Background:Successful liver resection in oncologic surgery depends on safety,precision,and efficacy,all of which require a thorough understanding of liver anatomy.Contrast-enhanced computed tomography(CT)-generated th...Background:Successful liver resection in oncologic surgery depends on safety,precision,and efficacy,all of which require a thorough understanding of liver anatomy.Contrast-enhanced computed tomography(CT)-generated three-dimensional(3D)models have been proposed as a valuable tool to enhance this understanding.However,a systematic comparison of different display modalities across professional groups has not yet been performed.Methods:In this prospective,monocentric randomized trial,we compared high-resolution twodimensional(2D)CT images of liver malignancies with their corresponding standardized,non-colored 3D virtual and printed models in facilitating anatomical and spatial understanding as well as surgical decision-making.A total of 91 participants,including 40 surgeons,10 radiologists,and 41 students,evaluated six clinical cases(three centrally and three peripherally located liver malignancies).Each participant assessed one central and one peripheral case per display modality,presented in a random order.Results:Compared to 2D CT images,both 3D virtual and printed models significantly improved the identification of tumor location(P<0.001),enhanced the comprehension of spatial relationships with adjacent liver and portal veins(P<0.001 and P=0.019,respectively),and facilitated clinical decisionmaking(P<0.001).No significant difference was observed between virtual and printed models in terms of effectiveness.Within the different groups,surgeons and students,but not radiologists,more accurately identified tumor location and spatial relationships with adjacent liver and portal veins using 3D models.Subjectively,most surgeons and students preferred 3D printed models over virtual models and 2D CT images.Conclusions:This study demonstrated that standardized,non-colored 3D virtual and printed models equally help preoperative anatomical understanding and decision-making,particularly for surgeons and students.By isolating the influence of display modality,our findings clarify prior inconsistent results and support the integration of cost-effective 3D visualization by applying virtual models into surgical planning and education.Preference for printed models despite comparable efficacy highlights the importance of user-centered implementation strategies.展开更多
四级核回波实验通常需要射频脉冲能够激发谱宽超过100 k Hz的信号.在最近的研究中,作者发现组合脉冲COM-II(9018090135 45)能够在氘核的四级核回波实验中实现宽带激发.此外,作者还结合了八步相位循环的方法,有效消除了由有限脉宽效应造...四级核回波实验通常需要射频脉冲能够激发谱宽超过100 k Hz的信号.在最近的研究中,作者发现组合脉冲COM-II(9018090135 45)能够在氘核的四级核回波实验中实现宽带激发.此外,作者还结合了八步相位循环的方法,有效消除了由有限脉宽效应造成的谱图扭曲现象.利用了平均哈密顿原理,对该方法进行了理论计算研究.作者采用了自旋为1的矩阵算符,通过计算解释了八步相位循环能够消除谱图扭曲的原因.展开更多
Nanosized Ba_(1-x)Bi_(x)Fe_(1-x)Cu_(x)O_(3)(12–50 nm)with x values of 0,0.01,0.05,and 0.1 system was prepared using the Pechini method.Structural,morphological,surface and optical characterizations were performed for...Nanosized Ba_(1-x)Bi_(x)Fe_(1-x)Cu_(x)O_(3)(12–50 nm)with x values of 0,0.01,0.05,and 0.1 system was prepared using the Pechini method.Structural,morphological,surface and optical characterizations were performed for the prepared samples.Cubic phase was the predominant phase for the undoped BaFeO_(3)and Bi and Cu co-doped BaFeO_(3)samples.Minor phases of monoclinic Ba_(2)Fe_(2)O_(5),orthorhombic BaFe_(2)O_(4)and orthorhombic BaCO_(3)were identified for all the prepared samples.Ba_(0.95)Bi_(0.05)Fe_(0.95)Cu_(0.05)O_(3)sample has the lowest band gap(2.43 e V).98.1%paracetamol removal was achieved with 0.75 g/L of Ba_(0.95)Bi_(0.05)Fe_(0.95)Cu_(0.05)O_(3)at pH9 after 120 min.The paracetamol degradation follows the pseudo first-order kinetics.HO·is the main oxidative species responsible for the paracetamol degradation.Gas chromatography–mass spectrometry(GC–MS)analysis was performed at the end of the photocatalytic degradation experiment under optimum operating condition using Ba_(0.95)Bi_(0.05)Fe_(0.95)Cu_(0.05)O_(3)to explain the reaction mechanism and identify the intermediate by-products which is confirmed by ultraviolet/visible(UV/Vis)spectroscopy study at different reaction times.展开更多
Environmental stability is a major bottleneck of perovskite solar cells.Only a handful of studies are investigating the effect of moisture on the structural degradation of the absorber.They mostly rely on ex situ expe...Environmental stability is a major bottleneck of perovskite solar cells.Only a handful of studies are investigating the effect of moisture on the structural degradation of the absorber.They mostly rely on ex situ experiments and on completely degraded samples,which restrict the assessment on initial and final stage.By combining in situ X-ray diffraction under controlled 85%relative humidity,and live observations of the water-induced degradation using liquid-cell transmission electron microscopy,we reveal two competitive degradation paths leading on one hand to the decomposition of state-of-theart mixed cation/anion(Cs_(0.05)(MA_(0.17)FA_(0.83))_(0.95)Pb(Br_(0.17)I_(0.83))_(3)(CsMAFA)into PbI_(2) through a dissolution/recrystallization mechanism and,on the other hand,to a non-equilibrium phase segregation leading to CsPb_(2)Br_(5) and a Cesium-poor/iodide-rich Cs_(0.05)-x(MA_(0.17)FA_(0.83))_(0.95)Pb(Br_(0.17-2y)I_(0.83)+2y)_(3) perovskite.This degradation mechanism is corroborated at atomic-scale resolution through solid-state ^(1)H and ^(133)Cs NMR analysis.Exposure to moisture leads to a film containing important heterogeneities in terms of morphology,photoluminescence intensities,and lifetimes.Our results provide new insights and consensus that complex perovskite compositions,though very performant as champion devices,are comparatively metastable,a trait that limits the chances to achieve long-term stability.展开更多
An integrated approach combining the development of an innovative catalyst and the research of a set of adequate operating conditions for the propane oxidative dehydrogenation （ODH） is described.The experimental set...An integrated approach combining the development of an innovative catalyst and the research of a set of adequate operating conditions for the propane oxidative dehydrogenation （ODH） is described.The experimental set-up,specially designed for steady-state and transient studies is presented.The preparation method,the characterization and the performances in steady-state and transient regimes of catalysts based on V2W4O194-Lindqvist isopolyanion used as a precursor and supported on alumina are reported.The influence of the preparation method of the catalyst and the role of water in the feed gas are more particularly discussed.展开更多
The synthesis and characterization of several dispersed molybdena catalysts on silica support (MoO3-SiO2) prepared from a variety of precursors (Mo(VI)-acetylacetonate, oxo-peroxo Mo-species, hydrated ammonium heptamo...The synthesis and characterization of several dispersed molybdena catalysts on silica support (MoO3-SiO2) prepared from a variety of precursors (Mo(VI)-acetylacetonate, oxo-peroxo Mo-species, hydrated ammonium heptamolybdate) and preparation methods (deposition of the Mo-phase on finite SiO2 support by aqueous and methanol impregnations, by adsorption, by oxo-peroxo route-like, and by one-step synthesis of MoO3-SiO2 system with molecular precursors) are presented. The molybdena concentration on silica was comprised in a large interval (1.5 - 14 wt%) depending on the preparation method which governed the Mo-loading on silica. Convenient comparisons among samples at similar Mo-concentration have been made discussing the morphologic-structural (XRD, XPS, UV-vis-DRS, and N2-adsorption) and physicochemical (TG-DTG, TPR, and n-butylamine-TPD) sample properties. Polymeric octahedral polymolybdate aggregates predominated in the samples prepared by aqueous and methanol impregnations, which were at high Mo-concentration. On the contrary, isolated Mo(VI) species in distorted Td symmetry predominated in the sample prepared by adsorption which was at very low Mo-concentration. The sample acidity was composed of a weak acidy site population, associated with the silica support, and a strong acid site population associated with the Mo-dispersed phase. Oxidation tests of formaldehyde, an oxygen-containing VOC (Volatile Organic Compound), were performed to determine the prevalent redox or acidic function of the Mo-species at the surface of the catalysts.展开更多
Nowadays the system of public health is constructed in such a manner so that its main objective is the recovery of an already sick person, while prediction and prevention receive little attention. Meanwhile the develo...Nowadays the system of public health is constructed in such a manner so that its main objective is the recovery of an already sick person, while prediction and prevention receive little attention. Meanwhile the development of these aspects of medicine can lead to the ability to control morbidity among the population, to identify chronic and genetic diseases in the early stages of development, and thus to prevent their further progression. This will reduce traditionally high costs of sick people treatment and the number of disabled population, and improve the quality and duration of life. The elaboration of new fields of science that are working on the study and interpretation of data obtained during laboratory and clinical research, creation of new methods for diagnosis, prognosis and treatment, provides an opportunity now to implement a new strategy, called PPPM, and gets promising results, which should lead to further development of an existing medicine.展开更多
BaM_(2)(PO_(4))_(2)(M^(2+)transition metals)compounds display a variety of polymorphs;among those,the wellknown rhombohedralγ-form stands at the origin of a series of(quasi)_(2)D-magnetic behaviors intensively studie...BaM_(2)(PO_(4))_(2)(M^(2+)transition metals)compounds display a variety of polymorphs;among those,the wellknown rhombohedralγ-form stands at the origin of a series of(quasi)_(2)D-magnetic behaviors intensively studied in the last few decades.We have prepared originalα-variants for M=Fe^(2+)and Mn_(2)+and investigated their stabilities and sequence of phase transitions by analogy to the already reported M=Co^(2+)case.Heating theα-phases leads to a variety of structural rearrangements betweenα,α’andβvariants,according to unified 1st order reconstructive transitions.However,spontaneous long-time transformations under ambient conditionsα→γ(Fe case)versusγ→α(Co case)denote a contrasted hierarchy of stable compounds verified by DFT calculations.Interestingly,inα-BaFe2(PO_(4))_(2)the quasi triangular Fe^(2+)O_(3)+2 coordination is rarely observed and relies on one very short Fe-O distance of ca.1.78A,destabilizing the edifice in favor of the most stable FeO6 in theγ-type,as verified by Crystal Orbital Hamilton Population(COHP)analysis.展开更多
The standard redox potentials of the Fe^(3+)/Fe^(2+)(+0.77 V)and H_(3)AsO_(4)/H_(3)AsO_(3)(+0.56 V)stabilize the easy crystallization of ferric arsenates.However,activating solvothermal reactions with a reducing agent...The standard redox potentials of the Fe^(3+)/Fe^(2+)(+0.77 V)and H_(3)AsO_(4)/H_(3)AsO_(3)(+0.56 V)stabilize the easy crystallization of ferric arsenates.However,activating solvothermal reactions with a reducing agent such as hydrazine or ethanol may destabilize the solid compounds towards ferric,ferrous or mixed Fe^(2+/3+)arsenites.Few of them have been reported and in this work we have prepared four new members with various counter cations(Ba^(2+))or anions(OH^(−),Cl^(−))and various iron valence.The versatile condensation of ortho-arsenites(AsO_(3)^(2−))into pyro–(As_(2)O_(5)^(4−)),rings or meta-arsenites favours the creation of effcient spacers,able to tune the magnetic dimensionality of the iron-based framework.These four new members cover from 0D(paramagnetic Ba_(2)Fe^(Ⅱ)(As_(3)^(3+)O_(6))_(2)·H_(2)O),1D(S=5/2 ladders in BaFe_(2)^(Ⅱ)(As_(2)O_(5))(AsO_(3))(OH)),2D(layers of S=5/2 dimers in Ba_(2)Fe_(2)^(Ⅲ)(As_(2)O_(5))_(2),up to 3D(T_(N)=97 K in Fe_(3)^(2.66+)(As_(2)O_(5))(AsO_(3))Cl with charge ordering)topologies.Their magnetic properties are analysed by means of combined structural,experimental results and ab initio calculations.展开更多
Human branding has become an essential issue in political marketing.It is exempli fied in the election of American Presidents.This paper examines the American experience to suggest a typology of human branding that ma...Human branding has become an essential issue in political marketing.It is exempli fied in the election of American Presidents.This paper examines the American experience to suggest a typology of human branding that may apply in both presidential and other political systems.It examines examples of presidential human brands from George Washington on but,given significant changes to electoral procedures,concentrates on first-time successful presidential candidates since 1901.The fourfold typology offers an interrelated set of ideal types that will augment the analysis of human branding.It is applied to presidents when they take up office rather than after serving.The typology draws on the source of primary brand association and relation to the core political system of each politician.展开更多
Microgrids are gaining popularity by facilitating distributed energy resources(DERs)and forming essential consumer/prosumer centric integrated energy systems.Integration,coordination and control of multiple DERs and m...Microgrids are gaining popularity by facilitating distributed energy resources(DERs)and forming essential consumer/prosumer centric integrated energy systems.Integration,coordination and control of multiple DERs and managing the energy transition in this environment is a strenuous task.Classical control techniques are not enough to support dynamic microgrid environments.Implementation of Artificial Intelligence(AI)techniques seems to be a promising solution to enhance the control and operation of microgrids in future smart grid networks.Therefore,this paper briefly reviews the control architectures,existing conventional controlling techniques,their drawbacks,the need for intelligent controllers and then extensively reviews the possibility of AI implementation in different control structures with a special focus on the hierarchical control layers.This paper also investigates the AI-based control strategies in networked/interconnected/multi-microgrids environments.It concludes with the summary and future scopes of AI implementation in hierarchical control layers and structures including single and networked microgrids environments.展开更多
Climate change is an ever-present issue,which has a vast variety of potential solutions,one of which being carbon capture.This paper aims to use bibliometric analysis techniques to find trends in carbon capture within...Climate change is an ever-present issue,which has a vast variety of potential solutions,one of which being carbon capture.This paper aims to use bibliometric analysis techniques to find trends in carbon capture within the technologies of adsorption,absorption,membranes,and hybrid technologies.The Web of Science core collection database performed bibliometric searches,with the‘Bibliometrix’plug-in for R software,performing the bibliometric analysis.Bibliometric data spanned across 1997–2020 and the investigation found that adsorption technologies dominated this period in terms of citations and articles,with hybrid technologies being the least produced but rising in scientific productivity and citations.The Analysis found China and the United States of America to be the dominant producers of articles,with global collaboration being central to carbon capture.The‘International Journal of Greenhouse Gas Control’ranked as the top producer of articles however,the‘ACS Applied Materials&Interfaces’was the leading journal in terms of H-index.展开更多
The combination of deep learning techniques and Raman spectroscopy shows great potential offering precise and prompt identification of pathogenic bacteria in clinical settings.However,the traditional closed-set classi...The combination of deep learning techniques and Raman spectroscopy shows great potential offering precise and prompt identification of pathogenic bacteria in clinical settings.However,the traditional closed-set classification approaches assume that all test samples belong to one of the known pathogens,and their applicability is limited since the clinical environment is inherently unpredictable and dynamic,unknown,or emerging pathogens may not be included in the available catalogs.We demonstrate that the current state-of-the-art neural networks identifying pathogens through Raman spectra are vulnerable to unknown inputs,resulting in an uncontrollable false positive rate.To address this issue,first we developed an ensemble of ResNet architectures combined with the attention mechanism that achieves a 30-isolate accuracy of 87.8±0.1%.Second,through the integration of feature regularization by the Objectosphere loss function,our model both achieves high accuracy in identifying known pathogens from the catalog and effectively separates unknown samples drastically reducing the false positive rate.Finally,the proposed feature regularization method during training significantly enhances the performance of out-of-distribution detectors during the inference phase improving the reliability of the detection of unknown classes.Our algorithm for Raman spectroscopy empowers the identification of previously unknown,uncataloged,and emerging pathogens ensuring adaptability to future pathogens that may surface.Moreover,it can be extended to enhance open-set medical image classification,bolstering its reliability in dynamic operational settings.展开更多
文摘Background:Successful liver resection in oncologic surgery depends on safety,precision,and efficacy,all of which require a thorough understanding of liver anatomy.Contrast-enhanced computed tomography(CT)-generated three-dimensional(3D)models have been proposed as a valuable tool to enhance this understanding.However,a systematic comparison of different display modalities across professional groups has not yet been performed.Methods:In this prospective,monocentric randomized trial,we compared high-resolution twodimensional(2D)CT images of liver malignancies with their corresponding standardized,non-colored 3D virtual and printed models in facilitating anatomical and spatial understanding as well as surgical decision-making.A total of 91 participants,including 40 surgeons,10 radiologists,and 41 students,evaluated six clinical cases(three centrally and three peripherally located liver malignancies).Each participant assessed one central and one peripheral case per display modality,presented in a random order.Results:Compared to 2D CT images,both 3D virtual and printed models significantly improved the identification of tumor location(P<0.001),enhanced the comprehension of spatial relationships with adjacent liver and portal veins(P<0.001 and P=0.019,respectively),and facilitated clinical decisionmaking(P<0.001).No significant difference was observed between virtual and printed models in terms of effectiveness.Within the different groups,surgeons and students,but not radiologists,more accurately identified tumor location and spatial relationships with adjacent liver and portal veins using 3D models.Subjectively,most surgeons and students preferred 3D printed models over virtual models and 2D CT images.Conclusions:This study demonstrated that standardized,non-colored 3D virtual and printed models equally help preoperative anatomical understanding and decision-making,particularly for surgeons and students.By isolating the influence of display modality,our findings clarify prior inconsistent results and support the integration of cost-effective 3D visualization by applying virtual models into surgical planning and education.Preference for printed models despite comparable efficacy highlights the importance of user-centered implementation strategies.
基金Key Project of Shanghai Committee of Science and Technology(11JC1403600)National Natural Science Foundation of China(21103050 and 21373086)+1 种基金National Key Basic Research Program of China(2013CB921800)Awards from the National Institute of General Medical Science of the National Institutes of Health(SC1 GM086268-08)
文摘四级核回波实验通常需要射频脉冲能够激发谱宽超过100 k Hz的信号.在最近的研究中,作者发现组合脉冲COM-II(9018090135 45)能够在氘核的四级核回波实验中实现宽带激发.此外,作者还结合了八步相位循环的方法,有效消除了由有限脉宽效应造成的谱图扭曲现象.利用了平均哈密顿原理,对该方法进行了理论计算研究.作者采用了自旋为1的矩阵算符,通过计算解释了八步相位循环能够消除谱图扭曲的原因.
文摘Nanosized Ba_(1-x)Bi_(x)Fe_(1-x)Cu_(x)O_(3)(12–50 nm)with x values of 0,0.01,0.05,and 0.1 system was prepared using the Pechini method.Structural,morphological,surface and optical characterizations were performed for the prepared samples.Cubic phase was the predominant phase for the undoped BaFeO_(3)and Bi and Cu co-doped BaFeO_(3)samples.Minor phases of monoclinic Ba_(2)Fe_(2)O_(5),orthorhombic BaFe_(2)O_(4)and orthorhombic BaCO_(3)were identified for all the prepared samples.Ba_(0.95)Bi_(0.05)Fe_(0.95)Cu_(0.05)O_(3)sample has the lowest band gap(2.43 e V).98.1%paracetamol removal was achieved with 0.75 g/L of Ba_(0.95)Bi_(0.05)Fe_(0.95)Cu_(0.05)O_(3)at pH9 after 120 min.The paracetamol degradation follows the pseudo first-order kinetics.HO·is the main oxidative species responsible for the paracetamol degradation.Gas chromatography–mass spectrometry(GC–MS)analysis was performed at the end of the photocatalytic degradation experiment under optimum operating condition using Ba_(0.95)Bi_(0.05)Fe_(0.95)Cu_(0.05)O_(3)to explain the reaction mechanism and identify the intermediate by-products which is confirmed by ultraviolet/visible(UV/Vis)spectroscopy study at different reaction times.
基金supported by Unité de Catalyse et Chimie du Solide (UCCS)sponsor of scholarship: China scholarship council and School of Environment, Tsinghua University
基金financial support from Region Hauts-de-France,FEDER,and Electricité de France(EDF)through PEROVSTAB programfinancial support from the IR-RMN-THC FR-3050 CNRS France for conducting solid-state NMR measurements.P.R.and G.N.M.R+1 种基金financial support from University of Lille and région Hauts-de-France.F.S“IMPRESSIVE”project which received funding from the European Union’s Horizon 2020 Research and Innovation Program under grant agreement number 826013.
文摘Environmental stability is a major bottleneck of perovskite solar cells.Only a handful of studies are investigating the effect of moisture on the structural degradation of the absorber.They mostly rely on ex situ experiments and on completely degraded samples,which restrict the assessment on initial and final stage.By combining in situ X-ray diffraction under controlled 85%relative humidity,and live observations of the water-induced degradation using liquid-cell transmission electron microscopy,we reveal two competitive degradation paths leading on one hand to the decomposition of state-of-theart mixed cation/anion(Cs_(0.05)(MA_(0.17)FA_(0.83))_(0.95)Pb(Br_(0.17)I_(0.83))_(3)(CsMAFA)into PbI_(2) through a dissolution/recrystallization mechanism and,on the other hand,to a non-equilibrium phase segregation leading to CsPb_(2)Br_(5) and a Cesium-poor/iodide-rich Cs_(0.05)-x(MA_(0.17)FA_(0.83))_(0.95)Pb(Br_(0.17-2y)I_(0.83)+2y)_(3) perovskite.This degradation mechanism is corroborated at atomic-scale resolution through solid-state ^(1)H and ^(133)Cs NMR analysis.Exposure to moisture leads to a film containing important heterogeneities in terms of morphology,photoluminescence intensities,and lifetimes.Our results provide new insights and consensus that complex perovskite compositions,though very performant as champion devices,are comparatively metastable,a trait that limits the chances to achieve long-term stability.
基金supported by CNRS standing for Centre National de la Recherche Scientifique (France),CAPES standing for Coordenao de Aperfeioamento de Pessoal de Nível Superior (Brazil),CNPq standing for Conselho Nacional de Desenvolvimento Científico e Tecnológico (Brazil) and FINEP standing for Financiadora de Estudos e Projetos (Brazil)
文摘An integrated approach combining the development of an innovative catalyst and the research of a set of adequate operating conditions for the propane oxidative dehydrogenation （ODH） is described.The experimental set-up,specially designed for steady-state and transient studies is presented.The preparation method,the characterization and the performances in steady-state and transient regimes of catalysts based on V2W4O194-Lindqvist isopolyanion used as a precursor and supported on alumina are reported.The influence of the preparation method of the catalyst and the role of water in the feed gas are more particularly discussed.
文摘The synthesis and characterization of several dispersed molybdena catalysts on silica support (MoO3-SiO2) prepared from a variety of precursors (Mo(VI)-acetylacetonate, oxo-peroxo Mo-species, hydrated ammonium heptamolybdate) and preparation methods (deposition of the Mo-phase on finite SiO2 support by aqueous and methanol impregnations, by adsorption, by oxo-peroxo route-like, and by one-step synthesis of MoO3-SiO2 system with molecular precursors) are presented. The molybdena concentration on silica was comprised in a large interval (1.5 - 14 wt%) depending on the preparation method which governed the Mo-loading on silica. Convenient comparisons among samples at similar Mo-concentration have been made discussing the morphologic-structural (XRD, XPS, UV-vis-DRS, and N2-adsorption) and physicochemical (TG-DTG, TPR, and n-butylamine-TPD) sample properties. Polymeric octahedral polymolybdate aggregates predominated in the samples prepared by aqueous and methanol impregnations, which were at high Mo-concentration. On the contrary, isolated Mo(VI) species in distorted Td symmetry predominated in the sample prepared by adsorption which was at very low Mo-concentration. The sample acidity was composed of a weak acidy site population, associated with the silica support, and a strong acid site population associated with the Mo-dispersed phase. Oxidation tests of formaldehyde, an oxygen-containing VOC (Volatile Organic Compound), were performed to determine the prevalent redox or acidic function of the Mo-species at the surface of the catalysts.
文摘Nowadays the system of public health is constructed in such a manner so that its main objective is the recovery of an already sick person, while prediction and prevention receive little attention. Meanwhile the development of these aspects of medicine can lead to the ability to control morbidity among the population, to identify chronic and genetic diseases in the early stages of development, and thus to prevent their further progression. This will reduce traditionally high costs of sick people treatment and the number of disabled population, and improve the quality and duration of life. The elaboration of new fields of science that are working on the study and interpretation of data obtained during laboratory and clinical research, creation of new methods for diagnosis, prognosis and treatment, provides an opportunity now to implement a new strategy, called PPPM, and gets promising results, which should lead to further development of an existing medicine.
基金carried out under the framework of the LOVE-ME project supported by the ANR(Grant ANR ANR-16-CE08-0023)。
文摘BaM_(2)(PO_(4))_(2)(M^(2+)transition metals)compounds display a variety of polymorphs;among those,the wellknown rhombohedralγ-form stands at the origin of a series of(quasi)_(2)D-magnetic behaviors intensively studied in the last few decades.We have prepared originalα-variants for M=Fe^(2+)and Mn_(2)+and investigated their stabilities and sequence of phase transitions by analogy to the already reported M=Co^(2+)case.Heating theα-phases leads to a variety of structural rearrangements betweenα,α’andβvariants,according to unified 1st order reconstructive transitions.However,spontaneous long-time transformations under ambient conditionsα→γ(Fe case)versusγ→α(Co case)denote a contrasted hierarchy of stable compounds verified by DFT calculations.Interestingly,inα-BaFe2(PO_(4))_(2)the quasi triangular Fe^(2+)O_(3)+2 coordination is rarely observed and relies on one very short Fe-O distance of ca.1.78A,destabilizing the edifice in favor of the most stable FeO6 in theγ-type,as verified by Crystal Orbital Hamilton Population(COHP)analysis.
基金supported by the ANR(Grant ANR ANR-16-CE08-0023).
文摘The standard redox potentials of the Fe^(3+)/Fe^(2+)(+0.77 V)and H_(3)AsO_(4)/H_(3)AsO_(3)(+0.56 V)stabilize the easy crystallization of ferric arsenates.However,activating solvothermal reactions with a reducing agent such as hydrazine or ethanol may destabilize the solid compounds towards ferric,ferrous or mixed Fe^(2+/3+)arsenites.Few of them have been reported and in this work we have prepared four new members with various counter cations(Ba^(2+))or anions(OH^(−),Cl^(−))and various iron valence.The versatile condensation of ortho-arsenites(AsO_(3)^(2−))into pyro–(As_(2)O_(5)^(4−)),rings or meta-arsenites favours the creation of effcient spacers,able to tune the magnetic dimensionality of the iron-based framework.These four new members cover from 0D(paramagnetic Ba_(2)Fe^(Ⅱ)(As_(3)^(3+)O_(6))_(2)·H_(2)O),1D(S=5/2 ladders in BaFe_(2)^(Ⅱ)(As_(2)O_(5))(AsO_(3))(OH)),2D(layers of S=5/2 dimers in Ba_(2)Fe_(2)^(Ⅲ)(As_(2)O_(5))_(2),up to 3D(T_(N)=97 K in Fe_(3)^(2.66+)(As_(2)O_(5))(AsO_(3))Cl with charge ordering)topologies.Their magnetic properties are analysed by means of combined structural,experimental results and ab initio calculations.
文摘Human branding has become an essential issue in political marketing.It is exempli fied in the election of American Presidents.This paper examines the American experience to suggest a typology of human branding that may apply in both presidential and other political systems.It examines examples of presidential human brands from George Washington on but,given significant changes to electoral procedures,concentrates on first-time successful presidential candidates since 1901.The fourfold typology offers an interrelated set of ideal types that will augment the analysis of human branding.It is applied to presidents when they take up office rather than after serving.The typology draws on the source of primary brand association and relation to the core political system of each politician.
文摘Microgrids are gaining popularity by facilitating distributed energy resources(DERs)and forming essential consumer/prosumer centric integrated energy systems.Integration,coordination and control of multiple DERs and managing the energy transition in this environment is a strenuous task.Classical control techniques are not enough to support dynamic microgrid environments.Implementation of Artificial Intelligence(AI)techniques seems to be a promising solution to enhance the control and operation of microgrids in future smart grid networks.Therefore,this paper briefly reviews the control architectures,existing conventional controlling techniques,their drawbacks,the need for intelligent controllers and then extensively reviews the possibility of AI implementation in different control structures with a special focus on the hierarchical control layers.This paper also investigates the AI-based control strategies in networked/interconnected/multi-microgrids environments.It concludes with the summary and future scopes of AI implementation in hierarchical control layers and structures including single and networked microgrids environments.
基金The Irish Research Council funded this study under the 2021 Environmental Protection Agency Postgraduate Scholarship GOIPG/2021/1523.
文摘Climate change is an ever-present issue,which has a vast variety of potential solutions,one of which being carbon capture.This paper aims to use bibliometric analysis techniques to find trends in carbon capture within the technologies of adsorption,absorption,membranes,and hybrid technologies.The Web of Science core collection database performed bibliometric searches,with the‘Bibliometrix’plug-in for R software,performing the bibliometric analysis.Bibliometric data spanned across 1997–2020 and the investigation found that adsorption technologies dominated this period in terms of citations and articles,with hybrid technologies being the least produced but rising in scientific productivity and citations.The Analysis found China and the United States of America to be the dominant producers of articles,with global collaboration being central to carbon capture.The‘International Journal of Greenhouse Gas Control’ranked as the top producer of articles however,the‘ACS Applied Materials&Interfaces’was the leading journal in terms of H-index.
文摘The combination of deep learning techniques and Raman spectroscopy shows great potential offering precise and prompt identification of pathogenic bacteria in clinical settings.However,the traditional closed-set classification approaches assume that all test samples belong to one of the known pathogens,and their applicability is limited since the clinical environment is inherently unpredictable and dynamic,unknown,or emerging pathogens may not be included in the available catalogs.We demonstrate that the current state-of-the-art neural networks identifying pathogens through Raman spectra are vulnerable to unknown inputs,resulting in an uncontrollable false positive rate.To address this issue,first we developed an ensemble of ResNet architectures combined with the attention mechanism that achieves a 30-isolate accuracy of 87.8±0.1%.Second,through the integration of feature regularization by the Objectosphere loss function,our model both achieves high accuracy in identifying known pathogens from the catalog and effectively separates unknown samples drastically reducing the false positive rate.Finally,the proposed feature regularization method during training significantly enhances the performance of out-of-distribution detectors during the inference phase improving the reliability of the detection of unknown classes.Our algorithm for Raman spectroscopy empowers the identification of previously unknown,uncataloged,and emerging pathogens ensuring adaptability to future pathogens that may surface.Moreover,it can be extended to enhance open-set medical image classification,bolstering its reliability in dynamic operational settings.
