Formulating oil-based drilling fluids(OBDFs)with an ultra-low oil-to-water ratio(OWR≤60:40)presents a formidable stability challenge due to the maximized interfacial area and intensified stress on the interfacial fil...Formulating oil-based drilling fluids(OBDFs)with an ultra-low oil-to-water ratio(OWR≤60:40)presents a formidable stability challenge due to the maximized interfacial area and intensified stress on the interfacial film under high-temperature,high-density conditions.To address this,we engineered a synergistic stabilization system through molecular and colloidal design.A novel hyperbranched polyamide emulsifier(epoxidized soybean oil polyamide)(ESOP),synthesized from epoxidized soybean oil,exhibits superior thermal stability and interfacial activity due to its hyperbranched architecture.Combined with calcium petroleum sulfonate(CPS)and hydrophobic nanosilica(HNs),it enables a high-performance OBDF with an ultra-low OWR of 60:40.The results show that the optimized formula achieves an excellent demulsification voltage of 1290 V,an ultra-low HTHP fluid loss of 1.5 mL,a yield point of 12.9 Pa,and a superior sag factor(SF)of 0.504,outperforming both base and commercial systems.Mechanistic studies reveal a multiscale stabilization strategy involving a dense composite interfacial film,Pickering stabilization,a 3D network,and a unique thermally triggered self-reinforcement effect.This work not only provides a cost-effective OBDF formulation but,more importantly,establishes a molecular topology engineering paradigm for stabilizing complex industrial fluids under extreme conditions.展开更多
RNA binding proteins(RBPs) are a crucial class of proteins that interact with RNA and play a key role in various biological process.Deficiencies or abnormalities of RBPs are closely linked to the occurrence and progre...RNA binding proteins(RBPs) are a crucial class of proteins that interact with RNA and play a key role in various biological process.Deficiencies or abnormalities of RBPs are closely linked to the occurrence and progression of numerous diseases,making RBPs potential therapeutic targets.However,the limited tissue penetration of 254 nm UV irradiation makes it difficult to efficiently crosslink weak and dynamic RNA-protein interactions in mammal tissues.Additionally,RNA degradation in metal catalyzed click reaction further hinders the enrichment of RNA-protein complexes(RPCs).Due to these inherent limitations,globally profiling the RNA binding proteome in mammal organs has long been a challenge.Herein,we proposed a novel method,which utilized a dual crosslinking with formaldehyde and 254 nm UV irradiation,metabolic labeling and metal-free thiol-yne click reaction to enable large-scale enrichment and identification of RBPs in mouse liver,called FTYc_UV.In this method,formaldehyde is first used to crosslink the crude RNA-protein complexes(cRPCs) in situ to address the problem of poor tissue penetration of 254 nm UV irradiation.Furthermore,this method integrates metabolic labeling with a metal-free thiol-yne click reaction to achieve non-destructive RNA tagging.After specifically RNA-RBPs crosslinking by 254 nm UV irradiation in tissue lysates,formaldehyde decrosslinking is employed to remove non-specific proteins,leading to effective enrichment of RPCs from mouse liver and thereby overcoming the poor specificity of formaldehyde crosslinking.Application of FTYc_UV in mouse liver successfully identified over 1600 RBPs covering approximately 75 % of previously reported RBPs.Furthermore,420 candidate RBPs,including 151metabolic enzymes,were also obtained,demonstrating the sensitivity of FTYc_UV and the potential of this method for in-depth exploration of RNA-protein interactions in biological and clinical research.展开更多
In-situ poly(1,3-dioxolane)(PDOL)-based electrolyte has received extensive attention in the research of lithium metal batteries due to its high stability to lithium anode and simple processing.However,it is still face...In-situ poly(1,3-dioxolane)(PDOL)-based electrolyte has received extensive attention in the research of lithium metal batteries due to its high stability to lithium anode and simple processing.However,it is still faced with defects such as low intrinsic ionic conductivity,a narrow electrochemical window,and poor thermal stability.A crosslinking and fluorination molecular design strategy toward PDOL is proposed to tackle the issues above.The amorphous crosslinked structure effectively improves ionic conductivity by inhibiting long-chain crystallization.Especially,the antioxidant–CF_(3)groups,stable crosslinked structure,and reduced terminal hydroxyl groups significantly enhance the electrochemical oxidation stability with a superb high-voltage window of 4.7 V.In addition,the designed electrolyte also exhibits obviously improved thermal stability with no deformation at 120°C for 5 min.Furthermore,the semi-solid NCM811||Li batteries exhibit a favourable capacity retention of 88.8%after 150 cycles at 0.5 C.Even assembled with NCM622 cathode working at 4.5 V,the semi-solid batteries can still show a satisfactory capacity retention of 85.3%after 100 cycles at 0.5 C.Also,a 0.1 Ah NCM811||Li pouch cell with active materials loading of 9 mg/cm2 demonstrates satisfactory cycling stability and working ability,which shows promising practical application prospects.展开更多
With the continuous advancement of social technology and the increasing awareness of health management,biomass-based triboelectric nanogenerator(TENG)displayed significant potential as flexible wearable electronics fo...With the continuous advancement of social technology and the increasing awareness of health management,biomass-based triboelectric nanogenerator(TENG)displayed significant potential as flexible wearable electronics for continuous foot gait monitoring.Nevertheless,existing biomass-based TENG often faces challenges of insufficient mechanical robustness and durability in practical applications,where they are prone to surface abrasion and structural fracture under continuous compression and friction,severely limiting their long-term performances.In order to address these challenges,this work proposed a multiscale crosslinking strategy,which strengthened the noncovalent interactions within the polymer by constructing multiple reinforcement networks,successfully fabricating a dual-network C-lignin-based triboelectric material(CLTM)with excellent durability and crack resistance.Among them,the optimal CLTM(PSGCL-0.2)exhibited high mechanical strength(strain 445%,tensile strength 41.56 MPa,Young's modulus 41.25 MPa,toughness 159.67 MJ/m^(3))and excellent cyclic stability(300 cycles)with versatile functionalities,including antibacterial,antioxidant,and UV-shielding properties,water stabilization(255.51 g/m^(2)/d),efficient photothermal conversion,and full recyclability.Furthermore,biomass-based TENG device assembled from PSGCL-0.2 achieved stable triboelectric output properties(102.5 V,2.9μA,and 61.3 nC),and sustainable for 2000 cycles,fast response time(68 ms),and excellent power density(325.9 mW/m^(2)),effectively converting mechanical energy into electrical energy.Especially,PSGCL 0.2 was also integrated into the wireless self-powered smart insole,successfully enabling real-time visual monitoring of plantar pressure distribution and dynamic gait.Meanwhile,combined with the machine learning algorithm,the self-powered smart insole achieved precise recognition and classification of eight different motion states with an accuracy of 98%.This study provides the feasible strategy for developing extremely stable and durable biomass-based TENG,aimed at advancing sustainable intelligent healthcare systems.展开更多
As the most abundant aromatic bio-based polymer,lignin has great potential as a sustainable feedstock for building crosslinked thermoset polymers as bio-based adhesives.However,the potential of hardwood kraft lignin(H...As the most abundant aromatic bio-based polymer,lignin has great potential as a sustainable feedstock for building crosslinked thermoset polymers as bio-based adhesives.However,the potential of hardwood kraft lignin(HKL)is limited due to its poor crosslinking reactivity.Hence,for the first time,the present study reports the facile oxidation of HKL involving a redox reaction with silver-ammonia complexes([(AgNH3)2]+),primarily focusing on oxidation to produce reactive quinones and promote C-C linkages during reaction.This study aims to increases reactivity of oxidized HKL for effective crosslinking with monoethanolamine(MEA)for the development of bio-based wood adhesives.The characterization,including 13C-nuclear magnetic resonance(NMR)and Fourier transform infrared(FT-IR)spectroscopy,confirms the oxidation reaction,such as the formation of quinones(C=O)and subsequent crosslinking between the oxidized HKL molecules and MEA.Additionally,gel permeation chromatography(GPC)confirms the C-C and C-O linkages with increased molecular weight after oxidation,and is supported by differential scanning calorimetry(DSC)which shows the exothermic reaction due to the crosslinking of the oxidized HKL molecules via condensation to form C-C and C-O linkages.The crosslinked HKL/MEA-based adhesives underwent mild reaction and achieved a maximum dry shear strength of 0.77 MPa,which exceeds the standard requirement of 0.6 MPa.These findings demonstrate not only a one-pot oxidation for improving the reactivity of HKL using silver complexes,but also its facile crosslinking with MEA for sustainable bio-based wood adhesives.展开更多
To address the issue of uneven temperature distribution in shale gas oil-based drill cuttings pyrolysis furnaces,a numerical model was developed using Fluent software.The effects of nitrogen flow rate,heating tube spa...To address the issue of uneven temperature distribution in shale gas oil-based drill cuttings pyrolysis furnaces,a numerical model was developed using Fluent software.The effects of nitrogen flow rate,heating tube spacing,and furnace dimensions on the internal temperature field were thoroughly analyzed from a mechanistic perspective.The results indicated that non-uniform radiation from the heating tubes and flow disturbances induced by the nitrogen stream were the primary causes of localized heat concentration.Under no-load conditions,the maximum deviation between simulated and on-site measured temperatures was 1.5%,validating the model’s accuracy.Further-more,this study investigated the trade-offs between temperature uniformity,energy consumption,and construction costs.The findings provide a crucial design basis and a reliable simulation platform for developing and optimizing pyrolysis equipment.展开更多
The oil-based mud(OBM) borehole measurement environment presents significant limitations on the application of existing electrical logging instruments in high-resistance formations. In this paper, we propose a novel l...The oil-based mud(OBM) borehole measurement environment presents significant limitations on the application of existing electrical logging instruments in high-resistance formations. In this paper, we propose a novel logging method for detection of high-resistance formations in OBM using highfrequency electrodes. The method addresses the issue of shallow depth of investigation(DOI) in existing electrical logging instruments, while simultaneously ensuring the vertical resolution. Based on the principle of current continuity, the total impedance of the loop is obtained by equating the measurement loop to the series form of a capacitively coupled circuit. and its validity is verified in a homogeneous formation model and a radial two-layer formation model with a mud standoff. Then, the instrument operating frequency and electrode system parameters were preferentially determined by numerical simulation, and the effect of mud gap on impedance measurement was investigated. Subsequently, the DOI of the instrument was investigated utilizing the pseudo-geometric factor defined by the real part of impedance. It was determined that the detection depth of the instrument is 8.74 cm, while the effective vertical resolution was not less than 2 cm. Finally, a focused high-frequency electrode-type instrument was designed by introducing a pair of focused electrodes, which effectively enhanced the DOI of the instrument and was successfully deployed in the Oklahoma formation model. The simulation results demonstrate that the novel method can achieve a detection depth of 17.40 cm in highly-resistive formations drilling with OBM, which is approximately twice the depth of detection of the existing oil-based mud microimager instruments. Furthermore, its effective vertical resolution remains at or above 2 cm,which is comparable to the resolution of the existing OBM electrical logging instrument.展开更多
Reader proteins that bind specific methyllysine are important to biological functions of lysine methylation,but readers of many methyllysine sites are still unknown.Therefore,development of covalent probes is importan...Reader proteins that bind specific methyllysine are important to biological functions of lysine methylation,but readers of many methyllysine sites are still unknown.Therefore,development of covalent probes is important to identify readers from cell samples so as to understand biological roles of lysine methylation.Generally,readers bind methyllysine via aromatic cages that contain tryptophan,tyrosine and phenylalanine,that offer a unique motif for selective crosslinking.We recently reported a site-selective tryptophan crosslinking strategy based on dimethylsulfonium that mimics dimethyllysine to crosslink tryptophan in aromatic cages of readers.Since tyrosine is a key residue for binding affinity to methyllysine,especially some readers that do not contain tryptophan residues in the binding pocket.Here we developed strategies of site-selective crosslinking to tyrosine.Ultraviolet(UV)source was applied to excite tyrosine at neutral pH or phenoxide at basic p H,and subsequent single-electron transfer(SET)from Tyr*to sulfonium inside the binding pocket enables selective crosslinking.In consequence,methyllysine readers with tyrosine-containing aromatic cages could be selectively crosslinked by site-specific sulfonium peptide probes.In addition,we expanded substrates from aromatic cages to tyrosine residues of proximate contact with sulfonium probes.The pair of LgBiT and SmBiT exhibited orthogonal crosslinking in complicated cell samples.As a result,we may expand sulfonium tools to target local tyrosine in future investigations.展开更多
Two-dimensional(2D) nanomaterials have always been regarded as having great development potential in the field of oil-based lubrication due to their designable structures,functional groups,and abundant active sites.Ho...Two-dimensional(2D) nanomaterials have always been regarded as having great development potential in the field of oil-based lubrication due to their designable structures,functional groups,and abundant active sites.However,understanding the structure-performance relationship between the chemical structure of 2D nanomaterials and their lubrication performance from a comprehensive perspective is crucial for guiding their future development.This review provides a timely and comprehensive overview of the applications of 2D nanomaterials in oil-based lubrication.First,the bottlenecks and mechanisms of action of 2D nanomaterials are outlined,including adsorption protective films,charge adsorption effects,tribochemical reaction films,interlayer slip,and synergistic effects.On this basis,the review summarizes recent structural regulation strategies for 2D nanomaterials,including doping engineering,surface modification,structural optimization,and interfacial mixing engineering.Then,the focus was on analyzing the structure-performance relationship between the chemical structure of 2D nanomaterials and their lubrication performance.The effects of thickness,number of layers,sheet diameter,interlayer spacing,Moiré patterns,wettability,functional groups,concentration,as well as interfacial compatibility and dispersion behavior of 2D nanomaterials were systematically investigated in oil-based lubrication,with the intrinsic correlations resolved through computational simulations.Finally,the review offers a preliminary summary of the significant challenges and future directions for 2D nanomaterials in oil-based lubrication.This review aims to provide valuable insights and development strategies for the rational design of high-performance oil-based lubrication materials.展开更多
BACKGROUND Oil-based iodinated contrast media have excellent contrast properties and are widely used for hysterosalpingographic evaluation of female infertility.On abdominal radiography and computed tomography(CT)scan...BACKGROUND Oil-based iodinated contrast media have excellent contrast properties and are widely used for hysterosalpingographic evaluation of female infertility.On abdominal radiography and computed tomography(CT)scans,their radiodensity is similar to that of metallic objects,which can sometimes lead to diagnostic confusion in the postoperative settings.In this case,retained oil-based contrast medium was observed on an abdominal radiograph following a cesarean section,making it difficult to differentiate from an intraperitoneal foreign body from surgery.The patient was a 37-year-old pregnant woman who was referred to our hospital at 32 weeks and 1 day of pregnancy due to complete placenta previa for mana-gement of pregnancy and delivery.An elective cesarean section was performed at 37 weeks and 3 days.A plain abdominal radiograph taken immediately after surgery revealed a near-round,hyperdense,mass-like shadow with a regular margin in the pelvic cavity.An intraperitoneal foreign body was suspected;therefore,an abdominal CT scan was performed.The foreign body was located on the left side of the pouch of Douglas and had a CT value of 7000 Hounsfield units,similar to that of metals.The CT value strongly suggested the presence of an artificial object.However,further inquiries with the patient and her previous physician revealed a history of hysterosalpingography.Accordingly,retained oil-based iodinated contrast medium was suspected,and observation of the object’s course was adopted.CONCLUSION When intraperitoneal foreign bodies are suspected on postoperative radiographs,the possibility of oil-based iodinated contrast medium retention should be considered.展开更多
Poly(vinyl alcohol)(PVA)hydrogels have garnered significant attention for tissue engineering,wound dressing,and electronic skin sensing applications.However,their poor mechanical performance severely restricts their m...Poly(vinyl alcohol)(PVA)hydrogels have garnered significant attention for tissue engineering,wound dressing,and electronic skin sensing applications.However,their poor mechanical performance severely restricts their multifunctional application in many scenarios.To address this limitation,PVA/tannic acid(TA)@carbon nanotubes(PVA/TA@CNTs)composite hydrogels with triple crosslinking networks were prepared through freezing-thawing and the solvent-induced shrinkage method,utilizing tannic acid-carbon nanotubes(TA@CNTs)as reinforcing units and a Ca^(2+)crosslinking strategy.The enhanced interfacial networks consisting of PVA crystalline domains,hydrogen bonding,and metal coordination endowed the composite hydrogel with a high mechanical strength,excellent flexibility,and fracture toughness,accompanied by a significant increase in crystallinity.The tensile strength and fracture toughness of the composite hydrogel reached up to about 7.0 MPa and 17.0MJ/m^(3),which were roughly 8 and 10 times higher than those of neat PVA hydrogel,respectively.The composite hydrogel demonstrated good cytocompatibility,significantly addressing the challenge of balancing structural reinforcement with biosafety in hydrogels.This methodology establishes a rational design for fabricating mechanically robust yet tough PVA hydrogels for biomedical applications.展开更多
Hydrogels are widely used in reservoir flow control to enhanced oil recovery.However,challenges such as environmental contamination from conventional crosslinkers,poor solubility of crosslinking agents,and short gelat...Hydrogels are widely used in reservoir flow control to enhanced oil recovery.However,challenges such as environmental contamination from conventional crosslinkers,poor solubility of crosslinking agents,and short gelation times under high-temperature conditions(e.g.,150℃)have hindered their practical application.Herein,we present the synthesis of amine-functionalized carbon quantum dots(NH_(2)-CQDs),which act as both a nano-crosslinker and a nano-reinforcing agent within hydrogel systems.The NH_(2)-CQDs-incorporated hydrogel can remain stability for 300 days under the conditions of a mineralization degree of 2.11×10^(4)mg/mL and 170℃,and has high tensile strength(371 kPa),good toughness(49.6 kJ/m^(3)),excellent viscoelasticity(G'=960 Pa,G"=460 Pa)and shear resistance.In addition,NH_(2)-CQDs adds many hydroxyl groups to the hydrogel,which can be attached to the surface of various substances.At the same time,micro-nano capsules containing NH_(2)-CQDs were formed by self-assembly of hydrophobic SiO_(2)on water droplets,the NH_(2)-CQDs solution is encapsulated in a capsule,and when stimulated by external conditions(temperature,pH,surfactant),the capsule releases the NH_(2)-CQDs solution,this method greatly delays the crosslinking time between polymer and crosslinker at high temperature.Under the condition of 170℃and pH=7,the gelation time of 10%hydrophobic SiO_(2)coated hydrogel is 44 times that of uncoated hydrogel,which can be effectively used for deep formation flow control,and CQD give hydrogels fluorescence properties that can be used for underground signal tracking.展开更多
Inorganic CsPbI_(3)perovskite with superior thermal stability and photoelectric properties has developed into a promising candidate for photovoltaic applications.Nevertheless,the power conversion efficiency(PCE)of CsP...Inorganic CsPbI_(3)perovskite with superior thermal stability and photoelectric properties has developed into a promising candidate for photovoltaic applications.Nevertheless,the power conversion efficiency(PCE)of CsPbI_(3)perovskite solar cells(PSCs)still lags far behind that of both organic-inorganic hybrid counterparts and the theoretical PCE limit,primarily restricted by severe fill factor(FF)and opencircuit voltage(VOC)deficits.Herein,an in-situ self-crosslinking strategy is proposed to construct high-performance inverted inorganic PSCs by incorporating acrylate monomers as additives into CsPbI_(3)perovskite precursors.During the thermal annealing process of perovskite films,acrylate monomers can form network structures by breaking the C=C groups through an in-situ polymerization reaction,mainly anchored at the grain boundaries(GBs)and on the surfaces of perovskite.Meanwhile,the C=O groups of acrylate polymers can favorably coordinate with uncoordinated Pb^(2+),thereby decreasing defect density and stabilizing the perovskite phase.Particularly,with multiple crosslinking and passivation sites,the incorporation of dipentaerythritol pentaacrylate(DPHA)can effectively improve the perovskite film quality,suppress nonradiative recombination,and block moisture erosion.Consequently,the DPHAbased PSC achieves a champion PCE of 20.05%with a record-high FF of 85.05%,both of which rank among the top in the performance of inverted CsPbI_(3)PSCs.Moreover,the unencapsulated DPHA-based device exhibits negligible hysteresis,remarkably improved long-term storage,and operational stability.This work offers a facile and useful strategy to simultaneously promote the efficiency and device stability of inverted inorganic PSCs.展开更多
Elastic electronics are increasingly prevalent in information storage,smart sensing and health monitoring due to their softness,stretchability and portability.Wearable electronic devices should possess elasticity and ...Elastic electronics are increasingly prevalent in information storage,smart sensing and health monitoring due to their softness,stretchability and portability.Wearable electronic devices should possess elasticity and stretchability that align with biological tissues.Specifically,their materials should be capable of elastic strain up to 50–80%,while the devices themselves must maintain electric stability under strains that accommodate body movements[1].展开更多
All-safe liquid-state lithium-ion batteries(ASLS-LIBs) is of great interest as they can potentially combine the safety of all-solid-state batteries with the high performance and low manufacturing cost of traditional l...All-safe liquid-state lithium-ion batteries(ASLS-LIBs) is of great interest as they can potentially combine the safety of all-solid-state batteries with the high performance and low manufacturing cost of traditional liquid-state LIBs. However, the practical success of ASLS-LIBs is bottlenecked by the lack of advanced separator technology that can simultaneously realize high performances in puncturing-tolerability,fire-resistance, and importantly, wetting-capability with non-flammable liquid-electrolytes. Here, we propose a concept of inorganic in-situ separator(IISS) by hybrid-sol physical crosslinking directly onto the electrode surface to address the above challenges. Particularly, the hybrid-sol is designed with silica nanoparticles as the building block and poly(vinylidene difluoride) nanoparticles as the crosslinking agent. The critical factors for controlling the IISS microstructures and properties have been systematically investigated. The advantages of the IISS have been confirmed by its fast wetting with various fireresistant liquid-electrolytes, customizable thickness and porous structures, robust interface with planar or three-dimensional(3D)-structured electrodes, and importantly, unexpected self-adaptability against puncturing. Enabled by the above merits, a fire-resistant ASLS-LIB is successfully assembled and demonstrated with stable electrochemical performance. This sol-crosslinked IISS may open an avenue for the studies on the next-generation separator technology, cell assembling, solid electrolyte processing as well as non-flammable secondary batteries.展开更多
AIM:To assess the visual outcomes and corneal biomechanical properties of myopia patients between laser in situ keratomileusis(LASIK)and LASIK combined with accelerated corneal crosslinking(LASIK Xtra).METHODS:This pr...AIM:To assess the visual outcomes and corneal biomechanical properties of myopia patients between laser in situ keratomileusis(LASIK)and LASIK combined with accelerated corneal crosslinking(LASIK Xtra).METHODS:This prospective study analyzed 52 consecutive myopia patients treated with LASIK Xtra and 45 consecutive myopia patients treated with LASIK.Only the right eyes in the two groups were analyzed.The uncorrected distance visual acuity(UDVA),keratometry values,postoperative central corneal thickness(CCT),corneal demarcation line depth,the corneal compensated intraocular pressure(IOPcc),Goldmann-correlated IOP(IOPg),corneal resistance factor(CRF)and corneal hysteresis(CH)from Ocular Response Analyzer(ORA)were analyzed.Further,the correlation between the demarcation line depth and ORA-related biomechanical parameters were analyzed.RESULTS:No significant differences in UDVA,postoperative CCT,or mean K values were found between the 2 groups at 1 to 12mo postoperative follow-up(all P>0.05).The changes of CRF was significantly lower in the LASIK Xtra group compared to the LASIK group(all P<0.05)at all the postoperative visits.The changes of CH were significantly higher in the LASIK Xtra group(all P<0.05).No significant differences were discovered regarding the changes of IOPcc and IOPg posperatively(all P>0.05).Out of 52 cases in the LASIK Xtra group,the demarcation line was present in 40 eyes(77%).The average depth of the demarcation was 220.73±42.70μm(136 to 288μm).No significant correlation was observed between the depth of the demarcation line and any of the ORA-related biomechanical parameters such as IOPcc,IOPg,CRF and CH at 12mo(all P>0.05).CONCLUSION:Both procedures demonstrate comparable outcomes in terms of visual acuity,refraction and ablation predictability.This study confirms that corneal biomechanical properties of the included patients weakened after both procedures,but the cornea after LASIK Xtra are stiffer than conventional LASIK.展开更多
The development of solar-driven interfacial evaporation technology is pivotal for addressing global water scarcity.However,it is hindered by the difficulty in synergizing high photothermal conversion with low water ev...The development of solar-driven interfacial evaporation technology is pivotal for addressing global water scarcity.However,it is hindered by the difficulty in synergizing high photothermal conversion with low water evaporation enthalpy into a single material.Herein,we propose an iron-aldehyde-cooperative dynamic covalent anchoring strategy,successfully constructing a covalently locked,hydroxymethyl-functionalized PEDOT-PVA integrated dual-network hydrogel(MEPH).This strategy employs Fe3+to achieve the one-step in situ oxidative polymerization of hydroxymethyl EDOT while concurrently forming a physical hybrid network with PVA,which is subsequently reinforced by covalent cross-linking using glutaraldehyde.This design endows the MEPH with exceptional broadband light absorption(>99%),efficient water transport,and regulated water state within the hydrogel matrix,leading to a reduced evaporation enthalpy of 732 J·g^(−1).The resulting evaporator achieves an ultrahigh evaporation rate of 4.95 kg·m^(−2)·h^(−1)under 1-sun illumination,corresponding to an energy conversion efficiency exceeding 95%,while maintaining stable,salt-resistant operation in high-salinity environments.Outdoor experiments validate its outstanding practicality for seawater and wastewater purification,with the produced freshwater significantly promoting plant growth,highlighting its great potential in sustainable agricultural water cycles.This iron-aldehyde-cooperative dynamic covalent anchoring strategy provides an innovative design paradigm for a new generation of high-performance and robust solar evaporators.展开更多
Liver is a vital organ in the human body and plays a central role in the metabolism and detoxification of endotoxins and exotoxins.Bilirubin is an endotoxin derived from hemoglobin(Hb).Removing excess bilirubin in the...Liver is a vital organ in the human body and plays a central role in the metabolism and detoxification of endotoxins and exotoxins.Bilirubin is an endotoxin derived from hemoglobin(Hb).Removing excess bilirubin in the blood is crucial for the treatment of liver diseases.Hemoperfusion,which relies on adsorbents to efficiently adsorb toxins,is a widely applied procedure for the removal of blood toxins.To broaden and improve the range and performance of hemoperfusion adsorbents,we synthesized cationic hyper crosslinked polymers(HCPs)with strong affinity for bilirubin.This material exhibited outstanding adsorption performance,with a maximum adsorption capacity of 934 mg/g and a removal efficiency of 96%.Further investigation confirmed their excellent selectivity,reusability,and biocompatibility.These findings expand the potential applications of HCPs and provide insight into strategies for constructing promising hemoperfusion adsorbent materials.展开更多
The metal‐reduction‐induced dechlorination coupling(MR-DC)strategy enables the first successful synthesis of an all‐inorganic crosslinked phosphazene network(aPN)from hexachlorocyclotriphosphazene(HCCP)under mild r...The metal‐reduction‐induced dechlorination coupling(MR-DC)strategy enables the first successful synthesis of an all‐inorganic crosslinked phosphazene network(aPN)from hexachlorocyclotriphosphazene(HCCP)under mild reaction conditions.Using Cu as a model,the resulting Cu-aPN(copper‐embedded all‐inorganic phosphazene network)retains the intrinsic N_(3)P_(3)backbone and exhibits an amorphous structure where Cu species are uniformly anchored at dense P/N coordination sites of the network.Time of flight secondary ion mass spectrometry(TOF‐SIMS)and X‐ray diffraction(XRD)reveal a gradual CuCl‐to‐CuO phase conversion during ammonia treatment,which effectively ensures the structural stability of the phosphazene framework.In 1 M KOH,Cu-aPN delivers an overpotential of 280 mV at 10 mA cm^(−2)and a Tafel slope of 48 mV dec^(−1),markedly outperforming Ga-aPN.In situ Raman and density functional theory(DFT)analyses indicate stronger Cu-P/N coordination coupling that lowers the*OH formation barrier(0.39 vs.0.88 eV for Ga).This MR-DC route furnishes a general and versatile pathway for constructing metal‐embedded all‐inorganic phosphazene frameworks with tunable coordination environments for advanced electrocatalytic applications.展开更多
Organic pollutants,a pivotal factor in water pollution,have persistently menaced the aquatic ecosystem,as well as the sustainable development of human health,economy,and society.Consequently,there is an urgent need fo...Organic pollutants,a pivotal factor in water pollution,have persistently menaced the aquatic ecosystem,as well as the sustainable development of human health,economy,and society.Consequently,there is an urgent need for advanced techniques to efficiently eliminate organic micropollutants from water.Here,we present the synthesis of three nonporous cavitand-crosslinked polymers capable of adsorbing diverse organic pollutants from aqueous solutions.These polymeric adsorbents exhibit outstanding adsorptive performance towards the tested micropollutants,characterized by high apparent adsorption rate constants(kobs)and maximum adsorption capacities(qmax,e).Notably,Compound NCCP-1 demonstrated a remarkable qmax,e of 459 mg/g for bisphenol A(BPA),ranking among the highest values reported for organic polymer adsorbents.In-depth investigation of the adsorption mechanism of the nonporous polymer revealed that it involves the recognition of pollutants by the deep cavities of the cavitand moieties and the interstitial spaces between them,primarily mediated by the hydrophobic effect.Furthermore,NCCP-1 was applied in situ water purification simulations and was proven to maintain its removal efficiency over more than four cycles,highlighting its potential for practical applications in water treatment.展开更多
基金supported by the Key Research and Development Program Project of Hubei Province(2023BCB070).
文摘Formulating oil-based drilling fluids(OBDFs)with an ultra-low oil-to-water ratio(OWR≤60:40)presents a formidable stability challenge due to the maximized interfacial area and intensified stress on the interfacial film under high-temperature,high-density conditions.To address this,we engineered a synergistic stabilization system through molecular and colloidal design.A novel hyperbranched polyamide emulsifier(epoxidized soybean oil polyamide)(ESOP),synthesized from epoxidized soybean oil,exhibits superior thermal stability and interfacial activity due to its hyperbranched architecture.Combined with calcium petroleum sulfonate(CPS)and hydrophobic nanosilica(HNs),it enables a high-performance OBDF with an ultra-low OWR of 60:40.The results show that the optimized formula achieves an excellent demulsification voltage of 1290 V,an ultra-low HTHP fluid loss of 1.5 mL,a yield point of 12.9 Pa,and a superior sag factor(SF)of 0.504,outperforming both base and commercial systems.Mechanistic studies reveal a multiscale stabilization strategy involving a dense composite interfacial film,Pickering stabilization,a 3D network,and a unique thermally triggered self-reinforcement effect.This work not only provides a cost-effective OBDF formulation but,more importantly,establishes a molecular topology engineering paradigm for stabilizing complex industrial fluids under extreme conditions.
基金financial support from the National Key R&D Program of China (No.2021YFA1302604)Scientific and technological innovation project of China Academy of Chinese Medical Sciences (No.CI2021B017)China Postdoctoral Science Foundation (No.2023T160727)。
文摘RNA binding proteins(RBPs) are a crucial class of proteins that interact with RNA and play a key role in various biological process.Deficiencies or abnormalities of RBPs are closely linked to the occurrence and progression of numerous diseases,making RBPs potential therapeutic targets.However,the limited tissue penetration of 254 nm UV irradiation makes it difficult to efficiently crosslink weak and dynamic RNA-protein interactions in mammal tissues.Additionally,RNA degradation in metal catalyzed click reaction further hinders the enrichment of RNA-protein complexes(RPCs).Due to these inherent limitations,globally profiling the RNA binding proteome in mammal organs has long been a challenge.Herein,we proposed a novel method,which utilized a dual crosslinking with formaldehyde and 254 nm UV irradiation,metabolic labeling and metal-free thiol-yne click reaction to enable large-scale enrichment and identification of RBPs in mouse liver,called FTYc_UV.In this method,formaldehyde is first used to crosslink the crude RNA-protein complexes(cRPCs) in situ to address the problem of poor tissue penetration of 254 nm UV irradiation.Furthermore,this method integrates metabolic labeling with a metal-free thiol-yne click reaction to achieve non-destructive RNA tagging.After specifically RNA-RBPs crosslinking by 254 nm UV irradiation in tissue lysates,formaldehyde decrosslinking is employed to remove non-specific proteins,leading to effective enrichment of RPCs from mouse liver and thereby overcoming the poor specificity of formaldehyde crosslinking.Application of FTYc_UV in mouse liver successfully identified over 1600 RBPs covering approximately 75 % of previously reported RBPs.Furthermore,420 candidate RBPs,including 151metabolic enzymes,were also obtained,demonstrating the sensitivity of FTYc_UV and the potential of this method for in-depth exploration of RNA-protein interactions in biological and clinical research.
基金the financial support from the National Natural Science Foundation of China (No. 52072390)the National High-Level Talents Special Support Program (Leading Talent of Technological Innovation)+2 种基金the China Postdoctoral Science Foundation (No. 2023M743648)the Young Scientists Fund of the National Natural Science Foundation of China (No. 52302330)the support from the Shanghai Emperor of Cleaning Hi-Tech Co.,LTD
文摘In-situ poly(1,3-dioxolane)(PDOL)-based electrolyte has received extensive attention in the research of lithium metal batteries due to its high stability to lithium anode and simple processing.However,it is still faced with defects such as low intrinsic ionic conductivity,a narrow electrochemical window,and poor thermal stability.A crosslinking and fluorination molecular design strategy toward PDOL is proposed to tackle the issues above.The amorphous crosslinked structure effectively improves ionic conductivity by inhibiting long-chain crystallization.Especially,the antioxidant–CF_(3)groups,stable crosslinked structure,and reduced terminal hydroxyl groups significantly enhance the electrochemical oxidation stability with a superb high-voltage window of 4.7 V.In addition,the designed electrolyte also exhibits obviously improved thermal stability with no deformation at 120°C for 5 min.Furthermore,the semi-solid NCM811||Li batteries exhibit a favourable capacity retention of 88.8%after 150 cycles at 0.5 C.Even assembled with NCM622 cathode working at 4.5 V,the semi-solid batteries can still show a satisfactory capacity retention of 85.3%after 100 cycles at 0.5 C.Also,a 0.1 Ah NCM811||Li pouch cell with active materials loading of 9 mg/cm2 demonstrates satisfactory cycling stability and working ability,which shows promising practical application prospects.
基金supported by the grants from National Natural Science Foundation of China(Nos.22278091,22278046)Young Elite Sci-entists Sponsorship Program by CAST(No.2024QNRC0387)+2 种基金the Guangxi Natural Science Foundation of China(Nos.2025GXNSFBA069146,2023GXNSFGA026001,GKAD25069076)the Foundation(No.202403)of Tianjin Key Laboratory of Pulp&Paper(Tianjin University of Science&Technology)P.R.China,and the Foundation of Guangxi Key Laboratory of Clean Pulp&Papermaking and Pollution Control,College of Light Industry and Food Engineering,Guangxi University(No.2021KF01).
文摘With the continuous advancement of social technology and the increasing awareness of health management,biomass-based triboelectric nanogenerator(TENG)displayed significant potential as flexible wearable electronics for continuous foot gait monitoring.Nevertheless,existing biomass-based TENG often faces challenges of insufficient mechanical robustness and durability in practical applications,where they are prone to surface abrasion and structural fracture under continuous compression and friction,severely limiting their long-term performances.In order to address these challenges,this work proposed a multiscale crosslinking strategy,which strengthened the noncovalent interactions within the polymer by constructing multiple reinforcement networks,successfully fabricating a dual-network C-lignin-based triboelectric material(CLTM)with excellent durability and crack resistance.Among them,the optimal CLTM(PSGCL-0.2)exhibited high mechanical strength(strain 445%,tensile strength 41.56 MPa,Young's modulus 41.25 MPa,toughness 159.67 MJ/m^(3))and excellent cyclic stability(300 cycles)with versatile functionalities,including antibacterial,antioxidant,and UV-shielding properties,water stabilization(255.51 g/m^(2)/d),efficient photothermal conversion,and full recyclability.Furthermore,biomass-based TENG device assembled from PSGCL-0.2 achieved stable triboelectric output properties(102.5 V,2.9μA,and 61.3 nC),and sustainable for 2000 cycles,fast response time(68 ms),and excellent power density(325.9 mW/m^(2)),effectively converting mechanical energy into electrical energy.Especially,PSGCL 0.2 was also integrated into the wireless self-powered smart insole,successfully enabling real-time visual monitoring of plantar pressure distribution and dynamic gait.Meanwhile,combined with the machine learning algorithm,the self-powered smart insole achieved precise recognition and classification of eight different motion states with an accuracy of 98%.This study provides the feasible strategy for developing extremely stable and durable biomass-based TENG,aimed at advancing sustainable intelligent healthcare systems.
基金supported by the National Research Foundation(NRF)of Korea,funded by the Korean Government(MSIT)(Grant No.RS-2023-00240043).
文摘As the most abundant aromatic bio-based polymer,lignin has great potential as a sustainable feedstock for building crosslinked thermoset polymers as bio-based adhesives.However,the potential of hardwood kraft lignin(HKL)is limited due to its poor crosslinking reactivity.Hence,for the first time,the present study reports the facile oxidation of HKL involving a redox reaction with silver-ammonia complexes([(AgNH3)2]+),primarily focusing on oxidation to produce reactive quinones and promote C-C linkages during reaction.This study aims to increases reactivity of oxidized HKL for effective crosslinking with monoethanolamine(MEA)for the development of bio-based wood adhesives.The characterization,including 13C-nuclear magnetic resonance(NMR)and Fourier transform infrared(FT-IR)spectroscopy,confirms the oxidation reaction,such as the formation of quinones(C=O)and subsequent crosslinking between the oxidized HKL molecules and MEA.Additionally,gel permeation chromatography(GPC)confirms the C-C and C-O linkages with increased molecular weight after oxidation,and is supported by differential scanning calorimetry(DSC)which shows the exothermic reaction due to the crosslinking of the oxidized HKL molecules via condensation to form C-C and C-O linkages.The crosslinked HKL/MEA-based adhesives underwent mild reaction and achieved a maximum dry shear strength of 0.77 MPa,which exceeds the standard requirement of 0.6 MPa.These findings demonstrate not only a one-pot oxidation for improving the reactivity of HKL using silver complexes,but also its facile crosslinking with MEA for sustainable bio-based wood adhesives.
基金funded by the key research on industrialization technologies of low-cost highenergy-density cathode materials(project number:2023GY008)the Sichuan Provincial Science and Technology Program(project number:2024NSFSC1406).
文摘To address the issue of uneven temperature distribution in shale gas oil-based drill cuttings pyrolysis furnaces,a numerical model was developed using Fluent software.The effects of nitrogen flow rate,heating tube spacing,and furnace dimensions on the internal temperature field were thoroughly analyzed from a mechanistic perspective.The results indicated that non-uniform radiation from the heating tubes and flow disturbances induced by the nitrogen stream were the primary causes of localized heat concentration.Under no-load conditions,the maximum deviation between simulated and on-site measured temperatures was 1.5%,validating the model’s accuracy.Further-more,this study investigated the trade-offs between temperature uniformity,energy consumption,and construction costs.The findings provide a crucial design basis and a reliable simulation platform for developing and optimizing pyrolysis equipment.
基金the National Natural Science Foundation of China(42074134,42474152,42374150)CNPC Innovation Found(2024DQ02-0152).
文摘The oil-based mud(OBM) borehole measurement environment presents significant limitations on the application of existing electrical logging instruments in high-resistance formations. In this paper, we propose a novel logging method for detection of high-resistance formations in OBM using highfrequency electrodes. The method addresses the issue of shallow depth of investigation(DOI) in existing electrical logging instruments, while simultaneously ensuring the vertical resolution. Based on the principle of current continuity, the total impedance of the loop is obtained by equating the measurement loop to the series form of a capacitively coupled circuit. and its validity is verified in a homogeneous formation model and a radial two-layer formation model with a mud standoff. Then, the instrument operating frequency and electrode system parameters were preferentially determined by numerical simulation, and the effect of mud gap on impedance measurement was investigated. Subsequently, the DOI of the instrument was investigated utilizing the pseudo-geometric factor defined by the real part of impedance. It was determined that the detection depth of the instrument is 8.74 cm, while the effective vertical resolution was not less than 2 cm. Finally, a focused high-frequency electrode-type instrument was designed by introducing a pair of focused electrodes, which effectively enhanced the DOI of the instrument and was successfully deployed in the Oklahoma formation model. The simulation results demonstrate that the novel method can achieve a detection depth of 17.40 cm in highly-resistive formations drilling with OBM, which is approximately twice the depth of detection of the existing oil-based mud microimager instruments. Furthermore, its effective vertical resolution remains at or above 2 cm,which is comparable to the resolution of the existing OBM electrical logging instrument.
基金the support from National Natural Science Foundation of China(No.22161132006)Key R&D Program of Zhejiang(No.2024SSYS0036)Westlake University Startup。
文摘Reader proteins that bind specific methyllysine are important to biological functions of lysine methylation,but readers of many methyllysine sites are still unknown.Therefore,development of covalent probes is important to identify readers from cell samples so as to understand biological roles of lysine methylation.Generally,readers bind methyllysine via aromatic cages that contain tryptophan,tyrosine and phenylalanine,that offer a unique motif for selective crosslinking.We recently reported a site-selective tryptophan crosslinking strategy based on dimethylsulfonium that mimics dimethyllysine to crosslink tryptophan in aromatic cages of readers.Since tyrosine is a key residue for binding affinity to methyllysine,especially some readers that do not contain tryptophan residues in the binding pocket.Here we developed strategies of site-selective crosslinking to tyrosine.Ultraviolet(UV)source was applied to excite tyrosine at neutral pH or phenoxide at basic p H,and subsequent single-electron transfer(SET)from Tyr*to sulfonium inside the binding pocket enables selective crosslinking.In consequence,methyllysine readers with tyrosine-containing aromatic cages could be selectively crosslinked by site-specific sulfonium peptide probes.In addition,we expanded substrates from aromatic cages to tyrosine residues of proximate contact with sulfonium probes.The pair of LgBiT and SmBiT exhibited orthogonal crosslinking in complicated cell samples.As a result,we may expand sulfonium tools to target local tyrosine in future investigations.
基金supported by the National Natural Science Foundation of China(No.51874036)the Natural Science Foundation of Ningxia(No.2024AAC02034)。
文摘Two-dimensional(2D) nanomaterials have always been regarded as having great development potential in the field of oil-based lubrication due to their designable structures,functional groups,and abundant active sites.However,understanding the structure-performance relationship between the chemical structure of 2D nanomaterials and their lubrication performance from a comprehensive perspective is crucial for guiding their future development.This review provides a timely and comprehensive overview of the applications of 2D nanomaterials in oil-based lubrication.First,the bottlenecks and mechanisms of action of 2D nanomaterials are outlined,including adsorption protective films,charge adsorption effects,tribochemical reaction films,interlayer slip,and synergistic effects.On this basis,the review summarizes recent structural regulation strategies for 2D nanomaterials,including doping engineering,surface modification,structural optimization,and interfacial mixing engineering.Then,the focus was on analyzing the structure-performance relationship between the chemical structure of 2D nanomaterials and their lubrication performance.The effects of thickness,number of layers,sheet diameter,interlayer spacing,Moiré patterns,wettability,functional groups,concentration,as well as interfacial compatibility and dispersion behavior of 2D nanomaterials were systematically investigated in oil-based lubrication,with the intrinsic correlations resolved through computational simulations.Finally,the review offers a preliminary summary of the significant challenges and future directions for 2D nanomaterials in oil-based lubrication.This review aims to provide valuable insights and development strategies for the rational design of high-performance oil-based lubrication materials.
文摘BACKGROUND Oil-based iodinated contrast media have excellent contrast properties and are widely used for hysterosalpingographic evaluation of female infertility.On abdominal radiography and computed tomography(CT)scans,their radiodensity is similar to that of metallic objects,which can sometimes lead to diagnostic confusion in the postoperative settings.In this case,retained oil-based contrast medium was observed on an abdominal radiograph following a cesarean section,making it difficult to differentiate from an intraperitoneal foreign body from surgery.The patient was a 37-year-old pregnant woman who was referred to our hospital at 32 weeks and 1 day of pregnancy due to complete placenta previa for mana-gement of pregnancy and delivery.An elective cesarean section was performed at 37 weeks and 3 days.A plain abdominal radiograph taken immediately after surgery revealed a near-round,hyperdense,mass-like shadow with a regular margin in the pelvic cavity.An intraperitoneal foreign body was suspected;therefore,an abdominal CT scan was performed.The foreign body was located on the left side of the pouch of Douglas and had a CT value of 7000 Hounsfield units,similar to that of metals.The CT value strongly suggested the presence of an artificial object.However,further inquiries with the patient and her previous physician revealed a history of hysterosalpingography.Accordingly,retained oil-based iodinated contrast medium was suspected,and observation of the object’s course was adopted.CONCLUSION When intraperitoneal foreign bodies are suspected on postoperative radiographs,the possibility of oil-based iodinated contrast medium retention should be considered.
基金financially supported by the China Postdoctoral Science Foundation(No.2024M751205)the Natural Science Foundation of Jiangsu Province(JSNSF)(No.BK20230694)。
文摘Poly(vinyl alcohol)(PVA)hydrogels have garnered significant attention for tissue engineering,wound dressing,and electronic skin sensing applications.However,their poor mechanical performance severely restricts their multifunctional application in many scenarios.To address this limitation,PVA/tannic acid(TA)@carbon nanotubes(PVA/TA@CNTs)composite hydrogels with triple crosslinking networks were prepared through freezing-thawing and the solvent-induced shrinkage method,utilizing tannic acid-carbon nanotubes(TA@CNTs)as reinforcing units and a Ca^(2+)crosslinking strategy.The enhanced interfacial networks consisting of PVA crystalline domains,hydrogen bonding,and metal coordination endowed the composite hydrogel with a high mechanical strength,excellent flexibility,and fracture toughness,accompanied by a significant increase in crystallinity.The tensile strength and fracture toughness of the composite hydrogel reached up to about 7.0 MPa and 17.0MJ/m^(3),which were roughly 8 and 10 times higher than those of neat PVA hydrogel,respectively.The composite hydrogel demonstrated good cytocompatibility,significantly addressing the challenge of balancing structural reinforcement with biosafety in hydrogels.This methodology establishes a rational design for fabricating mechanically robust yet tough PVA hydrogels for biomedical applications.
基金support and funding from the National Natural Science Foundation of China(No.52174047)。
文摘Hydrogels are widely used in reservoir flow control to enhanced oil recovery.However,challenges such as environmental contamination from conventional crosslinkers,poor solubility of crosslinking agents,and short gelation times under high-temperature conditions(e.g.,150℃)have hindered their practical application.Herein,we present the synthesis of amine-functionalized carbon quantum dots(NH_(2)-CQDs),which act as both a nano-crosslinker and a nano-reinforcing agent within hydrogel systems.The NH_(2)-CQDs-incorporated hydrogel can remain stability for 300 days under the conditions of a mineralization degree of 2.11×10^(4)mg/mL and 170℃,and has high tensile strength(371 kPa),good toughness(49.6 kJ/m^(3)),excellent viscoelasticity(G'=960 Pa,G"=460 Pa)and shear resistance.In addition,NH_(2)-CQDs adds many hydroxyl groups to the hydrogel,which can be attached to the surface of various substances.At the same time,micro-nano capsules containing NH_(2)-CQDs were formed by self-assembly of hydrophobic SiO_(2)on water droplets,the NH_(2)-CQDs solution is encapsulated in a capsule,and when stimulated by external conditions(temperature,pH,surfactant),the capsule releases the NH_(2)-CQDs solution,this method greatly delays the crosslinking time between polymer and crosslinker at high temperature.Under the condition of 170℃and pH=7,the gelation time of 10%hydrophobic SiO_(2)coated hydrogel is 44 times that of uncoated hydrogel,which can be effectively used for deep formation flow control,and CQD give hydrogels fluorescence properties that can be used for underground signal tracking.
基金supported by the Program for Science and Technology Innovation Team in Zhejiang(Grant No.2021R01004)the Natural Science Foundation of Ningbo City(No.2023J119)+1 种基金the Ningbo Youth Science and Technology Innovation Leading Talent Project(2023QL029)K.C.Wong Magna Fund in Ningbo University,China。
文摘Inorganic CsPbI_(3)perovskite with superior thermal stability and photoelectric properties has developed into a promising candidate for photovoltaic applications.Nevertheless,the power conversion efficiency(PCE)of CsPbI_(3)perovskite solar cells(PSCs)still lags far behind that of both organic-inorganic hybrid counterparts and the theoretical PCE limit,primarily restricted by severe fill factor(FF)and opencircuit voltage(VOC)deficits.Herein,an in-situ self-crosslinking strategy is proposed to construct high-performance inverted inorganic PSCs by incorporating acrylate monomers as additives into CsPbI_(3)perovskite precursors.During the thermal annealing process of perovskite films,acrylate monomers can form network structures by breaking the C=C groups through an in-situ polymerization reaction,mainly anchored at the grain boundaries(GBs)and on the surfaces of perovskite.Meanwhile,the C=O groups of acrylate polymers can favorably coordinate with uncoordinated Pb^(2+),thereby decreasing defect density and stabilizing the perovskite phase.Particularly,with multiple crosslinking and passivation sites,the incorporation of dipentaerythritol pentaacrylate(DPHA)can effectively improve the perovskite film quality,suppress nonradiative recombination,and block moisture erosion.Consequently,the DPHAbased PSC achieves a champion PCE of 20.05%with a record-high FF of 85.05%,both of which rank among the top in the performance of inverted CsPbI_(3)PSCs.Moreover,the unencapsulated DPHA-based device exhibits negligible hysteresis,remarkably improved long-term storage,and operational stability.This work offers a facile and useful strategy to simultaneously promote the efficiency and device stability of inverted inorganic PSCs.
基金supported by generous grants from the Natural Science Foundation of Zhejiang Province(LR24E030003)Zhejiang Province Qianjiang Talent Program(ZJ-QJRC-2020-32).
文摘Elastic electronics are increasingly prevalent in information storage,smart sensing and health monitoring due to their softness,stretchability and portability.Wearable electronic devices should possess elasticity and stretchability that align with biological tissues.Specifically,their materials should be capable of elastic strain up to 50–80%,while the devices themselves must maintain electric stability under strains that accommodate body movements[1].
基金National Natural Science Foundation of China (52203123)Sichuan Science and Technology Program (2023NSFSC0991)+2 种基金State Key Laboratory of Polymer Materials Engineering (sklpme-2023-1-05 and sklpme-2024-2-04)Fundamental Research Funds for the Central UniversitiesThis research was also partially sponsored by the Double First-Class Construction Funds of Sichuan University。
文摘All-safe liquid-state lithium-ion batteries(ASLS-LIBs) is of great interest as they can potentially combine the safety of all-solid-state batteries with the high performance and low manufacturing cost of traditional liquid-state LIBs. However, the practical success of ASLS-LIBs is bottlenecked by the lack of advanced separator technology that can simultaneously realize high performances in puncturing-tolerability,fire-resistance, and importantly, wetting-capability with non-flammable liquid-electrolytes. Here, we propose a concept of inorganic in-situ separator(IISS) by hybrid-sol physical crosslinking directly onto the electrode surface to address the above challenges. Particularly, the hybrid-sol is designed with silica nanoparticles as the building block and poly(vinylidene difluoride) nanoparticles as the crosslinking agent. The critical factors for controlling the IISS microstructures and properties have been systematically investigated. The advantages of the IISS have been confirmed by its fast wetting with various fireresistant liquid-electrolytes, customizable thickness and porous structures, robust interface with planar or three-dimensional(3D)-structured electrodes, and importantly, unexpected self-adaptability against puncturing. Enabled by the above merits, a fire-resistant ASLS-LIB is successfully assembled and demonstrated with stable electrochemical performance. This sol-crosslinked IISS may open an avenue for the studies on the next-generation separator technology, cell assembling, solid electrolyte processing as well as non-flammable secondary batteries.
基金Supported by Wu Jieping Medical Foundation(No.320.6750.2021-04-15).
文摘AIM:To assess the visual outcomes and corneal biomechanical properties of myopia patients between laser in situ keratomileusis(LASIK)and LASIK combined with accelerated corneal crosslinking(LASIK Xtra).METHODS:This prospective study analyzed 52 consecutive myopia patients treated with LASIK Xtra and 45 consecutive myopia patients treated with LASIK.Only the right eyes in the two groups were analyzed.The uncorrected distance visual acuity(UDVA),keratometry values,postoperative central corneal thickness(CCT),corneal demarcation line depth,the corneal compensated intraocular pressure(IOPcc),Goldmann-correlated IOP(IOPg),corneal resistance factor(CRF)and corneal hysteresis(CH)from Ocular Response Analyzer(ORA)were analyzed.Further,the correlation between the demarcation line depth and ORA-related biomechanical parameters were analyzed.RESULTS:No significant differences in UDVA,postoperative CCT,or mean K values were found between the 2 groups at 1 to 12mo postoperative follow-up(all P>0.05).The changes of CRF was significantly lower in the LASIK Xtra group compared to the LASIK group(all P<0.05)at all the postoperative visits.The changes of CH were significantly higher in the LASIK Xtra group(all P<0.05).No significant differences were discovered regarding the changes of IOPcc and IOPg posperatively(all P>0.05).Out of 52 cases in the LASIK Xtra group,the demarcation line was present in 40 eyes(77%).The average depth of the demarcation was 220.73±42.70μm(136 to 288μm).No significant correlation was observed between the depth of the demarcation line and any of the ORA-related biomechanical parameters such as IOPcc,IOPg,CRF and CH at 12mo(all P>0.05).CONCLUSION:Both procedures demonstrate comparable outcomes in terms of visual acuity,refraction and ablation predictability.This study confirms that corneal biomechanical properties of the included patients weakened after both procedures,but the cornea after LASIK Xtra are stiffer than conventional LASIK.
基金financially supported by the Natural Science Foundation of Jiangxi Province(No.20232ACB204002)the Jiangxi Provincial Key Laboratory of Flexible Electronics(No.20242BCC32010).
文摘The development of solar-driven interfacial evaporation technology is pivotal for addressing global water scarcity.However,it is hindered by the difficulty in synergizing high photothermal conversion with low water evaporation enthalpy into a single material.Herein,we propose an iron-aldehyde-cooperative dynamic covalent anchoring strategy,successfully constructing a covalently locked,hydroxymethyl-functionalized PEDOT-PVA integrated dual-network hydrogel(MEPH).This strategy employs Fe3+to achieve the one-step in situ oxidative polymerization of hydroxymethyl EDOT while concurrently forming a physical hybrid network with PVA,which is subsequently reinforced by covalent cross-linking using glutaraldehyde.This design endows the MEPH with exceptional broadband light absorption(>99%),efficient water transport,and regulated water state within the hydrogel matrix,leading to a reduced evaporation enthalpy of 732 J·g^(−1).The resulting evaporator achieves an ultrahigh evaporation rate of 4.95 kg·m^(−2)·h^(−1)under 1-sun illumination,corresponding to an energy conversion efficiency exceeding 95%,while maintaining stable,salt-resistant operation in high-salinity environments.Outdoor experiments validate its outstanding practicality for seawater and wastewater purification,with the produced freshwater significantly promoting plant growth,highlighting its great potential in sustainable agricultural water cycles.This iron-aldehyde-cooperative dynamic covalent anchoring strategy provides an innovative design paradigm for a new generation of high-performance and robust solar evaporators.
基金financially supported by the International Cooperation Program of the Ministry of Science and Technology of Hubei Province(No.2023EHA069)Shenzhen Science and Technology Program(No.JCYJ20230807143702005)the National Foreign Experts Program(No.G2022027015L)。
文摘Liver is a vital organ in the human body and plays a central role in the metabolism and detoxification of endotoxins and exotoxins.Bilirubin is an endotoxin derived from hemoglobin(Hb).Removing excess bilirubin in the blood is crucial for the treatment of liver diseases.Hemoperfusion,which relies on adsorbents to efficiently adsorb toxins,is a widely applied procedure for the removal of blood toxins.To broaden and improve the range and performance of hemoperfusion adsorbents,we synthesized cationic hyper crosslinked polymers(HCPs)with strong affinity for bilirubin.This material exhibited outstanding adsorption performance,with a maximum adsorption capacity of 934 mg/g and a removal efficiency of 96%.Further investigation confirmed their excellent selectivity,reusability,and biocompatibility.These findings expand the potential applications of HCPs and provide insight into strategies for constructing promising hemoperfusion adsorbent materials.
基金financially supported by the National Natural Science Foundation of China(Grant 22205173)the Innovation Capability Support Program of Shaanxi(Grant 2024CX‐GXPT‐12)。
文摘The metal‐reduction‐induced dechlorination coupling(MR-DC)strategy enables the first successful synthesis of an all‐inorganic crosslinked phosphazene network(aPN)from hexachlorocyclotriphosphazene(HCCP)under mild reaction conditions.Using Cu as a model,the resulting Cu-aPN(copper‐embedded all‐inorganic phosphazene network)retains the intrinsic N_(3)P_(3)backbone and exhibits an amorphous structure where Cu species are uniformly anchored at dense P/N coordination sites of the network.Time of flight secondary ion mass spectrometry(TOF‐SIMS)and X‐ray diffraction(XRD)reveal a gradual CuCl‐to‐CuO phase conversion during ammonia treatment,which effectively ensures the structural stability of the phosphazene framework.In 1 M KOH,Cu-aPN delivers an overpotential of 280 mV at 10 mA cm^(−2)and a Tafel slope of 48 mV dec^(−1),markedly outperforming Ga-aPN.In situ Raman and density functional theory(DFT)analyses indicate stronger Cu-P/N coordination coupling that lowers the*OH formation barrier(0.39 vs.0.88 eV for Ga).This MR-DC route furnishes a general and versatile pathway for constructing metal‐embedded all‐inorganic phosphazene frameworks with tunable coordination environments for advanced electrocatalytic applications.
基金supported by the National Natural Science Foundation of China(Nos.22322107,22101169 and 22071144)by Shanghai Scientific and Technological Committee(No.22010500300).
文摘Organic pollutants,a pivotal factor in water pollution,have persistently menaced the aquatic ecosystem,as well as the sustainable development of human health,economy,and society.Consequently,there is an urgent need for advanced techniques to efficiently eliminate organic micropollutants from water.Here,we present the synthesis of three nonporous cavitand-crosslinked polymers capable of adsorbing diverse organic pollutants from aqueous solutions.These polymeric adsorbents exhibit outstanding adsorptive performance towards the tested micropollutants,characterized by high apparent adsorption rate constants(kobs)and maximum adsorption capacities(qmax,e).Notably,Compound NCCP-1 demonstrated a remarkable qmax,e of 459 mg/g for bisphenol A(BPA),ranking among the highest values reported for organic polymer adsorbents.In-depth investigation of the adsorption mechanism of the nonporous polymer revealed that it involves the recognition of pollutants by the deep cavities of the cavitand moieties and the interstitial spaces between them,primarily mediated by the hydrophobic effect.Furthermore,NCCP-1 was applied in situ water purification simulations and was proven to maintain its removal efficiency over more than four cycles,highlighting its potential for practical applications in water treatment.
