The semiconductor gas sensors used for xylene gas detection in real time has been restricted by the inadequate sensitivity and selectivity.Constructing a bilayer cascade sensor with the catalysis-gas sensitivity syner...The semiconductor gas sensors used for xylene gas detection in real time has been restricted by the inadequate sensitivity and selectivity.Constructing a bilayer cascade sensor with the catalysis-gas sensitivity synergistic is considered as an effective solution.Herein,the Ag@CeO_(2)nanosheets are synthesized by heat treating the Ag@Ce-MOF,which synthesized via solvothermal method.The morphological evolution of cerium metalorganic framework(Ce-MOF),regulated by Ag ions,is investigated,and the transformation mechanism is proposed.The bilayer sensors were constructed by using WO_(3)nanofibers,prepared via the electrospinning method,as the sensitive layer and the Ag@CeO_(2)nanosheets as the catalytic layer,respectively.The bilayer sensors exhibit remarkable performance in response to xylene.The response value(R_(a)/R_(g))of WO_(3)/Ag@CeO_(2)sensor to10 ppm xylene gas reaches 32.13 at the operating temperature of 160℃.Additionally,the sensor displays an exceptional response to even trace amounts of xylene,as low as parts per billion(ppb).The catalysis-gas sensitivity synergistic mechanism was elucidated by capturing catalytic intermediates using online mass spectrometry.These findings provide a novel strategy for benzene series(BTEX)sensor and offer a novel approach to prepare twodimensional Ce-MOF and its derived materials with tailored properties.展开更多
In this study,a framework for predicting the gas-sensitive properties of gas-sensitive materials by combining machine learning and density functional theory(DFT)has been proposed.The framework rapidly predicts the gas...In this study,a framework for predicting the gas-sensitive properties of gas-sensitive materials by combining machine learning and density functional theory(DFT)has been proposed.The framework rapidly predicts the gas response of materials by establishing relationships between multisource physical parameters and gas-sensitive properties.In order to prove its effectiveness,the perovskite Cs_(3)Cu_(2)I_(5) has been selected as the representative material.The physical parameters before and after the adsorption of various gases have been calculated using DFT,and then a machine learning model has been trained based on these parameters.Previous studies have shown that a single physical parameter alone is not enough to accurately predict the gas sensitivity of materials.Therefore,a variety of physical parameters have been selected for machine learning,and the final machine learning model achieved 92%accuracy in predicting gas sensitivity.It is important to note that although there have been no previous reports on the response of Cs_(3)Cu_(2)I_(5) to hydrogen sulfide,the resulting model predicts the gas response of H2S;it is subsequently confirmed experimentally.This method not only enhances the understanding of the gas sensing mechanism,but also has a universal nature,making it suitable for the development of various new gas-sensitive materials.展开更多
Zeolitic Imidazolate Framework-8(ZIF-8)material was prepared by chemical precipitation method.The microstructure and physical properties of the as-prepared samples were characterized by XRD,BET,FESEM and UV spectropho...Zeolitic Imidazolate Framework-8(ZIF-8)material was prepared by chemical precipitation method.The microstructure and physical properties of the as-prepared samples were characterized by XRD,BET,FESEM and UV spectrophotometer.The self-made four-channel measurement device was used to test the gas sensitivity of ZIF-8 material toward ethanol gas under photo-thermal synergistic excitation.The results showed that the sample was typical ZIF-8(E_(g)=4.96 eV)with a regular dodecahedron shape and the specific surface is up to 1793 m^(2)/g.The as-prepared ZIF-8 has a gas response value of 55.04 to 100 ppm ethanol at 75℃ and it shows good gas sensing selectivity and repeated stability.The excellent gas sensitivity can be attributed to the increase of free electron concentration in the ZIF-8 conduction band by photo-thermal synergistic excitation,and the large specific surface area of ZIF-8 material provides more active sites for gas-solid surface reaction.The reaction mechanism of ZIF-8 material under multi-field excitation was also discussed.展开更多
Hydrothermal methods are widely used in chemical synthesis of target products with specific morphology and nanostructure.Those methods are very efficient for the preparation of well-controlled structures but the react...Hydrothermal methods are widely used in chemical synthesis of target products with specific morphology and nanostructure.Those methods are very efficient for the preparation of well-controlled structures but the reaction time is usually long.The assistance of microwave makes the reaction system heat up faster,more uniformly and reactions are accelerated,it also can be utilized to change the morphology or structure of materials,which improves the physic-chemical properties of synthesized products and influences its gas-sensing performance.Copper oxide(CuO)is widely applied in semiconductor gas sensors because of its good reactivity and stability.This review article briefly introduces the principle,mechanism and recent development of CuO nanostructures obtained by microwave-as sis ted hydrothermal synthesis(MWHS)process.It also discussed the relation between endopathic factors of material and its gas-sensitive performance.The technical challenges and prospective solutions for highperformance CuO-based gas-sensitive materials with unique nanostructure are proposed.It is pointed out that the hierarchical CuO-based nanostructures and their composite materials prepared by MWHS process are efficacious methods to improve the gas-sensitive performance of the materials.On the basis of the morphology,the materials are divided into nanorods,nanoflowers,nanosheets,nanospheres and other nanostructures.The influence of microwave parameters on the properties of synthetic products is analyzed.The influence followed by metal element loading on the structure and properties of CuO-based materials by MWHS process is further discussed.Then this review summarizes the research progress of graphene-CuO and metal oxide-CuO composites prepared by MWHS process in recent years.展开更多
A model for describing the adsorption process of hydrogen on surface of tungsten oxide was proposed based on the first-principle calculations. Multiple factors such as type of active surface, adsorption site and distr...A model for describing the adsorption process of hydrogen on surface of tungsten oxide was proposed based on the first-principle calculations. Multiple factors such as type of active surface, adsorption site and distribution of oxygen vacancies were considered to evaluate the hydrogen adsorption capability of tungsten oxide. The adsorption Gibbs free energies, electronic structures and bonding characteristics under various conditions were examined to reveal the influence of oxygen vacancies on the surface. It is found that the capability of hydrogen adsorption of tungsten oxide can be significantly enhanced by adjusting the oxygen vacancy on the outermost layer of certain active surfaces. The modeling predicts that the surface structure stability and gas adsorption ability of tungsten oxide can be simultaneously improved through the formation of W–H bonds. The proposed strategy for moderating surface provides a new approach to obtain excellent gas-sensitive metal oxide materials.展开更多
Thin nanocomposite fflms based on tin dioxide with a low content of zinc oxide(0.5–5 mol.%)were obtained by the sol–gel method.The synthesized fflms are 300–600 nm thick and contains pore sizes of 19–29 nm.The res...Thin nanocomposite fflms based on tin dioxide with a low content of zinc oxide(0.5–5 mol.%)were obtained by the sol–gel method.The synthesized fflms are 300–600 nm thick and contains pore sizes of 19–29 nm.The resulting ZnO–SnO_(2) fflms were comprehensively studied by atomic force and Kelvin probe force microscopy,X-ray diffraction,scanning electron microscopy,and high-resolution X-ray photoelectron spectroscopy spectra.The photoconductivity parameters on exposure to light with a wavelength of 470 nm were also studied.The study of the photosensitivity kinetics of ZnO–SnO_(2) fflms showed that the fflm with the Zn:Sn ratio equal to 0.5:99.5 has the minimum value of the charge carrier generation time constant.Measurements of the activation energy of the conductivity,potential barrier,and surface potential of ZnO–SnO_(2) fflms showed that these parameters have maxima at ZnO concentrations of 0.5 mol.%and 1 mol.%.Films with 1 mol.%ZnO exhibit high response values when exposed to 5–50 ppm of nitrogen dioxide at operating temperatures of 200℃ and 250℃.展开更多
基金financially supported by the National Natural Science Foundation of China(Nos.62471303,62071300,22176127,22301181,22406130 and 22476131)Shanghai Sailing Program(Nos.23YF1429000 and 22YF1430400)
文摘The semiconductor gas sensors used for xylene gas detection in real time has been restricted by the inadequate sensitivity and selectivity.Constructing a bilayer cascade sensor with the catalysis-gas sensitivity synergistic is considered as an effective solution.Herein,the Ag@CeO_(2)nanosheets are synthesized by heat treating the Ag@Ce-MOF,which synthesized via solvothermal method.The morphological evolution of cerium metalorganic framework(Ce-MOF),regulated by Ag ions,is investigated,and the transformation mechanism is proposed.The bilayer sensors were constructed by using WO_(3)nanofibers,prepared via the electrospinning method,as the sensitive layer and the Ag@CeO_(2)nanosheets as the catalytic layer,respectively.The bilayer sensors exhibit remarkable performance in response to xylene.The response value(R_(a)/R_(g))of WO_(3)/Ag@CeO_(2)sensor to10 ppm xylene gas reaches 32.13 at the operating temperature of 160℃.Additionally,the sensor displays an exceptional response to even trace amounts of xylene,as low as parts per billion(ppb).The catalysis-gas sensitivity synergistic mechanism was elucidated by capturing catalytic intermediates using online mass spectrometry.These findings provide a novel strategy for benzene series(BTEX)sensor and offer a novel approach to prepare twodimensional Ce-MOF and its derived materials with tailored properties.
基金supported by Natural Science Foundation of Jiangsu Province(No.BK20210494)National Natural Science Foundation of China(No.52303356).
文摘In this study,a framework for predicting the gas-sensitive properties of gas-sensitive materials by combining machine learning and density functional theory(DFT)has been proposed.The framework rapidly predicts the gas response of materials by establishing relationships between multisource physical parameters and gas-sensitive properties.In order to prove its effectiveness,the perovskite Cs_(3)Cu_(2)I_(5) has been selected as the representative material.The physical parameters before and after the adsorption of various gases have been calculated using DFT,and then a machine learning model has been trained based on these parameters.Previous studies have shown that a single physical parameter alone is not enough to accurately predict the gas sensitivity of materials.Therefore,a variety of physical parameters have been selected for machine learning,and the final machine learning model achieved 92%accuracy in predicting gas sensitivity.It is important to note that although there have been no previous reports on the response of Cs_(3)Cu_(2)I_(5) to hydrogen sulfide,the resulting model predicts the gas response of H2S;it is subsequently confirmed experimentally.This method not only enhances the understanding of the gas sensing mechanism,but also has a universal nature,making it suitable for the development of various new gas-sensitive materials.
基金supported by the National Natural Science Foundation of China(No.51864028)the Yunnan Province Science and Technology Major Project for Materials Genetic Engineering of Rare and Precious Metal(No.202002AB080001)+2 种基金the Yunnan Province Funds for Distinguished Young Scientists,(No.2019FJ005)the Science Research Foundation of Yunnan Provincial Education Department(No.2022J0441)the Sichuan Science and Technology Program(No.22QYCX0097)。
文摘Zeolitic Imidazolate Framework-8(ZIF-8)material was prepared by chemical precipitation method.The microstructure and physical properties of the as-prepared samples were characterized by XRD,BET,FESEM and UV spectrophotometer.The self-made four-channel measurement device was used to test the gas sensitivity of ZIF-8 material toward ethanol gas under photo-thermal synergistic excitation.The results showed that the sample was typical ZIF-8(E_(g)=4.96 eV)with a regular dodecahedron shape and the specific surface is up to 1793 m^(2)/g.The as-prepared ZIF-8 has a gas response value of 55.04 to 100 ppm ethanol at 75℃ and it shows good gas sensing selectivity and repeated stability.The excellent gas sensitivity can be attributed to the increase of free electron concentration in the ZIF-8 conduction band by photo-thermal synergistic excitation,and the large specific surface area of ZIF-8 material provides more active sites for gas-solid surface reaction.The reaction mechanism of ZIF-8 material under multi-field excitation was also discussed.
基金financially supported by the National Key Research and Development Program of China(No.2017YFE0115900)the Natural Science Foundation of China(No.51872254)Yangzhou City-Yangzhou University Cooperation Foundation(No.YZU201801)。
文摘Hydrothermal methods are widely used in chemical synthesis of target products with specific morphology and nanostructure.Those methods are very efficient for the preparation of well-controlled structures but the reaction time is usually long.The assistance of microwave makes the reaction system heat up faster,more uniformly and reactions are accelerated,it also can be utilized to change the morphology or structure of materials,which improves the physic-chemical properties of synthesized products and influences its gas-sensing performance.Copper oxide(CuO)is widely applied in semiconductor gas sensors because of its good reactivity and stability.This review article briefly introduces the principle,mechanism and recent development of CuO nanostructures obtained by microwave-as sis ted hydrothermal synthesis(MWHS)process.It also discussed the relation between endopathic factors of material and its gas-sensitive performance.The technical challenges and prospective solutions for highperformance CuO-based gas-sensitive materials with unique nanostructure are proposed.It is pointed out that the hierarchical CuO-based nanostructures and their composite materials prepared by MWHS process are efficacious methods to improve the gas-sensitive performance of the materials.On the basis of the morphology,the materials are divided into nanorods,nanoflowers,nanosheets,nanospheres and other nanostructures.The influence of microwave parameters on the properties of synthetic products is analyzed.The influence followed by metal element loading on the structure and properties of CuO-based materials by MWHS process is further discussed.Then this review summarizes the research progress of graphene-CuO and metal oxide-CuO composites prepared by MWHS process in recent years.
基金supported by the National Key Program of Research and Development (2021YFB3501502, 2021YFB3501504)the National Natural Science Foundation of China (51631002, 92163107)the Beijing Natural Science Foundation (2214067)
文摘A model for describing the adsorption process of hydrogen on surface of tungsten oxide was proposed based on the first-principle calculations. Multiple factors such as type of active surface, adsorption site and distribution of oxygen vacancies were considered to evaluate the hydrogen adsorption capability of tungsten oxide. The adsorption Gibbs free energies, electronic structures and bonding characteristics under various conditions were examined to reveal the influence of oxygen vacancies on the surface. It is found that the capability of hydrogen adsorption of tungsten oxide can be significantly enhanced by adjusting the oxygen vacancy on the outermost layer of certain active surfaces. The modeling predicts that the surface structure stability and gas adsorption ability of tungsten oxide can be simultaneously improved through the formation of W–H bonds. The proposed strategy for moderating surface provides a new approach to obtain excellent gas-sensitive metal oxide materials.
基金The authors are grateful to the PHENMA 2021–2022 conference for the possibility of manuscript publication.The research was carried out at the expense of the grant of the Russian Science Foundation No.22-29-00621,(https://rscf.ru/project/22-29-00621/)at the Southern Federal University.
文摘Thin nanocomposite fflms based on tin dioxide with a low content of zinc oxide(0.5–5 mol.%)were obtained by the sol–gel method.The synthesized fflms are 300–600 nm thick and contains pore sizes of 19–29 nm.The resulting ZnO–SnO_(2) fflms were comprehensively studied by atomic force and Kelvin probe force microscopy,X-ray diffraction,scanning electron microscopy,and high-resolution X-ray photoelectron spectroscopy spectra.The photoconductivity parameters on exposure to light with a wavelength of 470 nm were also studied.The study of the photosensitivity kinetics of ZnO–SnO_(2) fflms showed that the fflm with the Zn:Sn ratio equal to 0.5:99.5 has the minimum value of the charge carrier generation time constant.Measurements of the activation energy of the conductivity,potential barrier,and surface potential of ZnO–SnO_(2) fflms showed that these parameters have maxima at ZnO concentrations of 0.5 mol.%and 1 mol.%.Films with 1 mol.%ZnO exhibit high response values when exposed to 5–50 ppm of nitrogen dioxide at operating temperatures of 200℃ and 250℃.
