The excellent irradiation resistance,high strength and plasticity exhibited by high-entropy alloys(HEAs)make it candidate for engin-eering applications.Diffusion bonding of Al_(0.3)CoCrFeNi single-phase HEAs was carri...The excellent irradiation resistance,high strength and plasticity exhibited by high-entropy alloys(HEAs)make it candidate for engin-eering applications.Diffusion bonding of Al_(0.3)CoCrFeNi single-phase HEAs was carried out using electric-assisted diffusion bonding(EADB),and the effect of bonding temperature on the evolution of the interfacial microstructure and the mechanical properties was investigated.The results indicate that as the bonding temperature increases,the pores at the interface gradually decrease in size and undergo closure.The electric current significantly promotes the pore closure mechanism dominated by plastic deformation at the diffusion interface and promotes the recrystallisation behavior at the interface,and the fracture mode changes from intergranular fracture at the interface to jagged fracture along the grains spanning the weld parent material.Due to the activation effect of EADB,higher-strength diffusion bonding of high-entropy alloys can be achieved at the same temperature compared with the conventional hot-pressure diffusion bonding(HPDB)process.展开更多
Cebu Province,a key hub in the Philippine archipelago,is known for its strategic location,abundant natural resources,and rich cultural heritage.Far across the sea in southern China,Guangxi Zhuang Autonomous Region shi...Cebu Province,a key hub in the Philippine archipelago,is known for its strategic location,abundant natural resources,and rich cultural heritage.Far across the sea in southern China,Guangxi Zhuang Autonomous Region shines with picturesque landscapes,vibrant ethnic cultures,and dynamic growth.Separated by vast waters yet linked through the China-ASEAN Expo(CAEXPO)in Nanning,the two regions have forged a strong bond of friendship.展开更多
Surface chemistry plays a critical role in the fields of electrochemistry,heterogeneous catalysis,adsorption,etc.[1–4].The representative D-band center theory reported through Hammer and Nørskov in surface chemi...Surface chemistry plays a critical role in the fields of electrochemistry,heterogeneous catalysis,adsorption,etc.[1–4].The representative D-band center theory reported through Hammer and Nørskov in surface chemistry has been widely used in early studies to predict adsorption strength[5,6].Generally,the adsorption strength of active sites correlates inversely with the downward shift of the D-band center(εd)relative to the Fermi level,as lower-energy positioning increases anti-bonding orbital occupancy,weakening surface interactions(Fig.1(a)).展开更多
Surface tension-induced shrinkage of heterogeneously bonded interfaces is a key factor in limiting the performance of nanostructures.Herein,we demonstrate a laser-induced thermo-compression bonding technology to suppr...Surface tension-induced shrinkage of heterogeneously bonded interfaces is a key factor in limiting the performance of nanostructures.Herein,we demonstrate a laser-induced thermo-compression bonding technology to suppress surface tension-induced shrinkage of Cu-Au bonded interface.A focused laser beam is used to apply localized heating and scattering force to the exposed Cu nanowire.The laser-induced scattering force and the heating can be adjusted by regulating the exposure intensity.When the ratio of scattering forces to the gravity of the exposed nanowire reaches 3.6×10^(3),the molten Cu nanowire is compressed into flattened shape rather than shrinking into nanosphere by the surface tension.As a result,the Cu-Au bonding interface is broadened fourfold by the scattering force,leading to a reduction in contact resistance of approximately 56%.This noncontact thermo-compression bonding technology provides significant possibilities for the interconnect packaging and integration of nanodevices.展开更多
Organofluorines play a crucial role in medicine,agrochemicals,and materials science.Adding fluorine to molecules creates structures with specific beneficial properties or tunes properties through interactions with the...Organofluorines play a crucial role in medicine,agrochemicals,and materials science.Adding fluorine to molecules creates structures with specific beneficial properties or tunes properties through interactions with their environment.Many popular pharmaceuticals and agrochemicals contain fluorine because it enhances hydrogen bonding at protein’s active sites.展开更多
Due to its superior nanoscale properties,cobalt(Co)is highly desirable for ultrahigh-density 3D integration into materials through metal/dielectric hybrid bonding.However,this process is very challenging through Co/Si...Due to its superior nanoscale properties,cobalt(Co)is highly desirable for ultrahigh-density 3D integration into materials through metal/dielectric hybrid bonding.However,this process is very challenging through Co/SiO_(2)hybrid bonding,as very hydrophilic SiO_(2)surfaces are needed for bonding during dehydration reactions and oxidation of the Co surfaces must be avoided.Additionally,the substantial coefficient of thermal expansion mismatch between the robust capping layers(Co and SiO_(2)layers)necessitates hybrid bonding with minimal thermal input and compression.In this study,we introduce a ternary plasma activation strategy employing an Ar/NH_(3)/H_(2)O gas mixture to facilitate Co/SiO_(2)hybrid bonding at temperatures as low as~200℃,which is markedly lower than the melting point of Co(~1500℃).Intriguingly,non-oxide metallization at the Co-Co interface can be realized without the hindrance of a bonding barrier,thereby reducing the electrical resistance by over 40%and compression force requirements.Moreover,the enhancement in the SiO_(2)surface energy through active group terminations fosters extensive interfacial hydration and strengthens the mechanical properties.This research paves the way for fine-tuning bonding surfaces using a material-selective strategy which should advance metal/dielectric hybrid bonding for future integration applications.展开更多
As more and more studies have shown that lipid molecules play an important role in the whole biology,in-depth analysis of lipid structure has become particularly important in lipidomics.Mass spectrometry(MS),as the pr...As more and more studies have shown that lipid molecules play an important role in the whole biology,in-depth analysis of lipid structure has become particularly important in lipidomics.Mass spectrometry(MS),as the preferred tool for lipid analysis,has greatly promoted the development of this field.However,the existing MS methods still face many difficulties in the in-depth or even comprehensive analysis of lipid structure.In this review,we discuss recent advances in MS methods based on double bond-specific chemistries for the resolving of C=C location and geometry isomers of lipids.This progress has greatly advanced the lipidomics analysis to a deeper structural level and facilitated the development of structural lipid biology.展开更多
The activation of the N≡N triple bond in N_(2) is a fascinating topic in nitrogen chemistry.The transition metals have been demonstrated to effectively modulate the reactivity of N_(2) molecules under high pressure,l...The activation of the N≡N triple bond in N_(2) is a fascinating topic in nitrogen chemistry.The transition metals have been demonstrated to effectively modulate the reactivity of N_(2) molecules under high pressure,leading to nitrogen-rich compounds.However,their use often results in a significant reduction in energy density.In this work,we propose a series of low-enthalpy nitrogen-rich phases in CN_(x)(x=3,...,7)compounds using a first-principles crystal structure search method.The results of calculations reveal that all these CN compounds are assembled from both CN_(4) tetrahedra and N_(x)(x=1,2,or 5)species.Strikingly,we find that the CN_(4) tetrahedron can effectively activate the N≡N bond through weakening of the π orbital of N_(2) under a pressure of 40 GPa,leading to stable CN polynitrides.The robust structural framework of CN polynitrides containing C-N and N-N bonds plays a crucial role in enhancing their structural stability,energy density,and hardness.Among these polynitrides,CN_(6) possesses not only a very high mass density of 3.19 g/cm^(3),but also an ultrahigh energy density of 28.94 kJ/cm^(3),which represents a significant advance in the development of energetic materials using high-pressure methods.This work provides new insights into the mechanism of N_(2) activation under high pressure,and offers a promising pathway to realize high-performance energetic materials.展开更多
Interfacial evolution and bonding mechanism of reduced activation ferritic/martensitic(RAFM)steel were systematically investigated through a series of hot compression tests conducted at various strains(0.15-0.8),strai...Interfacial evolution and bonding mechanism of reduced activation ferritic/martensitic(RAFM)steel were systematically investigated through a series of hot compression tests conducted at various strains(0.15-0.8),strain rates(0.001-1 s^(-1)),and temperatures(950-1050℃).Interfacial microstructural analysis revealed that plastic deformation of surface asperities effectively removes interfacial voids,and the evolution of dynamic recrystallization(DRX)aids in achieving a joint characterized by homogeneously refined microstructure and adequate interfacial grain boundary(IGB)migration.Electron backscattered diffraction analysis demonstrated that the continuous dynamic recrystallization,characterized by progressive subgrain rotation,is the prevailing DRX nucleation mechanism in RAFM steel during hot compression bonding.During DRX evolution,emerging DRX grains in the interfacial region expand into adjacent areas,transforming T-type triple junction grain boundaries into equal form,and resulting in a serrated and intricate interface.Elevated temperatures and strains,coupled with reduced strain rates,augment DRX grain nucleation and IGB migration,thus enhancing RAFM joint quality with regard to the interface bonding ratio and the interface migration ratio.展开更多
Silicene,a silicon analog of graphene,holds promise for next-generation electronics due to its tunable bandgap and larger spin-orbit coupling.Despite extensive efforts to synthesize and characterize silicene on metal ...Silicene,a silicon analog of graphene,holds promise for next-generation electronics due to its tunable bandgap and larger spin-orbit coupling.Despite extensive efforts to synthesize and characterize silicene on metal substrates,bondresolved imaging of its atomic structure has remained elusive.Here,we report the fabrication and bond-resolved characterization of silicene on Au(111)substrate.Three silicene phases tuned by surface reconstruction and annealing temperatures are achieved.Using CO-terminated scanning tunneling microscopy(STM)tips,we resolve these silicene phases with atomic precision,determining their bond lengths,local strain,and geometric configurations.Furthermore,we correlate these structural features with their electronic properties,revealing the effect of strain and substrate interactions on the electronic properties of silicene.This work establishes silicene's intrinsic bonding topology and resolves longstanding controversies in silicene research.展开更多
Efficient conversion and synergistic solar energy utilization are critical for advancing low-carbon and sustainable development.In this study,two Pt(Ⅱ)-based metal/halogen-bonded organic frameworks(MXOFBen and MXOF-A...Efficient conversion and synergistic solar energy utilization are critical for advancing low-carbon and sustainable development.In this study,two Pt(Ⅱ)-based metal/halogen-bonded organic frameworks(MXOFBen and MXOF-Anth)were designed to enhance photoconversion efficiency and enable multifunctional integration.The ligand L-terpyr is formed by coupling tripyridine with diphenylamine dipyridine,in which the tripyridine effectively acts as a metal-ligand to lower the band gap and promote nonradiative leaps,thereby enhancing the photoconversion ability.Meanwhile,diphenylamine dipyridine serves as a[N…I^(+)…N]halogen-bonding acceptor,imparting superhydrophilicity to the materials and increasing carrier density,further improving photocatalytic performance.Experimental results demonstrate that these two MXOFs achieve impressive interfacial water evaporation efficiencies of up to87.8%and 94.0%,respectively.Additionally,the materials exhibit excellent performance in photothermal power generation and photocatalysis of H_(2)O_(2).Notably,the MXOFs also deliver strong overall performance in integrated systems combining interfacial water evaporation with photothermal power generation or photocatalysis,underscoring their exceptional photoconversion efficiency and multifunctional potential.This work introduces a novel strategy by incorporating metal-ligand and halogen bonds,offering a pathway to enhance photoconversion efficiency and develop versatile materials for advanced solar energy applications,thereby fostering the progress of high-efficiency solar energy conversion and multifunctional organic materials.展开更多
The intrinsic symmetrical electron distribution in crystalline metal sulfides usually causes an improper electronic configuration between catalytic S atoms and H intermediates(H_(ad))to form strong S-H_(ad) bonds,resu...The intrinsic symmetrical electron distribution in crystalline metal sulfides usually causes an improper electronic configuration between catalytic S atoms and H intermediates(H_(ad))to form strong S-H_(ad) bonds,resulting in a low photocatalytic H_(2) evolution activity.Herein,a cobalt-induced asymmetric electronic distribution is justified as an effective strategy to optimize the electronic configuration of catalytic S sites in NiCoS cocatalysts for highly active photocatalytic H_(2) evolution.To this end,Co atoms are uniformly incorporated in NiS nanoparticles to fabricate homogeneous NiCoS cocatalyst on TiO_(2) surface by a facile photosynthesis strategy.It is revealed that the incorporated Co atoms break the electron distribution symmetry in NiS,thus essentially increasing the electron density of S atoms to form active electron-enriched S^(2+δ)–sites.The electron-enriched S^(2+δ)–sites could interact with Had via an increased antibonding orbital occupancy,which weakens S–Had bonds for efficient H_(ad) adsorption and desorption,endowing the NiCoS cocatalysts with a highly active H_(2) evolution process.Consequently,the optimized NiCoS/TiO_(2)(1:2)photocatalyst displays the highest H_(2) production performance,outperforming the NiS/TiO_(2) and CoS/TiO_(2) samples by factors of 2.1 and 2.5,respectively.This work provides novel insights on breaking electron distribution symmetry to optimize catalytic efficiency of active sites.展开更多
Acidic-stable oxygen evolution reaction(OER)catalysts based on earth-abundant materials are important but rare for the proton exchange membrane-based water electrolysis.In this study,a metal-containing hydrogen-bonded...Acidic-stable oxygen evolution reaction(OER)catalysts based on earth-abundant materials are important but rare for the proton exchange membrane-based water electrolysis.In this study,a metal-containing hydrogen-bonded organic framework(HOF)of manganese coordinated with 2,2'-bipyridine-6,6'-dicarboxylate ligands,Mn(bda),interconnected through hydrogen bonding and π-π stacking is used as a heterogeneous OER catalyst(Mn(bda)-HOF)for acidic water oxidation and exhibits a considerable OER performance.Electrochemical results show that Mn(bda)-HOF displays a turn of frequency of 1 s^(-1) at an overpotential of 870 mV.Meanwhile,this Mn(bda)-HOF shows an unusual pH dependence on performance,where the reaction rate increases with the decrease of pH.A comprehensive mechanistic study reveals that the charge transfer triggered coupling of two metal-oxo species Mn^(5+)(O)is the rate-determining step,which leads to this unusual pH dependence on the OER performance.展开更多
The persistent stability of ruthenium dioxide(RuO_(2))in acidic oxygen evolution reactions(OER)is compromised by the involvement of lattice oxygen(LO)and metal dissolution during the OER process.Heteroatom doping has ...The persistent stability of ruthenium dioxide(RuO_(2))in acidic oxygen evolution reactions(OER)is compromised by the involvement of lattice oxygen(LO)and metal dissolution during the OER process.Heteroatom doping has been recognized as a viable strategy to foster the stability of RuO_(2)for acidic OER applications.This study presented an ion that does not readily gain or lose electrons,Ba^(2+),into RuO_(2)(Ba-RuO_(2))nanosheet(NS)catalyst that increased the number of exposed active sites,achieving a current density of 10 mA/cm^(2)with an overpotential of only 229 mV and sustaining this output for over 250 h.According to density functional theory(DFT)and X-ray absorption spectroscopy,Ba doping resulted in a longer Ru-O bond length,which in turn diminished the covalency of the bond.This alteration curtailed the involvement of LO and the dissolution of ruthenium(Ru),thereby markedly improving the durability of the catalyst over extended periods.Additionally,attenuated total reflectance-surface enhanced infrared absorption spectroscopy analysis substantiated that the OER mechanism shifted from a LO-mediated pathway to an adsorbate evolution pathway due to Ba doping,thereby circumventing Ru over-oxidation and further enhancing the stability of RuO_(2).Furthermore,DFT findings uncovered that Ba doping optimizes the adsorption energy of intermediates,thus enhancing the OER activity in acidic environments.This study offers a potent strategy to guide future developments on Ru-based oxide catalysts'stability in an acidic environment.展开更多
Gels and conductive polymer composites,including hydrogen bonds(HBs),have emerged as promising materials for electro-magnetic wave(EMW)absorption across various applications.However,the relationship between conduction...Gels and conductive polymer composites,including hydrogen bonds(HBs),have emerged as promising materials for electro-magnetic wave(EMW)absorption across various applications.However,the relationship between conduction loss in EMW-absorbing materials and charge transfer in HB remains to be fully understood.In this study,we developed a series of deep eutectic gels to fine-tune the quantity of HB by adjusting the molar ratio of choline chloride(ChCl)and ethylene glycol(EG).Owing to the unique properties of deep eutectic gels,the effects of magnetic loss and polarization loss on EMW attenuation can be disregarded.Our results indicate that the quantity of HB initially increases and then decreases with the introduction of EG,with HB-induced conductive loss following similar pat-terns.At a ChCl and EG molar ratio of 2.4,the gel labeled G22-CE2.4 exhibited the best EMW absorption performance,characterized by an effective absorption bandwidth of 8.50 GHz and a thickness of 2.54 mm.This superior performance is attributed to the synergistic ef-fects of excellent conductive loss and impedance matching generated by the optimal number of HB.This work elucidates the role of HB in dielectric loss for the first time and provides valuable insights into the optimal design of supramolecular polymer absorbers.展开更多
Mn-based layered oxides(KMO)have emerged as one of the promising low-cost cathodes for potassiumion batteries(PIBs).However,due to the multiple-phase transitions and the distortion in the MnO6structure induced by the ...Mn-based layered oxides(KMO)have emerged as one of the promising low-cost cathodes for potassiumion batteries(PIBs).However,due to the multiple-phase transitions and the distortion in the MnO6structure induced by the Jahn-Teller(JT)effect associated with Mn-ion,the cathode exhibits poor structural stability.Herein,we propose a strategy to enhance structural stability by introducing robust metal-oxygen(M-O)bonds,which can realize the pinning effect to constrain the distortion in the transition metal(TM)layer.Concurrently,all the elements employed have exceptionally high crustal abundance.As a proof of concept,the designed K_(0.5)Mn_(0.9)Mg_(0.025)Ti_(0.025)Al_(0.05)O_(2)cathode exhibited a discharge capacity of approximately 100 mA h g^(-1)at 20 mA g^(-1)with 79%capacity retention over 50 cycles,and 73%capacity retention over 200 cycles at 200 mA g^(-1),showcased much better battery performance than the designed cathode with less robust M-O bonds.The properties of the formed M-O bonds were investigated using theoretical calculations.The enhanced dynamics,mitigated JT effect,and improved structural stability were elucidated through the in-situ X-ray diffractometer(XRD),in-situ electrochemical impedance spectroscopy(EIS)(and distribution of relaxation times(DRT)method),and ex-situ X-ray absorption fine structure(XAFS)tests.This study holds substantial reference value for the future design of costeffective Mn-based layered cathodes for PIBs.展开更多
Determination of Shear Bond strength(SBS)at interlayer of double-layer asphalt concrete is crucial in flexible pavement structures.The study used three Machine Learning(ML)models,including K-Nearest Neighbors(KNN),Ext...Determination of Shear Bond strength(SBS)at interlayer of double-layer asphalt concrete is crucial in flexible pavement structures.The study used three Machine Learning(ML)models,including K-Nearest Neighbors(KNN),Extra Trees(ET),and Light Gradient Boosting Machine(LGBM),to predict SBS based on easily determinable input parameters.Also,the Grid Search technique was employed for hyper-parameter tuning of the ML models,and cross-validation and learning curve analysis were used for training the models.The models were built on a database of 240 experimental results and three input variables:temperature,normal pressure,and tack coat rate.Model validation was performed using three statistical criteria:the coefficient of determination(R2),the Root Mean Square Error(RMSE),and the mean absolute error(MAE).Additionally,SHAP analysis was also used to validate the importance of the input variables in the prediction of the SBS.Results show that these models accurately predict SBS,with LGBM providing outstanding performance.SHAP(Shapley Additive explanation)analysis for LGBM indicates that temperature is the most influential factor on SBS.Consequently,the proposed ML models can quickly and accurately predict SBS between two layers of asphalt concrete,serving practical applications in flexible pavement structure design.展开更多
This study investigates the bond performance at the interfacial region shared by Ultra-High Performance Concrete(UHPC)and steel tubes through push-out tests.This study examines how changes in steel fiber volumetric ra...This study investigates the bond performance at the interfacial region shared by Ultra-High Performance Concrete(UHPC)and steel tubes through push-out tests.This study examines how changes in steel fiber volumetric ratio and thickness of steel tube influence the bond strength characteristics.The results show that as the enhancement of the steel tube wall thickness,the ultimate bond strength at the interface improves significantly,whereas the initial bond strength exhibits only slight variations.The influence of steel fiber volumetric ratio presents a nonlinear trend,with initial bond strength decreasing at low fiber content and increasing significantly as fiber content rises.Additionally,finite element(FE)simulations were applied to replicate the experimental conditions,and the outcomes showed strong correlation with the experimental data,confirming the exactitude of the FE model in predicting the bond behavior at the UHPC-Steel interface.These findings provide valuable insights for optimizing the design of UHPC-Filled steel tubes in high-performance structure.展开更多
Removing H_(2)S and CO_(2)is of great significance for natural gas purification.With excellent gas affinity and tunable structure,ionic liquids(ILs) have been regarded as nontrivial candidates for fabricating polymer-...Removing H_(2)S and CO_(2)is of great significance for natural gas purification.With excellent gas affinity and tunable structure,ionic liquids(ILs) have been regarded as nontrivial candidates for fabricating polymer-based membranes.Herein,we firstly reported the incorporation of protic ILs (PILs) having ether-rich and carboxylate sites (ECPILs) into poly(ether-block-amide)(Pebax) matrix for efficient separation H_(2)S and CO_(2)from CH_(4).Notably,the optimal permeability of H_(2)S reaches up to 4310 Barrer (40C,0.50 bar) in Pebax/ECPIL membranes,along with H_(2)S/CH_(4)and (H_(2)StCO_(2))/CH_(4)selectivity of 97.7 and 112.3,respectively.These values are increased by 1125%,160.8%and 145.9%compared to those in neat Pebax membrane.Additionally,the solubility and diffusion coefficients of the gases were measured,demonstrating that ECPIL can simultaneously strengthen the dissolution and diffusion of H_(2)S and CO_(2),thus elevating the permeability and permselectivity.By using quantum chemical calculations and FT-IR spectroscopy,the highly reversible multi-site hydrogen bonding interaction between ECPILs and H_(2)S was revealed,which is responsible for the fast permeation of H_(2)S and good selectivity.Furthermore,H_(2)S/CO_(2)/CH_(4)(3/3/94 mol/mol) ternary mixed gas can be efficiently and stably separated by Pebax/ECPIL membrane for at least 100 h.Overall,this work not only illustrates that PILs with ether-rich and carboxylate hydrogen bonding sites are outstanding materials for simultaneous removal of H_(2)S and CO_(2),but may also provide a novel insight into the design of membrane materials for natural gas upgrading.展开更多
基金support from National Natural Science Foundation of China(NSFC,Grant numbers U22A20185,U21A20128,52175302 and 52305353)Aeronautical Science Foundation(ASFC-20230036077001)Fundamental Research Funds for the Central Universities(2022FRFK060009,HIT.DZI1.2023012).
文摘The excellent irradiation resistance,high strength and plasticity exhibited by high-entropy alloys(HEAs)make it candidate for engin-eering applications.Diffusion bonding of Al_(0.3)CoCrFeNi single-phase HEAs was carried out using electric-assisted diffusion bonding(EADB),and the effect of bonding temperature on the evolution of the interfacial microstructure and the mechanical properties was investigated.The results indicate that as the bonding temperature increases,the pores at the interface gradually decrease in size and undergo closure.The electric current significantly promotes the pore closure mechanism dominated by plastic deformation at the diffusion interface and promotes the recrystallisation behavior at the interface,and the fracture mode changes from intergranular fracture at the interface to jagged fracture along the grains spanning the weld parent material.Due to the activation effect of EADB,higher-strength diffusion bonding of high-entropy alloys can be achieved at the same temperature compared with the conventional hot-pressure diffusion bonding(HPDB)process.
文摘Cebu Province,a key hub in the Philippine archipelago,is known for its strategic location,abundant natural resources,and rich cultural heritage.Far across the sea in southern China,Guangxi Zhuang Autonomous Region shines with picturesque landscapes,vibrant ethnic cultures,and dynamic growth.Separated by vast waters yet linked through the China-ASEAN Expo(CAEXPO)in Nanning,the two regions have forged a strong bond of friendship.
文摘Surface chemistry plays a critical role in the fields of electrochemistry,heterogeneous catalysis,adsorption,etc.[1–4].The representative D-band center theory reported through Hammer and Nørskov in surface chemistry has been widely used in early studies to predict adsorption strength[5,6].Generally,the adsorption strength of active sites correlates inversely with the downward shift of the D-band center(εd)relative to the Fermi level,as lower-energy positioning increases anti-bonding orbital occupancy,weakening surface interactions(Fig.1(a)).
基金supported by the National Natural Science Foundation of China(Nos.52305612 and U20A6004)Open Fund of Hubei Key Laboratory of Electronic Manufacturing and Packaging Integration(Wuhan University)(NO.EMPI2023015).
文摘Surface tension-induced shrinkage of heterogeneously bonded interfaces is a key factor in limiting the performance of nanostructures.Herein,we demonstrate a laser-induced thermo-compression bonding technology to suppress surface tension-induced shrinkage of Cu-Au bonded interface.A focused laser beam is used to apply localized heating and scattering force to the exposed Cu nanowire.The laser-induced scattering force and the heating can be adjusted by regulating the exposure intensity.When the ratio of scattering forces to the gravity of the exposed nanowire reaches 3.6×10^(3),the molten Cu nanowire is compressed into flattened shape rather than shrinking into nanosphere by the surface tension.As a result,the Cu-Au bonding interface is broadened fourfold by the scattering force,leading to a reduction in contact resistance of approximately 56%.This noncontact thermo-compression bonding technology provides significant possibilities for the interconnect packaging and integration of nanodevices.
文摘Organofluorines play a crucial role in medicine,agrochemicals,and materials science.Adding fluorine to molecules creates structures with specific beneficial properties or tunes properties through interactions with their environment.Many popular pharmaceuticals and agrochemicals contain fluorine because it enhances hydrogen bonding at protein’s active sites.
基金supported by the National Natural Science Foundation of China(Grant Nos.92164105 and 51975151)the Heilongjiang Provincial Natural Science Foundation of China under grant LH2019E041+1 种基金the Heilongjiang Touyan Innovation Team Program(HITTY-20190013)State Key Laboratory of Precision Welding&Joining of Materials and Structures(No.24-T-04)。
文摘Due to its superior nanoscale properties,cobalt(Co)is highly desirable for ultrahigh-density 3D integration into materials through metal/dielectric hybrid bonding.However,this process is very challenging through Co/SiO_(2)hybrid bonding,as very hydrophilic SiO_(2)surfaces are needed for bonding during dehydration reactions and oxidation of the Co surfaces must be avoided.Additionally,the substantial coefficient of thermal expansion mismatch between the robust capping layers(Co and SiO_(2)layers)necessitates hybrid bonding with minimal thermal input and compression.In this study,we introduce a ternary plasma activation strategy employing an Ar/NH_(3)/H_(2)O gas mixture to facilitate Co/SiO_(2)hybrid bonding at temperatures as low as~200℃,which is markedly lower than the melting point of Co(~1500℃).Intriguingly,non-oxide metallization at the Co-Co interface can be realized without the hindrance of a bonding barrier,thereby reducing the electrical resistance by over 40%and compression force requirements.Moreover,the enhancement in the SiO_(2)surface energy through active group terminations fosters extensive interfacial hydration and strengthens the mechanical properties.This research paves the way for fine-tuning bonding surfaces using a material-selective strategy which should advance metal/dielectric hybrid bonding for future integration applications.
基金financially supported by the National Natural Science Foundation of China(No.22074111)National Key Research and Development Program of China(No.2021YFC2700700)the Opening fund of Hubei Key Laboratory of Bioinorganic Chemistry&Materia Medica(No.BCMM202303)。
文摘As more and more studies have shown that lipid molecules play an important role in the whole biology,in-depth analysis of lipid structure has become particularly important in lipidomics.Mass spectrometry(MS),as the preferred tool for lipid analysis,has greatly promoted the development of this field.However,the existing MS methods still face many difficulties in the in-depth or even comprehensive analysis of lipid structure.In this review,we discuss recent advances in MS methods based on double bond-specific chemistries for the resolving of C=C location and geometry isomers of lipids.This progress has greatly advanced the lipidomics analysis to a deeper structural level and facilitated the development of structural lipid biology.
基金supported by the Higher Educational Youth Innovation Science and Technology Program Shandong Province(Grant Nos.2022KJ183 and 2022KJ175)the Natural Science Foundation of Shandong Province(Grant Nos.ZR2023MA016 and ZR2023JQ001)+1 种基金the National Natural Science Foundation of China(Grant Nos.11974208 and 12374012)financial support from the award of Taishan Scholar(Grant No.tsqn202211128).
文摘The activation of the N≡N triple bond in N_(2) is a fascinating topic in nitrogen chemistry.The transition metals have been demonstrated to effectively modulate the reactivity of N_(2) molecules under high pressure,leading to nitrogen-rich compounds.However,their use often results in a significant reduction in energy density.In this work,we propose a series of low-enthalpy nitrogen-rich phases in CN_(x)(x=3,...,7)compounds using a first-principles crystal structure search method.The results of calculations reveal that all these CN compounds are assembled from both CN_(4) tetrahedra and N_(x)(x=1,2,or 5)species.Strikingly,we find that the CN_(4) tetrahedron can effectively activate the N≡N bond through weakening of the π orbital of N_(2) under a pressure of 40 GPa,leading to stable CN polynitrides.The robust structural framework of CN polynitrides containing C-N and N-N bonds plays a crucial role in enhancing their structural stability,energy density,and hardness.Among these polynitrides,CN_(6) possesses not only a very high mass density of 3.19 g/cm^(3),but also an ultrahigh energy density of 28.94 kJ/cm^(3),which represents a significant advance in the development of energetic materials using high-pressure methods.This work provides new insights into the mechanism of N_(2) activation under high pressure,and offers a promising pathway to realize high-performance energetic materials.
基金The authors are grateful to the National Natural Science Foundation of China(Grant Nos.52034004 and 52271111)the National Key R&D Program of China(2022YFB3705300)for grant and financial support.
文摘Interfacial evolution and bonding mechanism of reduced activation ferritic/martensitic(RAFM)steel were systematically investigated through a series of hot compression tests conducted at various strains(0.15-0.8),strain rates(0.001-1 s^(-1)),and temperatures(950-1050℃).Interfacial microstructural analysis revealed that plastic deformation of surface asperities effectively removes interfacial voids,and the evolution of dynamic recrystallization(DRX)aids in achieving a joint characterized by homogeneously refined microstructure and adequate interfacial grain boundary(IGB)migration.Electron backscattered diffraction analysis demonstrated that the continuous dynamic recrystallization,characterized by progressive subgrain rotation,is the prevailing DRX nucleation mechanism in RAFM steel during hot compression bonding.During DRX evolution,emerging DRX grains in the interfacial region expand into adjacent areas,transforming T-type triple junction grain boundaries into equal form,and resulting in a serrated and intricate interface.Elevated temperatures and strains,coupled with reduced strain rates,augment DRX grain nucleation and IGB migration,thus enhancing RAFM joint quality with regard to the interface bonding ratio and the interface migration ratio.
基金Project supported by the National Natural Science Foundation of China(Grant No.12474181)the Guangdong Basic and Applied Basic Research Foundation(Grant Nos.2021B0301030002 and 2024A1515010656)the Guangdong Science and Technology Project(Grant No.2021QN02X859)。
文摘Silicene,a silicon analog of graphene,holds promise for next-generation electronics due to its tunable bandgap and larger spin-orbit coupling.Despite extensive efforts to synthesize and characterize silicene on metal substrates,bondresolved imaging of its atomic structure has remained elusive.Here,we report the fabrication and bond-resolved characterization of silicene on Au(111)substrate.Three silicene phases tuned by surface reconstruction and annealing temperatures are achieved.Using CO-terminated scanning tunneling microscopy(STM)tips,we resolve these silicene phases with atomic precision,determining their bond lengths,local strain,and geometric configurations.Furthermore,we correlate these structural features with their electronic properties,revealing the effect of strain and substrate interactions on the electronic properties of silicene.This work establishes silicene's intrinsic bonding topology and resolves longstanding controversies in silicene research.
基金supported by the National Natural Science Foundation of China(Nos.22371218,21702153,52270070,and 21801194)the Wuhan Science and Technology Bureau(No.whkxjsj009)+1 种基金support of the Core Facility of Wuhan Universitythe Large-scale Instrument and Equipment Sharing Foundation of Wuhan University。
文摘Efficient conversion and synergistic solar energy utilization are critical for advancing low-carbon and sustainable development.In this study,two Pt(Ⅱ)-based metal/halogen-bonded organic frameworks(MXOFBen and MXOF-Anth)were designed to enhance photoconversion efficiency and enable multifunctional integration.The ligand L-terpyr is formed by coupling tripyridine with diphenylamine dipyridine,in which the tripyridine effectively acts as a metal-ligand to lower the band gap and promote nonradiative leaps,thereby enhancing the photoconversion ability.Meanwhile,diphenylamine dipyridine serves as a[N…I^(+)…N]halogen-bonding acceptor,imparting superhydrophilicity to the materials and increasing carrier density,further improving photocatalytic performance.Experimental results demonstrate that these two MXOFs achieve impressive interfacial water evaporation efficiencies of up to87.8%and 94.0%,respectively.Additionally,the materials exhibit excellent performance in photothermal power generation and photocatalysis of H_(2)O_(2).Notably,the MXOFs also deliver strong overall performance in integrated systems combining interfacial water evaporation with photothermal power generation or photocatalysis,underscoring their exceptional photoconversion efficiency and multifunctional potential.This work introduces a novel strategy by incorporating metal-ligand and halogen bonds,offering a pathway to enhance photoconversion efficiency and develop versatile materials for advanced solar energy applications,thereby fostering the progress of high-efficiency solar energy conversion and multifunctional organic materials.
文摘The intrinsic symmetrical electron distribution in crystalline metal sulfides usually causes an improper electronic configuration between catalytic S atoms and H intermediates(H_(ad))to form strong S-H_(ad) bonds,resulting in a low photocatalytic H_(2) evolution activity.Herein,a cobalt-induced asymmetric electronic distribution is justified as an effective strategy to optimize the electronic configuration of catalytic S sites in NiCoS cocatalysts for highly active photocatalytic H_(2) evolution.To this end,Co atoms are uniformly incorporated in NiS nanoparticles to fabricate homogeneous NiCoS cocatalyst on TiO_(2) surface by a facile photosynthesis strategy.It is revealed that the incorporated Co atoms break the electron distribution symmetry in NiS,thus essentially increasing the electron density of S atoms to form active electron-enriched S^(2+δ)–sites.The electron-enriched S^(2+δ)–sites could interact with Had via an increased antibonding orbital occupancy,which weakens S–Had bonds for efficient H_(ad) adsorption and desorption,endowing the NiCoS cocatalysts with a highly active H_(2) evolution process.Consequently,the optimized NiCoS/TiO_(2)(1:2)photocatalyst displays the highest H_(2) production performance,outperforming the NiS/TiO_(2) and CoS/TiO_(2) samples by factors of 2.1 and 2.5,respectively.This work provides novel insights on breaking electron distribution symmetry to optimize catalytic efficiency of active sites.
基金supported by the National Natural Science Foundation of China(Nos.22172011,22088102,and 22301248)the National Key R&D Program of China(2022YFA0911900)the Fundamental Research Funds for the Central Universities(DUT23LAB611).
文摘Acidic-stable oxygen evolution reaction(OER)catalysts based on earth-abundant materials are important but rare for the proton exchange membrane-based water electrolysis.In this study,a metal-containing hydrogen-bonded organic framework(HOF)of manganese coordinated with 2,2'-bipyridine-6,6'-dicarboxylate ligands,Mn(bda),interconnected through hydrogen bonding and π-π stacking is used as a heterogeneous OER catalyst(Mn(bda)-HOF)for acidic water oxidation and exhibits a considerable OER performance.Electrochemical results show that Mn(bda)-HOF displays a turn of frequency of 1 s^(-1) at an overpotential of 870 mV.Meanwhile,this Mn(bda)-HOF shows an unusual pH dependence on performance,where the reaction rate increases with the decrease of pH.A comprehensive mechanistic study reveals that the charge transfer triggered coupling of two metal-oxo species Mn^(5+)(O)is the rate-determining step,which leads to this unusual pH dependence on the OER performance.
基金supported by Young Project of Education Department in Guizhou Province(No.2022099)the Natural Science Special of Guizhou University(No.X202220 Special Post A)the National Natural Science Foundation of China(Grant No.22208071)。
文摘The persistent stability of ruthenium dioxide(RuO_(2))in acidic oxygen evolution reactions(OER)is compromised by the involvement of lattice oxygen(LO)and metal dissolution during the OER process.Heteroatom doping has been recognized as a viable strategy to foster the stability of RuO_(2)for acidic OER applications.This study presented an ion that does not readily gain or lose electrons,Ba^(2+),into RuO_(2)(Ba-RuO_(2))nanosheet(NS)catalyst that increased the number of exposed active sites,achieving a current density of 10 mA/cm^(2)with an overpotential of only 229 mV and sustaining this output for over 250 h.According to density functional theory(DFT)and X-ray absorption spectroscopy,Ba doping resulted in a longer Ru-O bond length,which in turn diminished the covalency of the bond.This alteration curtailed the involvement of LO and the dissolution of ruthenium(Ru),thereby markedly improving the durability of the catalyst over extended periods.Additionally,attenuated total reflectance-surface enhanced infrared absorption spectroscopy analysis substantiated that the OER mechanism shifted from a LO-mediated pathway to an adsorbate evolution pathway due to Ba doping,thereby circumventing Ru over-oxidation and further enhancing the stability of RuO_(2).Furthermore,DFT findings uncovered that Ba doping optimizes the adsorption energy of intermediates,thus enhancing the OER activity in acidic environments.This study offers a potent strategy to guide future developments on Ru-based oxide catalysts'stability in an acidic environment.
基金supported by the National Nat-ural Science Foundation of China(Nos.51872238,52074227,and 21806129)the Fundamental Research Funds for the Central Universities,China(Nos.3102018zy045 and 3102019AX11)+2 种基金the Guangdong Basic and Applied Basic Research Foundation,China(No.2024A1515010298)the Natural Science Basic Research Plan in Shaanxi Province of China(Nos.2017JQ5116 and 2020JM-118)the Key Laboratory of Icing and Anti/De-icing of CARDC(No.IADL20220401).
文摘Gels and conductive polymer composites,including hydrogen bonds(HBs),have emerged as promising materials for electro-magnetic wave(EMW)absorption across various applications.However,the relationship between conduction loss in EMW-absorbing materials and charge transfer in HB remains to be fully understood.In this study,we developed a series of deep eutectic gels to fine-tune the quantity of HB by adjusting the molar ratio of choline chloride(ChCl)and ethylene glycol(EG).Owing to the unique properties of deep eutectic gels,the effects of magnetic loss and polarization loss on EMW attenuation can be disregarded.Our results indicate that the quantity of HB initially increases and then decreases with the introduction of EG,with HB-induced conductive loss following similar pat-terns.At a ChCl and EG molar ratio of 2.4,the gel labeled G22-CE2.4 exhibited the best EMW absorption performance,characterized by an effective absorption bandwidth of 8.50 GHz and a thickness of 2.54 mm.This superior performance is attributed to the synergistic ef-fects of excellent conductive loss and impedance matching generated by the optimal number of HB.This work elucidates the role of HB in dielectric loss for the first time and provides valuable insights into the optimal design of supramolecular polymer absorbers.
基金financially supported by the National Natural Science Foundation of China(NSFC)(52274295)the Natural Science Foundation of Hebei Province(E2021501029)+3 种基金the Fundamental Research Funds for the Central Universities(N2423051,N2423053,N2302016,N2423019,N2323013,N2423005)the Science and Technology Project of Hebei Education Department(QN2024238)the Basic Research Program Project of Shijiazhuang City for Universities Stationed in Hebei Province(241790937A)the Science and Technology Project of Qinhuangdao City in 2023.
文摘Mn-based layered oxides(KMO)have emerged as one of the promising low-cost cathodes for potassiumion batteries(PIBs).However,due to the multiple-phase transitions and the distortion in the MnO6structure induced by the Jahn-Teller(JT)effect associated with Mn-ion,the cathode exhibits poor structural stability.Herein,we propose a strategy to enhance structural stability by introducing robust metal-oxygen(M-O)bonds,which can realize the pinning effect to constrain the distortion in the transition metal(TM)layer.Concurrently,all the elements employed have exceptionally high crustal abundance.As a proof of concept,the designed K_(0.5)Mn_(0.9)Mg_(0.025)Ti_(0.025)Al_(0.05)O_(2)cathode exhibited a discharge capacity of approximately 100 mA h g^(-1)at 20 mA g^(-1)with 79%capacity retention over 50 cycles,and 73%capacity retention over 200 cycles at 200 mA g^(-1),showcased much better battery performance than the designed cathode with less robust M-O bonds.The properties of the formed M-O bonds were investigated using theoretical calculations.The enhanced dynamics,mitigated JT effect,and improved structural stability were elucidated through the in-situ X-ray diffractometer(XRD),in-situ electrochemical impedance spectroscopy(EIS)(and distribution of relaxation times(DRT)method),and ex-situ X-ray absorption fine structure(XAFS)tests.This study holds substantial reference value for the future design of costeffective Mn-based layered cathodes for PIBs.
基金the University of Transport Technology under grant number DTTD2022-12.
文摘Determination of Shear Bond strength(SBS)at interlayer of double-layer asphalt concrete is crucial in flexible pavement structures.The study used three Machine Learning(ML)models,including K-Nearest Neighbors(KNN),Extra Trees(ET),and Light Gradient Boosting Machine(LGBM),to predict SBS based on easily determinable input parameters.Also,the Grid Search technique was employed for hyper-parameter tuning of the ML models,and cross-validation and learning curve analysis were used for training the models.The models were built on a database of 240 experimental results and three input variables:temperature,normal pressure,and tack coat rate.Model validation was performed using three statistical criteria:the coefficient of determination(R2),the Root Mean Square Error(RMSE),and the mean absolute error(MAE).Additionally,SHAP analysis was also used to validate the importance of the input variables in the prediction of the SBS.Results show that these models accurately predict SBS,with LGBM providing outstanding performance.SHAP(Shapley Additive explanation)analysis for LGBM indicates that temperature is the most influential factor on SBS.Consequently,the proposed ML models can quickly and accurately predict SBS between two layers of asphalt concrete,serving practical applications in flexible pavement structure design.
基金supported by grants from the Natural Science Foundation of Fujian Province(2021J011062)Minjiang Scholars Funding(GY-633Z21067).
文摘This study investigates the bond performance at the interfacial region shared by Ultra-High Performance Concrete(UHPC)and steel tubes through push-out tests.This study examines how changes in steel fiber volumetric ratio and thickness of steel tube influence the bond strength characteristics.The results show that as the enhancement of the steel tube wall thickness,the ultimate bond strength at the interface improves significantly,whereas the initial bond strength exhibits only slight variations.The influence of steel fiber volumetric ratio presents a nonlinear trend,with initial bond strength decreasing at low fiber content and increasing significantly as fiber content rises.Additionally,finite element(FE)simulations were applied to replicate the experimental conditions,and the outcomes showed strong correlation with the experimental data,confirming the exactitude of the FE model in predicting the bond behavior at the UHPC-Steel interface.These findings provide valuable insights for optimizing the design of UHPC-Filled steel tubes in high-performance structure.
基金sponsored by the National Natural Science Foundation of China (Nos. 22308145, 22208140, 22178159, 22078145)Natural Science Foundation of Jiangsu Province (BK20230791)Postgraduate Research Innovation Program of Jiangsu Province (KYCX24_0165)。
文摘Removing H_(2)S and CO_(2)is of great significance for natural gas purification.With excellent gas affinity and tunable structure,ionic liquids(ILs) have been regarded as nontrivial candidates for fabricating polymer-based membranes.Herein,we firstly reported the incorporation of protic ILs (PILs) having ether-rich and carboxylate sites (ECPILs) into poly(ether-block-amide)(Pebax) matrix for efficient separation H_(2)S and CO_(2)from CH_(4).Notably,the optimal permeability of H_(2)S reaches up to 4310 Barrer (40C,0.50 bar) in Pebax/ECPIL membranes,along with H_(2)S/CH_(4)and (H_(2)StCO_(2))/CH_(4)selectivity of 97.7 and 112.3,respectively.These values are increased by 1125%,160.8%and 145.9%compared to those in neat Pebax membrane.Additionally,the solubility and diffusion coefficients of the gases were measured,demonstrating that ECPIL can simultaneously strengthen the dissolution and diffusion of H_(2)S and CO_(2),thus elevating the permeability and permselectivity.By using quantum chemical calculations and FT-IR spectroscopy,the highly reversible multi-site hydrogen bonding interaction between ECPILs and H_(2)S was revealed,which is responsible for the fast permeation of H_(2)S and good selectivity.Furthermore,H_(2)S/CO_(2)/CH_(4)(3/3/94 mol/mol) ternary mixed gas can be efficiently and stably separated by Pebax/ECPIL membrane for at least 100 h.Overall,this work not only illustrates that PILs with ether-rich and carboxylate hydrogen bonding sites are outstanding materials for simultaneous removal of H_(2)S and CO_(2),but may also provide a novel insight into the design of membrane materials for natural gas upgrading.
