Thermoelectric(TE)devices can realize the conversion of heat energy and electrical power based on Seebeck effect and Peltier effect.Among them,flexible TE devices have received more attention recently due to their bet...Thermoelectric(TE)devices can realize the conversion of heat energy and electrical power based on Seebeck effect and Peltier effect.Among them,flexible TE devices have received more attention recently due to their better attachment to various heat sources and aimed components with arbitrary shapes.To improve the performance of flexible TE devices for various application scenarios,large efforts have been made to design the leg patterns,the electrical and thermal contact issues,and the substrate and encapsulation materials for the decrease of heat loss.This paper is to review the advancements about the design of flexible inorganic TE devices over the last decade.Firstly,the design of flexible thin-film TE devices based on the direction of temperature gradient,including the patterns of TE legs,the fabrication methods,and the flexible substrate materials is summarized.Secondly,the design of wearable TE devices that contains common architecture of the module,the substrates and encapsulations,the electrical and thermal contact,and some thin-film based wearable devices with curving TE legs is demonstrated.Thirdly,the characterizations of the flexibility of TE devices and the current applications are outlined.Moreover,some views about the future development for TE devices are proposed.展开更多
The electrochemical water splitting to produce hydrogen converts electric energy into clean hydrogen energy,which is a groundbreaking concept of energy optimization.To achieve high efficiency,numerous strategies have ...The electrochemical water splitting to produce hydrogen converts electric energy into clean hydrogen energy,which is a groundbreaking concept of energy optimization.To achieve high efficiency,numerous strategies have been developed to enhance the performance of electrocatalysts.Among these,interface engineering with molecules/ions/groups,serves as a versatile approach for optimizing the performance of electrocatalysts in water splitting.On the basis of numerous achievements in high-performance electrocatalysts engineered through molecules/ions/groups at interface,a comprehensive understanding of these advancements is crucial for guiding future progress.Herein,after providing a concise overview of the background,the interface engineering via molecules/ions/groups for electrocatalytic water splitting is demonstrated from three perspectives.Firstly,the engineering of electronic state of electrocatalysts by molecules/ions/groups at interface to reduce the Gibbs free energy of the corresponding reactions.Secondly,the modification of local microenvironment surrounding electrocatalysts via molecules/ions/groups at interface to enhance the transfer of reactants and products.Thirdly,the protection of electrocatalysts with molecule/ion/group fences improves their durability,including protecting active sites from leaching and defending them against harmful species.The fundamental principles of these three aspects are outlined for each,along with pertinent comments.Finally,several research directions and challenges are proposed.展开更多
The inter-nanocrystal （NC） distance, necking degree, ordering level, and NC surface ligands all affect the electronic and optoelectronic properties of NC solids. Herein, we introduce a unique PbS structure of neckin...The inter-nanocrystal （NC） distance, necking degree, ordering level, and NC surface ligands all affect the electronic and optoelectronic properties of NC solids. Herein, we introduce a unique PbS structure of necking percolative superlattices to exclude the morphological factors and study the effect of ligands on the NC properties. X-ray photoelectron spectroscopy data indicate that 1,2-ethanedithiol （EDT）, oxalic acid, mercaptopropionic acid, and NH4SCN （SCN） ligands were attached to the surface of NCs by substrate-supported Iigand exchange. Field-effect transistors were tested and photodetector measurements were performed to compare these NC solids. An SCN-treated film had the highest mobility and responsivity under high-power intensity irradiation owing to its high carrier density, whereas an EDT-treated film had the lowest mobility, photocurrent, and dark current. These findings introduce new avenues for choosing suitable ligands for NC applications.展开更多
Alkaline hydrogen evolution reaction(HER)offers a near-zero-emission approach to advance hydrogen energy.However,the activity limited by the multiple reaction steps involving H_(2)O molecules transfer,absorption,and a...Alkaline hydrogen evolution reaction(HER)offers a near-zero-emission approach to advance hydrogen energy.However,the activity limited by the multiple reaction steps involving H_(2)O molecules transfer,absorption,and activation still unqualified the thresholds of economic viability.Herein,we proposed a multisite complementary strategy that incorporates hydrophilic Mo and electrophilic V into Ni-based catalysts to divide the distinct steps on atomically dispersive sites and thus realize sequential regulation of the HER process.The Isotopic labeled in situ Raman spectroscopy describes 4-coordinated hydrogen bonded H_(2)O to be free H_(2)O passing the inner Helmholtz plane in the vicinity of the catalysts under the action of hydrophilic Mo sites.Furthermore,potential-dependent electrochemical impedance spectroscopy(EIS)reveals that electrophilic V sites with abundant 3d empty orbitals could activate the lone-pair electrons in the free H_(2)O molecules to produce more protic hydrogen,and dimerize into H_(2) at the Ni sites.By the sequential management of reactive H_(2)O molecules,NiMoV oxides multisite catalysts surpass Pt/C hydrogen evolution activity(49 mV@10 mA∙cm^(-2) over 140 h).Profoundly,this study provides a tangible model to deepen the comprehension of the catalyst–electrolyte interface and create efficient catalysts for diverse reactions.展开更多
基金The authors acknowledge financial support from the National Basic Research Program of China(No.2015CB932600)the National Key R&D Program of China(No.2017YFA0208000)+7 种基金the National Natural Science Foundation of China(Nos.21525523,21802130,21874121,21722507 and 21574048)the National Key Basic Research Program of China(Nos.2014CB931801 and 2016YFA0200700,Z.Y.T.)National Natural Science Foundation of China(Nos.21475029 and 91427302,Z.Y.T.)Frontier Science Key Project of the Chinese Academy of Sciences(No.QYZDJ-SSW-SLH038,Z.Y.T.)Instrument Developing Project of the Chinese Academy of Sciences(No.YZ201311,Z.Y.T.)CAS-CSIRO Cooperative Research Program(No.GJHZ1503,Z.Y.T.)“Strategic Priority Research Program”of Chinese Academy of Sciences(No.XDA09040100,Z.Y.T.)K.C.Wong Education Foundation,and Fundamental Research Funds for the Central Universities,China University of Geosciences(Wuhan)(No.CUG170669).
文摘Thermoelectric(TE)devices can realize the conversion of heat energy and electrical power based on Seebeck effect and Peltier effect.Among them,flexible TE devices have received more attention recently due to their better attachment to various heat sources and aimed components with arbitrary shapes.To improve the performance of flexible TE devices for various application scenarios,large efforts have been made to design the leg patterns,the electrical and thermal contact issues,and the substrate and encapsulation materials for the decrease of heat loss.This paper is to review the advancements about the design of flexible inorganic TE devices over the last decade.Firstly,the design of flexible thin-film TE devices based on the direction of temperature gradient,including the patterns of TE legs,the fabrication methods,and the flexible substrate materials is summarized.Secondly,the design of wearable TE devices that contains common architecture of the module,the substrates and encapsulations,the electrical and thermal contact,and some thin-film based wearable devices with curving TE legs is demonstrated.Thirdly,the characterizations of the flexibility of TE devices and the current applications are outlined.Moreover,some views about the future development for TE devices are proposed.
基金supported by the National Natural Science Foundation of China(Nos.22071069,22090050,22176180,21874121 and 21974128)the National Key Research and Development Program of China(Nos.2018YFE0206900 and 2021YFA1200400)+2 种基金Zhejiang Provincial Natural Science Foundation of China under Grant(Nos.LY20B050002 and LD21B050001)Hubei Provincial Natural Science Foundation of China(No.2020CFA037)the Foundation of Basic and Applied Basic Research of Guangdong Province(No.2019B1515120087).
文摘The electrochemical water splitting to produce hydrogen converts electric energy into clean hydrogen energy,which is a groundbreaking concept of energy optimization.To achieve high efficiency,numerous strategies have been developed to enhance the performance of electrocatalysts.Among these,interface engineering with molecules/ions/groups,serves as a versatile approach for optimizing the performance of electrocatalysts in water splitting.On the basis of numerous achievements in high-performance electrocatalysts engineered through molecules/ions/groups at interface,a comprehensive understanding of these advancements is crucial for guiding future progress.Herein,after providing a concise overview of the background,the interface engineering via molecules/ions/groups for electrocatalytic water splitting is demonstrated from three perspectives.Firstly,the engineering of electronic state of electrocatalysts by molecules/ions/groups at interface to reduce the Gibbs free energy of the corresponding reactions.Secondly,the modification of local microenvironment surrounding electrocatalysts via molecules/ions/groups at interface to enhance the transfer of reactants and products.Thirdly,the protection of electrocatalysts with molecule/ion/group fences improves their durability,including protecting active sites from leaching and defending them against harmful species.The fundamental principles of these three aspects are outlined for each,along with pertinent comments.Finally,several research directions and challenges are proposed.
基金Acknowledgements This work was supported financially by Chinese ministry of science and technology （No. 2016YFA0200700）, National Basic Research Program of China （No. 2014CB931801, Z. Y. T.）, National Natural Science Foundation of China （No. 21473044, C. G. L. Nos. 21475029 and 91427302, Z. Y. T.）, Instrument Developing Project of the Chinese Academy of Sciences （No. YZ201311, Z. Y. T.）, CAS-CSIRO Cooperative Research Program （No. GJHZ1503, Z. Y. T.）, and ＂Strategic Priority Research Program＂ of Chinese Academy of Sciences （No. XDA09040100, Z. Y. T.）.
文摘The inter-nanocrystal （NC） distance, necking degree, ordering level, and NC surface ligands all affect the electronic and optoelectronic properties of NC solids. Herein, we introduce a unique PbS structure of necking percolative superlattices to exclude the morphological factors and study the effect of ligands on the NC properties. X-ray photoelectron spectroscopy data indicate that 1,2-ethanedithiol （EDT）, oxalic acid, mercaptopropionic acid, and NH4SCN （SCN） ligands were attached to the surface of NCs by substrate-supported Iigand exchange. Field-effect transistors were tested and photodetector measurements were performed to compare these NC solids. An SCN-treated film had the highest mobility and responsivity under high-power intensity irradiation owing to its high carrier density, whereas an EDT-treated film had the lowest mobility, photocurrent, and dark current. These findings introduce new avenues for choosing suitable ligands for NC applications.
文摘Alkaline hydrogen evolution reaction(HER)offers a near-zero-emission approach to advance hydrogen energy.However,the activity limited by the multiple reaction steps involving H_(2)O molecules transfer,absorption,and activation still unqualified the thresholds of economic viability.Herein,we proposed a multisite complementary strategy that incorporates hydrophilic Mo and electrophilic V into Ni-based catalysts to divide the distinct steps on atomically dispersive sites and thus realize sequential regulation of the HER process.The Isotopic labeled in situ Raman spectroscopy describes 4-coordinated hydrogen bonded H_(2)O to be free H_(2)O passing the inner Helmholtz plane in the vicinity of the catalysts under the action of hydrophilic Mo sites.Furthermore,potential-dependent electrochemical impedance spectroscopy(EIS)reveals that electrophilic V sites with abundant 3d empty orbitals could activate the lone-pair electrons in the free H_(2)O molecules to produce more protic hydrogen,and dimerize into H_(2) at the Ni sites.By the sequential management of reactive H_(2)O molecules,NiMoV oxides multisite catalysts surpass Pt/C hydrogen evolution activity(49 mV@10 mA∙cm^(-2) over 140 h).Profoundly,this study provides a tangible model to deepen the comprehension of the catalyst–electrolyte interface and create efficient catalysts for diverse reactions.
