The gelation of crude oil with high wax and asphaltene content at low temperatures often results in the block of transportation pipeline in Africa. In recent years, it was reported that surface hydrophobicmodified nan...The gelation of crude oil with high wax and asphaltene content at low temperatures often results in the block of transportation pipeline in Africa. In recent years, it was reported that surface hydrophobicmodified nanoparticles have important applications in crude oil flow modification. In this work, four kinds of core-shell hybride nanoparticles by grafting poly(octadecyl, docosyl acrylate) and poly(acrylate-α-olefin) onto the surface of nano-sized SiO_(2) were synthesized by grafting polymerization method.The chemical structure of nanoparticles was analyzed by Fourier transform infrared spectroscopy(FT-IR),scanning electron microscopy(SEM) and thermogravimetric analysis(TGA). The rheological behaviors of crude oil and precipitation of asphaltenes in the presence of nanoparticles were studied by measuring the viscose-temperature relationship curve, the cumulative wax precipitation amount, and morphology of waxes and asphaltenes. The results indicate that the docosyl polyacrylate@SiO_(2) nanoparticle(PDA@SiO_(2)) can reduce the cumulative wax precipitation amount of crude oil by 72.8%, decline the viscosity of crude oil by 85.6% at 20℃, reduce the average size of wax crystals by 89.7%, and inhibit the agglomeration of asphaltene by 74.8%. Therefore, the nanoparticles not only adjust the crystalline behaviors of waxes, but also inhibit the agglomeration of asphaltenes. Apparently, core-shell hybride nanoparticles provides more heterogeneous nucleation sites for the crystallization of wax molecules,thus inhibiting the formation of three-dimensional network structure. The core-shell polymer@SiO_(2) hybride nanoparticles are one of promising additives for inhibiting crystallization of waxes and agglomeration of asphaltenes in crude oil.展开更多
The rational design of metal single-atom catalysts(SACs)for electrochemical nitrogen reduction reaction(NRR)is challenging.Two-dimensional metal-organic frameworks(2DMOFs)is a unique class of promising SACs.Up to now,...The rational design of metal single-atom catalysts(SACs)for electrochemical nitrogen reduction reaction(NRR)is challenging.Two-dimensional metal-organic frameworks(2DMOFs)is a unique class of promising SACs.Up to now,the roles of individual metals,coordination atoms,and their synergy effect on the electroanalytic performance remain unclear.Therefore,in this work,a series of 2DMOFs with different metals and coordinating atoms are systematically investigated as electrocatalysts for ammonia synthesis using density functional theory calculations.For a specific metal,a proper metal-intermediate atoms p-d orbital hybridization interaction strength is found to be a key indicator for their NRR catalytic activities.The hybridization interaction strength can be quantitatively described with the p-/d-band center energy difference(Δd-p),which is found to be a sufficient descriptor for both the p-d hybridization strength and the NRR performance.The maximum free energy change(ΔG_(max))andΔd-p have a volcanic relationship with OsC_(4)(Se)_(4)located at the apex of the volcanic curve,showing the best NRR performance.The asymmetrical coordination environment could regulate the band structure subtly in terms of band overlap and positions.This work may shed new light on the application of orbital engineering in electrocatalytic NRR activity and especially promotes the rational design for SACs.展开更多
Precisely refining the electronic structure of electrocatalysts represents a powerful approach to further optimize the electrocatalytic performance.Herein,we demonstrate an ingenious d-d orbital hybridization concept ...Precisely refining the electronic structure of electrocatalysts represents a powerful approach to further optimize the electrocatalytic performance.Herein,we demonstrate an ingenious d-d orbital hybridization concept to construct Mo-doped Co_(9)S_(8) nanorod arrays aligned on carbon cloth(CC)substrate(abbreviated as Mo-Co_(9)S_(8)@CC hereafter)as a high-efficiency bifunctional electrocatalyst toward water electrolysis.It has experimentally and theoretically validated that the 4d-3d orbital coupling between Mo dopant and Co site can effectively optimize the H_(2)O activation energy and lower H^(*)adsorption energy barrier,thereby leading to enhanced hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)activities.Thanks to the unique electronic and geometrical advantages,the optimized Mo-Co_(9)S_(8)@CC with appropriate Mo content exhibits outstanding bifunctional performance in alkaline solution,with the overpotentials of 75 and 234 mV for the delivery of a current density of 10 mA cm^(-2),small Tafel slopes of 53.8 and 39.9 mV dec~(-1)and long-term stabilities for at least 32 and 30 h for HER and OER,respectively.More impressively,a water splitting electrolylzer assembled by the self-supported Mo-Co_(9)S_(8)@CC electrode requires a low cell voltage of 1.53 V at 10 mA cm^(-2)and shows excellent stability and splendid reversibility,demonstrating a huge potential for affordable and scalable electrochemical H_(2) production.The innovational orbital hybridization strategy for electronic regulation herein provides an inspirable avenue for developing progressive electrocatalysts toward new energy systems.展开更多
Siliconated polyurethane (Si-PU) was synthesized using isophorone diisocyanate (IPDI), hydroxybutyl-terminated polydimethylsiloxane (PDMS), polytetramethylene ether glycol (PTMG), polypropylene glycol (PPG),...Siliconated polyurethane (Si-PU) was synthesized using isophorone diisocyanate (IPDI), hydroxybutyl-terminated polydimethylsiloxane (PDMS), polytetramethylene ether glycol (PTMG), polypropylene glycol (PPG), 1,6-hexanediol (HDO), dimethylol propionic acid (DMPA) and triethylamine (TEA). Based on butyl acrylate (BA), 2, 2, 2-trifluoroethylmethacrylate (TFEMA) and Si-PU as a seed emulsion, a novel core-shell type acrylic-polyurethane hybrid emulsion, containing siloxane and fluorine (F-Si-PU), was prepared by seeded emulsion polymerization. The contents of siloxane and fluorine were determined according to the feed ratio. Fourier transform infrared spectroscopy (FTIR) was used to identify the chain structures of Si-PU and F-Si-PU. Investigation of transmission electron microscopy (TEM) confirmed the core-shell structure of F-Si-PU emulsion. Measurement results of water contact angle and the swelling ratio in water and n-octane for cured film showed that the water and the oil resistances for F-Si-PU had been significantly improved at a suitable content of fluorine and siloxane.展开更多
A core-shell composite consisting of ZSM-5 zeolite as the core and ordered mesoporous silica as the shell was prepared by a surfactant-controlled sol-gel process and using tetradecylamine(TDA) as the template and Tetr...A core-shell composite consisting of ZSM-5 zeolite as the core and ordered mesoporous silica as the shell was prepared by a surfactant-controlled sol-gel process and using tetradecylamine(TDA) as the template and Tetraethylorthosilicate(TEOS) as the silica precursor.The pores of the silica shell were found to be ordered and perpendicular to the crystal faces of the zeolite core.The thickness of the shell in the coreshell structured composite can be adjusted in the range of 20-90 nm,while the surface morphology and the pore size distribution were modified by changing the mass ratio of TEOS to zeolite.The composite molecular sieves have higher surface area for capturing molecules than ZSM-5,and with the increase of mesoporous shell layer,the ZSM-5@SiO_(2)-x composites show stronger adsorption capacity of butyraldehyde.However,when the shell thickness exceeds 90 nm,the adsorption capacity of butyraldehyde decreases instead.The composites have a huge potential for environmental applications.展开更多
As the global electric vehicle market continues to grow,the recycling of Li-ion battery (LIB) becomes more important worldwide and the resynthesis of cathode materials would be the most value-added recycling approach ...As the global electric vehicle market continues to grow,the recycling of Li-ion battery (LIB) becomes more important worldwide and the resynthesis of cathode materials would be the most value-added recycling approach taking into account limited metal resources.Although resynthesized homogenous LiNi_(x)Co_(y)Mn_(z)O_(2)(NCM) from spent LIB leachate shows comparable battery performance to pristine NCM from virgin materials,there is general concern in its cycling performance.Here,we synthesize core–shell(CS) Ni-rich NCM,which consists of Ni-rich NCM as the core and NCM derived from the original or purified leachate of spent LIBs as the shell.Resynthesized CS Ni-rich NCM exhibits improved rate capability resulting from expanded interslab thickness in the NCM structure.CS Ni-rich NCM from purified LIB leachate shows improvement in cycling performance and thermal stability.It specifically delivers a capacity retention of 86.6%at a high temperature after 80 cycles compared to that (75.0%) of pristine CS Ni-rich NCM.These improvements are caused by a relatively high Mg content on the shell and the widespread distribution of Al through the CS structure.CS Ni-rich NCM derived from spent LIB leachate provides a new alternative approach to conventional LIB recycling methods,which would utilize efficiently limited metal resources for the sustainable LIB production.展开更多
Semiconductor photocatalysis holds great promise for renewable energy generation and environment remediation,but generally suffers from the serious drawbacks on light absorption,charge generation and transport,and str...Semiconductor photocatalysis holds great promise for renewable energy generation and environment remediation,but generally suffers from the serious drawbacks on light absorption,charge generation and transport,and structural stability that limit the performance.The core-shell semiconductorgraphene(CSSG)nanoarchitectures may address these issues due to their unique structures with exceptional physical and chemical properties.This review explores recent advances of the CSSG nanoarchitectures in the photocatalytic performance.It starts with the classification of the CSSG nanoarchitectures by the dimensionality.Then,the construction methods under internal and external driving forces were introduced and compared with each other.Afterward,the physicochemical properties and photocatalytic applications of these nanoarchitectures were discussed,with a focus on their role in photocatalysis.It ends with a summary and some perspectives on future development of the CSSG nanoarchitectures toward highly efficient photocatalysts with extensive application.By harnessing the synergistic capabilities of the CSSG architectures,we aim to address pressing environmental and energy challenges and drive scientific progress in these fields.展开更多
Building a covalently connected structure with accelerated photo-induced electrons and charge-carrier separation between semiconductors could enhance the photocatalytic performance.In this work,we report a facile and ...Building a covalently connected structure with accelerated photo-induced electrons and charge-carrier separation between semiconductors could enhance the photocatalytic performance.In this work,we report a facile and novel seed growth method to coat NH2-MIL-125 MOFs with crystalline and porous covalent organic frameworks(COFs)materials and form a range of NH2-MIL-125@TAPB-PDA nanocomposites with different thicknesses of COF shell.The introduction of appropriate content of COF could not only modify the intrinsic electronic and optical properties,but also enhance the photocatalytic activity distinctly.Especially,NH2-MIL-125@TAPB-PDA-3 with COF shell thickness of around 20nm exhibited the highest yield(94.7%)of benzaldehyde which is approximately 2.5 and 15.5 times as that of parental NH2-MIL-125 and COF,respectively.The promoted photocatalytic performance of hybrid materials was mainly owing to the enhanced photo-induced charge carriers transfer between the MOF and COF through the covalent bond.In addition,a possible mechanism to elucidate the process of photocatalysis was explored.Therefore,this kind of MOF-based photocatalysts possesses great potentials in future green organic synthesis.展开更多
Direct conversion of solar energy into chemical energy in an environmentally friendly manner is one of the most promising strategies to deal with the environmental pollution and energy crisis.Among a variety of materi...Direct conversion of solar energy into chemical energy in an environmentally friendly manner is one of the most promising strategies to deal with the environmental pollution and energy crisis.Among a variety of materials developed as photocatalysts,the core-shell metal/covalent-organic framework(MOF or COF)photocatalysts have garnered significant attention due to their highly porous structure and the adjustability in both structure and functionality.The existing reviews on core-shell organic framework photocatalytic materials have mainly focused on core-shell MOF materials.However,there is still a lack of indepth reviews specifically addressing the photocatalytic performance of core-shell COFs and MOFs@COFs.Simultaneously,there is an urgent need for a comprehensive review encompassing these three types of core-shell structures.Based on this,this review aims to provide a comprehensive understanding and useful guidelines for the exploration of suitable core-shell organic framework photocatalysts towards appropriate photocatalytic energy conversion and environmental governance.Firstly,the classification,synthesis,formation mechanisms,and reasonable regulation of core-shell organic framework were summarized.Then,the photocatalytic applications of these three kinds of core-shell structures in different areas,such as H_(2)evolution,CO_(2)reduction,and pollutants degradation are emphasized.Finally,the main challenges and development prospects of core-shell organic framework photocatalysts were introduced.This review aims to provide insights into the development of a novel generation of efficient and stable core-shell organic framework materials for energy conversion and environmental remediation.展开更多
Using interface engineering,a highly efficient catalyst with a shell@core structure was successfully synthesized by growing an amorphous material composed of Ni,Mo,and P on Cu nanowires(Ni-MoP@CuNWs).This catalyst onl...Using interface engineering,a highly efficient catalyst with a shell@core structure was successfully synthesized by growing an amorphous material composed of Ni,Mo,and P on Cu nanowires(Ni-MoP@CuNWs).This catalyst only requires an overpotential of 35 mV to reach a current density of 10 mA cm^(-2).The exceptional hydrogen evolution reaction(HER)activity is attributed to the unique amorphous rod-like nature of NiMoP@CuNWs,which possesses a special hydrophilic feature,en-hances mass transfer,promotes effective contact between the electrode and electrolyte solution,and exposes more active sites during the catalytic process.Density functional theory revealed that the introduction of Mo weakens the binding strength of the Ni site on the catalyst surface with the H atom and promotes the desorption process of the H_(2) product significantly.Owing to its facile syn-thesis,low cost,and high catalytic performance,this electrocatalyst is a promising option for com-mercial applications as a water electrolysis catalyst.展开更多
The massive use of antibiotics has led to the aggravation of bacterial resistance and also brought environmental pollution problems.This poses a great threat to human health.If the dosage of antibiotics is reduced by ...The massive use of antibiotics has led to the aggravation of bacterial resistance and also brought environmental pollution problems.This poses a great threat to human health.If the dosage of antibiotics is reduced by increasing its bactericidal performance,the emergence of drug resistance is certainly delayed,so that there's not enough time for developing drug resistance during treatment.Therefore,we selected typical representative materials of metal Ag and semiconductor ZnO nano-bactericides to design and synthesize Ag/ZnO hollow core-shell structures(AZ for short).Antibiotics are grafted on the surface of AZ through rational modification to form a composite sterilization system.The research results show that the antibacterial efficiency of the composite system is significantly increased,from the sum(34.7%+22.8%-57.5%)of the antibacterial efficiency of AZ and gentamicin to 80.2%,net synergizes 22.7%,which fully reflects the effect of 1+1>2.Therefore,the dosage of antibiotics can be drastically reduced in this way,which makes both the possibility of bacterial resistance and medical expenses remarkably decrease.Subsequently,residual antibiotics can be degraded under simple illumination using AZ-self as a photocatalyst,which cuts off the path of environmental pollution.In short,such an innovative route has guiding significance for drug resistance.展开更多
A machine learning(ML)-based random forest(RF)classification model algorithm was employed to investigate the main factors affecting the formation of the core-shell structure of BaTiO_(3)-based ceramics and their inter...A machine learning(ML)-based random forest(RF)classification model algorithm was employed to investigate the main factors affecting the formation of the core-shell structure of BaTiO_(3)-based ceramics and their interpretability was analyzed by using Shapley additive explanations(SHAP).An F1-score changed from 0.8795 to 0.9310,accuracy from 0.8450 to 0.9070,precision from 0.8714 to 0.9000,recall from 0.8929 to 0.9643,and ROC/AUC value of 0.97±0.03 was achieved by the RF classification with the optimal set of features containing only 5 features,demonstrating the high accuracy of our model and its high robustness.During the interpretability analysis of the model,it was found that the electronegativity,melting point,and sintering temperature of the dopant contribute highly to the formation of the core-shell structure,and based on these characteristics,specific ranges were delineated and twelve elements were finally obtained that met all the requirements,namely Si,Sc,Mn,Fe,Co,Ni,Pd,Er,Tm,Lu,Pa,and Cm.In the process of exploring the structure of the core-shell,the doping elements can be effectively localized to be selected by choosing the range of features.展开更多
Lysine is one of the essential amino acids for human body,and its imbalance is a major cause to anemia,aging process,leukemia cell proliferation and tumor growth.Therefore,its monitoring is dominative to the preventio...Lysine is one of the essential amino acids for human body,and its imbalance is a major cause to anemia,aging process,leukemia cell proliferation and tumor growth.Therefore,its monitoring is dominative to the prevention the disease progress and guidance to the clinical treatment.However,traditional inhospital detection methods,such as colorimetry and fluorometric,often suffer the disadvantages of high cost and long time-consuming.These drawbacks show a difficulty in the home-in and dairy monitoring for the lysine regulation in body.In this study,we have proposed an ultrasensitive microchipbased portable device to achieve the onsite and precise determination of lysine within only 10 s.This microchip was functionalized through constructing a center-concave nanosheet of core-shell WO_(3)@Prussian blue(WO_(3)@PB)to remarkably strengthen the generation and transfer of the detection signal.In this special architecture,the core WO_(3)nanosheet can be exposed at the center region of this nanocomposite to effectively promote the enzymatic oxidation,while the PB shell enables to strongly reduce the H_(2)O_(2)produced by the enzymatic reaction.Under above synergetic effects,a handheld device was designed to support the plug-and-play microchip,which performed an outstanding accuracy for the lysine detection in blood.展开更多
The weak interface interaction and solid-solid phase transition have long been a conundrum for 1,3,5,7-tetranitro-1,3,5,7-tetraazacyclooctane(HMX)-based polymer-bonded explosives(PBX).A two-step strategy that involves...The weak interface interaction and solid-solid phase transition have long been a conundrum for 1,3,5,7-tetranitro-1,3,5,7-tetraazacyclooctane(HMX)-based polymer-bonded explosives(PBX).A two-step strategy that involves the pretreatment of HMX to endow—OH groups on the surface via polyalcohol bonding agent modification and in situ coating with nitrate ester-containing polymer,was proposed to address the problem.Two types of energetic polyether—glycidyl azide polymer(GAP)and nitrate modified GAP(GNP)were grafted onto HMX crystal based on isocyanate addition reaction bridged through neutral polymeric bonding agent(NPBA)layer.The morphology and structure of the HMX-based composites were characterized in detail and the core-shell structure was validated.The grafted polymers obviously enhanced the adhesion force between HMX crystals and fluoropolymer(F2314)binder.Due to the interfacial reinforcement among the components,the two HMX-based composites exhibited a remarkable increment of phase transition peak temperature by 10.2°C and 19.6°C with no more than 1.5%shell content,respectively.Furthermore,the impact and friction sensitivity of the composites decreased significantly as a result of the barrier produced by the grafted polymers.These findings will enhance the future prospects for the interface design of energetic composites aiming to solve the weak interface and safety concerns.展开更多
In overlapping distribution areas of Sorbus pohuashanensis and S.discolor in North China(Mount Tuoliang,Mount Xiling and Mount Baihua),Sorbus indi-viduals were found with pink fruit,which have never been recorded for ...In overlapping distribution areas of Sorbus pohuashanensis and S.discolor in North China(Mount Tuoliang,Mount Xiling and Mount Baihua),Sorbus indi-viduals were found with pink fruit,which have never been recorded for the flora of China.Fourteen morphological characters combined with four chloroplast DNA markers and internal transcribed spacer(ITS)were used to analyze the origin of the Sorbus individuals with pink fruits and their relationship to S.pohuashanensis and S.discolor.PCA,SDA and one-way(taxon)ANOVA of morphological characters provided convincing evidence of the hybrid ori-gin of Sorbus individuals with pink fruits based on a novel morphological character and many intermediate characters.Haplotype analysis based on four cpDNA markers showed that either S.pohuashanensis or S.discolor were maternal parents of Sorbus individuals with pink fruits.Incongru-ence of the position of Sorbus individuals with pink fruits between cpDNA and ITS in cluster trees supported by DNA sequence comparative analysis,implying former hybridiza-tion events between S.pohuashanensis and S.discolor.Mul-tiple hybridization events between S.pohuashanensis and S.discolor might have contributed to the generation of Sorbus individuals with pink fruits.This study has provided insights into hybridization between species of the same genus in sympatric areas,which is of great significance for the study of interspecific hybridization.展开更多
Incorporating a selenium(Se)positive electrode into aluminum(Al)-ion batteries is an effective strategy for improving the overall battery performance.However,the cycling stability of Se positive electrodes has challen...Incorporating a selenium(Se)positive electrode into aluminum(Al)-ion batteries is an effective strategy for improving the overall battery performance.However,the cycling stability of Se positive electrodes has challenges due to the dissolution of intermediate reaction products.In this work,we aim to harness the advantages of Se while reducing its limitations by preparing a core-shell mesoporous carbon hollow sphere with a titanium nitride(C@TiN)host to load 63.9wt%Se as the positive electrode material for Al-Se batteries.Using the physical and chemical confinement offered by the hollow mesoporous carbon and TiN,the obtained core-shell mesoporous carbon hollow spheres coated with Se(Se@C@TiN)display superior utilization of the active material and remarkable cycling stability.As a result,Al-Se batteries equipped with the as-prepared Se@C@TiN composite positive electrodes show an initial discharge specific capacity of 377 mAh·g^(-1)at a current density of 1000 mA·g^(-1)while maintaining a discharge specific capacity of 86.0 mAh·g^(-1)over 200 cycles.This improved cycling performance is ascribed to the high electrical conductivity of the core-shell mesoporous carbon hollow spheres and the unique three-dimensional hierarchical architecture of Se@C@TiN.展开更多
The development of efficient single-atom catalysts(SACs) for the oxygen reduction reaction(ORR)remains a formidable challenge,primarily due to the symmetric charge distribution of metal singleatom sites(M-N_(4)).To ad...The development of efficient single-atom catalysts(SACs) for the oxygen reduction reaction(ORR)remains a formidable challenge,primarily due to the symmetric charge distribution of metal singleatom sites(M-N_(4)).To address such issue,herein,Fe-N_(x) sites coupled synergistic catalysts fabrication strategy is presented to break the uniform electronic distribution,thus enhancing the intrinsic catalytic activity.Precisely,atomically dispersed Fe-N_(x) sites supported on N/S-doped mesoporous carbon(NSC)coupled with FeS@C core-shell nanoparticles(FAS-NSC@950) is synthesized by a facile hydrothermal reaction and subsequent pyrolysis.Due to the presence of an in situ-grown conductive graphitic layer(shell),the FeS nanoparticles(core) effectively adjust the electronic structure of single-atom Fe sites and facilitate the ORR kinetics via short/long-range coupling interactions.Consequently,FAS-NSC@950displays a more positive half-wave potential(E_(1/2)) of 0.871 V with a significantly boosted ORR kinetics(Tafel slope=52.2 mV dec^(-1)),outpacing the commercial Pt/C(E_(1/2)=0.84 V and Tafel slope=54.6 mV dec^(-1)).As a bifunctional electrocatalyst,it displays a smaller bifunctional activity parameter(ΔE) of 0.673 V,surpassing the Pt/C-RuO_(2) combination(ΔE=0.724 V).Besides,the FAS-NSC@950-based zincair battery(ZAB) displays superior power density,specific capacity,and long-term cycling performance to the Pt/C-Ir/C-based ZAB.This work significantly contributes to the field by offering a promising strategy to enhance the catalytic activity of SACs for ORR,with potential implications for energy conversion and storage technologies.展开更多
Herein,we demonstrate the synthesis of bifunctional nickel cobalt selenide@nickel telluride(Ni_(x)Co_(12-x)Se@NiTe)core-shell heterostructures via an electrodeposition approach for overall urea electrolysis and superc...Herein,we demonstrate the synthesis of bifunctional nickel cobalt selenide@nickel telluride(Ni_(x)Co_(12-x)Se@NiTe)core-shell heterostructures via an electrodeposition approach for overall urea electrolysis and supercapacitors.The 3D vertically orientated NiTe dendritic frameworks induce the homogeneous nucleation of 2D Ni_(x)Co_(12-x)Se nanosheet arrays along similar crystal directions and bring a strong interfacial binding between the integrated active components.In particular,the optimized Ni_(6)Co_(6)Se@NiTe with an interface coupling effect works in concert to tune the intrinsic activity.It only needs a low overpotential of 1.33 V to yield a current density of 10 mA cm^(-2)for alkaline urea electrolysis.Meanwhile,the full urea catalysis driven only by Ni_(6)Co_(6)Se@NiTe achieves 10 mA cm^(-2)at a potential of 1.38 V and can approach a constant level of the current response for 40 h.Besides,the integrated Ni_(6)Co_(6)Se@NiTe electrode delivers an enhanced specific capacity(223 mA h g^(-1)at 1 A g^(-1))with a high cycling stability.Consequently,a hybrid asymmetric supercapacitor(HASC)device based on Ni_(6)Co_(6)Se@NiTe exhibits a favorable rate capability and reaches a high energy density of 67.7 Wh kg^(-1)and a power density of 724.8 W kg^(-1)with an exceptional capacity retention of 92.4%after sequential 12000 cycles at 5 A g^(-1).展开更多
A novel core-shell hydrogel bead was fabricated for effective removal of methylene blue dye from aqueous solutions.The core,made of sodium alginate-g-polyacrylamide and attapulgite nanofibers,was cross-linked by Calci...A novel core-shell hydrogel bead was fabricated for effective removal of methylene blue dye from aqueous solutions.The core,made of sodium alginate-g-polyacrylamide and attapulgite nanofibers,was cross-linked by Calcium ions(Ca^(2+)).The shell,composed of a chitosan/activated carbon mixture,was then coated onto the core.Fourier transform infrared spectroscopy confirmed the grafting polymerization of acrylamide onto sodium alginate.Scanning electron microscopy images showed the core-shell structure.The core exhibited a high water uptake ratio,facilitating the diffusion of methylene blue into the core.During the diffusion process,the methylene blue was first adsorbed by the shell and then further adsorbed by the core.Adsorption tests showed that the coreshell structure had a larger adsorption capacity than the core alone.The shell effectively enhanced the adsorption capacity to methylene blue compared to the single core.Methylene blue was adsorbed by activated carbon and chitosan in the shell,and the residual methylene blue diffused into the core and was further adsorbed.展开更多
Understanding the evolutionary and ecological processes involved in population differentiation and speciation provides critical insights into biodiversity formation. In this study, we employed 29,865 single nucleotide...Understanding the evolutionary and ecological processes involved in population differentiation and speciation provides critical insights into biodiversity formation. In this study, we employed 29,865 single nucleotide polymorphisms(SNPs) and complete plastomes to examine genomic divergence and hybridization in Gentiana aristata, which is endemic to the Qinghai-Tibet Plateau(QTP) region. Genetic clustering revealed that G. aristata is characterized by geographic genetic structures with five clusters(West, East, Central, South and North). The West cluster has a specific morphological character(i.e., blue corolla) and higher values of FSTcompared to the remaining clusters, likely the result of the geological barrier formed by the Yangtze River. The West cluster diverged from the other clusters in the Early Pliocene;these remaining clusters diverged from one another in the Early Quaternary. Phylogenetic reconstructions based on SNPs and plastid data revealed substantial cyto-nuclear conflicts. Genetic clustering and D-statistics demonstrated rampant hybridization between the Central and North clusters,along the Bayankala Mountains, which form the geological barrier between the Central and North clusters. Species distribution modeling demonstrated the range of G. aristata expanded since the Last Interglacial period. Our findings provide genetic and morphological evidence of cryptic diversity in G. aristata, and identified rampant hybridization between genetic clusters along a geological barrier.These findings suggest that geological barriers and climatic fluctuations have an important role in triggering diversification as well as hybridization, indicating that cryptic diversity and hybridization are essential factors in biodiversity formation within the QTP region.展开更多
基金Financial support by project of China Petroleum Engineering Corp., Ltd (CPEC), Study on microstructural regulation of polyacrylate and applying as pour-point depressant for crude oil (2021ZYGC-01-01)。
文摘The gelation of crude oil with high wax and asphaltene content at low temperatures often results in the block of transportation pipeline in Africa. In recent years, it was reported that surface hydrophobicmodified nanoparticles have important applications in crude oil flow modification. In this work, four kinds of core-shell hybride nanoparticles by grafting poly(octadecyl, docosyl acrylate) and poly(acrylate-α-olefin) onto the surface of nano-sized SiO_(2) were synthesized by grafting polymerization method.The chemical structure of nanoparticles was analyzed by Fourier transform infrared spectroscopy(FT-IR),scanning electron microscopy(SEM) and thermogravimetric analysis(TGA). The rheological behaviors of crude oil and precipitation of asphaltenes in the presence of nanoparticles were studied by measuring the viscose-temperature relationship curve, the cumulative wax precipitation amount, and morphology of waxes and asphaltenes. The results indicate that the docosyl polyacrylate@SiO_(2) nanoparticle(PDA@SiO_(2)) can reduce the cumulative wax precipitation amount of crude oil by 72.8%, decline the viscosity of crude oil by 85.6% at 20℃, reduce the average size of wax crystals by 89.7%, and inhibit the agglomeration of asphaltene by 74.8%. Therefore, the nanoparticles not only adjust the crystalline behaviors of waxes, but also inhibit the agglomeration of asphaltenes. Apparently, core-shell hybride nanoparticles provides more heterogeneous nucleation sites for the crystallization of wax molecules,thus inhibiting the formation of three-dimensional network structure. The core-shell polymer@SiO_(2) hybride nanoparticles are one of promising additives for inhibiting crystallization of waxes and agglomeration of asphaltenes in crude oil.
基金supported by the National Natural Science Foundation of China(21905253,51973200,and 52122308)the Natural Science Foundation of Henan(202300410372)the National Supercomputing Center in Zhengzhou
文摘The rational design of metal single-atom catalysts(SACs)for electrochemical nitrogen reduction reaction(NRR)is challenging.Two-dimensional metal-organic frameworks(2DMOFs)is a unique class of promising SACs.Up to now,the roles of individual metals,coordination atoms,and their synergy effect on the electroanalytic performance remain unclear.Therefore,in this work,a series of 2DMOFs with different metals and coordinating atoms are systematically investigated as electrocatalysts for ammonia synthesis using density functional theory calculations.For a specific metal,a proper metal-intermediate atoms p-d orbital hybridization interaction strength is found to be a key indicator for their NRR catalytic activities.The hybridization interaction strength can be quantitatively described with the p-/d-band center energy difference(Δd-p),which is found to be a sufficient descriptor for both the p-d hybridization strength and the NRR performance.The maximum free energy change(ΔG_(max))andΔd-p have a volcanic relationship with OsC_(4)(Se)_(4)located at the apex of the volcanic curve,showing the best NRR performance.The asymmetrical coordination environment could regulate the band structure subtly in terms of band overlap and positions.This work may shed new light on the application of orbital engineering in electrocatalytic NRR activity and especially promotes the rational design for SACs.
基金financially supported by the National Natural Science Foundation of China(21972068,22072067,22232004)the High-level Talents Project of Jinling Institute of Technology(jit-b-202164)。
文摘Precisely refining the electronic structure of electrocatalysts represents a powerful approach to further optimize the electrocatalytic performance.Herein,we demonstrate an ingenious d-d orbital hybridization concept to construct Mo-doped Co_(9)S_(8) nanorod arrays aligned on carbon cloth(CC)substrate(abbreviated as Mo-Co_(9)S_(8)@CC hereafter)as a high-efficiency bifunctional electrocatalyst toward water electrolysis.It has experimentally and theoretically validated that the 4d-3d orbital coupling between Mo dopant and Co site can effectively optimize the H_(2)O activation energy and lower H^(*)adsorption energy barrier,thereby leading to enhanced hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)activities.Thanks to the unique electronic and geometrical advantages,the optimized Mo-Co_(9)S_(8)@CC with appropriate Mo content exhibits outstanding bifunctional performance in alkaline solution,with the overpotentials of 75 and 234 mV for the delivery of a current density of 10 mA cm^(-2),small Tafel slopes of 53.8 and 39.9 mV dec~(-1)and long-term stabilities for at least 32 and 30 h for HER and OER,respectively.More impressively,a water splitting electrolylzer assembled by the self-supported Mo-Co_(9)S_(8)@CC electrode requires a low cell voltage of 1.53 V at 10 mA cm^(-2)and shows excellent stability and splendid reversibility,demonstrating a huge potential for affordable and scalable electrochemical H_(2) production.The innovational orbital hybridization strategy for electronic regulation herein provides an inspirable avenue for developing progressive electrocatalysts toward new energy systems.
基金Financial supports from the National Natural Science Foundation of China(No.50273035)Hangzhou Zhijiang Silicone Chemical Industry Co.,Ltd.are acknowledged.
文摘Siliconated polyurethane (Si-PU) was synthesized using isophorone diisocyanate (IPDI), hydroxybutyl-terminated polydimethylsiloxane (PDMS), polytetramethylene ether glycol (PTMG), polypropylene glycol (PPG), 1,6-hexanediol (HDO), dimethylol propionic acid (DMPA) and triethylamine (TEA). Based on butyl acrylate (BA), 2, 2, 2-trifluoroethylmethacrylate (TFEMA) and Si-PU as a seed emulsion, a novel core-shell type acrylic-polyurethane hybrid emulsion, containing siloxane and fluorine (F-Si-PU), was prepared by seeded emulsion polymerization. The contents of siloxane and fluorine were determined according to the feed ratio. Fourier transform infrared spectroscopy (FTIR) was used to identify the chain structures of Si-PU and F-Si-PU. Investigation of transmission electron microscopy (TEM) confirmed the core-shell structure of F-Si-PU emulsion. Measurement results of water contact angle and the swelling ratio in water and n-octane for cured film showed that the water and the oil resistances for F-Si-PU had been significantly improved at a suitable content of fluorine and siloxane.
文摘A core-shell composite consisting of ZSM-5 zeolite as the core and ordered mesoporous silica as the shell was prepared by a surfactant-controlled sol-gel process and using tetradecylamine(TDA) as the template and Tetraethylorthosilicate(TEOS) as the silica precursor.The pores of the silica shell were found to be ordered and perpendicular to the crystal faces of the zeolite core.The thickness of the shell in the coreshell structured composite can be adjusted in the range of 20-90 nm,while the surface morphology and the pore size distribution were modified by changing the mass ratio of TEOS to zeolite.The composite molecular sieves have higher surface area for capturing molecules than ZSM-5,and with the increase of mesoporous shell layer,the ZSM-5@SiO_(2)-x composites show stronger adsorption capacity of butyraldehyde.However,when the shell thickness exceeds 90 nm,the adsorption capacity of butyraldehyde decreases instead.The composites have a huge potential for environmental applications.
基金supported by Basic Science Research Program through the National Research Foundation of Korea (NRF) funded by the Ministry of Science and ICT (2023R1A2C100571511,RS-2023-00254424)the Ministry of Education(2020R1A6A1A03038540)。
文摘As the global electric vehicle market continues to grow,the recycling of Li-ion battery (LIB) becomes more important worldwide and the resynthesis of cathode materials would be the most value-added recycling approach taking into account limited metal resources.Although resynthesized homogenous LiNi_(x)Co_(y)Mn_(z)O_(2)(NCM) from spent LIB leachate shows comparable battery performance to pristine NCM from virgin materials,there is general concern in its cycling performance.Here,we synthesize core–shell(CS) Ni-rich NCM,which consists of Ni-rich NCM as the core and NCM derived from the original or purified leachate of spent LIBs as the shell.Resynthesized CS Ni-rich NCM exhibits improved rate capability resulting from expanded interslab thickness in the NCM structure.CS Ni-rich NCM from purified LIB leachate shows improvement in cycling performance and thermal stability.It specifically delivers a capacity retention of 86.6%at a high temperature after 80 cycles compared to that (75.0%) of pristine CS Ni-rich NCM.These improvements are caused by a relatively high Mg content on the shell and the widespread distribution of Al through the CS structure.CS Ni-rich NCM derived from spent LIB leachate provides a new alternative approach to conventional LIB recycling methods,which would utilize efficiently limited metal resources for the sustainable LIB production.
基金supported by the National Natural Science Foundation of China(61974125)the Open Innovation Fund for undergraduate students of Xiamen University(KFJJ-202411).
文摘Semiconductor photocatalysis holds great promise for renewable energy generation and environment remediation,but generally suffers from the serious drawbacks on light absorption,charge generation and transport,and structural stability that limit the performance.The core-shell semiconductorgraphene(CSSG)nanoarchitectures may address these issues due to their unique structures with exceptional physical and chemical properties.This review explores recent advances of the CSSG nanoarchitectures in the photocatalytic performance.It starts with the classification of the CSSG nanoarchitectures by the dimensionality.Then,the construction methods under internal and external driving forces were introduced and compared with each other.Afterward,the physicochemical properties and photocatalytic applications of these nanoarchitectures were discussed,with a focus on their role in photocatalysis.It ends with a summary and some perspectives on future development of the CSSG nanoarchitectures toward highly efficient photocatalysts with extensive application.By harnessing the synergistic capabilities of the CSSG architectures,we aim to address pressing environmental and energy challenges and drive scientific progress in these fields.
基金the National Key Research and Development Program of China(No.2016YFB0701100)the National Natural Science Foundation of China(Nos.51802015 and 51890893)Fundamental Research Funds for the Central Universities(FRFTP-16-028A1)。
文摘Building a covalently connected structure with accelerated photo-induced electrons and charge-carrier separation between semiconductors could enhance the photocatalytic performance.In this work,we report a facile and novel seed growth method to coat NH2-MIL-125 MOFs with crystalline and porous covalent organic frameworks(COFs)materials and form a range of NH2-MIL-125@TAPB-PDA nanocomposites with different thicknesses of COF shell.The introduction of appropriate content of COF could not only modify the intrinsic electronic and optical properties,but also enhance the photocatalytic activity distinctly.Especially,NH2-MIL-125@TAPB-PDA-3 with COF shell thickness of around 20nm exhibited the highest yield(94.7%)of benzaldehyde which is approximately 2.5 and 15.5 times as that of parental NH2-MIL-125 and COF,respectively.The promoted photocatalytic performance of hybrid materials was mainly owing to the enhanced photo-induced charge carriers transfer between the MOF and COF through the covalent bond.In addition,a possible mechanism to elucidate the process of photocatalysis was explored.Therefore,this kind of MOF-based photocatalysts possesses great potentials in future green organic synthesis.
基金supported by the National Natural Science Foundation of China(52161145409,21976116)SAFEA of China("Belt and Road”Innovative Talent Exchange Foreign Expert Project#2023041004L)(High-end Foreign Expert Project#G2023041021L)the Alexander-von-Humboldt Foundation of Germany(GroupLinkage Program)。
文摘Direct conversion of solar energy into chemical energy in an environmentally friendly manner is one of the most promising strategies to deal with the environmental pollution and energy crisis.Among a variety of materials developed as photocatalysts,the core-shell metal/covalent-organic framework(MOF or COF)photocatalysts have garnered significant attention due to their highly porous structure and the adjustability in both structure and functionality.The existing reviews on core-shell organic framework photocatalytic materials have mainly focused on core-shell MOF materials.However,there is still a lack of indepth reviews specifically addressing the photocatalytic performance of core-shell COFs and MOFs@COFs.Simultaneously,there is an urgent need for a comprehensive review encompassing these three types of core-shell structures.Based on this,this review aims to provide a comprehensive understanding and useful guidelines for the exploration of suitable core-shell organic framework photocatalysts towards appropriate photocatalytic energy conversion and environmental governance.Firstly,the classification,synthesis,formation mechanisms,and reasonable regulation of core-shell organic framework were summarized.Then,the photocatalytic applications of these three kinds of core-shell structures in different areas,such as H_(2)evolution,CO_(2)reduction,and pollutants degradation are emphasized.Finally,the main challenges and development prospects of core-shell organic framework photocatalysts were introduced.This review aims to provide insights into the development of a novel generation of efficient and stable core-shell organic framework materials for energy conversion and environmental remediation.
文摘Using interface engineering,a highly efficient catalyst with a shell@core structure was successfully synthesized by growing an amorphous material composed of Ni,Mo,and P on Cu nanowires(Ni-MoP@CuNWs).This catalyst only requires an overpotential of 35 mV to reach a current density of 10 mA cm^(-2).The exceptional hydrogen evolution reaction(HER)activity is attributed to the unique amorphous rod-like nature of NiMoP@CuNWs,which possesses a special hydrophilic feature,en-hances mass transfer,promotes effective contact between the electrode and electrolyte solution,and exposes more active sites during the catalytic process.Density functional theory revealed that the introduction of Mo weakens the binding strength of the Ni site on the catalyst surface with the H atom and promotes the desorption process of the H_(2) product significantly.Owing to its facile syn-thesis,low cost,and high catalytic performance,this electrocatalyst is a promising option for com-mercial applications as a water electrolysis catalyst.
基金supported by the National Natural Science Foundation of China(Nos.22176145,82172612)the State Key Laboratory of Fine Chemicals,Dalian University of Technology(KF 2001)the Fundamental Research Funds for the Central Universities(22120210137).
文摘The massive use of antibiotics has led to the aggravation of bacterial resistance and also brought environmental pollution problems.This poses a great threat to human health.If the dosage of antibiotics is reduced by increasing its bactericidal performance,the emergence of drug resistance is certainly delayed,so that there's not enough time for developing drug resistance during treatment.Therefore,we selected typical representative materials of metal Ag and semiconductor ZnO nano-bactericides to design and synthesize Ag/ZnO hollow core-shell structures(AZ for short).Antibiotics are grafted on the surface of AZ through rational modification to form a composite sterilization system.The research results show that the antibacterial efficiency of the composite system is significantly increased,from the sum(34.7%+22.8%-57.5%)of the antibacterial efficiency of AZ and gentamicin to 80.2%,net synergizes 22.7%,which fully reflects the effect of 1+1>2.Therefore,the dosage of antibiotics can be drastically reduced in this way,which makes both the possibility of bacterial resistance and medical expenses remarkably decrease.Subsequently,residual antibiotics can be degraded under simple illumination using AZ-self as a photocatalyst,which cuts off the path of environmental pollution.In short,such an innovative route has guiding significance for drug resistance.
基金Funded by the National Key Research and Development Program of China(No.2023YFB3812200)。
文摘A machine learning(ML)-based random forest(RF)classification model algorithm was employed to investigate the main factors affecting the formation of the core-shell structure of BaTiO_(3)-based ceramics and their interpretability was analyzed by using Shapley additive explanations(SHAP).An F1-score changed from 0.8795 to 0.9310,accuracy from 0.8450 to 0.9070,precision from 0.8714 to 0.9000,recall from 0.8929 to 0.9643,and ROC/AUC value of 0.97±0.03 was achieved by the RF classification with the optimal set of features containing only 5 features,demonstrating the high accuracy of our model and its high robustness.During the interpretability analysis of the model,it was found that the electronegativity,melting point,and sintering temperature of the dopant contribute highly to the formation of the core-shell structure,and based on these characteristics,specific ranges were delineated and twelve elements were finally obtained that met all the requirements,namely Si,Sc,Mn,Fe,Co,Ni,Pd,Er,Tm,Lu,Pa,and Cm.In the process of exploring the structure of the core-shell,the doping elements can be effectively localized to be selected by choosing the range of features.
基金financially supported by the National Key Research and Development Program of China(2021YFC2103300)the National Natural Science Foundation of China Youth Found(22308154 and 22108120)the Natural Science Foundation of Jiangsu Province(BK20231518 and BK20210549).
文摘Lysine is one of the essential amino acids for human body,and its imbalance is a major cause to anemia,aging process,leukemia cell proliferation and tumor growth.Therefore,its monitoring is dominative to the prevention the disease progress and guidance to the clinical treatment.However,traditional inhospital detection methods,such as colorimetry and fluorometric,often suffer the disadvantages of high cost and long time-consuming.These drawbacks show a difficulty in the home-in and dairy monitoring for the lysine regulation in body.In this study,we have proposed an ultrasensitive microchipbased portable device to achieve the onsite and precise determination of lysine within only 10 s.This microchip was functionalized through constructing a center-concave nanosheet of core-shell WO_(3)@Prussian blue(WO_(3)@PB)to remarkably strengthen the generation and transfer of the detection signal.In this special architecture,the core WO_(3)nanosheet can be exposed at the center region of this nanocomposite to effectively promote the enzymatic oxidation,while the PB shell enables to strongly reduce the H_(2)O_(2)produced by the enzymatic reaction.Under above synergetic effects,a handheld device was designed to support the plug-and-play microchip,which performed an outstanding accuracy for the lysine detection in blood.
基金the support for this work by National Natural Science Foundation of China(Grant Nos.22175139 and 22105156)。
文摘The weak interface interaction and solid-solid phase transition have long been a conundrum for 1,3,5,7-tetranitro-1,3,5,7-tetraazacyclooctane(HMX)-based polymer-bonded explosives(PBX).A two-step strategy that involves the pretreatment of HMX to endow—OH groups on the surface via polyalcohol bonding agent modification and in situ coating with nitrate ester-containing polymer,was proposed to address the problem.Two types of energetic polyether—glycidyl azide polymer(GAP)and nitrate modified GAP(GNP)were grafted onto HMX crystal based on isocyanate addition reaction bridged through neutral polymeric bonding agent(NPBA)layer.The morphology and structure of the HMX-based composites were characterized in detail and the core-shell structure was validated.The grafted polymers obviously enhanced the adhesion force between HMX crystals and fluoropolymer(F2314)binder.Due to the interfacial reinforcement among the components,the two HMX-based composites exhibited a remarkable increment of phase transition peak temperature by 10.2°C and 19.6°C with no more than 1.5%shell content,respectively.Furthermore,the impact and friction sensitivity of the composites decreased significantly as a result of the barrier produced by the grafted polymers.These findings will enhance the future prospects for the interface design of energetic composites aiming to solve the weak interface and safety concerns.
基金This study was supported by the National Natural Science Foundation of China,Grant/Award Number:32071779.
文摘In overlapping distribution areas of Sorbus pohuashanensis and S.discolor in North China(Mount Tuoliang,Mount Xiling and Mount Baihua),Sorbus indi-viduals were found with pink fruit,which have never been recorded for the flora of China.Fourteen morphological characters combined with four chloroplast DNA markers and internal transcribed spacer(ITS)were used to analyze the origin of the Sorbus individuals with pink fruits and their relationship to S.pohuashanensis and S.discolor.PCA,SDA and one-way(taxon)ANOVA of morphological characters provided convincing evidence of the hybrid ori-gin of Sorbus individuals with pink fruits based on a novel morphological character and many intermediate characters.Haplotype analysis based on four cpDNA markers showed that either S.pohuashanensis or S.discolor were maternal parents of Sorbus individuals with pink fruits.Incongru-ence of the position of Sorbus individuals with pink fruits between cpDNA and ITS in cluster trees supported by DNA sequence comparative analysis,implying former hybridiza-tion events between S.pohuashanensis and S.discolor.Mul-tiple hybridization events between S.pohuashanensis and S.discolor might have contributed to the generation of Sorbus individuals with pink fruits.This study has provided insights into hybridization between species of the same genus in sympatric areas,which is of great significance for the study of interspecific hybridization.
基金supported by the National Natural Science Foundation of China(No.52374350)China Postdoctoral Science Foundation(Nos.2020M680347 and 2021T140051)the Fundamental Research Funds for the Central Universities(No.FRF-TP-20-045A1)。
文摘Incorporating a selenium(Se)positive electrode into aluminum(Al)-ion batteries is an effective strategy for improving the overall battery performance.However,the cycling stability of Se positive electrodes has challenges due to the dissolution of intermediate reaction products.In this work,we aim to harness the advantages of Se while reducing its limitations by preparing a core-shell mesoporous carbon hollow sphere with a titanium nitride(C@TiN)host to load 63.9wt%Se as the positive electrode material for Al-Se batteries.Using the physical and chemical confinement offered by the hollow mesoporous carbon and TiN,the obtained core-shell mesoporous carbon hollow spheres coated with Se(Se@C@TiN)display superior utilization of the active material and remarkable cycling stability.As a result,Al-Se batteries equipped with the as-prepared Se@C@TiN composite positive electrodes show an initial discharge specific capacity of 377 mAh·g^(-1)at a current density of 1000 mA·g^(-1)while maintaining a discharge specific capacity of 86.0 mAh·g^(-1)over 200 cycles.This improved cycling performance is ascribed to the high electrical conductivity of the core-shell mesoporous carbon hollow spheres and the unique three-dimensional hierarchical architecture of Se@C@TiN.
基金financially supported by the National Natural Science Foundation of China(21773024)the Natural Science Foundation of Sichuan Province of China(2023NSFC0084)the China Postdoctoral Science Foundation(2019M663469)。
文摘The development of efficient single-atom catalysts(SACs) for the oxygen reduction reaction(ORR)remains a formidable challenge,primarily due to the symmetric charge distribution of metal singleatom sites(M-N_(4)).To address such issue,herein,Fe-N_(x) sites coupled synergistic catalysts fabrication strategy is presented to break the uniform electronic distribution,thus enhancing the intrinsic catalytic activity.Precisely,atomically dispersed Fe-N_(x) sites supported on N/S-doped mesoporous carbon(NSC)coupled with FeS@C core-shell nanoparticles(FAS-NSC@950) is synthesized by a facile hydrothermal reaction and subsequent pyrolysis.Due to the presence of an in situ-grown conductive graphitic layer(shell),the FeS nanoparticles(core) effectively adjust the electronic structure of single-atom Fe sites and facilitate the ORR kinetics via short/long-range coupling interactions.Consequently,FAS-NSC@950displays a more positive half-wave potential(E_(1/2)) of 0.871 V with a significantly boosted ORR kinetics(Tafel slope=52.2 mV dec^(-1)),outpacing the commercial Pt/C(E_(1/2)=0.84 V and Tafel slope=54.6 mV dec^(-1)).As a bifunctional electrocatalyst,it displays a smaller bifunctional activity parameter(ΔE) of 0.673 V,surpassing the Pt/C-RuO_(2) combination(ΔE=0.724 V).Besides,the FAS-NSC@950-based zincair battery(ZAB) displays superior power density,specific capacity,and long-term cycling performance to the Pt/C-Ir/C-based ZAB.This work significantly contributes to the field by offering a promising strategy to enhance the catalytic activity of SACs for ORR,with potential implications for energy conversion and storage technologies.
基金supported by the open fund of the National Defense Key Discipline Laboratory of New Micro/Nano Devices and System Technology,Zhejiang Provincial Natural Science Foundation of China,under Grant No.LY19E020014NSFC(Grant Nos 21303162 and 11604295)
文摘Herein,we demonstrate the synthesis of bifunctional nickel cobalt selenide@nickel telluride(Ni_(x)Co_(12-x)Se@NiTe)core-shell heterostructures via an electrodeposition approach for overall urea electrolysis and supercapacitors.The 3D vertically orientated NiTe dendritic frameworks induce the homogeneous nucleation of 2D Ni_(x)Co_(12-x)Se nanosheet arrays along similar crystal directions and bring a strong interfacial binding between the integrated active components.In particular,the optimized Ni_(6)Co_(6)Se@NiTe with an interface coupling effect works in concert to tune the intrinsic activity.It only needs a low overpotential of 1.33 V to yield a current density of 10 mA cm^(-2)for alkaline urea electrolysis.Meanwhile,the full urea catalysis driven only by Ni_(6)Co_(6)Se@NiTe achieves 10 mA cm^(-2)at a potential of 1.38 V and can approach a constant level of the current response for 40 h.Besides,the integrated Ni_(6)Co_(6)Se@NiTe electrode delivers an enhanced specific capacity(223 mA h g^(-1)at 1 A g^(-1))with a high cycling stability.Consequently,a hybrid asymmetric supercapacitor(HASC)device based on Ni_(6)Co_(6)Se@NiTe exhibits a favorable rate capability and reaches a high energy density of 67.7 Wh kg^(-1)and a power density of 724.8 W kg^(-1)with an exceptional capacity retention of 92.4%after sequential 12000 cycles at 5 A g^(-1).
文摘A novel core-shell hydrogel bead was fabricated for effective removal of methylene blue dye from aqueous solutions.The core,made of sodium alginate-g-polyacrylamide and attapulgite nanofibers,was cross-linked by Calcium ions(Ca^(2+)).The shell,composed of a chitosan/activated carbon mixture,was then coated onto the core.Fourier transform infrared spectroscopy confirmed the grafting polymerization of acrylamide onto sodium alginate.Scanning electron microscopy images showed the core-shell structure.The core exhibited a high water uptake ratio,facilitating the diffusion of methylene blue into the core.During the diffusion process,the methylene blue was first adsorbed by the shell and then further adsorbed by the core.Adsorption tests showed that the coreshell structure had a larger adsorption capacity than the core alone.The shell effectively enhanced the adsorption capacity to methylene blue compared to the single core.Methylene blue was adsorbed by activated carbon and chitosan in the shell,and the residual methylene blue diffused into the core and was further adsorbed.
基金financial support provided by the Foundation of Henan Educational Committee (22A180024)Natural Science Foundation of Henan Province (232300420212)。
文摘Understanding the evolutionary and ecological processes involved in population differentiation and speciation provides critical insights into biodiversity formation. In this study, we employed 29,865 single nucleotide polymorphisms(SNPs) and complete plastomes to examine genomic divergence and hybridization in Gentiana aristata, which is endemic to the Qinghai-Tibet Plateau(QTP) region. Genetic clustering revealed that G. aristata is characterized by geographic genetic structures with five clusters(West, East, Central, South and North). The West cluster has a specific morphological character(i.e., blue corolla) and higher values of FSTcompared to the remaining clusters, likely the result of the geological barrier formed by the Yangtze River. The West cluster diverged from the other clusters in the Early Pliocene;these remaining clusters diverged from one another in the Early Quaternary. Phylogenetic reconstructions based on SNPs and plastid data revealed substantial cyto-nuclear conflicts. Genetic clustering and D-statistics demonstrated rampant hybridization between the Central and North clusters,along the Bayankala Mountains, which form the geological barrier between the Central and North clusters. Species distribution modeling demonstrated the range of G. aristata expanded since the Last Interglacial period. Our findings provide genetic and morphological evidence of cryptic diversity in G. aristata, and identified rampant hybridization between genetic clusters along a geological barrier.These findings suggest that geological barriers and climatic fluctuations have an important role in triggering diversification as well as hybridization, indicating that cryptic diversity and hybridization are essential factors in biodiversity formation within the QTP region.