Elastomers with outstanding strength,toughness and healing efficiency are highly promising for many emerging fields.However,it is still a challenge to integrate all these beneficial features in one elastomer.Herein,an...Elastomers with outstanding strength,toughness and healing efficiency are highly promising for many emerging fields.However,it is still a challenge to integrate all these beneficial features in one elastomer.Herein,an asymmetric alicyclic structure adjacent to aromatic disulfide was tactfully introduced into the backbone of polyurethane(PU)elastomer.Specifically,such elastomer(PU-HPS)was fabricated by polycondensing polytetramethylene ether glycol(PTMEG),isophorone diisocyanate(IPDI)and p-hydroxydiphenyl disulfide(HPS)via one-pot method.The molecular mobility and phase morphology of PU-HPS can be tuned by adjusting the HPS content.Consequently,the dynamic exchange of hydrogen and disulfide bonds in the hard segment domains can also be tailored.The optimized sample manifests outstanding tensile strength(46.4 MPa),high toughness(109.1 MJ/m^(3)),high self-healing efficiency after fracture(90.3%),complete scratch recovery(100%)and good puncture resistance.Therefore,this work provides a facile strategy for developing robust self-healing polymers.展开更多
The self-healing solid polymer electrolytes(SHSPEs)can spontaneously eliminate mechanical damages or micro-cracks generated during the assembly or operation of lithium-ion batteries(LIBs),significantly improving cycli...The self-healing solid polymer electrolytes(SHSPEs)can spontaneously eliminate mechanical damages or micro-cracks generated during the assembly or operation of lithium-ion batteries(LIBs),significantly improving cycling performance and extending service life of LIBs.Here,we report a novel cross-linked network SHSPE(PDDP)containing hydrogen bonds and dynamic disulfide bonds with excellent self-healing properties and nonflammability.The combination of hydrogen bonding between urea groups and the metathesis reaction of dynamic disulfide bonds endows PDDP with rapid self-healing capacity at 28°C without external stimulation.Furthermore,the addition of 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide(EMIMTFSI)improves the ionic conductivity(1.13×10^(−4)S cm^(−1)at 28°C)and non-flammability of PDDP.The assembled Li/PDDP/LiFePO_(4)cell exhibits excellent cycling performance with a discharge capacity of 137 mA h g^(−1)after 300 cycles at 0.2 C.More importantly,the self-healed PDDP can recover almost the same ionic conductivity and cycling performance as the original PDDP.展开更多
Each possible pair of residues inβ-1,4 glucanase for disulfide formation was assessed using online websites,and four pairs L28C-S256C,Q41C-P278C,S122C-N163C and A184C-A215C were selected.Accordingly,four recombinant ...Each possible pair of residues inβ-1,4 glucanase for disulfide formation was assessed using online websites,and four pairs L28C-S256C,Q41C-P278C,S122C-N163C and A184C-A215C were selected.Accordingly,four recombinant plasmids pET28a(+)EccslH28,pET28a(+)EccslH41,pET28a(+)EccslH122 and pET28a(+)EccslH184 were prepared and transformed into E.coli to express the recombinant enzymes.Then analysis on enzymatic properties showed that T50 of the recombinant enzymes was increased from 10 min for EccslHt2 to 90 min for EccslH28 and 40 min for EccslH41 at 70℃,while their optimum pH value and pH stability were not affected,which proved that the introduction of disulfide bond improved the thermal stability ofβ-1,4 glucanase.展开更多
Decorsin, an antagonist of integrin glycoprotein IIb/IIIa, contains Arg-Gly-Asp （RGD） sequence and three disulfide bridges. The function of RGD sequence has already been well defined, but the roles of conserved disu...Decorsin, an antagonist of integrin glycoprotein IIb/IIIa, contains Arg-Gly-Asp （RGD） sequence and three disulfide bridges. The function of RGD sequence has already been well defined, but the roles of conserved disulfide bonds in antihemostatic proteins still remain unclear. Herein we use the fusion expression and characterization of mutant decorsin to study the func- tions of disulfide bonds in protein structure, stability and biological activity. The purified protein shows an apparent inhibition of activity to platelet aggregation induced by ADP with IC50 of 500 nM. The removal of cys7-cysl5 （from cysteine to serine） at the N-terminal causes a thirty-fold decrease of the inhibition activity with IC50 of 15 ~tM, whereas the mutation of cys22-cys38 at the C-terminal completely impairs the biological activity of decorsin. The overall secondary and tertiary struc- tures of decorsin are disrupted inevitably without disulfide bonds. Using a domain insertion mutation, the retaining of RGD loop and the adjacent disulfide bond produces a week antihemostatic activity of decorsin. This reveals that the overall structure of decorsin stabilized by the three conserved disulfide bridges is cooperative for antihemostatic function. Our study on the ef- fect of disulfide bonds together with RGD-sequence on the protein function is helpful for structure-based drug design of an- tithrombotic research.展开更多
Thanks to their excellent bond strength,phenyl-based molecules with thiol anchoring groups are extensively employed to form stable single-molecule junctions.However,two critical questions are still not answered which ...Thanks to their excellent bond strength,phenyl-based molecules with thiol anchoring groups are extensively employed to form stable single-molecule junctions.However,two critical questions are still not answered which seriously hinder high-yield establishing reliable molecular functional devices:(1)Whether molecular dimer junctions will be formed,and if this is the case,whether the dimerization is caused by intermolecular disulfide bonds orπ–πstacking of phenyl rings;(2)Upon a mechanical-compression force,is it possible that both anchoring groups of the molecule bond to the same electrode instead of bridging two opposite electrodes,which would drastically reduce the yield of the molecular junctions.Here,combining UV-Vis/Raman spectroscopy of bulk molecules and conductance/flicker-noise measurements of single molecules,we give compelling evidence that molecular dimers naturally form under ambient conditions,primarily via disulfide bonds rather than byπ–πstacking.We further proposed a technique,named electrode-compression-hold-on(ECHO),and reveal that the two thiol groups of phenyl-backboned molecules will bond to the same electrode upon a compression force with a prolongated ECHO time.In contrast,the compression-time-dependent phenomenon is not observed for alkyl-backboned molecules.The underlying mechanism for these unprecedented observations is elucidated,shedding light on the yield of molecular junctions.展开更多
Monitoring subtle changes in ionic current flow through a nanopore could be applied to observe single molecule reaction. Here,we introduced cysteine to substitute for lysine at position 238 constructing a mutant aerol...Monitoring subtle changes in ionic current flow through a nanopore could be applied to observe single molecule reaction. Here,we introduced cysteine to substitute for lysine at position 238 constructing a mutant aerolysin K238 C. It could be regarded as a nanoreactor to efficiently visualize chemical bonds making and breaking. The compound 5,5′-dithiobis-(2-nitrobenzoic acid)(DTNB) was selected as a reactant coming into collisions on the interface of the pore to occur a reversible reaction. Our results showed that the mutant aerolysin could respond to three molecules of DTNB simultaneously and reflect corresponding levels with distinguishable current signals. Therefore, this method constitutes a simple, generic tool for monitoring single molecule reaction, which evokes a guidance for the mutant aerolysin towards the application of tracking other more reactions at single molecule level.展开更多
The most widely used bisphenol A-type epoxy resin(DGEBA)in electrical engineering demonstrates excellent mechanical and electrical properties.However,the insoluble and infusible characteristics of cured DGEBA make it ...The most widely used bisphenol A-type epoxy resin(DGEBA)in electrical engineering demonstrates excellent mechanical and electrical properties.However,the insoluble and infusible characteristics of cured DGEBA make it difficult to efficiently degrade and recycle decommissioned electrical equipment.In this study,a degradable itaconic acid-based epoxy resin incorporating dynamic covalent bonds was prepared through the integration of ester bonds and disulfide bonds,with itaconic acid as the precursor.The covalent bonding effects on the mechanical,thermal,electrical,and degradation characteristics were systematically evaluated.The experimental results revealed that the introduction of dynamic ester bonds enhanced the mechanical properties and thermal stability of the resin system,achieving a flexural strength of 141.57 MPa and an initial decomposition temperature T_(5%)of up to 344.9℃.The resin system containing dynamic disulfide bonds exhibited a dielectric breakdown strength of 41.11 k V/mm.Simultaneously,the incorporation of disulfide bonds endowed the epoxy resin with remarkable degradability,enabling complete dissolution within 1.5 h at 90℃ in a mixed solution of dithiothreitol(DTT)and N-methylpyrrolidone(NMP).This research provides a valuable reference for the application of itaconic acid-based vitrimer with dynamic covalent bonds in electrical materials,contributing to the development and utilization of environmentally friendly electrical equipment.展开更多
In order to prepare pyrimidine nucleoside-peptide conjugate concisely, we developed a one-pot synthetic strategy. Started from uridine, 5-S-acetyl-thiomethyl-2＇,3 ＇-di-O-isopropylidene-uridine （4） was synthesized ...In order to prepare pyrimidine nucleoside-peptide conjugate concisely, we developed a one-pot synthetic strategy. Started from uridine, 5-S-acetyl-thiomethyl-2＇,3 ＇-di-O-isopropylidene-uridine （4） was synthesized as the key intermediate in four steps. Under acidic condition, compound 4 was deprotected and reacted with PySS-R （8, 12, 15, Py = 2-pyridyl, R = amino acid or peptide） in one pot to form uridine conjugates （9, 13, 2） with disulfide bond as linker.展开更多
Self-healing polymers based on dynamic crosslinkers have drawn rapidly increasing interest over the last decade.Here,a self-healable epoxy network with exchangeable disulfide bonds was synthesized by polymerizing two ...Self-healing polymers based on dynamic crosslinkers have drawn rapidly increasing interest over the last decade.Here,a self-healable epoxy network with exchangeable disulfide bonds was synthesized by polymerizing two epoxies with an aromatic amine containing a disulfide bond.The bisphenol A diglycidyl ether(DGEBA)and poly(ethylene glycol)diglycidyl ether(DER736)were used as rigid and soft components,respectively.The crosslinking densities of studied polymers decreased with the increasing amount of DER736,resulting in the lower glassy temperature and weaker mechanical strength.The dynamic covalent network character of disulfide bond and its low active energy were also investigated through stress relaxation experiments at various temperatures.The self-healing performance of healable epoxy resins with varied flexibility was measured by tensile tests.The tensile strength of a full-cut sample was restored to 84%(13 MPa)of the initial values(16 MPa)at moderate temperature.Its healed fracture strain was up to 505%.Moreover,the effect of healing time and temperature on the self-healing properties was also studied.A model was proposed to investigate the self-repairing efficiency evolution with healing time,suggesting that hydrogen bonds mainly contributed to the initial sticking or interfacial adhesion while disulfide links and chain interdiffusion assisted time dependent reformation of networks to restore the original mechanical strength.展开更多
Disulfide bond-bridging strategy has been extensively utilized to construct tumor specificity-responsive aliphatic prodrug nanoparticles(PNPs) for precise cancer therapy. Yet, there is no research shedding light on th...Disulfide bond-bridging strategy has been extensively utilized to construct tumor specificity-responsive aliphatic prodrug nanoparticles(PNPs) for precise cancer therapy. Yet, there is no research shedding light on the impacts of the saturation and cis-trans configuration of aliphatic tails on the self-assembly capacity of disulfide bond-linked prodrugs and the in vivo delivery fate of PNPs. Herein, five disulfide bond-linked docetaxelfatty acid prodrugs are designed and synthesized by using stearic acid, elaidic acid, oleic acid, linoleic acid and linolenic acid as the aliphatic tails, respectively. Interestingly, the cistrans configuration of aliphatic tails significantly influences the self-assembly features of prodrugs, and elaidic acid-linked prodrug with a trans double bond show poor self-assembly capacity. Although the aliphatic tails have almost no effect on the redox-sensitive drug release and cytotoxicity, different aliphatic tails significantly influence the chemical stability of prodrugs and the colloidal stability of PNPs, thus affecting the in vivo pharmacokinetics, biodistribution and antitumor efficacy of PNPs. Our findings illustrate how aliphatic tails affect the assembly characteristic of disulfide bond-linked aliphatic prodrugs and the in vivo delivery fate of PNPs, and thus provide theoretical basis for future development of disulfide bond-bridged aliphatic prodrugs.展开更多
Stimulus-responsive polymers containing dynamic bonds enable fascinating properties of self-healing,recycling and reprocessing due to enhanced relaxation of polymer chain/network with labile linkages.Here,we study the...Stimulus-responsive polymers containing dynamic bonds enable fascinating properties of self-healing,recycling and reprocessing due to enhanced relaxation of polymer chain/network with labile linkages.Here,we study the structure and properties of a new type of thermoplastic polyurethanes(TPUs)with trapped dynamic covalent bonds in the hard-phase domain and report the frustrated relaxation of TPUs containing weak dynamic bond andπ-πinteraction in hard segments.As detected by rheometry,the aromatic TPUs with alkyl disulfide in the hard segments possess the maximum network relaxation time in contrast to those without dynamic bonds and alicyclic TPUs.In situ FTIR and small-angle scattering results reveal that the alkyl disulfide facilitates stronger intermolecular interaction and more stable micro-phase morphology inπ-πinteraction based aromatic TPUs.Molecular dynamics simulation for pure hard segments of model molecules verify that the presence of disulfide bonds leads to strongerπ-πstacking of aromatic rings due to both enhanced assembling thermodynamics and kinetics.The enhancedπ-πpacking and micro-phase structure in TPUs further kinetically immobilize the dynamic bond.This kinetically interlocking between the weak dynamic bonds and strong molecular interaction in hard segments leads to much slower network relaxation of TPU.This work provides a new insight in tuning the network relaxation and heat resistance as well as molecular self-assembly in stimulus-responsive dynamic polymers by both molecular design and micro-phase control toward the functional applications of advanced materials.展开更多
One of the major barriers in utilizing prodrug nanocarriers for cancer therapy is the slow release of parent drug in tumors.Tumor cells generally display the higher oxidative level than normal cells,and also displayed...One of the major barriers in utilizing prodrug nanocarriers for cancer therapy is the slow release of parent drug in tumors.Tumor cells generally display the higher oxidative level than normal cells,and also displayed the heterogeneity in terms of redox homeostasis level.We previously found that the disulfide bond-linkage demonstrates surprising oxidationsensitivity to form the hydrophilic sulfoxide and sulphone groups.Herein,we develop oxidation-strengthened prodrug nanosystem loaded with pyropheophorbide a(PPa)to achieve light-activatable cascade drug release and enhance therapeutic efficacy.The disulfide bond-driven prodrug nanosystems not only respond to the redox-heterogeneity in tumor,but also respond to the exogenous oxidant(singlet oxygen)elicited by photosensitizers.Once the prodrug nanoparticles(NPs)are activated under irradiation,they would undergo an oxidative self-strengthened process,resulting in a facilitated drug cascade release.The IC50 value of the PPa@PTX-S-S NPs without irradiation was 2-fold higher than those of NPs plus irradiation.In vivo,the PPa@PTX prodrug NPs display prolonged systemic circulation and increased accumulation in tumor site.The PPa@PTXS-S NPs showed much higher efficiency than free PTX or the PPa@PTX-C-C NPs to suppress the growth of 4 T1 tumors.Therefore,this novel oxidation-strengthened disulfide-bridged prodrug-nanosystem has a great potential in the enhanced efficacy of cancer synergetic photochemotherapy.展开更多
AIM: To study the influence of redox environment of Escherichia coli (E(?) coli) cytoplasm on disulfide bond formation of recombinant proteins. METHODS: Bovine fibrobllast growth factor (BbFGF) was selected as a model...AIM: To study the influence of redox environment of Escherichia coli (E(?) coli) cytoplasm on disulfide bond formation of recombinant proteins. METHODS: Bovine fibrobllast growth factor (BbFGF) was selected as a model of simple proteins with a single disulfide bond and free cysteines. Anti-HBsAg single-chain Fv (HBscFv), an artificial multidomain protein, was selected as the model molecule of complex protein with 2 disulfide bonds. A BbFGF-producing plasmid, pJN-BbFGF, and a HBscFv producing-plasmid, pQE-HBscFv, were constructed and transformed into E(?)coli strains BL21(DE3) and M15[pREP4] respectively. At the same time, both plasmids were transformed into a reductase-deficient host strain,E(?)coli Origami(DE3). The 4 recombinant E(?)coli strains were cultured and the target proteins were purified. Solubility and bioactivity of recombinant BbFGF and HBscFv produced in different host strains were analyzed and compared respectively. RESULTS: All recombinant E(?)coli strains could efficiently produce target proteins. The level of BbFGF in BL21(DE3) was 15-23% of the total protein, and was 5-10% in Origami (DE3). In addition, 65% of the BbFGF produced in BL21(DE3) formed into inclusion body in the cytoplasm, and all the target proteins became soluble in Origami (DE3). The bioactivity of BbFGF purified from Origami(DE3) was higher than its counterpart from BL21(DE3). The ED50 of BbFGF from Origami(DE3) and BL21(DE3) was 1.6 μg/L and 2.2 μg/L, respectively. Both HBscFv formed into inclusion body in the cytoplasm of M15[pQE-HBscFv] or Origami[pQE-HBscFv]. But the supernatant of Origami [pQE-HBscFv] lysate displayed weak bioactivity and its counterpart from M15[pQE-HBscFv] did not display any bioactivity. The soluble HBscFv in Origami[pQE-HBscFv] was purified to be 1-2 mg/L and its affinity constant was determined to be 2.62×107 mol/L. The yield of native HBscFv refolded from inclusion body in M15[pQE-HBscFv] was 30-35 mg/L and the affinity constant was 1.98×107 mol/L. There was no significant difference between the bioactivity of HBscFvs refolded from the inclusion bodies produced in different host strains. CONCLUSION: Modification of the redox environment of E(?)coli cytoplasm can significantly improve the folding of recombinant disulfide-bonded proteins produced in it.展开更多
Combining photocatalytic organic reactions with CO_(2)reduction is an efficient solar energy utilization mode,but it is still limited by the organic species that can be matched and the low conversion.Herein,ultrathin ...Combining photocatalytic organic reactions with CO_(2)reduction is an efficient solar energy utilization mode,but it is still limited by the organic species that can be matched and the low conversion.Herein,ultrathin organic polymer with p-πconjugated structure(TPP)was rationally designed and prepared,and showed a high yield of CO(15.2 mmol g^(-1))and conversion of SAS coupled products(100%),far exceeding the organic polymer with P=O structure.The enhanced photoredox activity of TPP is ascribed to the orbital interaction between the p-orbital on phosphorus and theπ-orbitals of aromatic,which can accelerate the photoinduced charge carrier separation and improve the CO_(2)adsorption capacity.TPP can also be used for the dehydrocoupling of various benzyl mercaptans to the corresponding SAS bond products.This work provides a new concept for the efficient synthesis of disulfide bonds combined with CO_(2)reduction in a photoreaction system.展开更多
Cysteine chemistry provides a low cost and convenient way for site-specific protein modification.However,recombinant expression of disulfide bonding containing protein with unpaired cysteine is technically challenging...Cysteine chemistry provides a low cost and convenient way for site-specific protein modification.However,recombinant expression of disulfide bonding containing protein with unpaired cysteine is technically challenging and the resulting protein often suffers from significantly reduced yield and activity.Here we used genetic code expansion technique to introduce a surface exposed self-paired dithiol functional group into proteins,which can be selectively reduced to afford active thiols.Two compounds containing self-paired disulfides were synthesized,and their genetic incorporations were validated using green fluorescent proteins(GFP).The compatibility of these self-paired di-thiols with natural disulfide bond was demonstrated using antibody fragment to afford site-specifically labeled antibody.This work provides another valuable building block into the chemical tool-box for site-specific labeling of proteins containing internal disulfides.展开更多
Enhancing the stability of biomolecules is one of the hot topics in industry.In this study,we enhanced the stability of an important protein called LEPTIN.LEPTIN is a hormone secreted by fat cells playing an essential...Enhancing the stability of biomolecules is one of the hot topics in industry.In this study,we enhanced the stability of an important protein called LEPTIN.LEPTIN is a hormone secreted by fat cells playing an essential role in body weight and composition,and its deficiency can result in several disorders.The treatment of related LEPTIN dysfunctions is often available in the form of injection.To decrease the cost and the frequency of its applications can be achieved by increasing its lifetime through engineering LEPTIN.In this study,to engineer LEPTIN,we have introduced disulfide bonds.Disulfide By Design server was used to predict the suitable nominate pairs,which suggested three pairs of amino acids to be mutated to cysteine for disulfide bond formation.Additionally,to further evaluate the effect of combined mutations,we combined these three nominated pairs to produce three more mutants.In order to assess the effect of introduced mutations,molecular dynamic(MD)simulation was performed.The result suggests that Mutant-1 is more stable in comparison to wild-type and the other mutants.Moreover,docking results showed that the introduced mutation does not affect the receptor binding performance;therefore,it can be considered a suitable choice for future protein engineering.展开更多
A prediction method of protein disulfide bond based on support vector machine and sample selection is proposed in this paper. First, the protein sequences selected are en-coded according to a certain encoding, input d...A prediction method of protein disulfide bond based on support vector machine and sample selection is proposed in this paper. First, the protein sequences selected are en-coded according to a certain encoding, input data for the prediction model of protein disulfide bond is generated;Then sample selection technique is used to select a portion of input data as training samples of support vector machine;finally the prediction model training samples trained is used to predict protein disulfide bond. The result of simulation experiment shows that the prediction model based on support vector ma-chine and sample selection can increase the prediction accuracy of protein disulfide bond.展开更多
Lost circulation of drilling fluid is an international engineering problem during drilling.Aiming at the problems of the first-time lost circulation control success rate and poor adaptability of traditional lost circu...Lost circulation of drilling fluid is an international engineering problem during drilling.Aiming at the problems of the first-time lost circulation control success rate and poor adaptability of traditional lost circulation materials,a new self-healing lost circulation material based on dynamic disulfide bonds was prepared and named CKSH.In this paper,the particle size of self-healing lost circulation material was from 0.1 to 5 mm.The structure was analyzed by modern characterization means,and the drilling fluid compatibility,self-healing performance were evaluated.The self-healing and bridging-filling-sealing mechanism of CKSH were revealed.The results showed that the healing rate of CKSH could reach100%after 12 h over 70℃.It showed good compatibility with drilling fluid,with no effect on rheology or filtration loss.It could be stably suspended in drilling fluid,and the temperature resistance reached140℃.Healing by self-healing lost circulation materials of different particle size,the pressure bearing capacity of plugging zone were over 12 MPa for fracture opening of 1–5 mm.It could play a synergistic role with traditional lost circulation materials by chemical bonding,and the repeated loss caused by physical plugging was avoided.The research results of this paper can improve the bridging plugging bearing pressure strength and the first-time lost circulation control success rate,which is of great significance for improving drilling efficiency and reducing non-productive time.展开更多
Neuregulin plays an important role in heart structure and function.Research discovered that recombinant neuregulin could reduce the degree of damage on myocardial cells caused by ischemia,hypoxia and viral infection.T...Neuregulin plays an important role in heart structure and function.Research discovered that recombinant neuregulin could reduce the degree of damage on myocardial cells caused by ischemia,hypoxia and viral infection.The primary structure,including N-terminal sequence,C-terminal sequence,PMF,accurate molecular mass,and disulfide bonding pattern of recombinant human neuregulin,have been identified by ESI-Q-TOF MS,Autoflex MALDI-TOF MS,9.4T Apex Q-FT MS and Ultraflex Ⅲ MALDI-TOF/TOF combining with two e]ymatic digestion.A abnormal peptide impurity in this drug was found and sequenced by Q-TOF MS and TOF/TOF MS,this is useful for the product quanlity control.展开更多
Polydimethylsiloxane(PDMS)is an electron-withdrawing material that is widely used in triboelectric nanogenerators(TENGs).However,PDMS has poor mechanical properties after curing and is easily damaged when subjected to...Polydimethylsiloxane(PDMS)is an electron-withdrawing material that is widely used in triboelectric nanogenerators(TENGs).However,PDMS has poor mechanical properties after curing and is easily damaged when subjected to long-term workloads.Thus,the long-term stable operation of TENGs under mechanical deformation cannot be guaranteed.In this work,multiple hydrogen bonds and aromatic disulfide bonds were introduced into PDMS elastomers.These elastomers exhibited high toughness(a tensile strength of 1.91 MPa and an elongation at break of 340%),good recyclability,and room-temperature self-healing properties(healing efficiency of 96.4%in 24 h).Recyclable sandwich-like triboelectric nanogenerators with excellent electrical output performance(13.5 V)and room-temperature self-healing performance(24 h,98%recovery of self-generating performance)were prepared by utilizing the hydrogen bonding between the PDMS elastomer and MXene.The work reported herein offers theoretical guidance and a compelling strategy for developing high-performance TENG negative friction layers.展开更多
基金supported by the National Natural Science Foundation of China(No.51873110)the Foundation of Guangdong Provincial Key Laboratory of Natural Rubber Processing and Key Laboratory of Carb on Fiber and Functio nal Polymers(Beijing University of Chemical Technology),Ministry of Educati on.
文摘Elastomers with outstanding strength,toughness and healing efficiency are highly promising for many emerging fields.However,it is still a challenge to integrate all these beneficial features in one elastomer.Herein,an asymmetric alicyclic structure adjacent to aromatic disulfide was tactfully introduced into the backbone of polyurethane(PU)elastomer.Specifically,such elastomer(PU-HPS)was fabricated by polycondensing polytetramethylene ether glycol(PTMEG),isophorone diisocyanate(IPDI)and p-hydroxydiphenyl disulfide(HPS)via one-pot method.The molecular mobility and phase morphology of PU-HPS can be tuned by adjusting the HPS content.Consequently,the dynamic exchange of hydrogen and disulfide bonds in the hard segment domains can also be tailored.The optimized sample manifests outstanding tensile strength(46.4 MPa),high toughness(109.1 MJ/m^(3)),high self-healing efficiency after fracture(90.3%),complete scratch recovery(100%)and good puncture resistance.Therefore,this work provides a facile strategy for developing robust self-healing polymers.
基金supported by R&D Program of Power Batteries with Low Temperature and High Energy,Science and Technology Bureau of Changchun(19SS013)Key Subject Construction of Physical Chemistry of Northeast Normal University+1 种基金the Fundamental Research Funds for the Central Universities(2412020FZ007,2412020FZ008)National Natural Science Foundation of China(22102020)
文摘The self-healing solid polymer electrolytes(SHSPEs)can spontaneously eliminate mechanical damages or micro-cracks generated during the assembly or operation of lithium-ion batteries(LIBs),significantly improving cycling performance and extending service life of LIBs.Here,we report a novel cross-linked network SHSPE(PDDP)containing hydrogen bonds and dynamic disulfide bonds with excellent self-healing properties and nonflammability.The combination of hydrogen bonding between urea groups and the metathesis reaction of dynamic disulfide bonds endows PDDP with rapid self-healing capacity at 28°C without external stimulation.Furthermore,the addition of 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide(EMIMTFSI)improves the ionic conductivity(1.13×10^(−4)S cm^(−1)at 28°C)and non-flammability of PDDP.The assembled Li/PDDP/LiFePO_(4)cell exhibits excellent cycling performance with a discharge capacity of 137 mA h g^(−1)after 300 cycles at 0.2 C.More importantly,the self-healed PDDP can recover almost the same ionic conductivity and cycling performance as the original PDDP.
基金Supported by the National Key Research and Development Plan of China(2019YFC1905902,2019YFC1905900)Key Research and Development Plan in Shandong Province(2020CXGC010603,2021ZDSYS10,2022CXGC020206)+2 种基金"Open Competition Mechanism"Project of Qilu University of Technology(Shandong Academy of Sciences)(2022JBZ01-06)Taishan Industry Leading Talent Program(tscy20180103)National Natural Science Foundation of China(31801527)。
文摘Each possible pair of residues inβ-1,4 glucanase for disulfide formation was assessed using online websites,and four pairs L28C-S256C,Q41C-P278C,S122C-N163C and A184C-A215C were selected.Accordingly,four recombinant plasmids pET28a(+)EccslH28,pET28a(+)EccslH41,pET28a(+)EccslH122 and pET28a(+)EccslH184 were prepared and transformed into E.coli to express the recombinant enzymes.Then analysis on enzymatic properties showed that T50 of the recombinant enzymes was increased from 10 min for EccslHt2 to 90 min for EccslH28 and 40 min for EccslH41 at 70℃,while their optimum pH value and pH stability were not affected,which proved that the introduction of disulfide bond improved the thermal stability ofβ-1,4 glucanase.
基金supported by the National Natural Science Foundation of China(91127026,11074115 and 61101056)the Open Project of State Key Laboratory of Bioelectronics of Southeast University(2011E14)supported by the Priority Academic Program Development of Jiangsu Higher Education Institutions
文摘Decorsin, an antagonist of integrin glycoprotein IIb/IIIa, contains Arg-Gly-Asp （RGD） sequence and three disulfide bridges. The function of RGD sequence has already been well defined, but the roles of conserved disulfide bonds in antihemostatic proteins still remain unclear. Herein we use the fusion expression and characterization of mutant decorsin to study the func- tions of disulfide bonds in protein structure, stability and biological activity. The purified protein shows an apparent inhibition of activity to platelet aggregation induced by ADP with IC50 of 500 nM. The removal of cys7-cysl5 （from cysteine to serine） at the N-terminal causes a thirty-fold decrease of the inhibition activity with IC50 of 15 ~tM, whereas the mutation of cys22-cys38 at the C-terminal completely impairs the biological activity of decorsin. The overall secondary and tertiary struc- tures of decorsin are disrupted inevitably without disulfide bonds. Using a domain insertion mutation, the retaining of RGD loop and the adjacent disulfide bond produces a week antihemostatic activity of decorsin. This reveals that the overall structure of decorsin stabilized by the three conserved disulfide bridges is cooperative for antihemostatic function. Our study on the ef- fect of disulfide bonds together with RGD-sequence on the protein function is helpful for structure-based drug design of an- tithrombotic research.
基金supported by the National Key R&D Program of China(No.2021YFA1200103)National Natural Science Foundation of China(Nos.11804170,22273041,91950116,and 11974217)+1 种基金Natural Science Foundation of Tianjin(Nos.19JCZDJC31000,19JCJQJC60900,and 22JCYBJC01310)Deutsche Forschungsgemeinschaft(DFG-German Research Foundation)through Project 406778771.
文摘Thanks to their excellent bond strength,phenyl-based molecules with thiol anchoring groups are extensively employed to form stable single-molecule junctions.However,two critical questions are still not answered which seriously hinder high-yield establishing reliable molecular functional devices:(1)Whether molecular dimer junctions will be formed,and if this is the case,whether the dimerization is caused by intermolecular disulfide bonds orπ–πstacking of phenyl rings;(2)Upon a mechanical-compression force,is it possible that both anchoring groups of the molecule bond to the same electrode instead of bridging two opposite electrodes,which would drastically reduce the yield of the molecular junctions.Here,combining UV-Vis/Raman spectroscopy of bulk molecules and conductance/flicker-noise measurements of single molecules,we give compelling evidence that molecular dimers naturally form under ambient conditions,primarily via disulfide bonds rather than byπ–πstacking.We further proposed a technique,named electrode-compression-hold-on(ECHO),and reveal that the two thiol groups of phenyl-backboned molecules will bond to the same electrode upon a compression force with a prolongated ECHO time.In contrast,the compression-time-dependent phenomenon is not observed for alkyl-backboned molecules.The underlying mechanism for these unprecedented observations is elucidated,shedding light on the yield of molecular junctions.
基金supported by the National Natural Science Foundation of China (21421004, 21777041, 21327807)the Program of Introducing Talents of Discipline to Universities (B16017)+1 种基金Innovation Program of Shanghai Municipal Education Commission (2017-0107-00-02-E00023)the Fundamental Research Funds for the Central Universities (222201718001, 222201717003)
文摘Monitoring subtle changes in ionic current flow through a nanopore could be applied to observe single molecule reaction. Here,we introduced cysteine to substitute for lysine at position 238 constructing a mutant aerolysin K238 C. It could be regarded as a nanoreactor to efficiently visualize chemical bonds making and breaking. The compound 5,5′-dithiobis-(2-nitrobenzoic acid)(DTNB) was selected as a reactant coming into collisions on the interface of the pore to occur a reversible reaction. Our results showed that the mutant aerolysin could respond to three molecules of DTNB simultaneously and reflect corresponding levels with distinguishable current signals. Therefore, this method constitutes a simple, generic tool for monitoring single molecule reaction, which evokes a guidance for the mutant aerolysin towards the application of tracking other more reactions at single molecule level.
基金financially supported by the National Natural Science Foundation of China(No.52377025)。
文摘The most widely used bisphenol A-type epoxy resin(DGEBA)in electrical engineering demonstrates excellent mechanical and electrical properties.However,the insoluble and infusible characteristics of cured DGEBA make it difficult to efficiently degrade and recycle decommissioned electrical equipment.In this study,a degradable itaconic acid-based epoxy resin incorporating dynamic covalent bonds was prepared through the integration of ester bonds and disulfide bonds,with itaconic acid as the precursor.The covalent bonding effects on the mechanical,thermal,electrical,and degradation characteristics were systematically evaluated.The experimental results revealed that the introduction of dynamic ester bonds enhanced the mechanical properties and thermal stability of the resin system,achieving a flexural strength of 141.57 MPa and an initial decomposition temperature T_(5%)of up to 344.9℃.The resin system containing dynamic disulfide bonds exhibited a dielectric breakdown strength of 41.11 k V/mm.Simultaneously,the incorporation of disulfide bonds endowed the epoxy resin with remarkable degradability,enabling complete dissolution within 1.5 h at 90℃ in a mixed solution of dithiothreitol(DTT)and N-methylpyrrolidone(NMP).This research provides a valuable reference for the application of itaconic acid-based vitrimer with dynamic covalent bonds in electrical materials,contributing to the development and utilization of environmentally friendly electrical equipment.
基金National Natural Science Foundation of China(Grant No.20332010)the Ministry of Science and Technology of China(Grant No.2005BA711A04,2006AA02Z144).
文摘In order to prepare pyrimidine nucleoside-peptide conjugate concisely, we developed a one-pot synthetic strategy. Started from uridine, 5-S-acetyl-thiomethyl-2＇,3 ＇-di-O-isopropylidene-uridine （4） was synthesized as the key intermediate in four steps. Under acidic condition, compound 4 was deprotected and reacted with PySS-R （8, 12, 15, Py = 2-pyridyl, R = amino acid or peptide） in one pot to form uridine conjugates （9, 13, 2） with disulfide bond as linker.
基金the Natural Science Foundation of Jiangxi Education Department(No.GJJ170680)the National Natural Science Foundation of China(Nos.51963010,21867011,and 51563011).
文摘Self-healing polymers based on dynamic crosslinkers have drawn rapidly increasing interest over the last decade.Here,a self-healable epoxy network with exchangeable disulfide bonds was synthesized by polymerizing two epoxies with an aromatic amine containing a disulfide bond.The bisphenol A diglycidyl ether(DGEBA)and poly(ethylene glycol)diglycidyl ether(DER736)were used as rigid and soft components,respectively.The crosslinking densities of studied polymers decreased with the increasing amount of DER736,resulting in the lower glassy temperature and weaker mechanical strength.The dynamic covalent network character of disulfide bond and its low active energy were also investigated through stress relaxation experiments at various temperatures.The self-healing performance of healable epoxy resins with varied flexibility was measured by tensile tests.The tensile strength of a full-cut sample was restored to 84%(13 MPa)of the initial values(16 MPa)at moderate temperature.Its healed fracture strain was up to 505%.Moreover,the effect of healing time and temperature on the self-healing properties was also studied.A model was proposed to investigate the self-repairing efficiency evolution with healing time,suggesting that hydrogen bonds mainly contributed to the initial sticking or interfacial adhesion while disulfide links and chain interdiffusion assisted time dependent reformation of networks to restore the original mechanical strength.
基金funding from the National Natural Science Foundation of China(No.81703451 and 81773656)the Excellent Youth Science Foundation of Liaoning Province(No.2020-YQ-06)+2 种基金the Liaoning Revitalization Talents Program(No.XLYC1808017 and XLYC1907129)the China Postdoctoral Science Foundation(No.2020M670794)the Science and Technology Major Project of Liaoning(No.2019JH1/10300004)。
文摘Disulfide bond-bridging strategy has been extensively utilized to construct tumor specificity-responsive aliphatic prodrug nanoparticles(PNPs) for precise cancer therapy. Yet, there is no research shedding light on the impacts of the saturation and cis-trans configuration of aliphatic tails on the self-assembly capacity of disulfide bond-linked prodrugs and the in vivo delivery fate of PNPs. Herein, five disulfide bond-linked docetaxelfatty acid prodrugs are designed and synthesized by using stearic acid, elaidic acid, oleic acid, linoleic acid and linolenic acid as the aliphatic tails, respectively. Interestingly, the cistrans configuration of aliphatic tails significantly influences the self-assembly features of prodrugs, and elaidic acid-linked prodrug with a trans double bond show poor self-assembly capacity. Although the aliphatic tails have almost no effect on the redox-sensitive drug release and cytotoxicity, different aliphatic tails significantly influence the chemical stability of prodrugs and the colloidal stability of PNPs, thus affecting the in vivo pharmacokinetics, biodistribution and antitumor efficacy of PNPs. Our findings illustrate how aliphatic tails affect the assembly characteristic of disulfide bond-linked aliphatic prodrugs and the in vivo delivery fate of PNPs, and thus provide theoretical basis for future development of disulfide bond-bridged aliphatic prodrugs.
基金financially supported by the National Natural Science Foundation of China(No.21774135)。
文摘Stimulus-responsive polymers containing dynamic bonds enable fascinating properties of self-healing,recycling and reprocessing due to enhanced relaxation of polymer chain/network with labile linkages.Here,we study the structure and properties of a new type of thermoplastic polyurethanes(TPUs)with trapped dynamic covalent bonds in the hard-phase domain and report the frustrated relaxation of TPUs containing weak dynamic bond andπ-πinteraction in hard segments.As detected by rheometry,the aromatic TPUs with alkyl disulfide in the hard segments possess the maximum network relaxation time in contrast to those without dynamic bonds and alicyclic TPUs.In situ FTIR and small-angle scattering results reveal that the alkyl disulfide facilitates stronger intermolecular interaction and more stable micro-phase morphology inπ-πinteraction based aromatic TPUs.Molecular dynamics simulation for pure hard segments of model molecules verify that the presence of disulfide bonds leads to strongerπ-πstacking of aromatic rings due to both enhanced assembling thermodynamics and kinetics.The enhancedπ-πpacking and micro-phase structure in TPUs further kinetically immobilize the dynamic bond.This kinetically interlocking between the weak dynamic bonds and strong molecular interaction in hard segments leads to much slower network relaxation of TPU.This work provides a new insight in tuning the network relaxation and heat resistance as well as molecular self-assembly in stimulus-responsive dynamic polymers by both molecular design and micro-phase control toward the functional applications of advanced materials.
基金financially supported by National Nature Science Foundation of China(No.81872816,81703451)Liaoning Revitalization Talents Program,No XLYC1808017+2 种基金Key projects of Technology bureau in Shenyang,No18400408Key projects of Liaoning Province Department of Education,No.2017LZD03supported by Heilongjiang Provincial Key Laboratory of Plant Genetic Engineering and Biological Fermentation Engineering for Cold Region。
文摘One of the major barriers in utilizing prodrug nanocarriers for cancer therapy is the slow release of parent drug in tumors.Tumor cells generally display the higher oxidative level than normal cells,and also displayed the heterogeneity in terms of redox homeostasis level.We previously found that the disulfide bond-linkage demonstrates surprising oxidationsensitivity to form the hydrophilic sulfoxide and sulphone groups.Herein,we develop oxidation-strengthened prodrug nanosystem loaded with pyropheophorbide a(PPa)to achieve light-activatable cascade drug release and enhance therapeutic efficacy.The disulfide bond-driven prodrug nanosystems not only respond to the redox-heterogeneity in tumor,but also respond to the exogenous oxidant(singlet oxygen)elicited by photosensitizers.Once the prodrug nanoparticles(NPs)are activated under irradiation,they would undergo an oxidative self-strengthened process,resulting in a facilitated drug cascade release.The IC50 value of the PPa@PTX-S-S NPs without irradiation was 2-fold higher than those of NPs plus irradiation.In vivo,the PPa@PTX prodrug NPs display prolonged systemic circulation and increased accumulation in tumor site.The PPa@PTXS-S NPs showed much higher efficiency than free PTX or the PPa@PTX-C-C NPs to suppress the growth of 4 T1 tumors.Therefore,this novel oxidation-strengthened disulfide-bridged prodrug-nanosystem has a great potential in the enhanced efficacy of cancer synergetic photochemotherapy.
基金Supported by the National Natural Science Foundation of China,No. 30371661 and No. 30400071and the Natural Science Foundation for Research Team of Guangdong Province, China, No. 2004E039213
文摘AIM: To study the influence of redox environment of Escherichia coli (E(?) coli) cytoplasm on disulfide bond formation of recombinant proteins. METHODS: Bovine fibrobllast growth factor (BbFGF) was selected as a model of simple proteins with a single disulfide bond and free cysteines. Anti-HBsAg single-chain Fv (HBscFv), an artificial multidomain protein, was selected as the model molecule of complex protein with 2 disulfide bonds. A BbFGF-producing plasmid, pJN-BbFGF, and a HBscFv producing-plasmid, pQE-HBscFv, were constructed and transformed into E(?)coli strains BL21(DE3) and M15[pREP4] respectively. At the same time, both plasmids were transformed into a reductase-deficient host strain,E(?)coli Origami(DE3). The 4 recombinant E(?)coli strains were cultured and the target proteins were purified. Solubility and bioactivity of recombinant BbFGF and HBscFv produced in different host strains were analyzed and compared respectively. RESULTS: All recombinant E(?)coli strains could efficiently produce target proteins. The level of BbFGF in BL21(DE3) was 15-23% of the total protein, and was 5-10% in Origami (DE3). In addition, 65% of the BbFGF produced in BL21(DE3) formed into inclusion body in the cytoplasm, and all the target proteins became soluble in Origami (DE3). The bioactivity of BbFGF purified from Origami(DE3) was higher than its counterpart from BL21(DE3). The ED50 of BbFGF from Origami(DE3) and BL21(DE3) was 1.6 μg/L and 2.2 μg/L, respectively. Both HBscFv formed into inclusion body in the cytoplasm of M15[pQE-HBscFv] or Origami[pQE-HBscFv]. But the supernatant of Origami [pQE-HBscFv] lysate displayed weak bioactivity and its counterpart from M15[pQE-HBscFv] did not display any bioactivity. The soluble HBscFv in Origami[pQE-HBscFv] was purified to be 1-2 mg/L and its affinity constant was determined to be 2.62×107 mol/L. The yield of native HBscFv refolded from inclusion body in M15[pQE-HBscFv] was 30-35 mg/L and the affinity constant was 1.98×107 mol/L. There was no significant difference between the bioactivity of HBscFvs refolded from the inclusion bodies produced in different host strains. CONCLUSION: Modification of the redox environment of E(?)coli cytoplasm can significantly improve the folding of recombinant disulfide-bonded proteins produced in it.
基金the financial support of the research fund of the Science and Technology Innovation Program of Hunan Province(2020RC2076)the General Project of Education Department of Hunan Province(21C008)+2 种基金the Open Research Fund of School of Chemistry and Chemical Engineering,Henan Normal University(2022C02)the Youth Science and Technology Talent Project of Hunan Province(2022RC1197)the Hunan Provincial Natural Science Foundation of China(2021JJ40529)。
文摘Combining photocatalytic organic reactions with CO_(2)reduction is an efficient solar energy utilization mode,but it is still limited by the organic species that can be matched and the low conversion.Herein,ultrathin organic polymer with p-πconjugated structure(TPP)was rationally designed and prepared,and showed a high yield of CO(15.2 mmol g^(-1))and conversion of SAS coupled products(100%),far exceeding the organic polymer with P=O structure.The enhanced photoredox activity of TPP is ascribed to the orbital interaction between the p-orbital on phosphorus and theπ-orbitals of aromatic,which can accelerate the photoinduced charge carrier separation and improve the CO_(2)adsorption capacity.TPP can also be used for the dehydrocoupling of various benzyl mercaptans to the corresponding SAS bond products.This work provides a new concept for the efficient synthesis of disulfide bonds combined with CO_(2)reduction in a photoreaction system.
基金financially supported by National Key Research and Development Program of China (No.2016YFA0201400)the National Natural Science Foundation of China (No.21778005)+1 种基金Peking University Health Science Center (Nos.BMU20160537 andBMU2017QQ006)the Youth Thousand-Talents Program of China for support
文摘Cysteine chemistry provides a low cost and convenient way for site-specific protein modification.However,recombinant expression of disulfide bonding containing protein with unpaired cysteine is technically challenging and the resulting protein often suffers from significantly reduced yield and activity.Here we used genetic code expansion technique to introduce a surface exposed self-paired dithiol functional group into proteins,which can be selectively reduced to afford active thiols.Two compounds containing self-paired disulfides were synthesized,and their genetic incorporations were validated using green fluorescent proteins(GFP).The compatibility of these self-paired di-thiols with natural disulfide bond was demonstrated using antibody fragment to afford site-specifically labeled antibody.This work provides another valuable building block into the chemical tool-box for site-specific labeling of proteins containing internal disulfides.
基金supported by China Postdoctoral Science Foundation Grant(2019M661742).
文摘Enhancing the stability of biomolecules is one of the hot topics in industry.In this study,we enhanced the stability of an important protein called LEPTIN.LEPTIN is a hormone secreted by fat cells playing an essential role in body weight and composition,and its deficiency can result in several disorders.The treatment of related LEPTIN dysfunctions is often available in the form of injection.To decrease the cost and the frequency of its applications can be achieved by increasing its lifetime through engineering LEPTIN.In this study,to engineer LEPTIN,we have introduced disulfide bonds.Disulfide By Design server was used to predict the suitable nominate pairs,which suggested three pairs of amino acids to be mutated to cysteine for disulfide bond formation.Additionally,to further evaluate the effect of combined mutations,we combined these three nominated pairs to produce three more mutants.In order to assess the effect of introduced mutations,molecular dynamic(MD)simulation was performed.The result suggests that Mutant-1 is more stable in comparison to wild-type and the other mutants.Moreover,docking results showed that the introduced mutation does not affect the receptor binding performance;therefore,it can be considered a suitable choice for future protein engineering.
文摘A prediction method of protein disulfide bond based on support vector machine and sample selection is proposed in this paper. First, the protein sequences selected are en-coded according to a certain encoding, input data for the prediction model of protein disulfide bond is generated;Then sample selection technique is used to select a portion of input data as training samples of support vector machine;finally the prediction model training samples trained is used to predict protein disulfide bond. The result of simulation experiment shows that the prediction model based on support vector ma-chine and sample selection can increase the prediction accuracy of protein disulfide bond.
基金supported by National Natural Science Foundation of China(52304006,52274032,and 51774062)the General Project of the Chongqing Natural Science Foundation(CSTB2022NSCQ-MSX1554 and CSTB2022NSCQ-MSX0349)Shaanxi Province Key Laboratory of Environmental Pollution Control and Reservoir Protection Technology of Oilfields and Engineering Research Center of Oil and Gas Field Chemistry,Universities of Shaanxi Province(XSYU-CCCE-2402).
文摘Lost circulation of drilling fluid is an international engineering problem during drilling.Aiming at the problems of the first-time lost circulation control success rate and poor adaptability of traditional lost circulation materials,a new self-healing lost circulation material based on dynamic disulfide bonds was prepared and named CKSH.In this paper,the particle size of self-healing lost circulation material was from 0.1 to 5 mm.The structure was analyzed by modern characterization means,and the drilling fluid compatibility,self-healing performance were evaluated.The self-healing and bridging-filling-sealing mechanism of CKSH were revealed.The results showed that the healing rate of CKSH could reach100%after 12 h over 70℃.It showed good compatibility with drilling fluid,with no effect on rheology or filtration loss.It could be stably suspended in drilling fluid,and the temperature resistance reached140℃.Healing by self-healing lost circulation materials of different particle size,the pressure bearing capacity of plugging zone were over 12 MPa for fracture opening of 1–5 mm.It could play a synergistic role with traditional lost circulation materials by chemical bonding,and the repeated loss caused by physical plugging was avoided.The research results of this paper can improve the bridging plugging bearing pressure strength and the first-time lost circulation control success rate,which is of great significance for improving drilling efficiency and reducing non-productive time.
文摘Neuregulin plays an important role in heart structure and function.Research discovered that recombinant neuregulin could reduce the degree of damage on myocardial cells caused by ischemia,hypoxia and viral infection.The primary structure,including N-terminal sequence,C-terminal sequence,PMF,accurate molecular mass,and disulfide bonding pattern of recombinant human neuregulin,have been identified by ESI-Q-TOF MS,Autoflex MALDI-TOF MS,9.4T Apex Q-FT MS and Ultraflex Ⅲ MALDI-TOF/TOF combining with two e]ymatic digestion.A abnormal peptide impurity in this drug was found and sequenced by Q-TOF MS and TOF/TOF MS,this is useful for the product quanlity control.
基金supported by the National Key Research and Development Program of China(No.2023YFB2407100)the National Natural Science Foundation of China(No.52173080)。
文摘Polydimethylsiloxane(PDMS)is an electron-withdrawing material that is widely used in triboelectric nanogenerators(TENGs).However,PDMS has poor mechanical properties after curing and is easily damaged when subjected to long-term workloads.Thus,the long-term stable operation of TENGs under mechanical deformation cannot be guaranteed.In this work,multiple hydrogen bonds and aromatic disulfide bonds were introduced into PDMS elastomers.These elastomers exhibited high toughness(a tensile strength of 1.91 MPa and an elongation at break of 340%),good recyclability,and room-temperature self-healing properties(healing efficiency of 96.4%in 24 h).Recyclable sandwich-like triboelectric nanogenerators with excellent electrical output performance(13.5 V)and room-temperature self-healing performance(24 h,98%recovery of self-generating performance)were prepared by utilizing the hydrogen bonding between the PDMS elastomer and MXene.The work reported herein offers theoretical guidance and a compelling strategy for developing high-performance TENG negative friction layers.
