Based on the knot theory and researching of network structures of glucomannan molecules, the polysaccharides were analyzed. The link prediction analysis is to further reveal the interactions between polysaccharides, t...Based on the knot theory and researching of network structures of glucomannan molecules, the polysaccharides were analyzed. The link prediction analysis is to further reveal the interactions between polysaccharides, to elaborate QSAR of polysaccharides, and to analyze the network conformation relationships among polysaccharides. We made a classification for glucomannan molecules based on the related domestic and international theories, and investigated their network structures and application prospects. The knot theory and the link predictions not only simplify the glucomannan microscopic descriptions but also play a guiding role in predicting and regulating the structures.展开更多
The interface problems in zinc-ion batteries severely limit their electrochemical performance,even in hydrogel(HG)electrolyte(HE).Herein,a strategy of reconfiguring the hydrogen bond networks by thermal gelation is pr...The interface problems in zinc-ion batteries severely limit their electrochemical performance,even in hydrogel(HG)electrolyte(HE).Herein,a strategy of reconfiguring the hydrogen bond networks by thermal gelation is proposed to enhance the battery interface stability.The strategy introduces methyl cellulose into acrylamide,which can effectively stabilize the electrode interface and reconstruct the hydrogen bond networks of the electrolyte through its unique thermos-gelation property.Methylcellulose is dissolved by heating and cooled to form gel.This thermal gelation strategy formed hydrogen bonds with a large amount of free water and methyl cellulose,which not only reduced the water activity but also enhanced the intermolecular polymerization network and also promoted the solvation of Zn^(2+).More importantly,the symmetric batteries with HE-HG hydrogel electrolyte exhibited a long cycling life of 8000 h.The Zn||Zn_(0.25)V_(2)O_(5)(Zn||ZVO)battery displays the low-capacity decay rate for 800 cycles at 1 C at−20°C.The pouch battery maintains a capacity of 255 mAh·g^(−1) after 100 cycles under 2.5 A·g^(−1) at−20°C.This study provides a new way to enhance the interfacial stability,which helps to realize the scale application of flexible zinc-ion batteries.展开更多
Aqueous Zn-metal batteries(AZMBs)performance is hampered by freezing water at low temperatures,which hampers their multi-scenario application.Hydrogen bonds(HBs)play a pivotal role in water freezing,and proton transpo...Aqueous Zn-metal batteries(AZMBs)performance is hampered by freezing water at low temperatures,which hampers their multi-scenario application.Hydrogen bonds(HBs)play a pivotal role in water freezing,and proton transport is indispensable for the establishment of HBs.Here,the accelerated proton transport modulates the dynamic hydrogen bonding network of a Zn(BF4)2/EMIMBF4impregnated polyacrylamide/poly(vinyl alcohol)/xanthan gum dual network eutectic gel electrolyte(PPX-ILZSE)for lowtemperature AZMBs.The PPX-ILZSE forms more HBs,shorter HBs lifetimes,higher tetrahedral entropy,and faster desolvation processes,as demonstrated by experimental and theoretical calculations.This enhanced dynamic proton transport promotes rapid cycling of HBs formation-failure,and for polyaniline cathode(PANI)abundant redox sites of proton,confers excellent low temperature electrochemical performance to the Zn//PANI full cell.Specific capacities for 1000 and 5000 cycles at 1 and 5 A g^(-1)were149.8 and 128.4 m A h g^(-1)at room temperature,respectively.Furthermore,specific capacities of 131.1 mA hg^(-1)(92.4%capacity retention)and 0.0066%capacity decay per lap were achieved for 3000and 3500 laps at-30 and 40℃,respectively,at 0.5 A g^(-1).Furthermore,in-situ protective layer of ZnOHF nano-arrays on the Zn anode surface to eliminate dendrite growth and accelerate Zn-ions adsorption and charge transfer.展开更多
The sensitivity and fidelity of surface electromyography(sEMG)signal monitoring is critical for muscle status and fatigue assessment,prosthetic control,and gesture recognition.However,the incompatible skin-electrode i...The sensitivity and fidelity of surface electromyography(sEMG)signal monitoring is critical for muscle status and fatigue assessment,prosthetic control,and gesture recognition.However,the incompatible skin-electrode interface and complex electrophysiological environment restrict the sensitive acquisition and accurate analysis of sEMG signals.Focused on the impedance of the skin-electrode interface issue,we developed an interfacial gel electrode patch with a tunable hydrogen bond network to simultaneously achieve a conformal interface,suitable adhesion,and high conductivity for sEMG signal monitoring.By exploiting hydroxyethylidene diphosphonic acid(HEDP)and 2-hydroxyphosphono-acetic acid(HPAA)as hydrogen bonding regulators were introduced into the polyvinyl alcohol(PVA)-based hydrogel network to regulate the hydrogen bond cross-linking network.As a result,the balance of elastic modulus,adhesion,and electrical conductivity of PVA-HEDP-HPAA(PHH)hydrogel are achieved.The reliable electrodeskin interface is manipulated to achieve conformal contact by matching the elastic modulus,reducing the gap of electrode-skin interface by adhesion,and promoting ion and electron conduction by electrical conductivity.The PHH electrode patches exhibit a lower interfacial impedance(12.56 kΩ)and a signal-to-noise ratio of 38.09±1.28 dB for accurate analysis of muscle strength and evaluation of the fatigue state.With the assistance of the artificial neural network algorithm,seven gestures can be recognized with 100%prediction accuracy.The interfacial gel electrode patch contributes a bio-matching electrophysiological platform for prosthetic control,human–machine interaction,and clinical or athletic auxiliary monitoring.展开更多
In this paper, the hydrogen bonding network models of konjac glucomannan （KGM） are predicted in the approach of molecular dynamics （MD）. These models have been proved by experiments whose results are consistent wi...In this paper, the hydrogen bonding network models of konjac glucomannan （KGM） are predicted in the approach of molecular dynamics （MD）. These models have been proved by experiments whose results are consistent with those from simulation. The results show that the hydrogen bonding network structures of KGM are stable and the key linking points of hydrogen bonding network are at the O（6） and O（2） positions on KGM ring. Moreover, acety has significant influence on hydrogen bonding network and hydrogen bonding network structures are more stable after deacetylation.展开更多
A new coordination compound [Mg（L）（H2 O）5·H2 O]（NKU-109, H2 L=5-（4 H-1,2,4-triazol-4-yl）benzene-1,3-dicarboxylic acid） was solvothermally synthesized, featuring a supramolecular hydrogen-bonding network. ...A new coordination compound [Mg（L）（H2 O）5·H2 O]（NKU-109, H2 L=5-（4 H-1,2,4-triazol-4-yl）benzene-1,3-dicarboxylic acid） was solvothermally synthesized, featuring a supramolecular hydrogen-bonding network. A good proton conductivity of 5.87×10^-4S/cm was recorded at 70℃ and a relative humidity of75% in alternating current（AC） impedance experiment, which sheds a new light on the design of proton conduction materials based on coordination compounds.展开更多
A novel complex, (H 3O) 2[Ni(2,6-pydc) 2]·2H 2O was synthesized in an aqueous solution and characterized by means of single-crystal X-ray diffraction, elemental analyses and IR spectra. The X-ray structural a...A novel complex, (H 3O) 2[Ni(2,6-pydc) 2]·2H 2O was synthesized in an aqueous solution and characterized by means of single-crystal X-ray diffraction, elemental analyses and IR spectra. The X-ray structural analysis revealed that the novel compound forms three-dimensional(3D) networks by both π-π stacking and hydrogen-bonding interactions. The crystal data for the complex are a=13.853(3) nm, b=9.6892(19) nm, c=13.732(3) nm, α=90.00°, β=115.52(3)°, γ=90.00°, Z=3, R 1=0.0786, wR 2=0.1522.展开更多
The Sb^(3+) doping strategy has been proven to be an effective way to regulate the band gap and improve the photophysical properties of organic-inorganic hybrid metal halides(OIHMHs).However,the emission of Sb^(3+) io...The Sb^(3+) doping strategy has been proven to be an effective way to regulate the band gap and improve the photophysical properties of organic-inorganic hybrid metal halides(OIHMHs).However,the emission of Sb^(3+) ions in OIHMHs is primarily confined to the low energy region,resulting in yellow or red emissions.To date,there are few reports about green emission of Sb^(3+)-doped OIHMHs.Here,we present a novel approach for regulating the luminescence of Sb^(3+) ions in 0D C_(10)H_(2)_(2)N_(6)InCl_(7)·H_(2)O via hydrogen bond network,in which water molecules act as agents for hydrogen bonding.Sb^(3+)-doped C_(10)H_(2)2N_(6)InCl_(7)·H_(2)O shows a broadband green emission peaking at 540 nm and a high photoluminescence quantum yield(PLQY)of 80%.It is found that the intense green emission stems from the radiative recombination of the self-trapped excitons(STEs).Upon removal of water molecules with heat,C_(10)H_(2)_(2)N_(6)In_(1-x)Sb_(x)Cl_(7) generates yellow emis-sion,attributed to the breaking of the hydrogen bond network and large structural distortions of excited state.Once water molecules are adsorbed by C_(10)H_(2)_(2)N_(6)In_(1-x)Sb_(x)Cl_(7),it can subsequently emit green light.This water-induced reversible emission switching is successfully used for optical security and information encryption.Our findings expand the under-standing of how the local coordination structure influences the photophysical mechanism in Sb^(3+)-doped metal halides and provide a novel method to control the STEs emission.展开更多
Hydrothermal reaction of MgCl2 and ethyl tetrazolate-5-carboxylate at 160 ℃unexpectedly yielded compound {（H3O）[Mg（H2O）6]Cl3} （1）. The result of X-ray diffraction analysis indicates that 1 crystallizes in the m...Hydrothermal reaction of MgCl2 and ethyl tetrazolate-5-carboxylate at 160 ℃unexpectedly yielded compound {（H3O）[Mg（H2O）6]Cl3} （1）. The result of X-ray diffraction analysis indicates that 1 crystallizes in the monoclinic system, space group C2/c with a = 9.2896（3）, b = 9.5570（4）, c = 13.3169（5） A, β = 90.1221（12）°, V= 1182.28（8） A3, Z = 4, Mr = 257.78, Dc = 1.448 g/cm3, μ = 0.824 mm^-1, F（000） = 536, R = 0.0265 and wR - 0.0706. 1 is composed of one hexa-aqua-magnesium（Ⅱ） ion, one hydroxonium ion, and three chlorine anions. These three components weave a perfect three-dimensional （3D） （4,4,6,12）-connected hydrogen bonding network within 1.展开更多
The crystal structure of the title compound [Na2(OH2)5]2+[C6H12N4H2]2-2+ [Mo7O24]6 ?4H2O, prepared from an aqueous solution of Na2MoO4 ?2H2O in the presence of MoCl3 and hexamethylene tetramine, has been determined by...The crystal structure of the title compound [Na2(OH2)5]2+[C6H12N4H2]2-2+ [Mo7O24]6 ?4H2O, prepared from an aqueous solution of Na2MoO4 ?2H2O in the presence of MoCl3 and hexamethylene tetramine, has been determined by single-crystal X-ray diffraction. The crystal is of orthorhombic, space group Pnma with a = 14.6113(2), b = 18.6833(1), c = 15.3712(2), V = 4196.14(8)3, Z = 4, Mr = 1548.13, F(000) = 3016, = 2.157 mm-1 and Dc = 2.451 g/cm3. The final R factor is 0.0526 for 3818 unique observed reflections (I > 2(I)). The structural analysis reveals that heptamolybdate anions in the title compound consist of seven edge-sharing MoO6 octahedra, and are linked into a three-dimensional framework by sodium ions and hydrogen bonds.展开更多
The emerging biomass-based epoxy vitrimers hold great potential to fulfill the requirements for sustainable development of society.Since the existence of dynamic chemical bonds in vitrimers often reduces both the ther...The emerging biomass-based epoxy vitrimers hold great potential to fulfill the requirements for sustainable development of society.Since the existence of dynamic chemical bonds in vitrimers often reduces both the thermal and mechanical properties of epoxy resins, it is challenging to produce recyclable epoxy vitrimers with both excellent mechanical properties and good thermal stability. Herein, a monomer 4-(((5-(hydroxymethyl)furan-2-yl)methylene)amino)phenol(FCN) containing furan ring with potential to form high density of hydrogen bonding among repeating units is designed and copolymerized with glycerol triglycidyl ether to yield epoxy resin(FCN-GTE), which intrinsically has dual hydrogen bond networks, dynamic imine structure and resultant high performance. Importantly, as compared to the BPA-GTE, the FCN-GTE exhibits significantly improved mechanical properties owing to the increased density of hydrogen bond network and physical crosslinking interaction. Furthermore, density functional theory(DFT) calculation and in situ FTIR analysis is conducted to decipher the formation mechanism of hydrogen bond network. In addition, the FCN-GTE possesses superior UV shielding, chemical degradation, and recyclability because of the existence of abundant imine bonds. Notably, the FCN-GTE-based carbon fiber composites could be completely recycled in an amine solution.This study provides a facile strategy for synthesizing recyclable biomass-based high-performance epoxy vitrimers and carbon fiber composites.展开更多
Aqueous zinc-ion batteries(AZIBs)are promising due to the advantages of metallic zinc,including the high specific capacity(820 mAh g^(-1)),low redox potential(−0.76 V vs.SHE),inherent safety,low cost,and environmental...Aqueous zinc-ion batteries(AZIBs)are promising due to the advantages of metallic zinc,including the high specific capacity(820 mAh g^(-1)),low redox potential(−0.76 V vs.SHE),inherent safety,low cost,and environmental sustainability.Despite these benefits,AZIBs face challenges such as uneven Zn deposition and excessive hydrogen evolution reaction(HER)at the Zn anode,which reduce the battery's coulombic efficiency and cycling life.This study introduces an ammonium formate(AF)additive into a 2.0 M ZnSO_(4) electrolyte to address these issues.The AF additive promotes the three-dimensional rapid diffusion of Zn^(2+)on the anode surface and induces the preferential Zn(002)plane deposition,thus inhibiting dendrite growth and enhancing cycling stability.It also disrupts the hydrogen bond network of electrolyte,reducing the number of active H2O molecules and suppressing H_(2)O-induced side reactions.Consequently,the Zn||Zn symmetric cell with the AF additive shows stable cycling over 2100 h at 5.0 mA cm^(−2) with an areal capacity of 1.0 mAh cm^(−2),and maintains stability over 9700 cycles at 30 mA cm^(−2).When applied in a Zn||VO_(2) full cell,it achieves capacity retention of 68.9%after 2000 cycles,which demonstrates significant performance improvements in AZIBs.展开更多
The aim of this work is to investigate the hydrogen-bonding interaction in poly(vinyl alcohol)(PVA)/poly(acrylic acid)(PAA) blending system and its influence on rheological properties in solution and the physical prop...The aim of this work is to investigate the hydrogen-bonding interaction in poly(vinyl alcohol)(PVA)/poly(acrylic acid)(PAA) blending system and its influence on rheological properties in solution and the physical properties in solid state. Introducing PAA into PVA solutions resulted in a thickening behavior of blend solutions.The viscosity of the solutions increased with PAA content increasing,and a maximum viscosity could be obtained when the ratio of PVA/PAA was 70/30. The intermolecular hydrogen-bonding and miscibility between PVA and PAA in solid state were investigated by differential scanning calorimetry(DSC),Fourier transform infrared spectroscopy(FTIR) and mechanical measurements.The results displayed the great influence of introducing PAA on the properties of blending films.The tensile strength increased from 89.31 MPa to 119.8 MPa and Young’s modulus improved by over 300%with increasing PAA concentration compared with those of pure PVA films.By systematically studying the rheological behaviors of solutions and the physical properties of films,the influence of hydrogen-bonding in solutions and solid states were discussed.展开更多
A new copper(Ⅱ) complex [Cu(PDA)(H 2O) 2] was synthesized and its structure was determined. Cu(Ⅱ) is five coordinated in a tetragonal pyramid geometry. The two coordinating water molecules are different and t...A new copper(Ⅱ) complex [Cu(PDA)(H 2O) 2] was synthesized and its structure was determined. Cu(Ⅱ) is five coordinated in a tetragonal pyramid geometry. The two coordinating water molecules are different and the two Cu-O bond lengths differ by nearly 0.02 nm. The whole crystal is linked to form a three dimensional network by means of hydrogen bonds. The X band ESR spectrum shows three different g tensors with a well resolved hyperfine structure in the g z signal, giving the ESR parameters g x=2 05, g y =2 065 and g z =2 29. The covalency of the coordinate bonds and the deviation from tetragonal pyramid geometry for the complex are discussed based on the ESR spectra.展开更多
Aqueous alkali metal-ion batteries(AAMIBs)have been recognized as emerging electrochemical energy storage technologies for grid-scale applications owning to their intrinsic safety,cost-effectiveness,and environmental ...Aqueous alkali metal-ion batteries(AAMIBs)have been recognized as emerging electrochemical energy storage technologies for grid-scale applications owning to their intrinsic safety,cost-effectiveness,and environmental sustainability.However,the practical application of AAMIBs is still severely constrained by the tendency of aqueous electrolytes to freeze at low temperatures and decompose at high temperatures,limiting their operational temperature range.Considering the urgent need for energy systems with higher adaptability and resilience at various application scenarios,designing novel electrolytes via structure modulation has increasingly emerged as a feasible and economical strategy for the performance optimization of wide-temperature AAMIBs.In this review,the latest advancement of wide-temperature electrolytes for AAMIBs is systematically and comprehensively summarized.Specifically,the key challenges,failure mechanisms,correlations between hydrogen bond behaviors and physicochemical properties,and thermodynamic and kinetic interpretations in aqueous electrolytes are discussed firstly.Additionally,we offer forward-looking insights and innovative design principles for developing aqueous electrolytes capable of operating across a broad temperature range.This review is expected to provide some guidance and reference for the rational design and regulation of widetemperature electrolytes for AAMIBs and promote their future development.展开更多
Two crystals of receptor 1, C（42）H（52）N（10）O4S2（anthracene-9,10-dicarbaldehyde bis-（phenyl-semithiocarbazone）） and-1-H2PO4, C（68）H（114）N（10）O（10）P2S2 were obtained at room temperature successfully, a...Two crystals of receptor 1, C（42）H（52）N（10）O4S2（anthracene-9,10-dicarbaldehyde bis-（phenyl-semithiocarbazone）） and-1-H2PO4, C（68）H（114）N（10）O（10）P2S2 were obtained at room temperature successfully, and their structures were characterized by X-ray crystallography diffraction. X-ray diffraction reveals that, receptor 1 crystallizes in monoclinic, space group P21/c, with a = 9.487（3）,b = 20.674（6）, c = 11.821（4）A, β = 113.416（8）o, Mr = 825.06, V = 2127.5（12） A^3, Z = 2, Dc = 1.288g/cm^3, μ = 0.18 mm^-1, F（000） = 876, MoK α radiation（λ = 0.71073 A）, the final R = 0.0472 and wR = 0.0930. A total of 3758 unique reflections were collected, of which 3313 with I 〉 2σ（I） were observed. Compound 1-H2PO4^-crystallizes in triclinic, space group P21/n, with a = 8.767（1）, b =13.6190（15）, c = 16.615（2） ？, α = 98.727（14）, β = 103.061（14）, γ = 91.382（16）°, Mr = 1357.75, V =1906.6（4） A^3, Z = 1, Dc = 1.183 g/cm^3, μ = 0.17 mm-（-1）, F（000） = 734, MoK α radiation（λ = 0.71073？）, the final R = 0.0769 and wR = 0.1884. A total of 6699 unique reflections were collected, of which 2989 with I 〉 2σ（I） were observed. As it was observed in the crystal structure of 1-H2PO4^-, 1bound H2PO4^-at a 1：2 ratio by intermolecular interaction of N-H···O hydrogen bond obviously.Another interesting feature was that H2PO4--groups assembled chains themselves via intramolecular hydrogen bond O-H···O and connected the 1 molecules together through the interaction of H-bonds,which improved the planarity of 1 and increased the stability of the entire structure.展开更多
A new compound [Zn3（C7NO4H3）3Cl4]·[C6NO2H6]4·4H2O （I） has been synthesized and structurally characterized by X-ray crystallography.It crystallizes in monoclinic,space group C2/c with a=16.9018（14）,b=12...A new compound [Zn3（C7NO4H3）3Cl4]·[C6NO2H6]4·4H2O （I） has been synthesized and structurally characterized by X-ray crystallography.It crystallizes in monoclinic,space group C2/c with a=16.9018（14）,b=12.6902（10）,c=25.1170（2）,β=90.54°,V=5387.0（8）3,Z=4,Zn3C45H41Cl4N7O24,Mr=1401.76,Dc=1.728 g/cm3,F（000）=2840,μ（MoKa）=1.615 mm-1,the R= 0.0758 and wR=0.2060 for 3468 observed reflections （I 〉 2σ（I））.Analysis of single-crystal X-ray diffraction data shows that compound I displays an interesting example of 3D supramolecular networks with perfect neutral and ionic hydrogen bonding array.展开更多
The stable nanobubbles adhered to mineral surfaces may facilitate their efficient separation via flotation in the mining industry.However,the state of nanobubbles on mineral solid surfaces is still elusive.In this stu...The stable nanobubbles adhered to mineral surfaces may facilitate their efficient separation via flotation in the mining industry.However,the state of nanobubbles on mineral solid surfaces is still elusive.In this study,molecular dynamics(MD)simulations are employed to examine mineral-like model surfaces with varying degrees of hydrophobicity,modulated by surface charges,to elucidate the adsorption behavior of nanobubbles at the interface.Our findings not only contribute to the fundamental understanding of nanobubbles but also have potential applications in the mining industry.We observed that as the surface charge increases,the contact angle of the nanobubbles increases accordingly with shape transformation from a pancake-like gas film to a cap-like shape,and ultimately forming a stable nanobubble upon an ordered water monolayer.When the solid–water interactions are weak with a small partial charge,the hydrophobic gas(N_(2))molecules accumulate near the solid surfaces.However,we have found,for the first time,that gas molecules assemble a nanobubble on the water monolayer adjacent to the solid surfaces with large partial charges.Such phenomena are attributed to the formation of a hydrophobic water monolayer with a hydrogen bond network structure near the surface.展开更多
Platinum-ruthenium alloys(PtRu)represent state-of-the-art alkaline hydrogen oxidation reaction(HOR)catalysts,yet the atomic-scale origin of their superiority over pure Pt remains incompletely understood.Here,we employ...Platinum-ruthenium alloys(PtRu)represent state-of-the-art alkaline hydrogen oxidation reaction(HOR)catalysts,yet the atomic-scale origin of their superiority over pure Pt remains incompletely understood.Here,we employ density functional theory calculations,ab initio molecular dynamics simulations,and microkinetic modeling on Pt(111)and PtRu(111)surfaces to systematically investigate the key factors,including active sites distribution,species adsorption,and solvent reorganization,that affect the HOR activity and decouple their contributions.The results reveal that while the moderate hydrogen binding energy and improved hydroxyl(OH)species adsorption both contribute to the enhanced activity,the dominant factor is the substantial reduction in solvent reorganization energy on the PtRu(111).This is facilitated by the spatial separation of active sites:Pt atoms preferentially stabilize adsorbed hydrogen,while Ru atoms strongly bind OH and interfacial water molecules.This configuration increases the probability of hydrogen interacting with OH/water and enhances the fraction of"H-up"water molecules,forming a well-organized hydrogen bond network within the electric double layer.The dynamically compatible interfacial water structure and HOR coordination promote H desorption and proton transfer in the Volmer step,thereby accelerating the HOR kinetics.展开更多
基金Supported by the National Natural Science Foundation of China(31271837 and 31071518)Specialized Research Fund for the Doctoral Program of Higher Education jointly funded by Ministry of Education(20113515110010)+2 种基金Special Research Funds from Ministry of Science and Technology(2012GA7200022)Major projects of industries,universities and research in Fujian Province(2013N5003)Natural Science Foundation of Fujian Province(2011J0101)
文摘Based on the knot theory and researching of network structures of glucomannan molecules, the polysaccharides were analyzed. The link prediction analysis is to further reveal the interactions between polysaccharides, to elaborate QSAR of polysaccharides, and to analyze the network conformation relationships among polysaccharides. We made a classification for glucomannan molecules based on the related domestic and international theories, and investigated their network structures and application prospects. The knot theory and the link predictions not only simplify the glucomannan microscopic descriptions but also play a guiding role in predicting and regulating the structures.
基金supported by the National Natural Science Foundation of China(Nos.52322708 and 52441702)Zhengzhou University Young Student Basic Research Projects(PhD students)(No.ZDBJ202512).
文摘The interface problems in zinc-ion batteries severely limit their electrochemical performance,even in hydrogel(HG)electrolyte(HE).Herein,a strategy of reconfiguring the hydrogen bond networks by thermal gelation is proposed to enhance the battery interface stability.The strategy introduces methyl cellulose into acrylamide,which can effectively stabilize the electrode interface and reconstruct the hydrogen bond networks of the electrolyte through its unique thermos-gelation property.Methylcellulose is dissolved by heating and cooled to form gel.This thermal gelation strategy formed hydrogen bonds with a large amount of free water and methyl cellulose,which not only reduced the water activity but also enhanced the intermolecular polymerization network and also promoted the solvation of Zn^(2+).More importantly,the symmetric batteries with HE-HG hydrogel electrolyte exhibited a long cycling life of 8000 h.The Zn||Zn_(0.25)V_(2)O_(5)(Zn||ZVO)battery displays the low-capacity decay rate for 800 cycles at 1 C at−20°C.The pouch battery maintains a capacity of 255 mAh·g^(−1) after 100 cycles under 2.5 A·g^(−1) at−20°C.This study provides a new way to enhance the interfacial stability,which helps to realize the scale application of flexible zinc-ion batteries.
基金supported by the National Natural Science Foundation of China(NSFC 52432002,52372041,and 52302087)China Postdoctoral Science Foundation(Grant No.2023 M740895)+1 种基金Heilongjiang Touyan Team Programthe Fundamental Research Funds for the Central Universities(Grant No.HIT.OCEF.2021003 and HIT.DZJJ.2025002)。
文摘Aqueous Zn-metal batteries(AZMBs)performance is hampered by freezing water at low temperatures,which hampers their multi-scenario application.Hydrogen bonds(HBs)play a pivotal role in water freezing,and proton transport is indispensable for the establishment of HBs.Here,the accelerated proton transport modulates the dynamic hydrogen bonding network of a Zn(BF4)2/EMIMBF4impregnated polyacrylamide/poly(vinyl alcohol)/xanthan gum dual network eutectic gel electrolyte(PPX-ILZSE)for lowtemperature AZMBs.The PPX-ILZSE forms more HBs,shorter HBs lifetimes,higher tetrahedral entropy,and faster desolvation processes,as demonstrated by experimental and theoretical calculations.This enhanced dynamic proton transport promotes rapid cycling of HBs formation-failure,and for polyaniline cathode(PANI)abundant redox sites of proton,confers excellent low temperature electrochemical performance to the Zn//PANI full cell.Specific capacities for 1000 and 5000 cycles at 1 and 5 A g^(-1)were149.8 and 128.4 m A h g^(-1)at room temperature,respectively.Furthermore,specific capacities of 131.1 mA hg^(-1)(92.4%capacity retention)and 0.0066%capacity decay per lap were achieved for 3000and 3500 laps at-30 and 40℃,respectively,at 0.5 A g^(-1).Furthermore,in-situ protective layer of ZnOHF nano-arrays on the Zn anode surface to eliminate dendrite growth and accelerate Zn-ions adsorption and charge transfer.
基金supported by the National Natural Science Foundation of China(grant nos.21874056 and 52003103)the National Key R&D Program of China(grant no.2016YFC1100502).
文摘The sensitivity and fidelity of surface electromyography(sEMG)signal monitoring is critical for muscle status and fatigue assessment,prosthetic control,and gesture recognition.However,the incompatible skin-electrode interface and complex electrophysiological environment restrict the sensitive acquisition and accurate analysis of sEMG signals.Focused on the impedance of the skin-electrode interface issue,we developed an interfacial gel electrode patch with a tunable hydrogen bond network to simultaneously achieve a conformal interface,suitable adhesion,and high conductivity for sEMG signal monitoring.By exploiting hydroxyethylidene diphosphonic acid(HEDP)and 2-hydroxyphosphono-acetic acid(HPAA)as hydrogen bonding regulators were introduced into the polyvinyl alcohol(PVA)-based hydrogel network to regulate the hydrogen bond cross-linking network.As a result,the balance of elastic modulus,adhesion,and electrical conductivity of PVA-HEDP-HPAA(PHH)hydrogel are achieved.The reliable electrodeskin interface is manipulated to achieve conformal contact by matching the elastic modulus,reducing the gap of electrode-skin interface by adhesion,and promoting ion and electron conduction by electrical conductivity.The PHH electrode patches exhibit a lower interfacial impedance(12.56 kΩ)and a signal-to-noise ratio of 38.09±1.28 dB for accurate analysis of muscle strength and evaluation of the fatigue state.With the assistance of the artificial neural network algorithm,seven gestures can be recognized with 100%prediction accuracy.The interfacial gel electrode patch contributes a bio-matching electrophysiological platform for prosthetic control,human–machine interaction,and clinical or athletic auxiliary monitoring.
基金supported by the National Natural Science Foundation of China(30371009, 30471218) Science Foundation of Fujian Department of Education (JA03059)
文摘In this paper, the hydrogen bonding network models of konjac glucomannan （KGM） are predicted in the approach of molecular dynamics （MD）. These models have been proved by experiments whose results are consistent with those from simulation. The results show that the hydrogen bonding network structures of KGM are stable and the key linking points of hydrogen bonding network are at the O（6） and O（2） positions on KGM ring. Moreover, acety has significant influence on hydrogen bonding network and hydrogen bonding network structures are more stable after deacetylation.
基金supported by the 973 Program of China (No. 2014CB845600)the National Natural Science Foundation of China (Nos. 21421001 and 21531005)the Natural Science Foundation of Tianjin(No. 15JCZDJC38800)
文摘A new coordination compound [Mg（L）（H2 O）5·H2 O]（NKU-109, H2 L=5-（4 H-1,2,4-triazol-4-yl）benzene-1,3-dicarboxylic acid） was solvothermally synthesized, featuring a supramolecular hydrogen-bonding network. A good proton conductivity of 5.87×10^-4S/cm was recorded at 70℃ and a relative humidity of75% in alternating current（AC） impedance experiment, which sheds a new light on the design of proton conduction materials based on coordination compounds.
基金Supported by the National Natural Science Foundation of China(No.2 0 1710 10)
文摘A novel complex, (H 3O) 2[Ni(2,6-pydc) 2]·2H 2O was synthesized in an aqueous solution and characterized by means of single-crystal X-ray diffraction, elemental analyses and IR spectra. The X-ray structural analysis revealed that the novel compound forms three-dimensional(3D) networks by both π-π stacking and hydrogen-bonding interactions. The crystal data for the complex are a=13.853(3) nm, b=9.6892(19) nm, c=13.732(3) nm, α=90.00°, β=115.52(3)°, γ=90.00°, Z=3, R 1=0.0786, wR 2=0.1522.
基金National Natural Science Foundation of China(11974063)Graduate research innovation project,School of Optoelectronic Engineering,Chongqing University(GDYKC2023002)+1 种基金Fundamental Research Funds for the Central Universities(2022CDJQY-010)The authors extend their appreciation to the Deputyship for Research and Innovation,Ministry of Education in Saudi Arabia for funding this research work through the project no.(IFKSUOR3-073-9).
文摘The Sb^(3+) doping strategy has been proven to be an effective way to regulate the band gap and improve the photophysical properties of organic-inorganic hybrid metal halides(OIHMHs).However,the emission of Sb^(3+) ions in OIHMHs is primarily confined to the low energy region,resulting in yellow or red emissions.To date,there are few reports about green emission of Sb^(3+)-doped OIHMHs.Here,we present a novel approach for regulating the luminescence of Sb^(3+) ions in 0D C_(10)H_(2)_(2)N_(6)InCl_(7)·H_(2)O via hydrogen bond network,in which water molecules act as agents for hydrogen bonding.Sb^(3+)-doped C_(10)H_(2)2N_(6)InCl_(7)·H_(2)O shows a broadband green emission peaking at 540 nm and a high photoluminescence quantum yield(PLQY)of 80%.It is found that the intense green emission stems from the radiative recombination of the self-trapped excitons(STEs).Upon removal of water molecules with heat,C_(10)H_(2)_(2)N_(6)In_(1-x)Sb_(x)Cl_(7) generates yellow emis-sion,attributed to the breaking of the hydrogen bond network and large structural distortions of excited state.Once water molecules are adsorbed by C_(10)H_(2)_(2)N_(6)In_(1-x)Sb_(x)Cl_(7),it can subsequently emit green light.This water-induced reversible emission switching is successfully used for optical security and information encryption.Our findings expand the under-standing of how the local coordination structure influences the photophysical mechanism in Sb^(3+)-doped metal halides and provide a novel method to control the STEs emission.
基金Supported by the Youth Foundation of Jiangxi Provincial Office of Education (GJJ09605)the Science Foundation of Jiangxi Provincial Office of Education (GJJ09637)
文摘Hydrothermal reaction of MgCl2 and ethyl tetrazolate-5-carboxylate at 160 ℃unexpectedly yielded compound {（H3O）[Mg（H2O）6]Cl3} （1）. The result of X-ray diffraction analysis indicates that 1 crystallizes in the monoclinic system, space group C2/c with a = 9.2896（3）, b = 9.5570（4）, c = 13.3169（5） A, β = 90.1221（12）°, V= 1182.28（8） A3, Z = 4, Mr = 257.78, Dc = 1.448 g/cm3, μ = 0.824 mm^-1, F（000） = 536, R = 0.0265 and wR - 0.0706. 1 is composed of one hexa-aqua-magnesium（Ⅱ） ion, one hydroxonium ion, and three chlorine anions. These three components weave a perfect three-dimensional （3D） （4,4,6,12）-connected hydrogen bonding network within 1.
基金This work was supported by Chinese Academy of Sciences the State Education Ministry+1 种基金 the State Personnel Ministry the NSFC (20073048)
文摘The crystal structure of the title compound [Na2(OH2)5]2+[C6H12N4H2]2-2+ [Mo7O24]6 ?4H2O, prepared from an aqueous solution of Na2MoO4 ?2H2O in the presence of MoCl3 and hexamethylene tetramine, has been determined by single-crystal X-ray diffraction. The crystal is of orthorhombic, space group Pnma with a = 14.6113(2), b = 18.6833(1), c = 15.3712(2), V = 4196.14(8)3, Z = 4, Mr = 1548.13, F(000) = 3016, = 2.157 mm-1 and Dc = 2.451 g/cm3. The final R factor is 0.0526 for 3818 unique observed reflections (I > 2(I)). The structural analysis reveals that heptamolybdate anions in the title compound consist of seven edge-sharing MoO6 octahedra, and are linked into a three-dimensional framework by sodium ions and hydrogen bonds.
基金financially supported by the National Natural Science Foundation of China (Nos.51973118, 22175121,52003160 and 22001175)Key-Area Research and Development Program of Guangdong Province (Nos.2019B010941001 and2019B010929002)+7 种基金the Natural Science Foundation of Guangdong Province (No.2020A1515010644)the Program for Guangdong Introducing Innovative and Entrepreneurial Teams(No.2019ZT08C642)Shenzhen Science and Technology Program (Nos.JCYJ20220818095810022, JSGGZD20220822095201003 and JCYJ20210324095412035)the start-up fund of Shenzhen University (No.000002110820)the Guangdong Natural Science Foundation (Nos.2022A1515011781 and2021A1515110086)Science and Technology Innovation Commission of Shenzhen,China (Nos.RCBS20200714114910141 and JCYJ20210324132816039)the Start-up Grant at Harbin Institute of Technology (Shenzhen),China (Nos.HA45001108 and HA11409049)Shenzhen Key Laboratory of Advanced Functional Carbon Materials Research and Comprehensive Application (No.ZDSYS20220527171407017)。
文摘The emerging biomass-based epoxy vitrimers hold great potential to fulfill the requirements for sustainable development of society.Since the existence of dynamic chemical bonds in vitrimers often reduces both the thermal and mechanical properties of epoxy resins, it is challenging to produce recyclable epoxy vitrimers with both excellent mechanical properties and good thermal stability. Herein, a monomer 4-(((5-(hydroxymethyl)furan-2-yl)methylene)amino)phenol(FCN) containing furan ring with potential to form high density of hydrogen bonding among repeating units is designed and copolymerized with glycerol triglycidyl ether to yield epoxy resin(FCN-GTE), which intrinsically has dual hydrogen bond networks, dynamic imine structure and resultant high performance. Importantly, as compared to the BPA-GTE, the FCN-GTE exhibits significantly improved mechanical properties owing to the increased density of hydrogen bond network and physical crosslinking interaction. Furthermore, density functional theory(DFT) calculation and in situ FTIR analysis is conducted to decipher the formation mechanism of hydrogen bond network. In addition, the FCN-GTE possesses superior UV shielding, chemical degradation, and recyclability because of the existence of abundant imine bonds. Notably, the FCN-GTE-based carbon fiber composites could be completely recycled in an amine solution.This study provides a facile strategy for synthesizing recyclable biomass-based high-performance epoxy vitrimers and carbon fiber composites.
基金supported by the Natural Science Foundation of Guangxi(2022JJD120011)the National Natural Science Foundation of China(22479031,22162004).
文摘Aqueous zinc-ion batteries(AZIBs)are promising due to the advantages of metallic zinc,including the high specific capacity(820 mAh g^(-1)),low redox potential(−0.76 V vs.SHE),inherent safety,low cost,and environmental sustainability.Despite these benefits,AZIBs face challenges such as uneven Zn deposition and excessive hydrogen evolution reaction(HER)at the Zn anode,which reduce the battery's coulombic efficiency and cycling life.This study introduces an ammonium formate(AF)additive into a 2.0 M ZnSO_(4) electrolyte to address these issues.The AF additive promotes the three-dimensional rapid diffusion of Zn^(2+)on the anode surface and induces the preferential Zn(002)plane deposition,thus inhibiting dendrite growth and enhancing cycling stability.It also disrupts the hydrogen bond network of electrolyte,reducing the number of active H2O molecules and suppressing H_(2)O-induced side reactions.Consequently,the Zn||Zn symmetric cell with the AF additive shows stable cycling over 2100 h at 5.0 mA cm^(−2) with an areal capacity of 1.0 mAh cm^(−2),and maintains stability over 9700 cycles at 30 mA cm^(−2).When applied in a Zn||VO_(2) full cell,it achieves capacity retention of 68.9%after 2000 cycles,which demonstrates significant performance improvements in AZIBs.
文摘The aim of this work is to investigate the hydrogen-bonding interaction in poly(vinyl alcohol)(PVA)/poly(acrylic acid)(PAA) blending system and its influence on rheological properties in solution and the physical properties in solid state. Introducing PAA into PVA solutions resulted in a thickening behavior of blend solutions.The viscosity of the solutions increased with PAA content increasing,and a maximum viscosity could be obtained when the ratio of PVA/PAA was 70/30. The intermolecular hydrogen-bonding and miscibility between PVA and PAA in solid state were investigated by differential scanning calorimetry(DSC),Fourier transform infrared spectroscopy(FTIR) and mechanical measurements.The results displayed the great influence of introducing PAA on the properties of blending films.The tensile strength increased from 89.31 MPa to 119.8 MPa and Young’s modulus improved by over 300%with increasing PAA concentration compared with those of pure PVA films.By systematically studying the rheological behaviors of solutions and the physical properties of films,the influence of hydrogen-bonding in solutions and solid states were discussed.
基金Supported by the National Natural Science Foundation of China(No.2 0 0 710 192 0 0 710 2 0 and5 0 172 0 2 ) and the Re-search Fund for Doctoral Program of Higher Education.
文摘A new copper(Ⅱ) complex [Cu(PDA)(H 2O) 2] was synthesized and its structure was determined. Cu(Ⅱ) is five coordinated in a tetragonal pyramid geometry. The two coordinating water molecules are different and the two Cu-O bond lengths differ by nearly 0.02 nm. The whole crystal is linked to form a three dimensional network by means of hydrogen bonds. The X band ESR spectrum shows three different g tensors with a well resolved hyperfine structure in the g z signal, giving the ESR parameters g x=2 05, g y =2 065 and g z =2 29. The covalency of the coordinate bonds and the deviation from tetragonal pyramid geometry for the complex are discussed based on the ESR spectra.
基金supported by the National Natural Science Foundation of China(52002297)National Key R&D Program of China(2022VFB2404800)+1 种基金Wuhan Yellow Crane Talents Program,China Postdoctoral Science Foundation(No.2024M752495)the Postdoctoral Fellowship Program of CPSF(No.GZB20230552).
文摘Aqueous alkali metal-ion batteries(AAMIBs)have been recognized as emerging electrochemical energy storage technologies for grid-scale applications owning to their intrinsic safety,cost-effectiveness,and environmental sustainability.However,the practical application of AAMIBs is still severely constrained by the tendency of aqueous electrolytes to freeze at low temperatures and decompose at high temperatures,limiting their operational temperature range.Considering the urgent need for energy systems with higher adaptability and resilience at various application scenarios,designing novel electrolytes via structure modulation has increasingly emerged as a feasible and economical strategy for the performance optimization of wide-temperature AAMIBs.In this review,the latest advancement of wide-temperature electrolytes for AAMIBs is systematically and comprehensively summarized.Specifically,the key challenges,failure mechanisms,correlations between hydrogen bond behaviors and physicochemical properties,and thermodynamic and kinetic interpretations in aqueous electrolytes are discussed firstly.Additionally,we offer forward-looking insights and innovative design principles for developing aqueous electrolytes capable of operating across a broad temperature range.This review is expected to provide some guidance and reference for the rational design and regulation of widetemperature electrolytes for AAMIBs and promote their future development.
基金supported by the China Postdoctoral Science Foundation(No.2014M551053)Natural Science Foundation of Hebei Province(No.B2015203124)Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education),Nankai University
文摘Two crystals of receptor 1, C（42）H（52）N（10）O4S2（anthracene-9,10-dicarbaldehyde bis-（phenyl-semithiocarbazone）） and-1-H2PO4, C（68）H（114）N（10）O（10）P2S2 were obtained at room temperature successfully, and their structures were characterized by X-ray crystallography diffraction. X-ray diffraction reveals that, receptor 1 crystallizes in monoclinic, space group P21/c, with a = 9.487（3）,b = 20.674（6）, c = 11.821（4）A, β = 113.416（8）o, Mr = 825.06, V = 2127.5（12） A^3, Z = 2, Dc = 1.288g/cm^3, μ = 0.18 mm^-1, F（000） = 876, MoK α radiation（λ = 0.71073 A）, the final R = 0.0472 and wR = 0.0930. A total of 3758 unique reflections were collected, of which 3313 with I 〉 2σ（I） were observed. Compound 1-H2PO4^-crystallizes in triclinic, space group P21/n, with a = 8.767（1）, b =13.6190（15）, c = 16.615（2） ？, α = 98.727（14）, β = 103.061（14）, γ = 91.382（16）°, Mr = 1357.75, V =1906.6（4） A^3, Z = 1, Dc = 1.183 g/cm^3, μ = 0.17 mm-（-1）, F（000） = 734, MoK α radiation（λ = 0.71073？）, the final R = 0.0769 and wR = 0.1884. A total of 6699 unique reflections were collected, of which 2989 with I 〉 2σ（I） were observed. As it was observed in the crystal structure of 1-H2PO4^-, 1bound H2PO4^-at a 1：2 ratio by intermolecular interaction of N-H···O hydrogen bond obviously.Another interesting feature was that H2PO4--groups assembled chains themselves via intramolecular hydrogen bond O-H···O and connected the 1 molecules together through the interaction of H-bonds,which improved the planarity of 1 and increased the stability of the entire structure.
基金supported by the Natural Science Foundation of Fujian Province (2006F3042)
文摘A new compound [Zn3（C7NO4H3）3Cl4]·[C6NO2H6]4·4H2O （I） has been synthesized and structurally characterized by X-ray crystallography.It crystallizes in monoclinic,space group C2/c with a=16.9018（14）,b=12.6902（10）,c=25.1170（2）,β=90.54°,V=5387.0（8）3,Z=4,Zn3C45H41Cl4N7O24,Mr=1401.76,Dc=1.728 g/cm3,F（000）=2840,μ（MoKa）=1.615 mm-1,the R= 0.0758 and wR=0.2060 for 3468 observed reflections （I 〉 2σ（I））.Analysis of single-crystal X-ray diffraction data shows that compound I displays an interesting example of 3D supramolecular networks with perfect neutral and ionic hydrogen bonding array.
基金supported by the National Natural Science Foundation of China(Grant Nos.12022508,12074394,and 22125604)Shanghai Supercomputer Center of ChinaShanghai Snowlake Technology Co.Ltd.
文摘The stable nanobubbles adhered to mineral surfaces may facilitate their efficient separation via flotation in the mining industry.However,the state of nanobubbles on mineral solid surfaces is still elusive.In this study,molecular dynamics(MD)simulations are employed to examine mineral-like model surfaces with varying degrees of hydrophobicity,modulated by surface charges,to elucidate the adsorption behavior of nanobubbles at the interface.Our findings not only contribute to the fundamental understanding of nanobubbles but also have potential applications in the mining industry.We observed that as the surface charge increases,the contact angle of the nanobubbles increases accordingly with shape transformation from a pancake-like gas film to a cap-like shape,and ultimately forming a stable nanobubble upon an ordered water monolayer.When the solid–water interactions are weak with a small partial charge,the hydrophobic gas(N_(2))molecules accumulate near the solid surfaces.However,we have found,for the first time,that gas molecules assemble a nanobubble on the water monolayer adjacent to the solid surfaces with large partial charges.Such phenomena are attributed to the formation of a hydrophobic water monolayer with a hydrogen bond network structure near the surface.
文摘Platinum-ruthenium alloys(PtRu)represent state-of-the-art alkaline hydrogen oxidation reaction(HOR)catalysts,yet the atomic-scale origin of their superiority over pure Pt remains incompletely understood.Here,we employ density functional theory calculations,ab initio molecular dynamics simulations,and microkinetic modeling on Pt(111)and PtRu(111)surfaces to systematically investigate the key factors,including active sites distribution,species adsorption,and solvent reorganization,that affect the HOR activity and decouple their contributions.The results reveal that while the moderate hydrogen binding energy and improved hydroxyl(OH)species adsorption both contribute to the enhanced activity,the dominant factor is the substantial reduction in solvent reorganization energy on the PtRu(111).This is facilitated by the spatial separation of active sites:Pt atoms preferentially stabilize adsorbed hydrogen,while Ru atoms strongly bind OH and interfacial water molecules.This configuration increases the probability of hydrogen interacting with OH/water and enhances the fraction of"H-up"water molecules,forming a well-organized hydrogen bond network within the electric double layer.The dynamically compatible interfacial water structure and HOR coordination promote H desorption and proton transfer in the Volmer step,thereby accelerating the HOR kinetics.
