In view of the fact that the proportion of tobacco leaves from Shandong in the stocks of a company is large,based on the premise of not affecting the quality of cigarettes,through the scientific evaluation,selection a...In view of the fact that the proportion of tobacco leaves from Shandong in the stocks of a company is large,based on the premise of not affecting the quality of cigarettes,through the scientific evaluation,selection and matching test,the proportion of tobacco leaves from Shandong in the formula of " Taishan" cigarette A has been increased,and the sensory quality of " Taishan" cigarette A before and after the test is basically stable.Moreover,the stocks of tobacco leaves from Shandong can be decreased in time.展开更多
[Objectives]This study was conducted to improve the sensory quality and industrial availability of tobacco extracts.[Methods]The L9(34)design was adopted to carried out an extraction experiment,in which formula tobacc...[Objectives]This study was conducted to improve the sensory quality and industrial availability of tobacco extracts.[Methods]The L9(34)design was adopted to carried out an extraction experiment,in which formula tobacco was extracted using supercritical CO2,and the extract was concentrated by vacuum distillation.Through sensory evaluation and chemical analysis,the function determination and chemical composition analysis of the tobacco extracts were carried out,and the optimal supercritical fluid extraction process was finally determined.[Results]The obtained optimal supercritical fluid extraction conditions were as follows:extraction temperature 55℃,extraction pressure 25 MPa,CO2 flow rate of 20 L/h,and entrainer of 95%ethanol.The tobacco extract obtained under the optimal conditions endowed the cigarettes with full and delicate aroma,less irritation and clean aftertaste and made the flavor of the cigarettes overall coordinated and softer,so the sensory quality was significantly improved.[Conclusions]The tobacco extract obtained by the supercritical CO2 extraction method from formula tobacco can effectively improve the quality of cigarettes.展开更多
Micro-energy systems contribute significantly to environmental improvement by reducing dependence on power grids through the utilization of multiple renewable energy sources.This study quantified the environmental imp...Micro-energy systems contribute significantly to environmental improvement by reducing dependence on power grids through the utilization of multiple renewable energy sources.This study quantified the environmental impact of a micro-energy network system in an industrial park through a life cycle assessment using the operation of the micro-energy network over a year as the functional unit and“cradle-to-gate”as the system boundary.Based on the baseline scenario,a natural gas generator set was added to replace central heating,and the light pipes were expanded to constitute the optimized scenario.The results showed that the key impact categories for both scenarios were global warming,fine particulate matter formation,human carcinogenic toxicity,and human non-carcinogenic toxicity.The overall environmental impact of the optimized scenario was reduced by 68%compared to the baseline scenario.A sensitivity analysis of the key factors showed that electricity from the power grid was the key impact factor in both scenarios,followed by central heating and natural gas.Therefore,to reduce the environmental impact of network systems,it is necessary to further optimize the grid power structure.The research approach can be used to optimize micro-energy networks and evaluate the environmental impact of different energy systems.展开更多
Although the tobacco industry is a significant contributor to energy consumption and carbon emissions its negative environmental impact has received inadequate attention globally.Cigarette factories are a key link in ...Although the tobacco industry is a significant contributor to energy consumption and carbon emissions its negative environmental impact has received inadequate attention globally.Cigarette factories are a key link in the tobacco industry’s production chain,and using data provided by a cigarette factory in China we conduct a life cycle assessment to account for the carbon footprint of cigar production in cigarette factories.The results of the assessment show that factory air conditioning is the most important contributor to the environmental load of the cigar manufacturing process,while electricity is the key factor that contributes the greatest envi‐ronmental load across all of the processes in the product life cycle.In addition,packaging,including small boxes and cigarette cartons,has a significant impact on the industry’s environmental footprint due to its use of raw materials.We find the carbon footprint of the entire production process for cigar products to be 383.59 kg CO_(2) eq.Based on our findings,we suggest ways to optimize cigar/cigarette factory processes to re‐duce carbon emissions that can help to promote sustainable development in related industries.展开更多
[Objectives]The extraction conditions of formula oolong tea were investigated by an orthogonal experiment.[Methods]The technical conditions were optimized by the 4C method,and the application of formula oolong tea ext...[Objectives]The extraction conditions of formula oolong tea were investigated by an orthogonal experiment.[Methods]The technical conditions were optimized by the 4C method,and the application of formula oolong tea extract in cigarettes was studied.[Results]①In the experimental range,the best sensory evaluation effect of formula oolong tea extract was obtained with extraction conditions of 70%ethanol as extraction solvent,extraction time h,extraction temperature 25℃,and ultrasonic frequency 80 kHz,and follow-up low-temperature concentration,low-temperature sedimentation and low-temperature centrifugation.②The effects of different centrifugal speeds on the quality of formula oolong tea extract were explored.The formula oolong tea extract obtained under the conditions of 3000 r/min and centrifugal time of 10 min showed the best evaluation effect with soft and delicate smoke,rich smoke fragrance,good comfort and refreshing mouthfeel.③The effective aroma components in the formula oolong tea extract were qualitatively analyzed by GC-MS.[Conclusions]This study provides high-quality raw materials and a theoretical basis for the research of independent flavor blending in cigarette industry enterprises.展开更多
[Objecdve] The aim was to observe the puff-by-puff transfer ratios of some flavors in cigarettes. [Method] Based on national stand- ards, the puff-by-puff transfer of tobacco of carbonyl flavors was analyzed. In the m...[Objecdve] The aim was to observe the puff-by-puff transfer ratios of some flavors in cigarettes. [Method] Based on national stand- ards, the puff-by-puff transfer of tobacco of carbonyl flavors was analyzed. In the meantime, by dint of simultaneous distillation and extraction equip- ment coupled to GC and GC/MS, the puff-by-puff transfer ratios to TPM of smoke were expounded and compared. [ Result] The puff-by-puff deliv- ery profiles of NFDPT,nicotine and carbon monoxide increased with increasing puff number. This trend was similar to that of particulate matters. The transfer ratio of flavored tobacco was increasing in general, but partial flavors augmented to the maximum value and then decreased slowly. [ Conclusion] The study provided reference for the application of carbonyl compounds in tobacco.展开更多
[Objectives]Laoshan black tea was subjected to supercritical CO_(2) extraction. [Methods]The extraction conditions of Laoshan black tea were studied by an orthogonal experiment and optimized by response surface method...[Objectives]Laoshan black tea was subjected to supercritical CO_(2) extraction. [Methods]The extraction conditions of Laoshan black tea were studied by an orthogonal experiment and optimized by response surface methodology. [Results] The optimum extraction conditions of black tea extract by supercritical CO_(2) extraction were as follows: extraction pressure 23.53 MPa, extraction time 1.73 h, and extraction temperature 49.75 ℃, with which the extract yield could reach 5.15% theoretically. [Conclusions] Based on the traditional extraction process, a supercritical extraction method optimized by response surface methodology and a unique extraction process were formed, which enriches the extraction processes and methods of natural raw materials.展开更多
In this work,dielectric ultracapacitors were designed and fabricated using a combination of phase boundary and nanograin strategies.These ultracapacitors are based on submicron-thick Ba(Zr_(0.2)Ti_(0.8))O_(3) ferroele...In this work,dielectric ultracapacitors were designed and fabricated using a combination of phase boundary and nanograin strategies.These ultracapacitors are based on submicron-thick Ba(Zr_(0.2)Ti_(0.8))O_(3) ferroelectric films sputterdeposited on Si at 500℃.With a composition near a polymorphic phase boundary(PPB),a compressive strain,and a high nucleation rate due to the lowered deposition temperature,these films exhibit a columnar nanograined microstructure with gradient phases along the growth direction.Such a microstructure presents three-dimensional polarization inhomogeneities on the nanoscale,thereby significantly delaying the saturation of the overall electric polarization.Consequently,a pseudolinear,ultraslim polarization(P)-electric field(E)hysteresis loop was obtained,featuring a high maximum applicable electric field(~5.7 MV/cm),low remnant polarization(~5.2μC/cm^(2))and high maximum polarization(~92.1μC/cm^(2)).This P-E loop corresponds to a high recyclable energy density(W_(rec)~208 J/cm^(3))and charge‒discharge efficiency(~88%).An indepth electron microscopy study revealed that the gradient ferroelectric phases consisted of tetragonal(T)and rhombohedral(R)polymorphs along the growth direction of the film.The T-rich phase is abundant near the bottom of the film and gradually transforms into the R-rich phase near the surface.These films also exhibited a high Curie temperature of~460℃and stable capacitive energy storage up to 200℃.These results suggest a feasible pathway for the design and fabrication of high-performance dielectric film capacitors.展开更多
To meet the expectation set by Moore’s law on transistors,the search for thickness-scalable high dielectric constant(k)gate layers has become an emergent research frontier.Previous investigations have failed to solve...To meet the expectation set by Moore’s law on transistors,the search for thickness-scalable high dielectric constant(k)gate layers has become an emergent research frontier.Previous investigations have failed to solve the“polarizability–scalability–insulation robustness”trilemma.In this work,we show that this trilemma can be solved by using a gate layer of a high k ferroelectric oxide in its superparaelectric(SPE)state.In the SPE,its polar order becomes local and is dispersed in an amorphous matrix with a crystalline size down to a few nanometers,leading to an excellent dimensional scalability and a good field-stability of the k value.As an example,a stable high k value(37±3)is shown in ultrathin SPE films of(Ba_(0.95),Sr_(0.05))(Zr_(0.2),Ti_(0.8))O_(3)deposited on LaNiO_(3)-buffered Pt/Ti/SiO_(2)/(100)Si down to a 4 nm thickness,leading to a small equivalent oxide thickness of~0.46 nm.The aforementioned characteristic microstructure endows the SPE film a high breakdown strength(~10.5 MV·cm^(−1)for the 4 nm film),and hence ensures a low leakage current for the operation of the complementary metal oxide semiconductor(CMOS)gate.Lastly,a high electrical fatigue resistance is displayed by the SPE films.These results reveal a great potential of superparaelectric materials as gate dielectrics in the next-generation microelectronics.展开更多
Due to its lead-free composition and a unique double polarization hysteresis loop with a large maximum polarization(Pmax)and a small remnant polarization(Pr),AgNbO_(3)-based antiferroelectrics(AFEs)have attracted exte...Due to its lead-free composition and a unique double polarization hysteresis loop with a large maximum polarization(Pmax)and a small remnant polarization(Pr),AgNbO_(3)-based antiferroelectrics(AFEs)have attracted extensive research interest for electric energy storage applications.However,a low dielectric breakdown field(Eb)limits an energy density and its further development.In this work,a highly efficient method was proposed to fabricate high-energy-density Ag(Nb,Ta)O_(3) capacitor films on Si substrates,using a two-step process combining radio frequency(RF)-magnetron sputtering at 450℃and post-deposition rapid thermal annealing(RTA).The RTA process at 700℃led to sufficient crystallization of nanograins in the film,hindering their lateral growth by employing short annealing time of 5 min.The obtained Ag(Nb,Ta)O_(3) films showed an average grain size(D)of~14 nm(obtained by Debye-Scherrer formula)and a slender room temperature(RT)polarization-electric field(P-E)loop(Pr≈3.8 mC·cm^(−2) and P_(max)≈38 mC·cm^(−2) under an electric field of~3.3 MV·cm^(−1)),the P-E loop corresponding to a high recoverable energy density(W_(rec))of~46.4 J·cm^(−3) and an energy efficiency(η)of~80.3%.Additionally,by analyzing temperature-dependent dielectric property of the film,a significant downshift of the diffused phase transition temperature(T_(M2-M3))was revealed,which indicated the existence of a stable relaxor-like AFE phase near the RT.The downshift of the T_(M2-M3) could be attributed to a nanograin size and residual tensile strain of the film,and it led to excellent temperature stability(20-240℃)of the energy storage performance of the film.Our results indicate that the Ag(Nb,Ta)O_(3) film is a promising candidate for electrical energy storage applications.展开更多
Achieving an excellent energy storage performance,together with high cycling reliability,is desirable for expanding technological applications of ferroelectric dielectrics.However,in well-crystallized ferroelectric ma...Achieving an excellent energy storage performance,together with high cycling reliability,is desirable for expanding technological applications of ferroelectric dielectrics.However,in well-crystallized ferroelectric materials,the concomitant high polarizability and low polarization saturation field have led to a square-shaped polarization–electric field loop,fatally impairing both recoverable energy density(W_(rec))and efficiency(η).Nanocrystalline ferroelectric films with a macroscopically amorphous structure have shown an improved W_(rec) andη,but their much lower polarizability demands an extremely high electric field to achieve such performances,which is undesirable from an economic viewpoint.Here,we propose a strategy to boost the energy storage performances and stability of ferroelectric capacitors simultaneously by constructing a tri-layer film in which a well-crystallized ferroelectric layer was sandwiched by two pseudo-linear dielectric layers with a dominant amorphous structure.In sol–gel-derived BaTiO_(3)/(Pb,La,Ca)TiO_(3)/BaTiO_(3)(BTO/PLCT/BTO)tri-layer films,we show that the above design is realized via rapid thermal annealing which fully crystallized the middle PLCT layer while left the top/bottom BTO cap layers in a poor crystallization status.This sandwiched structure is endowed with an enhanced maximum polarization while a small remnant one and a much-delayed polarization saturation,which corresponds to large W_(rec)≈80 J/cm^(3) and highη≈86%.Furthermore,the film showed an outstanding cycling stability:its W_(rec) andηremain essentially unchanged after 10^(9) electric cycles(DW/W<4%,Dη/η<2%).These good energy storage characteristics have proved the effectiveness of our proposed strategy,paving a way for the utilization of sandwiched films in applications of electric power systems and advanced pulsed-discharge devices.展开更多
文摘In view of the fact that the proportion of tobacco leaves from Shandong in the stocks of a company is large,based on the premise of not affecting the quality of cigarettes,through the scientific evaluation,selection and matching test,the proportion of tobacco leaves from Shandong in the formula of " Taishan" cigarette A has been increased,and the sensory quality of " Taishan" cigarette A before and after the test is basically stable.Moreover,the stocks of tobacco leaves from Shandong can be decreased in time.
文摘[Objectives]This study was conducted to improve the sensory quality and industrial availability of tobacco extracts.[Methods]The L9(34)design was adopted to carried out an extraction experiment,in which formula tobacco was extracted using supercritical CO2,and the extract was concentrated by vacuum distillation.Through sensory evaluation and chemical analysis,the function determination and chemical composition analysis of the tobacco extracts were carried out,and the optimal supercritical fluid extraction process was finally determined.[Results]The obtained optimal supercritical fluid extraction conditions were as follows:extraction temperature 55℃,extraction pressure 25 MPa,CO2 flow rate of 20 L/h,and entrainer of 95%ethanol.The tobacco extract obtained under the optimal conditions endowed the cigarettes with full and delicate aroma,less irritation and clean aftertaste and made the flavor of the cigarettes overall coordinated and softer,so the sensory quality was significantly improved.[Conclusions]The tobacco extract obtained by the supercritical CO2 extraction method from formula tobacco can effectively improve the quality of cigarettes.
基金funded by the National Key R&D Project[Grant No.2019YFC1903900]Key R&D Province[Grant No.2023SFGC0101]Taishan Scholar Project[Grant No.tsqn202103010].
文摘Micro-energy systems contribute significantly to environmental improvement by reducing dependence on power grids through the utilization of multiple renewable energy sources.This study quantified the environmental impact of a micro-energy network system in an industrial park through a life cycle assessment using the operation of the micro-energy network over a year as the functional unit and“cradle-to-gate”as the system boundary.Based on the baseline scenario,a natural gas generator set was added to replace central heating,and the light pipes were expanded to constitute the optimized scenario.The results showed that the key impact categories for both scenarios were global warming,fine particulate matter formation,human carcinogenic toxicity,and human non-carcinogenic toxicity.The overall environmental impact of the optimized scenario was reduced by 68%compared to the baseline scenario.A sensitivity analysis of the key factors showed that electricity from the power grid was the key impact factor in both scenarios,followed by central heating and natural gas.Therefore,to reduce the environmental impact of network systems,it is necessary to further optimize the grid power structure.The research approach can be used to optimize micro-energy networks and evaluate the environmental impact of different energy systems.
基金supported by Shandong Natural Science Founda‐tion[Grant No.ZR2023MD079]Shandong Province Social Science Planning Research Project[Grant No.22CKRJ04]+2 种基金Taishan Scholar Project[Grant No.tsqn202103010]Department of Science and Tech‐nology of Shandong Province[Grant No.2021SFGC0904-05]Zaozhuang Science and Technology Bureau[Grant No.2021GH22].
文摘Although the tobacco industry is a significant contributor to energy consumption and carbon emissions its negative environmental impact has received inadequate attention globally.Cigarette factories are a key link in the tobacco industry’s production chain,and using data provided by a cigarette factory in China we conduct a life cycle assessment to account for the carbon footprint of cigar production in cigarette factories.The results of the assessment show that factory air conditioning is the most important contributor to the environmental load of the cigar manufacturing process,while electricity is the key factor that contributes the greatest envi‐ronmental load across all of the processes in the product life cycle.In addition,packaging,including small boxes and cigarette cartons,has a significant impact on the industry’s environmental footprint due to its use of raw materials.We find the carbon footprint of the entire production process for cigar products to be 383.59 kg CO_(2) eq.Based on our findings,we suggest ways to optimize cigar/cigarette factory processes to re‐duce carbon emissions that can help to promote sustainable development in related industries.
文摘[Objectives]The extraction conditions of formula oolong tea were investigated by an orthogonal experiment.[Methods]The technical conditions were optimized by the 4C method,and the application of formula oolong tea extract in cigarettes was studied.[Results]①In the experimental range,the best sensory evaluation effect of formula oolong tea extract was obtained with extraction conditions of 70%ethanol as extraction solvent,extraction time h,extraction temperature 25℃,and ultrasonic frequency 80 kHz,and follow-up low-temperature concentration,low-temperature sedimentation and low-temperature centrifugation.②The effects of different centrifugal speeds on the quality of formula oolong tea extract were explored.The formula oolong tea extract obtained under the conditions of 3000 r/min and centrifugal time of 10 min showed the best evaluation effect with soft and delicate smoke,rich smoke fragrance,good comfort and refreshing mouthfeel.③The effective aroma components in the formula oolong tea extract were qualitatively analyzed by GC-MS.[Conclusions]This study provides high-quality raw materials and a theoretical basis for the research of independent flavor blending in cigarette industry enterprises.
文摘[Objecdve] The aim was to observe the puff-by-puff transfer ratios of some flavors in cigarettes. [Method] Based on national stand- ards, the puff-by-puff transfer of tobacco of carbonyl flavors was analyzed. In the meantime, by dint of simultaneous distillation and extraction equip- ment coupled to GC and GC/MS, the puff-by-puff transfer ratios to TPM of smoke were expounded and compared. [ Result] The puff-by-puff deliv- ery profiles of NFDPT,nicotine and carbon monoxide increased with increasing puff number. This trend was similar to that of particulate matters. The transfer ratio of flavored tobacco was increasing in general, but partial flavors augmented to the maximum value and then decreased slowly. [ Conclusion] The study provided reference for the application of carbonyl compounds in tobacco.
文摘[Objectives]Laoshan black tea was subjected to supercritical CO_(2) extraction. [Methods]The extraction conditions of Laoshan black tea were studied by an orthogonal experiment and optimized by response surface methodology. [Results] The optimum extraction conditions of black tea extract by supercritical CO_(2) extraction were as follows: extraction pressure 23.53 MPa, extraction time 1.73 h, and extraction temperature 49.75 ℃, with which the extract yield could reach 5.15% theoretically. [Conclusions] Based on the traditional extraction process, a supercritical extraction method optimized by response surface methodology and a unique extraction process were formed, which enriches the extraction processes and methods of natural raw materials.
基金the financial support from the Natural Science Foundation of Shandong Province(Nos.ZR2022ZD39,ZR2022ME031,ZR2023QB119,ZR2023QE138,ZR2020QE042,and ZR2022QB138)the National Natural Science Foundation of China(No.52002192)+3 种基金the Science,Education and Industry Integration Pilot Projects of Qilu University of Technology(Shandong Academy of Sciences)(Nos.2022GH018,2023PX062,and 2023PX041)the Training Plan Project of Qilu University of Technology(Nos.2023RCKY093 and 2023RCKY095)the support from the Jinan City Science and Technology Bureau(No.2021GXRC055)the Education Department of Hunan Province/Xiangtan University(No.KZ0807969)。
文摘In this work,dielectric ultracapacitors were designed and fabricated using a combination of phase boundary and nanograin strategies.These ultracapacitors are based on submicron-thick Ba(Zr_(0.2)Ti_(0.8))O_(3) ferroelectric films sputterdeposited on Si at 500℃.With a composition near a polymorphic phase boundary(PPB),a compressive strain,and a high nucleation rate due to the lowered deposition temperature,these films exhibit a columnar nanograined microstructure with gradient phases along the growth direction.Such a microstructure presents three-dimensional polarization inhomogeneities on the nanoscale,thereby significantly delaying the saturation of the overall electric polarization.Consequently,a pseudolinear,ultraslim polarization(P)-electric field(E)hysteresis loop was obtained,featuring a high maximum applicable electric field(~5.7 MV/cm),low remnant polarization(~5.2μC/cm^(2))and high maximum polarization(~92.1μC/cm^(2)).This P-E loop corresponds to a high recyclable energy density(W_(rec)~208 J/cm^(3))and charge‒discharge efficiency(~88%).An indepth electron microscopy study revealed that the gradient ferroelectric phases consisted of tetragonal(T)and rhombohedral(R)polymorphs along the growth direction of the film.The T-rich phase is abundant near the bottom of the film and gradually transforms into the R-rich phase near the surface.These films also exhibited a high Curie temperature of~460℃and stable capacitive energy storage up to 200℃.These results suggest a feasible pathway for the design and fabrication of high-performance dielectric film capacitors.
基金the National Natural Science Foundation of China(Nos.51772175 and 52002192)the Natural Science Foundation of Shandong Province(Nos.ZR2022ZD39,ZR2020QE042,ZR2022ME031,and ZR2022QB138)+2 种基金the Science,Education and Industry Integration Pilot Projects of Qilu University of Technology(Shandong Academy of Sciences)(Nos.2022GH018 and 2022PY055)Jun Ouyang acknowledges the support from the Jinan City Science and Technology Bureau(No.2021GXRC055)the Education Department of Hunan Province/Xiangtan University(No.KZ0807969).
文摘To meet the expectation set by Moore’s law on transistors,the search for thickness-scalable high dielectric constant(k)gate layers has become an emergent research frontier.Previous investigations have failed to solve the“polarizability–scalability–insulation robustness”trilemma.In this work,we show that this trilemma can be solved by using a gate layer of a high k ferroelectric oxide in its superparaelectric(SPE)state.In the SPE,its polar order becomes local and is dispersed in an amorphous matrix with a crystalline size down to a few nanometers,leading to an excellent dimensional scalability and a good field-stability of the k value.As an example,a stable high k value(37±3)is shown in ultrathin SPE films of(Ba_(0.95),Sr_(0.05))(Zr_(0.2),Ti_(0.8))O_(3)deposited on LaNiO_(3)-buffered Pt/Ti/SiO_(2)/(100)Si down to a 4 nm thickness,leading to a small equivalent oxide thickness of~0.46 nm.The aforementioned characteristic microstructure endows the SPE film a high breakdown strength(~10.5 MV·cm^(−1)for the 4 nm film),and hence ensures a low leakage current for the operation of the complementary metal oxide semiconductor(CMOS)gate.Lastly,a high electrical fatigue resistance is displayed by the SPE films.These results reveal a great potential of superparaelectric materials as gate dielectrics in the next-generation microelectronics.
基金support from the National Natural Science Foundation of China (Grant Nos.51772175,52072218,and 52002192)Natural Science Foundation of Shandong Province (Grant Nos.ZR2020QE042,ZR2022ZD39,and ZR2022ME031)+6 种基金the Science,Education and Industry Integration Pilot Projects of Qilu University of Technology (Shandong Academy of Sciences) (Grant Nos.2022GH018 and 2022PY055)support from the Jinan City Science and Technology Bureau (Grant No.2021GXRC055)the Education Department of Hunan Province/Xiangtan University (Grant No.KZ0807969)funding for top talents at Qilu University of Technology (Shandong Academy of Sciences)support from the Jiangsu Province NSFC (Grant No.BK20180764)support from the National Key R&D Program of China (Grant No.2021YFB3601504)Natural Science Foundation of Shandong Province (Grant No.ZR2020KE019).
文摘Due to its lead-free composition and a unique double polarization hysteresis loop with a large maximum polarization(Pmax)and a small remnant polarization(Pr),AgNbO_(3)-based antiferroelectrics(AFEs)have attracted extensive research interest for electric energy storage applications.However,a low dielectric breakdown field(Eb)limits an energy density and its further development.In this work,a highly efficient method was proposed to fabricate high-energy-density Ag(Nb,Ta)O_(3) capacitor films on Si substrates,using a two-step process combining radio frequency(RF)-magnetron sputtering at 450℃and post-deposition rapid thermal annealing(RTA).The RTA process at 700℃led to sufficient crystallization of nanograins in the film,hindering their lateral growth by employing short annealing time of 5 min.The obtained Ag(Nb,Ta)O_(3) films showed an average grain size(D)of~14 nm(obtained by Debye-Scherrer formula)and a slender room temperature(RT)polarization-electric field(P-E)loop(Pr≈3.8 mC·cm^(−2) and P_(max)≈38 mC·cm^(−2) under an electric field of~3.3 MV·cm^(−1)),the P-E loop corresponding to a high recoverable energy density(W_(rec))of~46.4 J·cm^(−3) and an energy efficiency(η)of~80.3%.Additionally,by analyzing temperature-dependent dielectric property of the film,a significant downshift of the diffused phase transition temperature(T_(M2-M3))was revealed,which indicated the existence of a stable relaxor-like AFE phase near the RT.The downshift of the T_(M2-M3) could be attributed to a nanograin size and residual tensile strain of the film,and it led to excellent temperature stability(20-240℃)of the energy storage performance of the film.Our results indicate that the Ag(Nb,Ta)O_(3) film is a promising candidate for electrical energy storage applications.
基金The authors are deeply grateful for the financial support from the National Natural Science Foundation of China(NSFC)(Grant Nos.52002192,51772175,and 52072150)the Natural Science Foundation of Shandong Province(Grant Nos.ZR2020QE042,ZR2022ZD39,ZR2022ME031,ZR2022ME075,and ZR2022QB138)+3 种基金the Science,Education and Industry Integration Pilot Projects of Qilu University of Technology(Shandong Academy of Sciences)(Grant Nos.2022PY055 and 2022GH018)Jun Ouyang acknowledges the support from the Jinan City Science and Technology Bureau(Grant No.2021GXRC055)the Education Department of Hunan Province/Xiangtan University(Grant No.KZ0807969)the Seed Funding for Top Talents at Qilu University of Technology(Shandong Academy of Sciences).
文摘Achieving an excellent energy storage performance,together with high cycling reliability,is desirable for expanding technological applications of ferroelectric dielectrics.However,in well-crystallized ferroelectric materials,the concomitant high polarizability and low polarization saturation field have led to a square-shaped polarization–electric field loop,fatally impairing both recoverable energy density(W_(rec))and efficiency(η).Nanocrystalline ferroelectric films with a macroscopically amorphous structure have shown an improved W_(rec) andη,but their much lower polarizability demands an extremely high electric field to achieve such performances,which is undesirable from an economic viewpoint.Here,we propose a strategy to boost the energy storage performances and stability of ferroelectric capacitors simultaneously by constructing a tri-layer film in which a well-crystallized ferroelectric layer was sandwiched by two pseudo-linear dielectric layers with a dominant amorphous structure.In sol–gel-derived BaTiO_(3)/(Pb,La,Ca)TiO_(3)/BaTiO_(3)(BTO/PLCT/BTO)tri-layer films,we show that the above design is realized via rapid thermal annealing which fully crystallized the middle PLCT layer while left the top/bottom BTO cap layers in a poor crystallization status.This sandwiched structure is endowed with an enhanced maximum polarization while a small remnant one and a much-delayed polarization saturation,which corresponds to large W_(rec)≈80 J/cm^(3) and highη≈86%.Furthermore,the film showed an outstanding cycling stability:its W_(rec) andηremain essentially unchanged after 10^(9) electric cycles(DW/W<4%,Dη/η<2%).These good energy storage characteristics have proved the effectiveness of our proposed strategy,paving a way for the utilization of sandwiched films in applications of electric power systems and advanced pulsed-discharge devices.