Reorganization energy(RE)is closely related to the charge transport properties and is one of the important parameters for screening novel organic semiconductors(OSCs).With the rise of data-driven technology,accurate a...Reorganization energy(RE)is closely related to the charge transport properties and is one of the important parameters for screening novel organic semiconductors(OSCs).With the rise of data-driven technology,accurate and efficient machine learning(ML)models for high-throughput screening novel organic molecules play an important role in the boom of material science.Comparing different molecular descriptors and algorithms,we construct a reasonable algorithm framework with molecular graphs to describe the compositional structure,convolutional neural networks to extract material features,and subsequently embedded fully connected neural networks to establish the mapping between features and predicted properties.With our well-designed judicious training pattern about feature-guided stratified random sampling,we have obtained a high-precision and robust reorganization energy prediction model,which can be used as one of the important descriptors for rapid screening potential OSCs.The root-meansquare error(RMSE)and the squared Pearson correlation coefficient(R^(2))of this model are 2.6 me V and0.99,respectively.More importantly,we confirm and emphasize that training pattern plays a crucial role in constructing supreme ML models.We are calling for more attention to designing innovative judicious training patterns in addition to high-quality databases,efficient material feature engineering and algorithm framework construction.展开更多
Implant-associated infections caused by biomedical catheters severely threaten patients'health.The use of electrochemical control on NO release from benign nitrite equipped in the catheter can potentially resolve ...Implant-associated infections caused by biomedical catheters severely threaten patients'health.The use of electrochemical control on NO release from benign nitrite equipped in the catheter can potentially resolve this issue with excellent biocompatibility.Inspired by nitrite reductase,a Cu-BDC(BDC:benzene-1,4-dicarboxylic acid)catalyst with coordinated Cu(Ⅱ)sites was constructed as a heterogeneous electrocatalyst to control nitrite reduction to nitric oxide for catheter antibacteria.The combined results of in situ and ex situ tests unveil the key function of interconversion between Cu(Ⅱ)and Cu(Ⅰ)species in NO_(2)^(-)reduction to NO.After being incorporated into the actual catheter,the Cu-BDC catalyst exhibits high electrocatalytic activity toward NO_(2)^(-)reduction to NO and excellent antibacteria efficacy with a sterilizing rate of 99.9%,paving the way for the development of advanced metal-organic frameworks(MOFs)electrocatalysts for catheter antibacteria.展开更多
The compatibility of the gate dielectrics with semiconductors is vital for constructing efficient conducting channel for high charge transport.However,it is still a highly challenging mission to clearly clarify the re...The compatibility of the gate dielectrics with semiconductors is vital for constructing efficient conducting channel for high charge transport.However,it is still a highly challenging mission to clearly clarify the relationship between the dielectric layers and the chemical structure of semiconductors,especially vacuum-deposited small molecules.Here,interfacial molecular screening of polyimide(Kapton)dielectric in organic field-effect transistors(OFETs)is comprehensively studied.It is found that the semiconducting small molecules with alkyl side chains prefer to form a high-quality charge transport layer on polyimide(PI)dielectrics compared with the molecules without alkyl side chains.On this basis,the fabricated transistors could reach the mobility of 1.2 cm^(2) V^(−1)s^(−1) the molecule with alkyl side chains on bare PI dielectric.What is more,the compatible semiconductor and dielectric would further produce a low activation energy(E_(A))of 3.01 meV towards efficient charge transport even at low temperature(e.g.,100 K,0.9 cm^(2) V^(−1)s^(−1)).Our research provides a guiding scheme for the construction of high-performance thin-film field-effect transistors based on PI dielectric layer at room and low temperatures.展开更多
A thioester-functionalized triphenylamine hole-transporting molecule(TPD-SAc) was synthesized and self-assembled to form a monolayer on an ultra-thin Au film supported on indium-tin oxide glass. The modified surface w...A thioester-functionalized triphenylamine hole-transporting molecule(TPD-SAc) was synthesized and self-assembled to form a monolayer on an ultra-thin Au film supported on indium-tin oxide glass. The modified surface was characterized by aqueous contact angle, ellipsometer, atomic force microscopy, X-ray photoelectron spectroscopy, and ultraviolet photoelectron spectrometer to substantiate the formation of compact and pinhole-free monolayers. The modified organic light emitting diode device [indium-tin oxide/Au(5 nm)/self-assembled monolayers(SAM)/TPD(50 nm)/Alq_3(40 nm)/TPBI(15 nm)/LiF(1 nm)/Al(100 nm)] showed a luminance of 7303.90 cd/m^2 and a current efficiency of 8.49 cd/A with 1.78 and 2.29-fold increase, respectively, compared to the control device without SAM. The improvements were attributed to the enhanced compatibility of the organic–inorganic interface, matched energy level by introduction of an energy mediating step and superior hole-injection property of SAM molecules.展开更多
Aqueous two-phase system features with ultralow interfacial tension and thick interfacial region,affording unique confined space for membrane assembly.Here,for the first time,an aqueous two-phase interfacial assembly ...Aqueous two-phase system features with ultralow interfacial tension and thick interfacial region,affording unique confined space for membrane assembly.Here,for the first time,an aqueous two-phase interfacial assembly method is proposed to fabricate covalent organic framework(COF)membranes.The aqueous solution containing polyethylene glycol and dextran undergoes segregated phase separation into two water-rich phases.By respectively distributing aldehyde and amine monomers into two aqueous phases,a series of COF membranes are fabricated at water-water interface.The resultant membranes exhibit high NaCl rejection of 93.0-93.6% and water permeance reaching 1.7-3.7 L m^(−2) h^(−1) bar^(−1),superior to most water desalination membranes.Interestingly,the interfacial tension is found to have pronounced effect on membrane structures.The appropriate interfacial tension range(0.1-1.0 mN m^(−1))leads to the tight and intact COF membranes.Furthermore,the method is extended to the fabrication of other COF and metal-organic polymer membranes.This work is the first exploitation of fabricating membranes in all-aqueous system,confering a green and generic method for advanced membrane manufacturing.展开更多
Due to the mechanical flexibility,light weight,aesthetics,absorption tunability and environmental friendliness,organic solar cells(OSCs)have superior application potential over their inorganic counterparts including s...Due to the mechanical flexibility,light weight,aesthetics,absorption tunability and environmental friendliness,organic solar cells(OSCs)have superior application potential over their inorganic counterparts including silicon and perovskite solar cells(PSCs).Thanks to these benefits,the past decade have witnessed the rapid growth of flexible OSCs,semitransparent OSCs and indoor OSCs.In this progress report,we firstly overview the recent advance of the applications of the three promising OSCs.Subsequently,we sketch the critical points for the three classes of OSCs and highlight the efforts paid by the research community to address these issues.Besides,we discuss some popular strategies to afford great performance of each kind of OSC,respectively,and underline the corresponding breakthrough directions.Last but not least,we present the remaining challenges for advancing the commercial applications of these three classes of OSCs.展开更多
Excessive nitrate in groundwater has emerged as a serious environmental concern. The elevated nitrate concentration in drinking water causes a serious threat to public health on account of the possible transformation ...Excessive nitrate in groundwater has emerged as a serious environmental concern. The elevated nitrate concentration in drinking water causes a serious threat to public health on account of the possible transformation of nitrate to nitrite, which is one of the main predisposing factors of methemoglobinemia [1].展开更多
In this study, we applied a novel, mild, and convenient synthetic method involving the oxidative cyclization of 1-(pyrazin-2-yl)guanidine derivatives to produce [1,2,4]triazolo[4,3-a ]pyrazin-3-amines. We optimized th...In this study, we applied a novel, mild, and convenient synthetic method involving the oxidative cyclization of 1-(pyrazin-2-yl)guanidine derivatives to produce [1,2,4]triazolo[4,3-a ]pyrazin-3-amines. We optimized the reaction procedure to easily obtain 5-chloro-[1,2,4]triazolo[4,3-a ]pyrazin-3-amine. Various types of halogenated pyrazines can successfully undergo this process. We synthesized a series of 1-(pyrazin-2-yl)guanidines and [1,2,4]triazolo[4,3-a ]pyrazin-3-amines, and then elucidated their structures based on their ~1H-NMR, ^(13)C-NMR, ESI-HRMS, and nuclear Overhauser effect spectra.展开更多
Precise spatial control of 2D materials is the key capability of engineering their optical,electronic,and mechanical properties.However,growth of novel 2D Mo2C on Cu surface by chemical vapor deposition method was rev...Precise spatial control of 2D materials is the key capability of engineering their optical,electronic,and mechanical properties.However,growth of novel 2D Mo2C on Cu surface by chemical vapor deposition method was revealed to be seed-induced 2D growth,limiting further synthesis of complex Mo2C spatial structures.In this research,we demonstrate the controlled growth of Mo2C pyramids with numerous morphologies,which are characterized with clear terraces within the structures.The whole evolution for Mo2C pyramids in the coursed of CVD process has been detected,posing significant potential in probing growth mechanism.The formation of the Mo2C pyramids arises from the supersaturation-induced nucleation and concentration-gradient driven diffused growth of a new Mo2C layer on the edged areas of intrinsic ones,as supported by STEM imaging.This work provides a novel Mo2C-based pyramid structure and further reveals a sliding growth mechanism,which could offer impetus for the design of new 3D spatial structures of Mo2C and other 2D materials.展开更多
This highlight indicates that the local electrostatic interactions between metal cations and key intermediates facilitate the electrocatalytic CO_(2) reduction reaction.Electrocatalytic CO_(2) reduction reaction(CO_(2...This highlight indicates that the local electrostatic interactions between metal cations and key intermediates facilitate the electrocatalytic CO_(2) reduction reaction.Electrocatalytic CO_(2) reduction reaction(CO_(2)RR)has been considered as a promising strategy to achieve a carbon-neutral cycle and produce valuable fuels and feedstocks.展开更多
Organic solar cells(OSCs) especially non-fullerene OSCs(NF-OSCs) are promising to become the next-generation of commercial applications and have received great attention from many researchers due to their typical adva...Organic solar cells(OSCs) especially non-fullerene OSCs(NF-OSCs) are promising to become the next-generation of commercial applications and have received great attention from many researchers due to their typical advantages of low cost,light weight,and flexibility [1,2].展开更多
Comprehensive Summary Since the concept of 2D inorganic molecular crystals(2DIMCs)was introduced,intensive attentions have been gradually devoted to this field.Herein,the very recent advances in growth,properties,and ...Comprehensive Summary Since the concept of 2D inorganic molecular crystals(2DIMCs)was introduced,intensive attentions have been gradually devoted to this field.Herein,the very recent advances in growth,properties,and applications of 2D inorganic molecular crystals are comprehensively reviewed.Firstly,the newly emerged 2DIMCs are classified into three categories.Then the two typical production methods are present,thus leading to discrepancy in size,distribution,morphology and structures of 2DIMCs.Moreover,the unique physicochemical properties of 2DIMCs are demonstrated on the basis of the as-obtained 2DIMCs,the various applications are exhibited,demonstrating significant potential in related fields.Finally,the perspective and prospects are outlooked to offer insights in further development of 2DIMCs.展开更多
Singlet fission(SF)has potential applications in high-efficiency photo-energy harvesting applications,but its practical application is hindered by the limited number of materials.In this work,we explored the bay aroma...Singlet fission(SF)has potential applications in high-efficiency photo-energy harvesting applications,but its practical application is hindered by the limited number of materials.In this work,we explored the bay aromatic substitution strategy for the design of new perylenediimide(PDI)based SF materials.A series of PDI derivatives with biphenyl or naphthalene units substituted at the bay posi-tions were designed and synthesized to investigate the effects of aromatic substitutes on their photodynamic behaviours.The bay substitutions do not shift the energy level of the PDI core significantly but give rise to different intermolecular coupling strengths in the thin films and affect the intermolecular SF efficiency.Femtosecond transient absorption(fsTA)spectroscopy reveals that appro-priate spacing configuration from the bay aromatic substitution groups enhances the SF yields by promoting the interaction of neighbouring PDI cores.Triplet exciton yields of up to 183%have been obtained from these new PDI derivatives,making them po-tential candidates in future SF-based optoelectronics.展开更多
The Ni-catalyzed highly selective diborylative cyclization of 1,6-enynes with diboron reagent has been developed. When pinB-Bdan was used, multiple types of boron-containing functional groups could be installed into o...The Ni-catalyzed highly selective diborylative cyclization of 1,6-enynes with diboron reagent has been developed. When pinB-Bdan was used, multiple types of boron-containing functional groups could be installed into organic molecule with great chemoselectivity and regioselectivity though this reaction. Meanwhile, if B_2pai_2 was employed, the asymmetric diborylative cyclization could be well induced by using strategy of dynamic kinetic resolution. Importantly, the above reactions could afford desired product with 100% atomic economy, and could be compatible with different series of substituents. The studies of further transformation well illustrated that different type products could serve diverse synthetic strategy. Notably, the reaction mechanism was intensively studied by density functional theory(DFT) calculations, which could reveal the mechanism of regio- and enantio-selective control.展开更多
Improving the complete ethanol electrooxidation on Pd-based catalysts in alkaline media has drawn widely attention due to the high mass energy density.However,the weak adsorption energy of CH_(3)CO^(*) on Pd restricts...Improving the complete ethanol electrooxidation on Pd-based catalysts in alkaline media has drawn widely attention due to the high mass energy density.However,the weak adsorption energy of CH_(3)CO^(*) on Pd restricts the C–C bond cleavage.Inspired by the molecular orbital theory,we proposed the d-state-editing strategy to construct more unoccupied d-states of Pd for the enhanced interaction with CH_(3)CO^(*) to break C–C bonds.As expected,the reduced number of e_g electrons and more unoccupied d-states of Pd successfully formed on as-prepared porous Rh Au–Pd Cu nanosheets(PNSs).Theoretical calculations show that the optimized d-states of Rh Au–Pd Cu PNS can effectively improve the adsorption of CH_(3)CO^(*) and drastically reduce the energy barrier of C–C bond cleavage,thus boosting the complete oxidation of ethanol.The charge ratio of C_1 pathway on Rh Au–Pd Cu PNSs is 51.5%,more than 2 times higher than that of Pd NSs.Our finding provides an innovative perspective for the design of highly-efficient noble-based electrocatalysts.展开更多
Thiolate-protected atomically precise nanoclusters(NCs)demonstrate a series of unique luminescent characteristics attributed to their various peculiar electronic structures.Therefore,fluorescent NCs present extraordin...Thiolate-protected atomically precise nanoclusters(NCs)demonstrate a series of unique luminescent characteristics attributed to their various peculiar electronic structures.Therefore,fluorescent NCs present extraordinary practical values in biosensing and bioimaging research fields.Nevertheless,restricted by the types of fluorescent NCs,there are great difficulties in promoting the development of NCs in fluorescent research areas.As a result,it is of significant necessity for researchers to develop new synthetic pathways to produce high-quality fluorescent NCs.According to the analysis about the structural characteristics of fluorescent NCs,some general features like longer motif and higher ligand-to-metal ratio can be found,consistent to some presented regularities in etching reaction.Consequently,in this work,we used Au_(25)(MHA)_(18)(MHA=6-mercaptohexanoic acid)as a model nanocluster and utilized the etching reaction to systematically explore etching products and their corresponding luminescent properties.Moreover,we also identified three main reaction processes in the entire etching reaction process,which can generate new metal nanocluster species with various fluorescent properties.Hence,the etching reaction will provide a good platform to produce new luminescent metal NC species.展开更多
Atomically precise metal nanoclusters(MNCs),as a potential type of photoacoustic(PA)contrast agent,are limited in application due to their low PA conversion efficiency(PACE).Here,with hydrophilic Au25SR18(SR=thiolate)...Atomically precise metal nanoclusters(MNCs),as a potential type of photoacoustic(PA)contrast agent,are limited in application due to their low PA conversion efficiency(PACE).Here,with hydrophilic Au25SR18(SR=thiolate)as model NCs,we present a result that weakly polar solvent induces aggregation,which effectively enhances PA intensity and PACE.The PA intensity and PACE are highly dependent on the degree of aggregation,while the aggregation-enhanced PA intensity(AEPA)positively correlates to the protected ligands.Such an AEPA phenomenon indicates that aggregation actually accelerates the intramolecular motion of Au NCs,and enlarges the proportion of excited state energy dissipated through vibrational relaxation.This result conflicts with the restriction of intramolecular motion mechanism of aggregation-induced emission.Further experiments show that the increased energy of AEPA originates from the aggregation inhibiting the intermolecular energy transfer from excited Au NCs to their surrounding medium molecules,including solvent molecule and dissolved oxygen,rather than restricting radiative relaxations.This study develops a new strategy for enhancing the PA intensity of Au NCs,and contributes to a deeper understanding of the origin of the PA signal and the excited state energy dissipation processes for MNCs.展开更多
Zinc-air batteries(ZABs)are widely studied because of their high theoretical energy density,high battery voltage,environmental protection,and low price.However,the slow kinetics of oxygen reduction reaction(ORR)and ox...Zinc-air batteries(ZABs)are widely studied because of their high theoretical energy density,high battery voltage,environmental protection,and low price.However,the slow kinetics of oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)on the air electrode limits the further application of ZABs,so that how to develop a cheap,efficient,and stable catalyst with bifunctional catalytic activity is the key to solving the development of ZABs.Transition metal compounds are widely used as cathode materials for ZABs due to their low cost,high electrocatalytic activity,and stable structure.This review summarizes the research progress of transition metal compounds as bifunctional catalysts for ZABs.The development history,operation principle,and mechanism of ORR and OER reactions are introduced first.The application and development of transition metal compounds as bifunctional catalysts for ZABs in recent years are systematically introduced,including transition metal oxides(TMOs),transition metal nitrides(TMNs),transition metal sulfides(TMSs),transition metal carbides(TMCs),transition metal phosphates(TMPs),and others.In addition,the shortcomings of transition metal compounds as bifunctional catalysts for ZABs were summarized and reasonable design strategies and improvement measures were put forward,aiming at providing a reference for the design and construction of high-performance ZABs cathode materials.Finally,the challenges and future in this field are discussed and prospected.展开更多
Electrocatalytic CO_(2) reduction reaction(CO_(2) RR) can store and transform the intermittent renewable energy in the form of chemical energy for industrial production of chemicals and fuels,which can dramatically re...Electrocatalytic CO_(2) reduction reaction(CO_(2) RR) can store and transform the intermittent renewable energy in the form of chemical energy for industrial production of chemicals and fuels,which can dramatically reduce CO_(2) emission and contribute to carbon-neutral cycle. E cient electrocatalytic reduction of chemically inert CO_(2) is challenging from thermodynamic and kinetic points of view. Therefore,low-cost,highly e cient,and readily available electrocatalysts have been the focus for promoting the conversion of CO_(2). Very recently,interface engineering has been considered as a highly e ective strategy to modulate the electrocatalytic performance through electronic and/or structural modulation,regulations of electron/proton/mass/intermediates,and the control of local reactant concentration,thereby achieving desirable reaction pathway,inhibiting competing hydrogen generation,breaking binding-energy scaling relations of intermediates,and promoting CO_(2) mass transfer. In this review,we aim to provide a comprehensive overview of current developments in interface engineering for CO_(2) RR from both a theoretical and experimental stand-point,involving interfaces between metal and metal,metal and metal oxide,metal and nonmetal,metal oxide and metal oxide,organic molecules and inorganic materials,electrode and electrolyte,molecular catalysts and electrode,etc. Finally,the opportunities and challenges of interface engineering for CO_(2) RR are proposed.展开更多
Skin is the largest organ of the human body and can perceive and respond to complex environmental stimulations.Recently,the development of electronic skin(E-skin)for the mimicry of the human sensory system has drawn g...Skin is the largest organ of the human body and can perceive and respond to complex environmental stimulations.Recently,the development of electronic skin(E-skin)for the mimicry of the human sensory system has drawn great attention due to its potential applications in wearable human health monitoring and care systems,advanced robotics,artificial intelligence,and human-machine interfaces.Tactile sense is one of the most important senses of human skin that has attracted special attention.The ability to obtain unique functions using diverse assembly processible methods has rapidly advanced the use of graphene,the most celebrated two-dimensional material,in electronic tactile sensing devices.With a special emphasis on the works achieved since 2016,this review begins with the assembly and modification of graphene materials and then critically and comprehensively summarizes the most advanced material assembly methods,device construction technologies and signal characterization approaches in pressure and strain detection based on graphene and its derivative materials.This review emphasizes on:(1)the underlying working principles of these types of sensors and the unique roles and advantages of graphene materials;(2)state-of-the-art protocols recently developed for high-performance tactile sensing,including representative examples;and(3)perspectives and current challenges for graphene-based tactile sensors in E-skin applications.A summary of these cutting-edge developments intends to provide readers with a deep understanding of the future design of high-quality tactile sensing devices and paves a path for their future commercial applications in the field of E-skin.展开更多
基金financially supported by the Ministry of Science and Technology of China (2017YFA0204503 and 2018YFA0703200)the National Natural Science Foundation of China (52121002,U21A6002 and 22003046)+1 种基金the Tianjin Natural Science Foundation (20JCJQJC00300)“A Multi-Scale and High-Efficiency Computing Platform for Advanced Functional Materials”program,funded by Haihe Laboratory in Tianjin (22HHXCJC00007)。
文摘Reorganization energy(RE)is closely related to the charge transport properties and is one of the important parameters for screening novel organic semiconductors(OSCs).With the rise of data-driven technology,accurate and efficient machine learning(ML)models for high-throughput screening novel organic molecules play an important role in the boom of material science.Comparing different molecular descriptors and algorithms,we construct a reasonable algorithm framework with molecular graphs to describe the compositional structure,convolutional neural networks to extract material features,and subsequently embedded fully connected neural networks to establish the mapping between features and predicted properties.With our well-designed judicious training pattern about feature-guided stratified random sampling,we have obtained a high-precision and robust reorganization energy prediction model,which can be used as one of the important descriptors for rapid screening potential OSCs.The root-meansquare error(RMSE)and the squared Pearson correlation coefficient(R^(2))of this model are 2.6 me V and0.99,respectively.More importantly,we confirm and emphasize that training pattern plays a crucial role in constructing supreme ML models.We are calling for more attention to designing innovative judicious training patterns in addition to high-quality databases,efficient material feature engineering and algorithm framework construction.
基金the financial support from National Postdoctoral Science Foundation of China(Nos.2021M702436 and BX2021211)Haihe Laboratory of Sustainable Chemical Transformations+1 种基金National Natural Science Foundation of China(Nos.22101202 and 22071173)Tianjin Science and Technology Programme(Nos.20JCJQJC00050 and 22ZYJDSS00060)。
文摘Implant-associated infections caused by biomedical catheters severely threaten patients'health.The use of electrochemical control on NO release from benign nitrite equipped in the catheter can potentially resolve this issue with excellent biocompatibility.Inspired by nitrite reductase,a Cu-BDC(BDC:benzene-1,4-dicarboxylic acid)catalyst with coordinated Cu(Ⅱ)sites was constructed as a heterogeneous electrocatalyst to control nitrite reduction to nitric oxide for catheter antibacteria.The combined results of in situ and ex situ tests unveil the key function of interconversion between Cu(Ⅱ)and Cu(Ⅰ)species in NO_(2)^(-)reduction to NO.After being incorporated into the actual catheter,the Cu-BDC catalyst exhibits high electrocatalytic activity toward NO_(2)^(-)reduction to NO and excellent antibacteria efficacy with a sterilizing rate of 99.9%,paving the way for the development of advanced metal-organic frameworks(MOFs)electrocatalysts for catheter antibacteria.
基金financial support from National Key Research and Development Program(Nos.2021YFA0717900,2022YFE0124200)National Natural Science Foundation of China(Nos.62004138,52273190,61905121,U2241221)Haihe Laboratory of Sustainable Chemical Transformations.
文摘The compatibility of the gate dielectrics with semiconductors is vital for constructing efficient conducting channel for high charge transport.However,it is still a highly challenging mission to clearly clarify the relationship between the dielectric layers and the chemical structure of semiconductors,especially vacuum-deposited small molecules.Here,interfacial molecular screening of polyimide(Kapton)dielectric in organic field-effect transistors(OFETs)is comprehensively studied.It is found that the semiconducting small molecules with alkyl side chains prefer to form a high-quality charge transport layer on polyimide(PI)dielectrics compared with the molecules without alkyl side chains.On this basis,the fabricated transistors could reach the mobility of 1.2 cm^(2) V^(−1)s^(−1) the molecule with alkyl side chains on bare PI dielectric.What is more,the compatible semiconductor and dielectric would further produce a low activation energy(E_(A))of 3.01 meV towards efficient charge transport even at low temperature(e.g.,100 K,0.9 cm^(2) V^(−1)s^(−1)).Our research provides a guiding scheme for the construction of high-performance thin-film field-effect transistors based on PI dielectric layer at room and low temperatures.
基金supported by the National Natural Science Foundation of China(Nos.21506151,21576195 and 21776207)
文摘A thioester-functionalized triphenylamine hole-transporting molecule(TPD-SAc) was synthesized and self-assembled to form a monolayer on an ultra-thin Au film supported on indium-tin oxide glass. The modified surface was characterized by aqueous contact angle, ellipsometer, atomic force microscopy, X-ray photoelectron spectroscopy, and ultraviolet photoelectron spectrometer to substantiate the formation of compact and pinhole-free monolayers. The modified organic light emitting diode device [indium-tin oxide/Au(5 nm)/self-assembled monolayers(SAM)/TPD(50 nm)/Alq_3(40 nm)/TPBI(15 nm)/LiF(1 nm)/Al(100 nm)] showed a luminance of 7303.90 cd/m^2 and a current efficiency of 8.49 cd/A with 1.78 and 2.29-fold increase, respectively, compared to the control device without SAM. The improvements were attributed to the enhanced compatibility of the organic–inorganic interface, matched energy level by introduction of an energy mediating step and superior hole-injection property of SAM molecules.
基金The authors gratefully acknowledge financial support from National Key Research and Development Program of China(Nos.2021YFC2101200 and 2021YFB3802200)National Natural Science Foundation of China(Nos.22178251,21878216,91934302,21838008 and 21878215)+1 种基金Program of Introducing Talents of Discipline to Universities(No.BP0618007)the Haihe Laboratory of Sustainable Chemical Transformations.
文摘Aqueous two-phase system features with ultralow interfacial tension and thick interfacial region,affording unique confined space for membrane assembly.Here,for the first time,an aqueous two-phase interfacial assembly method is proposed to fabricate covalent organic framework(COF)membranes.The aqueous solution containing polyethylene glycol and dextran undergoes segregated phase separation into two water-rich phases.By respectively distributing aldehyde and amine monomers into two aqueous phases,a series of COF membranes are fabricated at water-water interface.The resultant membranes exhibit high NaCl rejection of 93.0-93.6% and water permeance reaching 1.7-3.7 L m^(−2) h^(−1) bar^(−1),superior to most water desalination membranes.Interestingly,the interfacial tension is found to have pronounced effect on membrane structures.The appropriate interfacial tension range(0.1-1.0 mN m^(−1))leads to the tight and intact COF membranes.Furthermore,the method is extended to the fabrication of other COF and metal-organic polymer membranes.This work is the first exploitation of fabricating membranes in all-aqueous system,confering a green and generic method for advanced membrane manufacturing.
基金the National Natural Science Foundation of China(No.52073207)the State Key Laboratory of Applied Optics(No.SKLAO2021001A17)for financial support.
文摘Due to the mechanical flexibility,light weight,aesthetics,absorption tunability and environmental friendliness,organic solar cells(OSCs)have superior application potential over their inorganic counterparts including silicon and perovskite solar cells(PSCs).Thanks to these benefits,the past decade have witnessed the rapid growth of flexible OSCs,semitransparent OSCs and indoor OSCs.In this progress report,we firstly overview the recent advance of the applications of the three promising OSCs.Subsequently,we sketch the critical points for the three classes of OSCs and highlight the efforts paid by the research community to address these issues.Besides,we discuss some popular strategies to afford great performance of each kind of OSC,respectively,and underline the corresponding breakthrough directions.Last but not least,we present the remaining challenges for advancing the commercial applications of these three classes of OSCs.
文摘Excessive nitrate in groundwater has emerged as a serious environmental concern. The elevated nitrate concentration in drinking water causes a serious threat to public health on account of the possible transformation of nitrate to nitrite, which is one of the main predisposing factors of methemoglobinemia [1].
基金supported by the National Nature Science Foundation of China(Nos.21576195 and 21776207)
文摘In this study, we applied a novel, mild, and convenient synthetic method involving the oxidative cyclization of 1-(pyrazin-2-yl)guanidine derivatives to produce [1,2,4]triazolo[4,3-a ]pyrazin-3-amines. We optimized the reaction procedure to easily obtain 5-chloro-[1,2,4]triazolo[4,3-a ]pyrazin-3-amine. Various types of halogenated pyrazines can successfully undergo this process. We synthesized a series of 1-(pyrazin-2-yl)guanidines and [1,2,4]triazolo[4,3-a ]pyrazin-3-amines, and then elucidated their structures based on their ~1H-NMR, ^(13)C-NMR, ESI-HRMS, and nuclear Overhauser effect spectra.
文摘Precise spatial control of 2D materials is the key capability of engineering their optical,electronic,and mechanical properties.However,growth of novel 2D Mo2C on Cu surface by chemical vapor deposition method was revealed to be seed-induced 2D growth,limiting further synthesis of complex Mo2C spatial structures.In this research,we demonstrate the controlled growth of Mo2C pyramids with numerous morphologies,which are characterized with clear terraces within the structures.The whole evolution for Mo2C pyramids in the coursed of CVD process has been detected,posing significant potential in probing growth mechanism.The formation of the Mo2C pyramids arises from the supersaturation-induced nucleation and concentration-gradient driven diffused growth of a new Mo2C layer on the edged areas of intrinsic ones,as supported by STEM imaging.This work provides a novel Mo2C-based pyramid structure and further reveals a sliding growth mechanism,which could offer impetus for the design of new 3D spatial structures of Mo2C and other 2D materials.
基金supported by the National Natural Science Foundation of China(22071172).
文摘This highlight indicates that the local electrostatic interactions between metal cations and key intermediates facilitate the electrocatalytic CO_(2) reduction reaction.Electrocatalytic CO_(2) reduction reaction(CO_(2)RR)has been considered as a promising strategy to achieve a carbon-neutral cycle and produce valuable fuels and feedstocks.
基金the Natural Science Foundation of China (52172048, 52103221, 51873172, 22205130, 12175298)the Shandon Provincial Natural Science Foundation of China (ZR2021QB024, ZR2021QB179, ZR2021ZD06)+2 种基金the Guangdong Natural Science Foundation of China (2023A1515012323, 2023A1515010943, 2022A1515110643)the National Key Research and Development Program of China (2022YFB4200400) funded by MOST of Chinathe Fundamental Research Funds of Shandong University from China。
文摘Organic solar cells(OSCs) especially non-fullerene OSCs(NF-OSCs) are promising to become the next-generation of commercial applications and have received great attention from many researchers due to their typical advantages of low cost,light weight,and flexibility [1,2].
基金the National Key R&D Program of China(2021YFA0717900)the National Natural Science Foundation of China(Grant 52002267)the Natural Science Foundation of Tianjin City(22JCJQJC00080,20JCQNJC01990).
文摘Comprehensive Summary Since the concept of 2D inorganic molecular crystals(2DIMCs)was introduced,intensive attentions have been gradually devoted to this field.Herein,the very recent advances in growth,properties,and applications of 2D inorganic molecular crystals are comprehensively reviewed.Firstly,the newly emerged 2DIMCs are classified into three categories.Then the two typical production methods are present,thus leading to discrepancy in size,distribution,morphology and structures of 2DIMCs.Moreover,the unique physicochemical properties of 2DIMCs are demonstrated on the basis of the as-obtained 2DIMCs,the various applications are exhibited,demonstrating significant potential in related fields.Finally,the perspective and prospects are outlooked to offer insights in further development of 2DIMCs.
基金supported by the National Natural Science Foundation of China(NSFC 51733004,51525303,21702085,21602093,21572086,22075117,92256202,U22A20399)the Fundamental Research Funds for the Central Universities(lzujbky-2022-kb01,Izujbky-2021-sp33,Izujbky-2021-27),and Supercomputing Center of Lanzhou University.
文摘Singlet fission(SF)has potential applications in high-efficiency photo-energy harvesting applications,but its practical application is hindered by the limited number of materials.In this work,we explored the bay aromatic substitution strategy for the design of new perylenediimide(PDI)based SF materials.A series of PDI derivatives with biphenyl or naphthalene units substituted at the bay posi-tions were designed and synthesized to investigate the effects of aromatic substitutes on their photodynamic behaviours.The bay substitutions do not shift the energy level of the PDI core significantly but give rise to different intermolecular coupling strengths in the thin films and affect the intermolecular SF efficiency.Femtosecond transient absorption(fsTA)spectroscopy reveals that appro-priate spacing configuration from the bay aromatic substitution groups enhances the SF yields by promoting the interaction of neighbouring PDI cores.Triplet exciton yields of up to 183%have been obtained from these new PDI derivatives,making them po-tential candidates in future SF-based optoelectronics.
基金supported by Tianjin University(B22021-010)the State Key Laboratory of Elemento-Organic Chemistrythe National Natural Science Foundation of China(22371203,22073066,21503143,21975179)。
文摘The Ni-catalyzed highly selective diborylative cyclization of 1,6-enynes with diboron reagent has been developed. When pinB-Bdan was used, multiple types of boron-containing functional groups could be installed into organic molecule with great chemoselectivity and regioselectivity though this reaction. Meanwhile, if B_2pai_2 was employed, the asymmetric diborylative cyclization could be well induced by using strategy of dynamic kinetic resolution. Importantly, the above reactions could afford desired product with 100% atomic economy, and could be compatible with different series of substituents. The studies of further transformation well illustrated that different type products could serve diverse synthetic strategy. Notably, the reaction mechanism was intensively studied by density functional theory(DFT) calculations, which could reveal the mechanism of regio- and enantio-selective control.
基金financially supported by the National Natural Science Foundation of China (22209039)Top-notch Personnel Fund of Henan Agricultural University (30500682)。
文摘Improving the complete ethanol electrooxidation on Pd-based catalysts in alkaline media has drawn widely attention due to the high mass energy density.However,the weak adsorption energy of CH_(3)CO^(*) on Pd restricts the C–C bond cleavage.Inspired by the molecular orbital theory,we proposed the d-state-editing strategy to construct more unoccupied d-states of Pd for the enhanced interaction with CH_(3)CO^(*) to break C–C bonds.As expected,the reduced number of e_g electrons and more unoccupied d-states of Pd successfully formed on as-prepared porous Rh Au–Pd Cu nanosheets(PNSs).Theoretical calculations show that the optimized d-states of Rh Au–Pd Cu PNS can effectively improve the adsorption of CH_(3)CO^(*) and drastically reduce the energy barrier of C–C bond cleavage,thus boosting the complete oxidation of ethanol.The charge ratio of C_1 pathway on Rh Au–Pd Cu PNSs is 51.5%,more than 2 times higher than that of Pd NSs.Our finding provides an innovative perspective for the design of highly-efficient noble-based electrocatalysts.
基金support from the National Natural Science Foundation of China(No.22071174)the Ministry of Eduction,Singapore(Academica Research Grant,Nos.R-279-000-538-114,R-279-000-580-112).
文摘Thiolate-protected atomically precise nanoclusters(NCs)demonstrate a series of unique luminescent characteristics attributed to their various peculiar electronic structures.Therefore,fluorescent NCs present extraordinary practical values in biosensing and bioimaging research fields.Nevertheless,restricted by the types of fluorescent NCs,there are great difficulties in promoting the development of NCs in fluorescent research areas.As a result,it is of significant necessity for researchers to develop new synthetic pathways to produce high-quality fluorescent NCs.According to the analysis about the structural characteristics of fluorescent NCs,some general features like longer motif and higher ligand-to-metal ratio can be found,consistent to some presented regularities in etching reaction.Consequently,in this work,we used Au_(25)(MHA)_(18)(MHA=6-mercaptohexanoic acid)as a model nanocluster and utilized the etching reaction to systematically explore etching products and their corresponding luminescent properties.Moreover,we also identified three main reaction processes in the entire etching reaction process,which can generate new metal nanocluster species with various fluorescent properties.Hence,the etching reaction will provide a good platform to produce new luminescent metal NC species.
基金Natural Science Foundation of Shandong Province,Grant/Award Number:ZR2020MB063Taishan Scholar Program of Shandong Province,Grant/Award Number:ts201511027。
文摘Atomically precise metal nanoclusters(MNCs),as a potential type of photoacoustic(PA)contrast agent,are limited in application due to their low PA conversion efficiency(PACE).Here,with hydrophilic Au25SR18(SR=thiolate)as model NCs,we present a result that weakly polar solvent induces aggregation,which effectively enhances PA intensity and PACE.The PA intensity and PACE are highly dependent on the degree of aggregation,while the aggregation-enhanced PA intensity(AEPA)positively correlates to the protected ligands.Such an AEPA phenomenon indicates that aggregation actually accelerates the intramolecular motion of Au NCs,and enlarges the proportion of excited state energy dissipated through vibrational relaxation.This result conflicts with the restriction of intramolecular motion mechanism of aggregation-induced emission.Further experiments show that the increased energy of AEPA originates from the aggregation inhibiting the intermolecular energy transfer from excited Au NCs to their surrounding medium molecules,including solvent molecule and dissolved oxygen,rather than restricting radiative relaxations.This study develops a new strategy for enhancing the PA intensity of Au NCs,and contributes to a deeper understanding of the origin of the PA signal and the excited state energy dissipation processes for MNCs.
基金the German Research Foundation(DFG:LE 2249/15-1)the Sino-German Center for Research Promotion(GZ1579)Y.R.and C.F.X.would like to appreciate the support from the China Scholarship Council(Nos.202207030010 and 20210637004).
文摘Zinc-air batteries(ZABs)are widely studied because of their high theoretical energy density,high battery voltage,environmental protection,and low price.However,the slow kinetics of oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)on the air electrode limits the further application of ZABs,so that how to develop a cheap,efficient,and stable catalyst with bifunctional catalytic activity is the key to solving the development of ZABs.Transition metal compounds are widely used as cathode materials for ZABs due to their low cost,high electrocatalytic activity,and stable structure.This review summarizes the research progress of transition metal compounds as bifunctional catalysts for ZABs.The development history,operation principle,and mechanism of ORR and OER reactions are introduced first.The application and development of transition metal compounds as bifunctional catalysts for ZABs in recent years are systematically introduced,including transition metal oxides(TMOs),transition metal nitrides(TMNs),transition metal sulfides(TMSs),transition metal carbides(TMCs),transition metal phosphates(TMPs),and others.In addition,the shortcomings of transition metal compounds as bifunctional catalysts for ZABs were summarized and reasonable design strategies and improvement measures were put forward,aiming at providing a reference for the design and construction of high-performance ZABs cathode materials.Finally,the challenges and future in this field are discussed and prospected.
基金supported by the National Natural Science Foundation of China (22071172)the Ministry of Science and Technology of China (2016YFB0401100,2017YFA0204503,and 2018YFA0703200)Shandong Provincial Natural Science Foundation (No. ZR2019BB025)。
文摘Electrocatalytic CO_(2) reduction reaction(CO_(2) RR) can store and transform the intermittent renewable energy in the form of chemical energy for industrial production of chemicals and fuels,which can dramatically reduce CO_(2) emission and contribute to carbon-neutral cycle. E cient electrocatalytic reduction of chemically inert CO_(2) is challenging from thermodynamic and kinetic points of view. Therefore,low-cost,highly e cient,and readily available electrocatalysts have been the focus for promoting the conversion of CO_(2). Very recently,interface engineering has been considered as a highly e ective strategy to modulate the electrocatalytic performance through electronic and/or structural modulation,regulations of electron/proton/mass/intermediates,and the control of local reactant concentration,thereby achieving desirable reaction pathway,inhibiting competing hydrogen generation,breaking binding-energy scaling relations of intermediates,and promoting CO_(2) mass transfer. In this review,we aim to provide a comprehensive overview of current developments in interface engineering for CO_(2) RR from both a theoretical and experimental stand-point,involving interfaces between metal and metal,metal and metal oxide,metal and nonmetal,metal oxide and metal oxide,organic molecules and inorganic materials,electrode and electrolyte,molecular catalysts and electrode,etc. Finally,the opportunities and challenges of interface engineering for CO_(2) RR are proposed.
基金supported by the National Key Research and Development Program of China(2017YFB0405400)National Natural Science Foundation of China(51732007)+1 种基金Major Innovation Projects in Shandong Province(2018YFJH0503)Natural Science Foundation of Shandong Province(ZR2018BEM010).
文摘Skin is the largest organ of the human body and can perceive and respond to complex environmental stimulations.Recently,the development of electronic skin(E-skin)for the mimicry of the human sensory system has drawn great attention due to its potential applications in wearable human health monitoring and care systems,advanced robotics,artificial intelligence,and human-machine interfaces.Tactile sense is one of the most important senses of human skin that has attracted special attention.The ability to obtain unique functions using diverse assembly processible methods has rapidly advanced the use of graphene,the most celebrated two-dimensional material,in electronic tactile sensing devices.With a special emphasis on the works achieved since 2016,this review begins with the assembly and modification of graphene materials and then critically and comprehensively summarizes the most advanced material assembly methods,device construction technologies and signal characterization approaches in pressure and strain detection based on graphene and its derivative materials.This review emphasizes on:(1)the underlying working principles of these types of sensors and the unique roles and advantages of graphene materials;(2)state-of-the-art protocols recently developed for high-performance tactile sensing,including representative examples;and(3)perspectives and current challenges for graphene-based tactile sensors in E-skin applications.A summary of these cutting-edge developments intends to provide readers with a deep understanding of the future design of high-quality tactile sensing devices and paves a path for their future commercial applications in the field of E-skin.