic activity of SrTiO3(La,Cr)prepared by the SHM has been ascribed to its more negative conduction‐band position,higher carrier concentration,and higher carrier mobility,demonstrating that the design and synthesis of an H2‐evolution photocatalyst with appropriate electronic properties is crucial for achieving Z‐scheme overall water splitting.展开更多
Elucidation of the CuOx-CeO2 interactions is of great interest and importance in understanding complex CuOx-CeO2 interfacial catalysis in various reactions. In the present work, we have investigated structures and cat...Elucidation of the CuOx-CeO2 interactions is of great interest and importance in understanding complex CuOx-CeO2 interfacial catalysis in various reactions. In the present work, we have investigated structures and catalytic activity in CO oxidation of CuOx species on CeO2 rods, cubes and polyhedra predominantly exposing {110}+{100}, {100} and {111} facets by the incipient wetness impregnation method with the lowest Cu loading of 0.025%. The structural evolution of CuOx species was found to depend on both the Cu loading and the CeO2 morphology. As the Cu loading increases, CuOx species are deposited preferentially on the surface defect of CeO2 and then aggregate and grow, accompanied by the formation of isolated Cu ions, CuOx clusters strongly/weakly interacting with the CeO2, highly dispersed Cu O nanoparticles, and large Cu O nanoparticles. The isolated Cu^+ species and CuOx clusters weakly interacting with the CeO2 were observed mainly on the O-terminated CeO2{100} facets. Meanwhile, more Cu(I) species are stabilized during CO reduction processes in CuOx/c-CeO2 catalysts than in CuOx/r-CeO2 and CuOx/p-CeO2 catalysts. The catalytic activities of various CuOx/CeO2 catalysts in CO oxidation vary with both the CuOx species and the CeO2 morphology. These results comprehensively elucidate the CuOx-CeO2 interactions and exemplify their morphology-dependence.展开更多
We report the fabrication and photocatalytic property of a composite of C/CaFe2O4nanorods(NRs)in an effort to reveal the influence of carbon modification.It is demonstrated that the photocatalytic degradation activity...We report the fabrication and photocatalytic property of a composite of C/CaFe2O4nanorods(NRs)in an effort to reveal the influence of carbon modification.It is demonstrated that the photocatalytic degradation activity is dependent on the mass ratio of C to CaFe2O4.The optimal carbon content is determined to be58wt%to yield a methylene blue(MB)degradation rate of0.0058min.1,which is4.8times higher than that of the pristine CaFe2O4NRs.The decoration of carbon on the surface of CaFe2O4NRs improves its adsorption capacity of the MB dye,which is specifically adsorbed on the surface as a monolayer according to the adsorption isotherm analysis.The trapping experiments of the reactive species indicate that superoxide radicals(.O2)are the main active species responsible for the removal of MB under visible‐light irradiation.Overall,the unique feature of carbon coating enables the efficient separation and transfer of photogenerated electrons and holes,strengthens the adsorption capacity of MB,and improves the light harvesting capability,hence enhancing the overall photocatalytic degradation of MB.展开更多
基金This work was financially supported by the National Natural Science Foundation of China(Nos.22303085,22102150 and 22172146)the Zhejiang Provincial Natural Science Foundation of China(LQ24B030014 andLQ21B030010).
文摘Polar surfaces are prevalent in metal oxides,the interactions between surface species with polar surfaces are different from those with non-polar surfaces,a thorough understanding of the interactions is key to regulate the performance of heterogeneous catalysts.In this work,we delve into the interaction of Pt_(n)(n=1-4)with polar ZnO(0001)-Zn and ZnO(0001)-O,and the influence of the surface polarity on the electronic structures and reactivity of Pt_(n)by using density functional theory calculations.The results suggest distinct differences in electronic structures of two exposed terminations,leading to different interactions with Pt_(n).The interaction between Pt_(n)and two terminations not only stabilizes the surface and clusters through polar compensation,but also induces opposite charges on the cluster at two terminations.Remarkably,the Pearson correlation coefficient reveals the interdependency between the electronic states of Pt_(n)and its performance in terms of small molecule adsorption/activation.These observations demonstrate the crucial role of surface polarity in regulating the electronic states and catalytic performance of active sites,and offer a possible design principle for supported catalysts.
文摘The direct synthesis of dimethyl carbonate(DMC)from CO_(2)and methanol has attracted much attention as an environmentally benign and alternative route for conventional routes.Herein,a series of cerium oxide catalysts with various textural features and surface properties were prepared by the one-pot synthesis method for the direct DMC synthesis from CO_(2)and methanol,and the structure-performance relationship was investigated in detail.Characterization results revealed that both of surface acid-base properties and the oxygen vacancies contents decreased with the rising crystallinity at increasingly higher calcination temperature accompanied by an unexpectedly volcano-shaped trend of DMC yield observed on the catalysts.In situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS)studies indicated that the adsorption rate of methanol is slower than that of CO_(2)and the methanol activation state largely influences the formation of key intermediate.Although the enhanced surface acidity-basicity and oxygen vacancies brought by low-temperature calcination could facilitate the activation of CO_(2),the presence of excess strongly basic sites on low-crystallinity sample was detrimental to DMC synthesis due to the preferred formation of unreactive mono/polydentate carbonates as well as the further impediment of methanol activation.Moreover,with the use of 2-cyanopyridine as a dehydration reagent,the DMC synthesis was found to be both influenced by the promotion from the rapid in situ removal of water and the inhibition from the competitive adsorption of hydration products on the same active sites.
基金supported by the National Natural Science Foundation of China(3237050031172142)。
文摘A peculiar sawfly genus from middle Asia,Cacosyndya Kirby,1883 and the type species Cacosyndya dimorpha(Freymuth,1870)are redescribed and illustrated.The systematic position of this genus in Tenthredinidae is discussed.The females in the genus are apterous,the only known apterous Symphytan,but the male is normally winged.Cacosyndya is not a member of Fenusinae or Heterarthrinae,but a member of Phymatocerini of Blennocampinae,Tenthredinidae as shown by the structure of the antenna,wing venation and body structure.The relationship between Cacosyndya and members of Phymatocerini is briefly discussed.
基金Research supported by the National Natural Science Foundation of China(12271220)postgraduate research and practice innovation program of Jiangsu Province(KYCX24-3010)。
文摘Dynamical behaviors of a class of second order Hopfield neural networks with time delays is investigated.The existence of a unique equilibrium point is proved by using Brouwer's fixed point theorem and the counter proof method,and some sufficient conditions for the global asymptotic stability of the equilibrium point are obtained through the combination of a suitable Lyapunov function and an algebraic inequality technique.
基金partly supported by the National Natural Science Foundation of China(323705003197044731672344)。
文摘Species of Pamphiliidae in the Himalaya region are quite rare.Only seven species belonging to three genera of this family have been recorded.Two new species of Pamphiliidae from Linzhi,Xizang of China are described:Cephalcia xizangica Wei sp.nov.and Onycholyda nigrothorax Wei sp.nov.Cephalcia is recorded from the Himalaya region for the first time.A key to currently known species of Pamphiliidae from Himalayas is provided.
文摘Background,aim,and scope Solar radiation is the main source of energy for terrestrial ecosystems.Small changes in the absorption of solar radiation at the ground surface can have a significant impact on the climatic environment.Natural and anthropogenic changes in ground cover are important factors affecting the absorption of solar radiation at the ground surface.This phenomenon is particularly pronounced in the mid and high latitudes.In order to quantify the inf luence of surface cover change on the absorption of solar radiation at the surface and to provide a scientific basis for changes in the climatic environment,this paper analyzed ground cover change,ground absorbed solar radiation change and the effect of ground cover change on ground absorbed solar radiation in the Three Northeastern Provinces of China from 2001 to 2018.Materials and methods In this study,the Three Northeastern Provinces of China were used as the study area.Firstly,satellite remote sensing data were used to obtain land cover data and albedo data for Aug.1st of each year in 2001,2005,2010,2015 and 2018.The albedo data were further used to calculate the absorbed solar radiation data at the ground surface.Next,the land cover data were used to count the area changes and shifts of different land classes over the five-year period.The land cover data were overlaid with the surface absorbed solar radiation data to obtain the mean and standard deviation of radiation absorption for different ground classes.The surface absorbed solar radiation data were subtracted to obtain the changes in surface absorbed solar radiation for 2001-2005,2005-2010,2010-2015 and 2015-2018.Ultimately,we used a combination of shifted changes in ground classes and changes in surface absorbed solar radiation data,with unchanged ground classes as a baseline and data such as slope orientation as an aid.We analyzed the effect of ground cover change on surface absorbed solar radiation at regional and pixel point scales.Results(1)The area of woodland and waters in the Three Northeastern Provinces of China increased and then decreased from 2001 to 2018,with an overall increase of 3.96%and 10.51%respectively.Cropland decreased and then increased,with a total decrease of 1.22%.Grassland continued to decrease,with an overall decrease of 19.36%.Building sites increased all the time,with a total increase of 11.08%.The main types of ground cover shifted were woodland,cropland and grassland.The main factors for the change in ground cover were China’s woodland protection policy and the saturation of the total woodland stock.(2)The five ground types absorb solar radiation in the order of waters>building sites>woodland>grassland>cropland.The surface absorption of solar radiation in the Songnen Plain,the Sanjiang Plain and the Songhua River Basin flowing through the Songnen Plain and the Sanjiang Plain varies significantly,by more than 25 W·m^(-2).(3)Changes in the ground cover type affected the absorption of solar radiation energy by the ground surface.There was a clear trend of interconversion between waters and cropland/grassland,cropland and woodland/grassland.In particular,the conversion of waters to both cropland and grassland radiation absorption values decreased significantly,while the opposite increased.The absolute difference between waters and cropland was a maximum of -156.66 W·m^(-2)in 2010-2015,and between waters and grassland was a maximum of 102.36 W·m^(-2) in 2005-2010.The radiative absorption values of woodland and grassland reclamation declined and conversely increased.The absolute difference between woodland and cropland was a maximum of-13.94 W·m^(-2) in 2010-2015 when woodland converted to cropland,and between grassland and cropland was a maximum of 22.36 W·m^(-2) in 2001-2005 when cropland converted to grassland,respectively.Discussion Ground cover changes in the Three Northeastern Provinces of China from 2001-2018 were inextricably linked to natural factors and the inf luence of Chinese national policies.The main inf luencing factors were China’s woodland protection policy,restoration of woodland fire sites,saturation of total woodland,optimization of cropland patterns,sanding of grassland,expansion of water conservancy projects,and urbanization expansion.There were differences in the radiation absorption characteristics of different ground cover types.This was due to the nature of the ground type itself and the regional environment.When ground cover types changed,their ability to absorb solar radiation also changed.The degree of change could be inf luenced by different ground types and different environmental factors.Different spatial scales can also produce variability.We need to consider the effects of ground cover change on the absorption of solar radiation at the surface in an integrated and comprehensive way.Conclusions The Three Northeastern Provinces of China had frequent changes in ground cover from 2001-2018,with the area of grassland decreased by almost 20%.These changes were due to natural environmental change and policies issued by China since the 21st century.The extent to which solar radiation was absorbed by different ground cover types was different,with grassland being the strongest and cropland the least.In the past few years,the Songnen Plain and Sanjiang Plain regions were the most significant changes in the absorption of solar radiation by the ground cover.The change in ground cover type led to a change in solar radiation absorption at the ground surface,with the conversion of waters to cropland or grassland and the conversion of cropland to woodland or grassland showing the greatest change in radiation absorption values,and vice versa.Of these,the absolute difference in the conversion of waters to cropland amounts to-156.66 W·m^(-2) in 2010-2015.The variation in the absorption of solar radiation at the ground surface was related to the characteristics of the ground class itself,but was also limited by the regional environment.Recommendations and perspectives This study showed that surface cover change can affect the absorption of solar radiation at the surface to varying degrees.The unchanged land classes were used as a comparative analysis in this paper,and it was clear from the paper that some of the unchanged land classes showed significant changes in radiation absorption that should be of interest in future studies.
基金financially supported by the National Natural Science Foundation of China(21773212,21872124)~~
文摘A series of Co–Cr–O mixed oxides with different Co/Cr molar ratios are synthesized and tested for the total oxidation of propane.The reaction behaviors are closely related to the structural features of the mixed oxides.The catalyst with a Co/Cr molar ratio of 1:2(1 Co2 Cr)and a spinel structure has the best activity(with a reaction rate of 1.38μmol g^–1 s^–1 at 250℃),which is attributed to the synergistic roles of its high surface acidity and good low-temperature reducibility,as evidenced by the temperature-programmed desorption of ammonia,reduction of hydrogen,and surface reaction of propane.Kinetic study shows that the reaction orders of propane and oxygen on the 1 Co2 Cr catalyst(0.58±0.03 and 0.34±0.05,respectively)are lower than those on the 2 Co1 Cr catalyst(0.77±0.02 and 0.98±0.16,respectively)and 1 Co5 Cr(0.66±0.05 and 1.30±0.11,respectively),indicating that the coverages of propane and oxygen on 1 Co2 Cr are higher than those on the other catalysts due to its higher surface acidity and higher reducibility.In addition,in-situ diffuse reflectance infrared spectroscopic investigation reveals that the main surface species on 1 Co2 Cr during the reaction are polydentate carbonate species,which accumulate on the surface at low temperatures(<250℃)but decompose at relatively high temperatures.
基金supported by the National Natural Science Foundation of China (21763013, 21473189)the National Key Research and Development Program of China (2017YFA0204804)~~
文摘The photocatalytic activity of a semiconductor‐based photocatalyst largely depends on the semiconductor’s intrinsic crystal and electronic properties.We have prepared two types of La and Cr co‐doped SrTiO3photocatalysts(SrTiO3(La,Cr))using the polymerized complex method(PCM)and sol‐gel hydrothermal method(SHM).Under?>420‐nm visible light irradiation,only the Pt‐loaded SrTiO3(La,Cr)prepared by the SHM showed efficient photocatalytic activities for both H2evolution in the presence of an I?sacrificial reagent and for Z‐scheme overall water splitting when it was coupled with the Pt‐loaded WO3in the presence of I?and IO3?as the shuttle redox mediator.The superior photocatalytic activity of SrTiO3(La,Cr)prepared by the SHM has been ascribed to its more negative conduction‐band position,higher carrier concentration,and higher carrier mobility,demonstrating that the design and synthesis of an H2‐evolution photocatalyst with appropriate electronic properties is crucial for achieving Z‐scheme overall water splitting.
文摘Elucidation of the CuOx-CeO2 interactions is of great interest and importance in understanding complex CuOx-CeO2 interfacial catalysis in various reactions. In the present work, we have investigated structures and catalytic activity in CO oxidation of CuOx species on CeO2 rods, cubes and polyhedra predominantly exposing {110}+{100}, {100} and {111} facets by the incipient wetness impregnation method with the lowest Cu loading of 0.025%. The structural evolution of CuOx species was found to depend on both the Cu loading and the CeO2 morphology. As the Cu loading increases, CuOx species are deposited preferentially on the surface defect of CeO2 and then aggregate and grow, accompanied by the formation of isolated Cu ions, CuOx clusters strongly/weakly interacting with the CeO2, highly dispersed Cu O nanoparticles, and large Cu O nanoparticles. The isolated Cu^+ species and CuOx clusters weakly interacting with the CeO2 were observed mainly on the O-terminated CeO2{100} facets. Meanwhile, more Cu(I) species are stabilized during CO reduction processes in CuOx/c-CeO2 catalysts than in CuOx/r-CeO2 and CuOx/p-CeO2 catalysts. The catalytic activities of various CuOx/CeO2 catalysts in CO oxidation vary with both the CuOx species and the CeO2 morphology. These results comprehensively elucidate the CuOx-CeO2 interactions and exemplify their morphology-dependence.
基金supported by the National Natural Science Foundation of China(21503100)Natural Science Foundation of Jiangxi Province(20161BAB213071,20151BAB213010)+1 种基金Project of Education Department of Jiangxi Province(GJJ150325)Sponsored Program for Cultivating Youths of Outstanding Ability in Jiangxi Normal University~~
文摘We report the fabrication and photocatalytic property of a composite of C/CaFe2O4nanorods(NRs)in an effort to reveal the influence of carbon modification.It is demonstrated that the photocatalytic degradation activity is dependent on the mass ratio of C to CaFe2O4.The optimal carbon content is determined to be58wt%to yield a methylene blue(MB)degradation rate of0.0058min.1,which is4.8times higher than that of the pristine CaFe2O4NRs.The decoration of carbon on the surface of CaFe2O4NRs improves its adsorption capacity of the MB dye,which is specifically adsorbed on the surface as a monolayer according to the adsorption isotherm analysis.The trapping experiments of the reactive species indicate that superoxide radicals(.O2)are the main active species responsible for the removal of MB under visible‐light irradiation.Overall,the unique feature of carbon coating enables the efficient separation and transfer of photogenerated electrons and holes,strengthens the adsorption capacity of MB,and improves the light harvesting capability,hence enhancing the overall photocatalytic degradation of MB.