Optical frequency combbased Fourier transform spectroscopy has the features of broad spectral bandwidth,high sensitivity,andmultiplexed trace gas detection,which has valuable application potential in the fields of pre...Optical frequency combbased Fourier transform spectroscopy has the features of broad spectral bandwidth,high sensitivity,andmultiplexed trace gas detection,which has valuable application potential in the fields of precision spectroscopy and trace gas detection.Here,we report the development of a mid-infrared Fourier transform spectrometer based on an optical frequency comb combined with a Herriott-type multipass cell.Using this instrument,the broadband absorption spectra of several important molecules,including methane,acetylene,water molecules and nitrous oxide,are measured by near real-time data acquisition in the 2800-3500 cm^(-1)spectral region.The achieved minimum detectable absorption of the instrument is 4.4×10^(-8)cm^(-1)·Hz^(-1/2)per spectral element.Broadband spectra of H_(2)0 are fited using the Voigt profile multispectral fitting technique and the consistency of the concentration inversion is 1%.Our system also enables precise spectroscopic measurements,and it allows the determination of the spectral line positions and upper state constants of N_(2)O in the(0002)-(1000)band,with results in good agreement with those reported by Toth[Appl.Opt.30,5289(1991)].展开更多
Hydrogen will be at the basis of the World’s energy policy in forthcoming decades, owing to its decarbonized nature, at least when produced from renewables. For now, hydrogen is still essentially produced from fossil...Hydrogen will be at the basis of the World’s energy policy in forthcoming decades, owing to its decarbonized nature, at least when produced from renewables. For now, hydrogen is still essentially produced from fossil feedstock(and to a minor extent from biomass);in consequence the present hydrogen gas on the market is containing non-negligible amounts of impurities that prevent its immediate usage in specialty chemistry or as an energy carrier in fuel cells, e.g. in transportation applications(cars, buses, trains, boats, etc.) that gradually spread on the planet. For these purposes, hydrogen must be of sufficient purity but also sufficiently compressed(at high pressures, typically 70 MPa), rendering purification and compression steps unavoidable in the hydrogen cycle. As shown in the first part of this contribution "Electrochemical hydrogen compression and purification versus competing technologies: Part I. pros and cons", electrochemical hydrogen compressors(EHCs), which enable both hydrogen purification and compression, exhibit many theoretical(thermodynamic) and practical(kinetics) advantages over their mechanical counterparts. However, in order to be competitive, EHCs must operate in very intensive conditions(high current density and low cell voltage) that can only be reached if their core materials, e.g. the membrane and the electrodes/electrocatalysts, are optimized. This contribution will particularly focus on the properties electrocatalysts must exhibit to be used in EHCs: they shall promote(very) fast hydrogen oxidation reaction(HOR) in presence of impurities, which implies that they are(very) tolerant to poisons as well. This consists of a prerequisite for the operation of the anode of an EHC used for the purification-compression of hydrogen, and the materials developed for poison-tolerance in the vast literature on low-temperature fuel cells, may not always satisfy these two criteria, as this contribution will review.展开更多
It is undisputed that hydrogen will play a great role in our future energetic mix, because it enables the storage of renewable electricity(power-to-H2) and the reversible conversion into electricity in fuel cell, not ...It is undisputed that hydrogen will play a great role in our future energetic mix, because it enables the storage of renewable electricity(power-to-H2) and the reversible conversion into electricity in fuel cell, not to speak of its wide use in the(petro)chemical industry. Whereas in these applications, pure hydrogen is required, today’s hydrogen production is still largely based on fossil fuels and can therefore not be considered pure. Therefore, purification of hydrogen is mandatory, at a large scale. In addition, hydrogen being the lightest gas, its volumetric energy content is well-below its competing fuels, unless it is compressed at high pressures(typically 70 MPa), making compression unavoidable as well. This contribution will detail the means available today for both purification and for compression of hydrogen. It will show that among the available technologies, the electrochemical hydrogen compressor(EHC), which also enables hydrogen purification, has numerous advantages compared to the classical technologies currently used at the industrial scale. EHC has their thermodynamic and operational advantages, but also their ease of use. However, the deployment of EHCs will be viable only if they reach sufficient performances, which implies some specifications that their base materials should stick to. The present contribution will detail these specifications.展开更多
A robust control strategy using the second-order integral sliding mode control(SOISMC)based on the variable speed grey wolf optimization(VGWO)is proposed.The aim is to maximize the wind power extraction of wind turbin...A robust control strategy using the second-order integral sliding mode control(SOISMC)based on the variable speed grey wolf optimization(VGWO)is proposed.The aim is to maximize the wind power extraction of wind turbine.Firstly,according to the uncertainty model of wind turbine,a SOISMC torque controller with fast convergence speed,strong robustness and effective chattering reduction is designed,which ensures that the torque controller can effectively track the reference speed.Secondly,given the strong local search ability of the grey wolf optimization(GWO)and the fast convergence speed and strong global search ability of the particle swarm optimization(PSO),the speed component of PSO is introduced into GWO,and VGWO with fast convergence speed,high solution accuracy and strong global search ability is used to optimize the parameters of wind turbine torque controller.Finally,the simulation is implemented based on Simulink/SimPowerSystem.The results demonstrate the effectiveness of the proposed strategy under both external disturbance and model uncertainty.展开更多
Cu/ZrO2/SiO2 are efficient catalysts for the selective hydrogenation of CO2 to CH3OH. In order to understand the role of ZrO2 in these mixed-oxides based catalysts, in situ X-ray absorption spectroscopy has been carri...Cu/ZrO2/SiO2 are efficient catalysts for the selective hydrogenation of CO2 to CH3OH. In order to understand the role of ZrO2 in these mixed-oxides based catalysts, in situ X-ray absorption spectroscopy has been carried out on the Cu and Zr K-edge. Under reaction conditions, Cu remains metallic, while Zr is present in three types of coordination environment associated with 1) bulk ZrO2, 2) coordinatively saturated and 3) unsaturated Zr(Ⅳ) surface sites. The amount of coordinatively unsaturated Zr surface sites can be quantified by linear combination fit of reference X-Ray absorption near edge structure (XANES) spectra and its amount correlates with CH3OH formation rates, thus indicating the importance of Zr(Ⅳ) Lewis acid surface sites in driving the selectivity toward CH3OH. This finding is consistent with the proposed mechanism, where CO2 is hydrogenated at the interface between the Cu nanoparticles that split H2 and Zr(Ⅳ) surface sites that stabilizes reaction intermediates.展开更多
Biodegradable polymers are highly attractive as potential alternatives to petroleum-based polymers in an attempt to achieve carbon neutrality whilst maintaining the mechanical properties of the structures.Among these ...Biodegradable polymers are highly attractive as potential alternatives to petroleum-based polymers in an attempt to achieve carbon neutrality whilst maintaining the mechanical properties of the structures.Among these polymers,polylactic acid(PLA)is particularly promising due to its good mechanical properties,biocompatibility and thermoplasticity.In this work,we aim to enhance the mechanical properties of PLA using mechanically-defibrated cellulose nanofibers(CNFs)that exhibit remarkable mechanical properties and biodegradability.We also employ fused deposition modeling(FDM),one of the three-dimensional printing methods for thermoplastic polymers,for the low-cost fabrication of the products.Mechanically-defibrated CNF-reinforced PLA matrix composites are fabricated by FDM.Their tensile properties are investigated in two printing directions(0°/90°and+45°/-45°).The discussion about the relationship between printing direction and tensile behavoir of mechanically-defibrated CNF-reinforced PLA matrix composite is the unique point of this study.We further discuss the microstructure and fracture surface of mechanically-defibrated CNF-reinforced PLA matrix composite by scanning electron microscope.展开更多
Gold catalysis had been considered a highly efficient candidate for heterogeneous catalysis.It is well established that reducible-material-supported Au NPs are more reactive than the unreducible materials,unless speci...Gold catalysis had been considered a highly efficient candidate for heterogeneous catalysis.It is well established that reducible-material-supported Au NPs are more reactive than the unreducible materials,unless specific modifications are carried out.However,unreducible materials such as carbon materials,silica,and alumina have particular advantages,including the easily controlled surface property,adjustable microscopic structure,earth-abundant reserves,and facile industrial manufacture.New strategies,influences,and mechanisms of modification to enhance the catalytic performance and thermal stability of unreducible-material-supported gold catalysts are among the most attractive research topics in gold catalysis.However,to the best of our knowledge,reports and reviews focused on unreducible-material-supported gold catalysts are lacking.Herein,the above concept will be thoroughly discussed regarding several typical unreducible supports,including the commonly used silica,alumina,carbon materials,and hydroxyapatite.The currently prevailing modification strategies will be summarized in detail from the aspects of theoretical conceptualization and practical methodology,including the ingenious synthesis method for catalyst with a specific structure,the currently prosperous electrostatic adsorption,colloid immobilization,and the applicative thermal gaseous treatment.The influences of physical and chemical modifications on the surface chemistry,electronic structure,interaction/synergy between Au-support/promoter,catalyst morphology and water precipitation will be also summarized.It is assumed that the review will shed light on significant studies on unreducible support in gold catalysis with the purpose of catalytic promotion and the promotion of the potential industrial demands in advance.Furthermore,the review will provide new insights into unreducible supports that can be potentially applied in gold catalysis.展开更多
A cloned cDNA designated as MS3 sequence can detect an RNA species with a size of about 6 kb in undifferentiated embryonaI carcinoma (EC) cell lines but not in several differentiated cell lines derived from EC cells.T...A cloned cDNA designated as MS3 sequence can detect an RNA species with a size of about 6 kb in undifferentiated embryonaI carcinoma (EC) cell lines but not in several differentiated cell lines derived from EC cells.This paper deals with the cytoplasmic distribution of this RNA species,MS3 RNA.NO MS3 RNA is observed in the cytoplasm of TDMI(trophoblastoma) cells.In the cytoplasm of PCC3 and F9(EC) cells,however。MS3 RNA is found in both polvsomal fraction and postpolysolnal fraction.About 20~55% MS3 RNA are included in polysome structure.This result implies that MS3 RNA is an actively translated message sequence and the protein specified by MS3 RNA will be a good marker for multipotent early embryonal cells.展开更多
The influence of the G‐quartet structural integrity on the catalytic activity of the G‐quadruplex(G4)was investigated by comparing the G4‐DNAzyme performances of a series of G4s with a G‐vacancy site and a G‐trip...The influence of the G‐quartet structural integrity on the catalytic activity of the G‐quadruplex(G4)was investigated by comparing the G4‐DNAzyme performances of a series of G4s with a G‐vacancy site and a G‐triplex(G‐tri).The results presented herein not only confirm that the structural integrity of the 3'‐end G‐quartet is necessary for G4s to be catalytically competent but also show how to remediate G‐vacancy‐mediated catalytic activity losses via the addition of guanine surrogates in an approach referred to as G‐vacancy complementation strategy that is applicable to parallel G4s only.Furthermore,this study demonstrates that the terminal G‐quartet could act as a proximal coordinating group and cooperate with the flanking nucleotide to activate the hemin cofactor.展开更多
基金supported by the National Natural Science Foundation China(No.42022051,No.U21A2028)Youth Innovation Promotion Association of the Chinese Academy of Sciences(No.Y202089)the HFIPS Director's Fund(No.YZJJ202101,No.BJPY2023A02).
文摘Optical frequency combbased Fourier transform spectroscopy has the features of broad spectral bandwidth,high sensitivity,andmultiplexed trace gas detection,which has valuable application potential in the fields of precision spectroscopy and trace gas detection.Here,we report the development of a mid-infrared Fourier transform spectrometer based on an optical frequency comb combined with a Herriott-type multipass cell.Using this instrument,the broadband absorption spectra of several important molecules,including methane,acetylene,water molecules and nitrous oxide,are measured by near real-time data acquisition in the 2800-3500 cm^(-1)spectral region.The achieved minimum detectable absorption of the instrument is 4.4×10^(-8)cm^(-1)·Hz^(-1/2)per spectral element.Broadband spectra of H_(2)0 are fited using the Voigt profile multispectral fitting technique and the consistency of the concentration inversion is 1%.Our system also enables precise spectroscopic measurements,and it allows the determination of the spectral line positions and upper state constants of N_(2)O in the(0002)-(1000)band,with results in good agreement with those reported by Toth[Appl.Opt.30,5289(1991)].
基金The authors thank the Auvergne Rhone-Alpes region for the funding of the PhD thesis of Marine TregaroPart of the work has been performed within the framework of the Centre of Excellence of Multifunctional Architectured Materials“CEMAM”no.ANR-10-LABX-44-01Both MT and MR make their PhD in the frame of the Eco-Sesa project,funded by IDEX Universite Grenoble Alpes.
文摘Hydrogen will be at the basis of the World’s energy policy in forthcoming decades, owing to its decarbonized nature, at least when produced from renewables. For now, hydrogen is still essentially produced from fossil feedstock(and to a minor extent from biomass);in consequence the present hydrogen gas on the market is containing non-negligible amounts of impurities that prevent its immediate usage in specialty chemistry or as an energy carrier in fuel cells, e.g. in transportation applications(cars, buses, trains, boats, etc.) that gradually spread on the planet. For these purposes, hydrogen must be of sufficient purity but also sufficiently compressed(at high pressures, typically 70 MPa), rendering purification and compression steps unavoidable in the hydrogen cycle. As shown in the first part of this contribution "Electrochemical hydrogen compression and purification versus competing technologies: Part I. pros and cons", electrochemical hydrogen compressors(EHCs), which enable both hydrogen purification and compression, exhibit many theoretical(thermodynamic) and practical(kinetics) advantages over their mechanical counterparts. However, in order to be competitive, EHCs must operate in very intensive conditions(high current density and low cell voltage) that can only be reached if their core materials, e.g. the membrane and the electrodes/electrocatalysts, are optimized. This contribution will particularly focus on the properties electrocatalysts must exhibit to be used in EHCs: they shall promote(very) fast hydrogen oxidation reaction(HOR) in presence of impurities, which implies that they are(very) tolerant to poisons as well. This consists of a prerequisite for the operation of the anode of an EHC used for the purification-compression of hydrogen, and the materials developed for poison-tolerance in the vast literature on low-temperature fuel cells, may not always satisfy these two criteria, as this contribution will review.
基金The authors thank the Auvergne Rhone-Alpes region for the funding of the PhD thesis of Marine TregaroPart of the work has been performed within the framework of the Centre of Excellence of Multifunctional Architectured Materials“CEMAM”no.ANR-10-LABX-44-01Both MR and MT make their PhD in the frame of the Eco-Sesa project,funded by IDEX Universite Grenoble Alpes.
文摘It is undisputed that hydrogen will play a great role in our future energetic mix, because it enables the storage of renewable electricity(power-to-H2) and the reversible conversion into electricity in fuel cell, not to speak of its wide use in the(petro)chemical industry. Whereas in these applications, pure hydrogen is required, today’s hydrogen production is still largely based on fossil fuels and can therefore not be considered pure. Therefore, purification of hydrogen is mandatory, at a large scale. In addition, hydrogen being the lightest gas, its volumetric energy content is well-below its competing fuels, unless it is compressed at high pressures(typically 70 MPa), making compression unavoidable as well. This contribution will detail the means available today for both purification and for compression of hydrogen. It will show that among the available technologies, the electrochemical hydrogen compressor(EHC), which also enables hydrogen purification, has numerous advantages compared to the classical technologies currently used at the industrial scale. EHC has their thermodynamic and operational advantages, but also their ease of use. However, the deployment of EHCs will be viable only if they reach sufficient performances, which implies some specifications that their base materials should stick to. The present contribution will detail these specifications.
基金This work was supported by the National Natural Science Foundation of China(No.51876089)the Fundamental Research Funds for the Central Universities(No.kfjj20190205).
文摘A robust control strategy using the second-order integral sliding mode control(SOISMC)based on the variable speed grey wolf optimization(VGWO)is proposed.The aim is to maximize the wind power extraction of wind turbine.Firstly,according to the uncertainty model of wind turbine,a SOISMC torque controller with fast convergence speed,strong robustness and effective chattering reduction is designed,which ensures that the torque controller can effectively track the reference speed.Secondly,given the strong local search ability of the grey wolf optimization(GWO)and the fast convergence speed and strong global search ability of the particle swarm optimization(PSO),the speed component of PSO is introduced into GWO,and VGWO with fast convergence speed,high solution accuracy and strong global search ability is used to optimize the parameters of wind turbine torque controller.Finally,the simulation is implemented based on Simulink/SimPowerSystem.The results demonstrate the effectiveness of the proposed strategy under both external disturbance and model uncertainty.
基金E.L.,K.L.,P.W.,and S.T.are supported by the SCCER-Heat and Energy Storage program
文摘Cu/ZrO2/SiO2 are efficient catalysts for the selective hydrogenation of CO2 to CH3OH. In order to understand the role of ZrO2 in these mixed-oxides based catalysts, in situ X-ray absorption spectroscopy has been carried out on the Cu and Zr K-edge. Under reaction conditions, Cu remains metallic, while Zr is present in three types of coordination environment associated with 1) bulk ZrO2, 2) coordinatively saturated and 3) unsaturated Zr(Ⅳ) surface sites. The amount of coordinatively unsaturated Zr surface sites can be quantified by linear combination fit of reference X-Ray absorption near edge structure (XANES) spectra and its amount correlates with CH3OH formation rates, thus indicating the importance of Zr(Ⅳ) Lewis acid surface sites in driving the selectivity toward CH3OH. This finding is consistent with the proposed mechanism, where CO2 is hydrogenated at the interface between the Cu nanoparticles that split H2 and Zr(Ⅳ) surface sites that stabilizes reaction intermediates.
基金supported by the Program for Creation of Interdisciplinary Research and Ensemble Program of Frontier Research Institute for Interdisciplinary Sciences,Tohoku University。
文摘Biodegradable polymers are highly attractive as potential alternatives to petroleum-based polymers in an attempt to achieve carbon neutrality whilst maintaining the mechanical properties of the structures.Among these polymers,polylactic acid(PLA)is particularly promising due to its good mechanical properties,biocompatibility and thermoplasticity.In this work,we aim to enhance the mechanical properties of PLA using mechanically-defibrated cellulose nanofibers(CNFs)that exhibit remarkable mechanical properties and biodegradability.We also employ fused deposition modeling(FDM),one of the three-dimensional printing methods for thermoplastic polymers,for the low-cost fabrication of the products.Mechanically-defibrated CNF-reinforced PLA matrix composites are fabricated by FDM.Their tensile properties are investigated in two printing directions(0°/90°and+45°/-45°).The discussion about the relationship between printing direction and tensile behavoir of mechanically-defibrated CNF-reinforced PLA matrix composite is the unique point of this study.We further discuss the microstructure and fracture surface of mechanically-defibrated CNF-reinforced PLA matrix composite by scanning electron microscope.
文摘Gold catalysis had been considered a highly efficient candidate for heterogeneous catalysis.It is well established that reducible-material-supported Au NPs are more reactive than the unreducible materials,unless specific modifications are carried out.However,unreducible materials such as carbon materials,silica,and alumina have particular advantages,including the easily controlled surface property,adjustable microscopic structure,earth-abundant reserves,and facile industrial manufacture.New strategies,influences,and mechanisms of modification to enhance the catalytic performance and thermal stability of unreducible-material-supported gold catalysts are among the most attractive research topics in gold catalysis.However,to the best of our knowledge,reports and reviews focused on unreducible-material-supported gold catalysts are lacking.Herein,the above concept will be thoroughly discussed regarding several typical unreducible supports,including the commonly used silica,alumina,carbon materials,and hydroxyapatite.The currently prevailing modification strategies will be summarized in detail from the aspects of theoretical conceptualization and practical methodology,including the ingenious synthesis method for catalyst with a specific structure,the currently prosperous electrostatic adsorption,colloid immobilization,and the applicative thermal gaseous treatment.The influences of physical and chemical modifications on the surface chemistry,electronic structure,interaction/synergy between Au-support/promoter,catalyst morphology and water precipitation will be also summarized.It is assumed that the review will shed light on significant studies on unreducible support in gold catalysis with the purpose of catalytic promotion and the promotion of the potential industrial demands in advance.Furthermore,the review will provide new insights into unreducible supports that can be potentially applied in gold catalysis.
文摘A cloned cDNA designated as MS3 sequence can detect an RNA species with a size of about 6 kb in undifferentiated embryonaI carcinoma (EC) cell lines but not in several differentiated cell lines derived from EC cells.This paper deals with the cytoplasmic distribution of this RNA species,MS3 RNA.NO MS3 RNA is observed in the cytoplasm of TDMI(trophoblastoma) cells.In the cytoplasm of PCC3 and F9(EC) cells,however。MS3 RNA is found in both polvsomal fraction and postpolysolnal fraction.About 20~55% MS3 RNA are included in polysome structure.This result implies that MS3 RNA is an actively translated message sequence and the protein specified by MS3 RNA will be a good marker for multipotent early embryonal cells.
文摘The influence of the G‐quartet structural integrity on the catalytic activity of the G‐quadruplex(G4)was investigated by comparing the G4‐DNAzyme performances of a series of G4s with a G‐vacancy site and a G‐triplex(G‐tri).The results presented herein not only confirm that the structural integrity of the 3'‐end G‐quartet is necessary for G4s to be catalytically competent but also show how to remediate G‐vacancy‐mediated catalytic activity losses via the addition of guanine surrogates in an approach referred to as G‐vacancy complementation strategy that is applicable to parallel G4s only.Furthermore,this study demonstrates that the terminal G‐quartet could act as a proximal coordinating group and cooperate with the flanking nucleotide to activate the hemin cofactor.