Dual-function communication radar systems use common Radio Frequency(RF)signals are used for both communication and detection.For better compatibility with existing communication systems,we adopt Multiple-Input Multip...Dual-function communication radar systems use common Radio Frequency(RF)signals are used for both communication and detection.For better compatibility with existing communication systems,we adopt Multiple-Input Multiple-Output(MIMO)Orthogonal Frequency Division Multiplexing(OFDM)signals as integrated signals and investigate the estimation performance of MIMO-OFDM signals.First,we analyze the Cramer-Rao Lower Bound(CRLB)of parameter estimation.Then,the transmit powers over different subcarriers are optimized to achieve the best tradeoff between the transmission rate and the estimation performance.Finally,we propose a more accurate estimation method that uses Canonical Polyadic Decomposition(CPD)of the third-order tensor to obtain the parameter matrices.Due to the characteristic of the column structure of the parameter matrices,we only need to use DFT/IDFT to recover the parameters of multiple targets.The simulation results show that tensor-based estimation method can achieve a performance close to CRLB,and the estimation performance can be improved by optimizing the transmit powers.展开更多
Wireless capsule endoscopy(WCE)has the potential to fully replace conventional wired counterparts for its low invasiveness.Recent studies have attempted to expand the functions of capsules toward this goal.However,lim...Wireless capsule endoscopy(WCE)has the potential to fully replace conventional wired counterparts for its low invasiveness.Recent studies have attempted to expand the functions of capsules toward this goal.However,limitations in space and energy supply have resulted in the inability to perform multiple diagnostic and treatment tasks using a single capsule.In this study,we developed a dual-functional capsule robot(DFCR)for drug delivery and tissue biopsy based on magnetic torsion spring technology.The delivery module was shown to rotate the push rod with a thrust of 894 mN to release approximately 0.3 mL of semisolid drug.The biopsy module used a built-in blade to cut tissue with a shear stress of 22.87 MPa,producing a sample of approximately 1.8 mm3.Additionally,a five-degree-of-freedom permanent magnet drive system was developed.By adjusting the strength of the unidirectional magnetic field generated by an external magnet,the capsule can be wirelessly controlled to sequentially trigger the two functions.Ex vivo tests on porcine stomachs confirmed the feasibility of the prototype capsule(12 mm in diameter and 45 mm in length)in active movement,medication,and tissue biopsy.The newly developed DFCR further expands the clinical application prospects of WCE robots in minimally invasive surgery.展开更多
The intrinsic poor electrical conductivity,severe dissolution of K x S y intermediates,and inferior conversion reaction reversibility extremely impede the practical application of the transition-metal chalcogenides(TM...The intrinsic poor electrical conductivity,severe dissolution of K x S y intermediates,and inferior conversion reaction reversibility extremely impede the practical application of the transition-metal chalcogenides(TMDs)anode for potassium-ion batteries(PIBs).Herein,a rationally designed Cu_(9)S_(5)/MoS_(2)/C heterostruc-ture hollow nanocage was synthesized with assistance from metal-organic frameworks(MOFs)precursor.During the K-storage process,the homogeneously distributed the sulfiphilic nature of Cu 0 reaction prod-uct could act as a dual-functional catalyst,not only facilitating the rapid charge transfer but also effec-tively anchoring(K x S y)polysulfides,thus boosting K-storage reactions reversibility during the conversion reaction process.When applied as an anode for PIBs,the as-prepared heterostructure exhibits excellent reversible capacity and long cycle lifespan(350.5 mAh g^(-1)at 0.1 A g^(-1)and 0.04%per cycle capacity de-cay at 1 A g^(-1)after 1000 cycles).Additionally,the potassium storage mechanism is distinctly revealed by in-situ characterizations.The nanoarchitecture designing strategy for the advanced electrode in this work could provide vital guidance for relevant energy storage materials.展开更多
In this paper,we investigate an reconfigurable intelligent surface-aided Integrated Sensing And Communication(ISAC)system.Our objective is to maximize the achievable sum rate of the multi-antenna communication users t...In this paper,we investigate an reconfigurable intelligent surface-aided Integrated Sensing And Communication(ISAC)system.Our objective is to maximize the achievable sum rate of the multi-antenna communication users through the joint active and passive beamforming.Specifically,the weighted minimum mean-square error method is first used to reformulate the original problem into an equivalent one.Then,we utilize an alternating optimization algorithm to decouple the optimization variables and decompose this challenging problem into two subproblems.Given reflecting coefficients,a penalty-based algorithm is utilized to deal with the non-convex radar Signal-to-Noise Ratio(SNR)constraints.For the given beamforming matrix of the base station,we apply majorization-minimization to transform the problem into a Quadratic Constraint Quadratic Programming(QCQP)problem,which is ultimately solved using a Semi-Definite Relaxation(SDR)based algorithm.Simulation results illustrate the advantage of deploying reconfigurable intelligent surface in the considered multi-user MultipleInput Multiple-Output(MIMO)ISAC systems.展开更多
Photocatalytic water splitting is a promising way to produce H_(2),a green and clean energy source.However,efficient H_(2) production typically relies on the addition of electron donors,such as alcohols and acids,whic...Photocatalytic water splitting is a promising way to produce H_(2),a green and clean energy source.However,efficient H_(2) production typically relies on the addition of electron donors,such as alcohols and acids,which are neither environmentally friendly nor cost-effective.Recently,we have witnessed a surge of studies in coupling photocatalytic H_(2) evolution with organic pollutant oxidation,which significantly promotes charge separation and improves the overall photocatalytic efficiency.It is thus an opportune time to critically assess the recent literature concerning dual-functional photocatalytic systems and provide perspectives for its future development.In this minireview,we begin with the working principles and requirements for synergistic photocatalytic systems.We then summarize and critically discuss the recent advances in photocatalytic H_(2) production and the degradation of various organic pollutants,including antibiotics,dyes,and phenols.Finally,we discuss the current challenges and suggest future directions for this field.展开更多
The development of an efficient dual-function catalytic-sorption system,which seamlessly integrates reaction and separation into a single step for extractant-free systems,represents a transformative advancement in oxi...The development of an efficient dual-function catalytic-sorption system,which seamlessly integrates reaction and separation into a single step for extractant-free systems,represents a transformative advancement in oxidative desulfurization(ODS)process.In this work,we introduce a novel dualfunction amphiphilic biochar(Mo/CBC)catalyst,functionalized with MoO_(3-x)featuring abundant oxygen vacancies,for highly effective extractant-free ODS.The polarity of the biochar was precisely tailored by varying the amount of KOH,leading to the creation of amphiphilic carriers.Subsequent ball milling facilitated the successful loading of MoO_(3-x)onto the biochar surface via an impregnation-calcination route leveraging carbon reduction,resulting in the synthesis of amphiphilic Mo/CBC catalysts.The amphiphilic nature of these catalysts ensures their stable dispersion within the oil phase,while also facilitating their interaction with the oxidant H2O2 and the adsorption of sulfur-containing oxidation products.Characterization techniques,including EPR,XPS,and in situ XRD,verified the existence of abundant oxygen vacancies obtained by carbon reduction on the amphiphilic Mo/CBC catalysts,which significantly boosted their activity in an extractant-free ODs system.Remarkably,the amphiphilic Mo/CBC catalyst displayed exceptional catalytic performance,achieving a desulfurization efficiency of 99.6%in just 10 min without extraction solvent.DFT theoretical calculations further revealed that H_(2)O_(2)readily dissociates into two OH radicals on the O_(vac)-MoO_(3),overcoming a low energy barrier.This process was identified as a key contributor to the catalyst's outstanding ODS performance.Furthermore,other biochar sources,such as rice straw,bamboo,rapeseed oil cake,and walnut oil cake,were investigated to produce Mo-based amphiphilic biochar catalysts,which all showed excellent desulfurization performance.This work establishes a versatile and highly efficient dual-function catalytic-sorption system by designing amphiphilic biochar catalysts enriched with oxygen vacancies,paving the way for the development of universally applicable ODS catalysts for industrial applications.展开更多
Herein,the Nd@g-C_(3)N_(4) dual-functional photocatalysis enabled fluoroalkylative heteroarylation of alkenes with R_(f)SO_(2)Cl under visible-light and ultrasound conditions was firstly reported.The photogenerated el...Herein,the Nd@g-C_(3)N_(4) dual-functional photocatalysis enabled fluoroalkylative heteroarylation of alkenes with R_(f)SO_(2)Cl under visible-light and ultrasound conditions was firstly reported.The photogenerated electron-driven reductive production of fluoroalkyl radical paired with photogenerated hole-driven oxidative production of chloride radical resulted in the full utilization of photogenerated carrier for bond formation.A wide range of N-heteroarenes,alkenes and R_(f)SO_(2)Cl,were well compatible for this reaction to access valuable fluoroalkylated N-heteroarenes with diverse structural features.The antitumor potential of synthesized fluoroalkylated N-heterocycles against Glioma 261 cells was evaluated by CCK8 assay.Notably,compound 4 aka demonstrated remarkable efficacy,exhibiting approximately sevenfold greater potency than temozolomide,a widely used chemotherapeutic agent.展开更多
Herein,the effect of the Ru:Ni bimetallic composition in dual-function materials(DFMs)for the integrated CO_(2)capture and methanation process(ICCU-Methanation)is systematically evaluated and combined with a thorough ...Herein,the effect of the Ru:Ni bimetallic composition in dual-function materials(DFMs)for the integrated CO_(2)capture and methanation process(ICCU-Methanation)is systematically evaluated and combined with a thorough material characterization,as well as a mechanistic(in-situ diffuse reflectance infrared fourier-transform spectroscopy(in-situ DRIFTS))and computational(computational fluid dynamics(CFD)modelling)investigation,in order to improve the performance of Ni-based DFMs.The bimetallic DFMs are comprised of a main Ni active metallic phase(20 wt%)and are modified with low Ru loadings in the 0.1-1 wt%range(to keep the material cost low),supported on Na_(2)O/Al_(2)O_(3).It is shown that the addition of even a very low Ru loading(0.1-0.2 wt%)can drastically improve the material reducibility,exposing a significantly higher amount of surface-active metallic sites,with Ru being highly dispersed over the support and the Ni phase,while also forming some small Ru particles.This manifests in a significant enhancement in the CH_(4)yield and the CH_(4)production kinetics during ICCU-Methanation(which mainly proceeds via formate intermediates),with 0.2 wt%Ru addition leading to the best results.This bimetallic DFM also shows high stability and a relatively good performance under an oxidizing CO_(2)capture atmosphere.The formation rate of CH_(4)during hydrogenation is then further validated via CFD modelling and the developed model is subsequently applied in the prediction of the effect of other parameters,including the inlet H_(2)concentration,inlet flow rate,dual-fu nction material weight,and reactor internal diameter.展开更多
Exploring cost-effective and efficient catalysts for oxygen reduction reaction(ORR)poses a significant challenge,espe-cially in the pursuit of alternatives to precious metals like platinum.Significant advancements hav...Exploring cost-effective and efficient catalysts for oxygen reduction reaction(ORR)poses a significant challenge,espe-cially in the pursuit of alternatives to precious metals like platinum.Significant advancements have driven electrochem-ists to develop efficient ORR catalysts using abundant materials,particularly iron(Fe)-based,known for their exceptional performance in ORR.While the crucial function of Fe in boosting ORR catalytic activity is recognized,the connection between material attributes and catalytic performance remains enigmatic.Understanding the dynamic processes involved in oxygen electrocatalysis is paramount for designing precious-metals-free ORR electrocatalysts.Mössbauer spectroscopy stands out as a powerful technique for deciphering the structural characteristics of Fe species in catalysis,facilitating the identification of active sites and the clarification of catalytic mechanisms.By showcasing noteworthy case studies within this review,we demonstrate the application of in-situ/operando 57Fe Mössbauer spectroscopy across diverse Fe-involved materials in ORR catalysis.This sheds light on various aspects of ORR catalysis,such as identifying active sites,assessing stability,and understanding the reaction mechanism.Our inquiry drives towards the opportunities and hurdles associ-ated with Mössbauer spectroscopy,unveiling potential breakthroughs and avenues for enhancement within this pivotal research realm.展开更多
The design and fabrication of ordered epitaxial MOF-on-MOF heterostructures as highly efficient electrocatalysts for water splitting is crucial but still challenging.In this study,a simple coordination-driven self-ass...The design and fabrication of ordered epitaxial MOF-on-MOF heterostructures as highly efficient electrocatalysts for water splitting is crucial but still challenging.In this study,a simple coordination-driven self-assembly method is used to fabricate controllable MOF-on-MOF multiscale heterostructures,where triangular host MOF(ZIF-67)nanosheets undergo in situ epitaxial growth to form uniform orthogonal vip MOF(CoFe PBA)nanosheets.Phosphorus(P)is further introduced in situ to fabricate CoP and Fe_(2)P heterostructured nanosheets(CoFe-P-NS),which exhibit excellent bifunctional electrocatalytic performance due to the enhancement of intrinsic electrocatalytic activity by p-d orbital hybridization.Specifically,the CoFe-P-NS requires low overpotential of 259 and 307 mV to reach 500 mA cm−2 for HER and OER,respectively.Remarkably,the assembled electrolysis cell maintained a large current density of 300 mA cm−2 for over 360 h with negligible voltage increase during alkaline seawater electrolysis.Experiments and theoretical calculations show that the synergistic catalytic activity of bimetallic phosphides arises from p-d orbital hybridization,where the CoP-P sites enhance HER by optimizing H*adsorption in the Volmer-Heyrovsky steps,while the Fe_(2)P-Fe sites accelerate OER by lowering the energy barrier of the rate-determining step from O*to OOH*.This study provides valuable insights into the design of a controllable MOF-on-MOF-based electrocatalyst toward alkaline seawater splitting.展开更多
Electrocatalytic nitrate-to-ammonia conversion offers dual environmental and sustainable synthesis benefits,but achieving high efficiency with low-cost catalysts remains a major challenge.This review focuses on cobalt...Electrocatalytic nitrate-to-ammonia conversion offers dual environmental and sustainable synthesis benefits,but achieving high efficiency with low-cost catalysts remains a major challenge.This review focuses on cobalt-based electrocatalysts,emphasizing their structural engineering for enhanced the performance of electrocatalytic nitrate reduction reaction(NO3RR)through dimensional control,compositional tuning,and coordination microenvironment modulation.Notably,by critically analyzing metallic cobalt,cobalt alloys,cobalt compounds,cobalt single atom and molecular catalyst configurations,we firstly establish correlations between atomic-scale structural features and catalytic performance in a coordination environment perspective for NO3RR,including the dynamic reconstruction during operation and its impact on active site.Synergizing experimental breakthroughs with computational modeling,we decode mechanisms underlying competitive hydrogen evolution suppression,intermediate adsorption-energy optimization,and durability enhancement in complex aqueous environments.The development of cobalt-based catalysts was summarized and prospected,and the emerging opportunities of machine learning in accelerating the research and development of high-performance catalysts and the configuration of series reactors for scalable nitrate-to-ammonia systems were also introduced.Bridging surface science and applications,it outlines a framework for designing multifunctional electrocatalysts to restore nitrogen cycle balance sustainably.展开更多
Structural engineering of Pt-based nanoalloys is crucial for the rational design and manufacturing of high-performance and low-cost electrocatalysts for hydrogen evolution reaction(HER).Here,we reported PtNi nanoparti...Structural engineering of Pt-based nanoalloys is crucial for the rational design and manufacturing of high-performance and low-cost electrocatalysts for hydrogen evolution reaction(HER).Here,we reported PtNi nanoparticles with a refined size of 2.71 nm and regular strains loaded on carbon black,synthesized using the high-temperature liquid shock(HTLS)method.This approach offers significant advantages over conventional synthesis methods,including high scalability,rapid reaction rates,and precise control over the size and shape of nanocrystals.Importantly,the synthesized PtNi electrocatalysts demonstrate outstanding catalytic activity and long-term stability for HER,achieving low overpotentials of 19 and 203 mV at current densities of 10 and 1000 mA/cm^(2),respectively.The superior performance can be attributed to the combination of a refined particle size,lattice strains,and synergistic effects between Pt and Ni.This rapid liquid-state synthesis demonstrated here holds great potential for scalable and industrial manufacturing of micro-/nano-catalysts.展开更多
Co_(3)S_(4)electrocatalysts with mixed valences of Co ions and excellent structural stability possess favorable oxygen evolution reaction(OER)activity,yet challenges remain in fabricating rechargeable lithiumoxygen ba...Co_(3)S_(4)electrocatalysts with mixed valences of Co ions and excellent structural stability possess favorable oxygen evolution reaction(OER)activity,yet challenges remain in fabricating rechargeable lithiumoxygen batteries(LOBs)due to their poor OER performance,resulting from poor electrical conductivity and overly strong intermediate adsorption.In this work,fancy double heterojunctions on 1T/2H-MoS_(2)@Co_(3)S_(4)(1T/2H-MCS)were constructed derived from the charge donation from Co to Mo ions,thus inducing the phase transformation of Mo S_(2)from 2H to 1T.The unique features of these double heterojunctions endow the1T/2H-MCS with complementary catalysis during charging and discharging processes.It is worth noting that 1T-Mo S2@Co3S4could provide fast Co-S-Mo electron transport channels to promote ORR/OER kinetics,and 2H-MoS_(2)@Co_(3)S_(4)contributed to enabling moderate egorbital occupancy when adsorbed with oxygen-containing intermediates.On the basis,the Li_(2)O_(2)nucleation route was changed to solution and surface dual pathways,improving reversible deposition and decomposition kinetics.As a result,1T/2H-MCS cathodes exhibit an improved electrocatalytic performance compared with those of Co_(3)S_(4)and Mo S2cathodes.This innovative heterostructure design provides a reliable strategy to construct efficient transition metal sulfide catalysts by improving electrical conductivity and modulating adsorption toward oxygenated intermediates for LOBs.展开更多
Hydrogen,as a green and clean next-generation fuel,is a key to achieving the goal of carbon neutrality.Constructing an electrocatalyst with bifunctional hydrogen evolution and oxygen evolution activity in the same ele...Hydrogen,as a green and clean next-generation fuel,is a key to achieving the goal of carbon neutrality.Constructing an electrocatalyst with bifunctional hydrogen evolution and oxygen evolution activity in the same electrolyte is a key technology for producing hydrogen via water splitting.Herein,a bimetallic active site catalyst,which possessed an edge-riched MoS_(2)nanoflakes array vertically growing on cubic CoS_(2),forming a nuclear-shell heterogeneous configuration,termed CSC-Mo S_(2)@Co S_(2).was reported The optimal CSC-Mo S_(2)@Co S_(2)-24 possessed good dualfunctional electrocatalytic activity(hydrogen evolution(HER),10 m A·cm^(-2)@241.5 m V and oxygen evolution(OER),10 m A·cm^(-2)@350 m V).Especially,CSC-Mo S_(2)@CoS_(2)-24 exhibited an extremely high mass activity for HER,and only required an overpotential of~550 m V when reaching a large current density of 1422 m A·mg^(-1),which was20.6-fold that of the bulk CoS_(2)(69 m A·mg^(-1)),as well as exhibiting stability of up to 100 h.The good electrocatalytic performance was attributed to the nuclear-shell heterostructure of Mo S_(2)@CoS_(2)hybrid could bring critical synergies,improving efficient mass transfer and electron transfer processes between Co S_(2)and Mo S_(2),which collaboratively promoted the electrocatalytic kinetics.It is foreseeable that the method proposed in this work will have guiding value for the preparation of dual-functional electrocatalysts with multi-interface heterostructures by assembling layered sulfides on cubic sulfides.展开更多
There is no study on food-derived peptide with both anticoagulant and angiotensin I-converting enzyme inhibitory (ACEI) activities yet. In this work, the anticoagulant and ACEI activities of the casein hydrolysates re...There is no study on food-derived peptide with both anticoagulant and angiotensin I-converting enzyme inhibitory (ACEI) activities yet. In this work, the anticoagulant and ACEI activities of the casein hydrolysates released by pepsin digestion were evaluated for the first time to the best of our knowledge. Results indicated that the casein hydrolysate exhibited potent anticoagulant activity by prolonging the thrombin time (TT) and the activated partial thromboplastin time (APTT). Compared with control samples, at 10 mg/mL, the TT and APTT of casein hydrolysate were 186.0 % ± 6.6 % and 163.5 % ± 7.4 %, respectively. The casein hydrolysate also showed a strong ACEI activity with an IC50 value of 1.775 mg/mL. The components of the bioactive casein hydrolysate were analyzed by nanoscale liquid chromatography quadrupole time-of-flight tandem mass spectrometry (NanoLC-Q-TOF-MS/MS). Total of 115 peptides were identified, among which 34, 9, 55 and 17 peptides were derived from α_(s1-), α_(s2-), β-, and κ-casein, respectively. The results of PeptideRanker and PepSite 2 analysis showed that 6 peptides (FRQFYQL, NENLLRF, NPWDQVKR, PVVVPPFLQ, PVRGPFPIIV, and ARHPHPHLSF) have both ACEI and anticoagulant activities by binding to the active sites of ACE and thrombin. This study indicated that casein is a potential functional food supplement that can be used for medical purposes.展开更多
Developing sulfur cathodes with high catalytic activity on accelerating the sluggish redox kinetics of lithium polysulfides(Li PSs) and unveiling their mechanisms are pivotal for advanced lithium–sulfur(Li–S)batteri...Developing sulfur cathodes with high catalytic activity on accelerating the sluggish redox kinetics of lithium polysulfides(Li PSs) and unveiling their mechanisms are pivotal for advanced lithium–sulfur(Li–S)batteries. Herein, MoS2 is verified to reduce the Gibbs free energy for rate-limiting step of sulfur reduction and the dissociation energy of lithium sulfide(Li2 S) for the first time employing theoretical calculations. The Mo S2 nanosheets coated on mesoporous hollow carbon spheres(MHCS) are then reasonably designed as a sulfur host for high-capacity and long-life Li–S battery, in which MHCS can guarantee the high sulfur loading and fast electron/ion transfer. It is revealed that the shuttle effect is efficiently inhibited because of the boosted conversion of Li PSs. As a result, the coin cell based on the MHCS@Mo S2-S cathode exhibits stable cycling performance maintaining 735.7 mAh g^(-1) after 500 cycles at 1.0 C. More importantly, the pouch cell employing the MHCS@Mo S2-S cathodes achieves high specific capacity of1353.2 m Ah g^(-1) and prominent cycle stability that remaining 960.0 m Ah g^(-1) with extraordinary capacity retention of 79.8% at 0.1 C after 170 cycles. Therefore, this work paves a new avenue for developing practical high specific energy and long-life pouch-type Li–S batteries.展开更多
Although extremely challenging,it is highly desirable to develop self-healing materials that exhibit high efficiency under environmental conditions for marine protection applications.In this work,polyurethane elastome...Although extremely challenging,it is highly desirable to develop self-healing materials that exhibit high efficiency under environmental conditions for marine protection applications.In this work,polyurethane elastomers with hydrogen bond and dimethylglyoxime-urethane(DOU)coordination complex were combined with in-situ dual-functional BiOI@Bi_(2)S_(3) to synthesize high-efficiency photothermal cyclic self-healing antibacterial coating.The photothermal efficiency of BiOI@Bi_(2)S_(3) is improved by 38% through interfacial regulation.BiOI@Bi_(2)S_(3)/PU rapidly rises by 50.2℃ within 300 s under near-infrared(NIR)light,which can trigger the hydrogen bond of polyurethane coating and recover the barrier properties of the coating through self-healing.Density functional theory was used to simulate and analyze the generation of multiple electron transfer paths after the vulcanization of BiOI,which improves the interfacial mobility of photogenerated carriers and generates more heat.Importantly,molecular dynamics verified the self-healing mechanism of hydrogen bond and the photothermal lifting mechanism of the coating.After 5th scratches and self-healing cycle tests,the coating has a self-healing efficiency of more than 80%,which can ensure the self-healing and anticorrosion protection performance of the coating for multiple cycles.The photocatalytic and photothermal properties of BiOI@Bi_(2)S_(3) enhance the antibacterial rate of the coating up to 99%.This work provides heuristic perspectives for the design of coatings with anti-corrosion,antibacterial and self-healing properties.展开更多
Binders could play crucial or even decisive roles in the fabrication of low-cost, stable and high-capacity electrodes. This is especially the case for the silicon (Si) anodes and sulfur (S) cathodes that undergo large...Binders could play crucial or even decisive roles in the fabrication of low-cost, stable and high-capacity electrodes. This is especially the case for the silicon (Si) anodes and sulfur (S) cathodes that undergo large volume change and active material loss in lithium-ion batteries during prolonged cycles. Herein, a hydrophilic polymer poly(methyl vinyl ether-alt-maleic acid) (PMVEMA) was explored as a dual-functional aqueous binder for the preparation of high-performance silicon anode and sulfur cathode. Benefiting from the dual functions of PMVEMA, i.e., the excellent dispersion ability and strong binding forces, the as-prepared electrodes exhibit improved capacity, rate capability and long-term cycling performance. In particular, the as-prepared Si electrode delivers a high initial discharge capacity of 1346.5 mAh g^(−1) at a high rate of 8.4 A/g and maintains 834.5 mAh g^(−1) after 300 cycles at 4.2 A/g, while the as-prepared S cathode exhibits enhanced cycling performance with high remaining discharge capacities of 663.4 mAh g^(−1) after 100 cycles at 0.2 C and 487.07 mAh g^(−1) after 300 cycles at 1 C, respectively. These encouraging results suggest that PMVEMA could be a universal binder to facilitate the green manufacture of both anode and cathode for high-capacity energy storage systems.展开更多
High-nickel single-crystal layered oxide material has become the most promising cathode material for electric vehicle power battery due to its high energy density.However,this material still suffers from structural de...High-nickel single-crystal layered oxide material has become the most promising cathode material for electric vehicle power battery due to its high energy density.However,this material still suffers from structural degradation during cycling and especially the severe interfacial reactions at elevated temperatures that exacerbate irreversible capacity loss.Here,a simple strategy was used to construct a dualfunction Li_(1.5)Al_(0.5)Ge_(1.5)P_(3)O_(12)(LAGP)protective layer on the surface of the high-nickel single-crystal(SC)cathode material,leading to SC@LAGP material.The strong Al-O bonding effectively inhibits the release of lattice oxygen(O)at elevated temperatures,which is supported by the positive formation energy of O vacancy from first-principal calculations.Besides,theoretical calculations demonstrate that the appropriate amount of Al doping accelerates the electron and Li^(+)transport,and thus reduces the kinetic barriers.In addition,the LAGP protective layer alleviates the stress accumulation during cycling and effectively reduces the erosion of materials from the electrolyte decomposition at elevated temperatures.The obtained SC@LAGP cathode material demonstrates much enhanced cycling stability even at high voltage(4.6 V)and elevated temperature(55℃),with a high capacity retention of 91.3%after 100 cycles.This work reports a simple dual-function coating strategy that simultaneously stabilizes the structure and interface of the single-crystal cathode material,which can be applied to design other cathode materials.展开更多
Photocatalytic dual-functional reaction under visible light irradiation represents a sustainable development strategy.In detail,H2production coupled with benzylamine oxidation can remarkably lower the cost by replacin...Photocatalytic dual-functional reaction under visible light irradiation represents a sustainable development strategy.In detail,H2production coupled with benzylamine oxidation can remarkably lower the cost by replacing sacrificial agents.In this work,Cd S quantum dots(Cd S QDs)were successfully loaded onto the surface of a porphyrinic metal-organic framework(Pd-PCN-222)by the electrostatic selfassembly at room temperature.The consequent Pd-PCN-222/CdS heterojunction composites displayed superb photocatalytic activity under visible light irradiation,achieving a H2production and benzylamine oxidation rate of 5069 and 3717μmol g^(-1)h^(-1)with>99%selectivity in 3 h.There is no noticeable loss of catalytic capability during three successive runs.Mechanistic studies by in situ electron spin resonance and X-ray photoelectron spectroscopy disclosed that CdS QDs injected photoexcited electrons to Pd-PCN-222 and then Zr6clusters under visible-light irradiation,and thus Cd S QDs and Zr6clusters behave as the photocatalytic oxidation and reduction centers,respectively.展开更多
基金supported by the National Natural Science Foundation of China under grants 62072229,U1936201,62071220,61976113joint project of China Mobile Research Institute&X-NET。
文摘Dual-function communication radar systems use common Radio Frequency(RF)signals are used for both communication and detection.For better compatibility with existing communication systems,we adopt Multiple-Input Multiple-Output(MIMO)Orthogonal Frequency Division Multiplexing(OFDM)signals as integrated signals and investigate the estimation performance of MIMO-OFDM signals.First,we analyze the Cramer-Rao Lower Bound(CRLB)of parameter estimation.Then,the transmit powers over different subcarriers are optimized to achieve the best tradeoff between the transmission rate and the estimation performance.Finally,we propose a more accurate estimation method that uses Canonical Polyadic Decomposition(CPD)of the third-order tensor to obtain the parameter matrices.Due to the characteristic of the column structure of the parameter matrices,we only need to use DFT/IDFT to recover the parameters of multiple targets.The simulation results show that tensor-based estimation method can achieve a performance close to CRLB,and the estimation performance can be improved by optimizing the transmit powers.
基金supported by the National Natural Science Foundation of China(No.52105072)Zhejiang Provincial Natural Science Foundation of China(No.LZ24E050004)+2 种基金Jiangsu Provincial Outstanding Youth Program(No.BK20230072)a grant from Suzhou Industrial Foresight and Key Core Technology Project(No.SYC2022044)grants from Jiangsu Qinglan Project and Jiangsu 333 High-level Talents.
文摘Wireless capsule endoscopy(WCE)has the potential to fully replace conventional wired counterparts for its low invasiveness.Recent studies have attempted to expand the functions of capsules toward this goal.However,limitations in space and energy supply have resulted in the inability to perform multiple diagnostic and treatment tasks using a single capsule.In this study,we developed a dual-functional capsule robot(DFCR)for drug delivery and tissue biopsy based on magnetic torsion spring technology.The delivery module was shown to rotate the push rod with a thrust of 894 mN to release approximately 0.3 mL of semisolid drug.The biopsy module used a built-in blade to cut tissue with a shear stress of 22.87 MPa,producing a sample of approximately 1.8 mm3.Additionally,a five-degree-of-freedom permanent magnet drive system was developed.By adjusting the strength of the unidirectional magnetic field generated by an external magnet,the capsule can be wirelessly controlled to sequentially trigger the two functions.Ex vivo tests on porcine stomachs confirmed the feasibility of the prototype capsule(12 mm in diameter and 45 mm in length)in active movement,medication,and tissue biopsy.The newly developed DFCR further expands the clinical application prospects of WCE robots in minimally invasive surgery.
基金financially supported by the National Natural Science Foundation of China (Nos.52070194,52073309,51902347,and 51908555)the Natural Science Foundation of Hunan Province (Nos.2022JJ20069 and 2020JJ5741).
文摘The intrinsic poor electrical conductivity,severe dissolution of K x S y intermediates,and inferior conversion reaction reversibility extremely impede the practical application of the transition-metal chalcogenides(TMDs)anode for potassium-ion batteries(PIBs).Herein,a rationally designed Cu_(9)S_(5)/MoS_(2)/C heterostruc-ture hollow nanocage was synthesized with assistance from metal-organic frameworks(MOFs)precursor.During the K-storage process,the homogeneously distributed the sulfiphilic nature of Cu 0 reaction prod-uct could act as a dual-functional catalyst,not only facilitating the rapid charge transfer but also effec-tively anchoring(K x S y)polysulfides,thus boosting K-storage reactions reversibility during the conversion reaction process.When applied as an anode for PIBs,the as-prepared heterostructure exhibits excellent reversible capacity and long cycle lifespan(350.5 mAh g^(-1)at 0.1 A g^(-1)and 0.04%per cycle capacity de-cay at 1 A g^(-1)after 1000 cycles).Additionally,the potassium storage mechanism is distinctly revealed by in-situ characterizations.The nanoarchitecture designing strategy for the advanced electrode in this work could provide vital guidance for relevant energy storage materials.
基金supported in part by the National Natural Science Foundation of China under Grants 62201137 and 62331023in part by the Fundamental Research Funds for the Central Universities under Grant 2242022k60001in part by the Fundamental Research Funds for the Central Universities under Grant 2242025K20001。
文摘In this paper,we investigate an reconfigurable intelligent surface-aided Integrated Sensing And Communication(ISAC)system.Our objective is to maximize the achievable sum rate of the multi-antenna communication users through the joint active and passive beamforming.Specifically,the weighted minimum mean-square error method is first used to reformulate the original problem into an equivalent one.Then,we utilize an alternating optimization algorithm to decouple the optimization variables and decompose this challenging problem into two subproblems.Given reflecting coefficients,a penalty-based algorithm is utilized to deal with the non-convex radar Signal-to-Noise Ratio(SNR)constraints.For the given beamforming matrix of the base station,we apply majorization-minimization to transform the problem into a Quadratic Constraint Quadratic Programming(QCQP)problem,which is ultimately solved using a Semi-Definite Relaxation(SDR)based algorithm.Simulation results illustrate the advantage of deploying reconfigurable intelligent surface in the considered multi-user MultipleInput Multiple-Output(MIMO)ISAC systems.
基金supported by the National Natural Science Foundation of China(Nos.22206113 and 22376124)the Outstanding Youth Science Fund(Overseas)of Shandong Provincial Natural Science Foundation(No.2022HWYQ-015)+4 种基金the Taishan Scholars Project Special Fund(No.tsqn202211039)the Guangdong Basic and Applied Basic Research Foundation(No.2021A1515111137)Qilu Youth Talent Program of Shandong University(No.61440082163171)the Natural Sciences and Engineering Research Council of Canadale Fonds de recherche du Quebec-Nature et technologies.
文摘Photocatalytic water splitting is a promising way to produce H_(2),a green and clean energy source.However,efficient H_(2) production typically relies on the addition of electron donors,such as alcohols and acids,which are neither environmentally friendly nor cost-effective.Recently,we have witnessed a surge of studies in coupling photocatalytic H_(2) evolution with organic pollutant oxidation,which significantly promotes charge separation and improves the overall photocatalytic efficiency.It is thus an opportune time to critically assess the recent literature concerning dual-functional photocatalytic systems and provide perspectives for its future development.In this minireview,we begin with the working principles and requirements for synergistic photocatalytic systems.We then summarize and critically discuss the recent advances in photocatalytic H_(2) production and the degradation of various organic pollutants,including antibiotics,dyes,and phenols.Finally,we discuss the current challenges and suggest future directions for this field.
基金supported by the National Natural Science Foundation of China(22162008)the Science and Technology Supporting Project of Guizhou Province([2022]208)+1 种基金the Guizhou Province Local Government Overseas Study Programthe open project of Guizhou Provincial Double Carbon and Renewable Energy Technology Innovation Research Institute.
文摘The development of an efficient dual-function catalytic-sorption system,which seamlessly integrates reaction and separation into a single step for extractant-free systems,represents a transformative advancement in oxidative desulfurization(ODS)process.In this work,we introduce a novel dualfunction amphiphilic biochar(Mo/CBC)catalyst,functionalized with MoO_(3-x)featuring abundant oxygen vacancies,for highly effective extractant-free ODS.The polarity of the biochar was precisely tailored by varying the amount of KOH,leading to the creation of amphiphilic carriers.Subsequent ball milling facilitated the successful loading of MoO_(3-x)onto the biochar surface via an impregnation-calcination route leveraging carbon reduction,resulting in the synthesis of amphiphilic Mo/CBC catalysts.The amphiphilic nature of these catalysts ensures their stable dispersion within the oil phase,while also facilitating their interaction with the oxidant H2O2 and the adsorption of sulfur-containing oxidation products.Characterization techniques,including EPR,XPS,and in situ XRD,verified the existence of abundant oxygen vacancies obtained by carbon reduction on the amphiphilic Mo/CBC catalysts,which significantly boosted their activity in an extractant-free ODs system.Remarkably,the amphiphilic Mo/CBC catalyst displayed exceptional catalytic performance,achieving a desulfurization efficiency of 99.6%in just 10 min without extraction solvent.DFT theoretical calculations further revealed that H_(2)O_(2)readily dissociates into two OH radicals on the O_(vac)-MoO_(3),overcoming a low energy barrier.This process was identified as a key contributor to the catalyst's outstanding ODS performance.Furthermore,other biochar sources,such as rice straw,bamboo,rapeseed oil cake,and walnut oil cake,were investigated to produce Mo-based amphiphilic biochar catalysts,which all showed excellent desulfurization performance.This work establishes a versatile and highly efficient dual-function catalytic-sorption system by designing amphiphilic biochar catalysts enriched with oxygen vacancies,paving the way for the development of universally applicable ODS catalysts for industrial applications.
基金financial support from Natural Science Foundation of Hunan Province(No.2025JJ50615)the Science and Technology Innovation Program of Hunan Province(No.2022RC4044)+2 种基金Hunan Provincial Health-Level Talent Scientific Research Project(No.R2023150)Clinical Research Center for Prevention and Treatment of Cognitive Impairment in Hunan Province(No.2023SK4050)University of South China Clinical Research 4310 Program(No.20224310NHYCG08)。
文摘Herein,the Nd@g-C_(3)N_(4) dual-functional photocatalysis enabled fluoroalkylative heteroarylation of alkenes with R_(f)SO_(2)Cl under visible-light and ultrasound conditions was firstly reported.The photogenerated electron-driven reductive production of fluoroalkyl radical paired with photogenerated hole-driven oxidative production of chloride radical resulted in the full utilization of photogenerated carrier for bond formation.A wide range of N-heteroarenes,alkenes and R_(f)SO_(2)Cl,were well compatible for this reaction to access valuable fluoroalkylated N-heteroarenes with diverse structural features.The antitumor potential of synthesized fluoroalkylated N-heterocycles against Glioma 261 cells was evaluated by CCK8 assay.Notably,compound 4 aka demonstrated remarkable efficacy,exhibiting approximately sevenfold greater potency than temozolomide,a widely used chemotherapeutic agent.
基金support of this work by the project“Development of new innovative low carbon energy technologies to improve excellence in the Region of Western Macedonia”(MIS 5047197),which is implemented under the Action“Reinforcement of the Research and Innovation Infrastructure”funded by the Operational Program“Competitiveness,Entrepreneurship and Innovation”(NSRF 2014-2020)co-financed by Greece and the European Union(European Regional Development Fund)+4 种基金the Hellenic Foundation for Research and Innovation(HFRI)for supporting this research work under the 3~(rd)Call for HFRI PhD Fellowships(Fellowship Number:6033)the support of ELECMI-LMA nodeNanbiosis ICTSsfunded by the Swiss National Science Foundation(Grant:206021_189629)the Research Council of Norway(Grant:296087)。
文摘Herein,the effect of the Ru:Ni bimetallic composition in dual-function materials(DFMs)for the integrated CO_(2)capture and methanation process(ICCU-Methanation)is systematically evaluated and combined with a thorough material characterization,as well as a mechanistic(in-situ diffuse reflectance infrared fourier-transform spectroscopy(in-situ DRIFTS))and computational(computational fluid dynamics(CFD)modelling)investigation,in order to improve the performance of Ni-based DFMs.The bimetallic DFMs are comprised of a main Ni active metallic phase(20 wt%)and are modified with low Ru loadings in the 0.1-1 wt%range(to keep the material cost low),supported on Na_(2)O/Al_(2)O_(3).It is shown that the addition of even a very low Ru loading(0.1-0.2 wt%)can drastically improve the material reducibility,exposing a significantly higher amount of surface-active metallic sites,with Ru being highly dispersed over the support and the Ni phase,while also forming some small Ru particles.This manifests in a significant enhancement in the CH_(4)yield and the CH_(4)production kinetics during ICCU-Methanation(which mainly proceeds via formate intermediates),with 0.2 wt%Ru addition leading to the best results.This bimetallic DFM also shows high stability and a relatively good performance under an oxidizing CO_(2)capture atmosphere.The formation rate of CH_(4)during hydrogenation is then further validated via CFD modelling and the developed model is subsequently applied in the prediction of the effect of other parameters,including the inlet H_(2)concentration,inlet flow rate,dual-fu nction material weight,and reactor internal diameter.
基金financially supported by the National Natural Science Foundation of China (22350410386,W2412116,22375200,U22A202175,21961142006)。
文摘Exploring cost-effective and efficient catalysts for oxygen reduction reaction(ORR)poses a significant challenge,espe-cially in the pursuit of alternatives to precious metals like platinum.Significant advancements have driven electrochem-ists to develop efficient ORR catalysts using abundant materials,particularly iron(Fe)-based,known for their exceptional performance in ORR.While the crucial function of Fe in boosting ORR catalytic activity is recognized,the connection between material attributes and catalytic performance remains enigmatic.Understanding the dynamic processes involved in oxygen electrocatalysis is paramount for designing precious-metals-free ORR electrocatalysts.Mössbauer spectroscopy stands out as a powerful technique for deciphering the structural characteristics of Fe species in catalysis,facilitating the identification of active sites and the clarification of catalytic mechanisms.By showcasing noteworthy case studies within this review,we demonstrate the application of in-situ/operando 57Fe Mössbauer spectroscopy across diverse Fe-involved materials in ORR catalysis.This sheds light on various aspects of ORR catalysis,such as identifying active sites,assessing stability,and understanding the reaction mechanism.Our inquiry drives towards the opportunities and hurdles associ-ated with Mössbauer spectroscopy,unveiling potential breakthroughs and avenues for enhancement within this pivotal research realm.
基金financial support of the National Natural Science Foundation of China (21875247,21072221, 21172252)the Project of Talent Cultivation for Carbon Peak and Carbon Neutrality of the University of Chinese of Academy of Science
文摘The design and fabrication of ordered epitaxial MOF-on-MOF heterostructures as highly efficient electrocatalysts for water splitting is crucial but still challenging.In this study,a simple coordination-driven self-assembly method is used to fabricate controllable MOF-on-MOF multiscale heterostructures,where triangular host MOF(ZIF-67)nanosheets undergo in situ epitaxial growth to form uniform orthogonal vip MOF(CoFe PBA)nanosheets.Phosphorus(P)is further introduced in situ to fabricate CoP and Fe_(2)P heterostructured nanosheets(CoFe-P-NS),which exhibit excellent bifunctional electrocatalytic performance due to the enhancement of intrinsic electrocatalytic activity by p-d orbital hybridization.Specifically,the CoFe-P-NS requires low overpotential of 259 and 307 mV to reach 500 mA cm−2 for HER and OER,respectively.Remarkably,the assembled electrolysis cell maintained a large current density of 300 mA cm−2 for over 360 h with negligible voltage increase during alkaline seawater electrolysis.Experiments and theoretical calculations show that the synergistic catalytic activity of bimetallic phosphides arises from p-d orbital hybridization,where the CoP-P sites enhance HER by optimizing H*adsorption in the Volmer-Heyrovsky steps,while the Fe_(2)P-Fe sites accelerate OER by lowering the energy barrier of the rate-determining step from O*to OOH*.This study provides valuable insights into the design of a controllable MOF-on-MOF-based electrocatalyst toward alkaline seawater splitting.
基金supported by the National Natural Science Foundation of China(Grant Nos.:21825201,52401244 and 52201227)Henan Province Key Research and Development and Promotion Program(Scientific and Technological Breakthrough Project:232102240088 and 252102230078)+3 种基金the Key Research&Development and Promotion of Special Project(Scientific Problem Tackling)of Henan Province(252102230078)Doctoral Research Startup Fund Project of Henan Open University(BSJH-2025-04)Zhejiang Provincial Natural Science Foundation of China(LQ24B020005,LQ23B030001)China Postdoctoral Science Foundation(2024M762442).
文摘Electrocatalytic nitrate-to-ammonia conversion offers dual environmental and sustainable synthesis benefits,but achieving high efficiency with low-cost catalysts remains a major challenge.This review focuses on cobalt-based electrocatalysts,emphasizing their structural engineering for enhanced the performance of electrocatalytic nitrate reduction reaction(NO3RR)through dimensional control,compositional tuning,and coordination microenvironment modulation.Notably,by critically analyzing metallic cobalt,cobalt alloys,cobalt compounds,cobalt single atom and molecular catalyst configurations,we firstly establish correlations between atomic-scale structural features and catalytic performance in a coordination environment perspective for NO3RR,including the dynamic reconstruction during operation and its impact on active site.Synergizing experimental breakthroughs with computational modeling,we decode mechanisms underlying competitive hydrogen evolution suppression,intermediate adsorption-energy optimization,and durability enhancement in complex aqueous environments.The development of cobalt-based catalysts was summarized and prospected,and the emerging opportunities of machine learning in accelerating the research and development of high-performance catalysts and the configuration of series reactors for scalable nitrate-to-ammonia systems were also introduced.Bridging surface science and applications,it outlines a framework for designing multifunctional electrocatalysts to restore nitrogen cycle balance sustainably.
基金supported by the National Natural Science Foundation of China(No.12205165)Hebei Province Innovation Ability Improvement Plan Project(No.225676111H).
文摘Structural engineering of Pt-based nanoalloys is crucial for the rational design and manufacturing of high-performance and low-cost electrocatalysts for hydrogen evolution reaction(HER).Here,we reported PtNi nanoparticles with a refined size of 2.71 nm and regular strains loaded on carbon black,synthesized using the high-temperature liquid shock(HTLS)method.This approach offers significant advantages over conventional synthesis methods,including high scalability,rapid reaction rates,and precise control over the size and shape of nanocrystals.Importantly,the synthesized PtNi electrocatalysts demonstrate outstanding catalytic activity and long-term stability for HER,achieving low overpotentials of 19 and 203 mV at current densities of 10 and 1000 mA/cm^(2),respectively.The superior performance can be attributed to the combination of a refined particle size,lattice strains,and synergistic effects between Pt and Ni.This rapid liquid-state synthesis demonstrated here holds great potential for scalable and industrial manufacturing of micro-/nano-catalysts.
基金financially supported by the National Natural Science Foundation of China(U21A20311,U24A2040,52171141,52272117)the Natural Science Foundation of Shandong Province(ZR2022JQ19)+3 种基金the Key Technology Research Project of Shandong Province(2023CXGC010202)the Taishan Industrial Experts Program(TSCX202306142)the Core Facility Sharing Platform of Shandong Universitythe Foundation of Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education),Nankai University。
文摘Co_(3)S_(4)electrocatalysts with mixed valences of Co ions and excellent structural stability possess favorable oxygen evolution reaction(OER)activity,yet challenges remain in fabricating rechargeable lithiumoxygen batteries(LOBs)due to their poor OER performance,resulting from poor electrical conductivity and overly strong intermediate adsorption.In this work,fancy double heterojunctions on 1T/2H-MoS_(2)@Co_(3)S_(4)(1T/2H-MCS)were constructed derived from the charge donation from Co to Mo ions,thus inducing the phase transformation of Mo S_(2)from 2H to 1T.The unique features of these double heterojunctions endow the1T/2H-MCS with complementary catalysis during charging and discharging processes.It is worth noting that 1T-Mo S2@Co3S4could provide fast Co-S-Mo electron transport channels to promote ORR/OER kinetics,and 2H-MoS_(2)@Co_(3)S_(4)contributed to enabling moderate egorbital occupancy when adsorbed with oxygen-containing intermediates.On the basis,the Li_(2)O_(2)nucleation route was changed to solution and surface dual pathways,improving reversible deposition and decomposition kinetics.As a result,1T/2H-MCS cathodes exhibit an improved electrocatalytic performance compared with those of Co_(3)S_(4)and Mo S2cathodes.This innovative heterostructure design provides a reliable strategy to construct efficient transition metal sulfide catalysts by improving electrical conductivity and modulating adsorption toward oxygenated intermediates for LOBs.
基金financially supported by the National Science Foundation of China(Nos.52203314,52071226 and 51872193)the Natural Science Foundations of Jiangsu Province(No.BK20210847)+1 种基金Jiangsu Key Laboratory for Biomass Energy and Material(No.JSBEM-S-201805)the Natural Science Foundations of the Jiangsu Higher Education Institutions of China(No.21KJB430042)。
文摘Hydrogen,as a green and clean next-generation fuel,is a key to achieving the goal of carbon neutrality.Constructing an electrocatalyst with bifunctional hydrogen evolution and oxygen evolution activity in the same electrolyte is a key technology for producing hydrogen via water splitting.Herein,a bimetallic active site catalyst,which possessed an edge-riched MoS_(2)nanoflakes array vertically growing on cubic CoS_(2),forming a nuclear-shell heterogeneous configuration,termed CSC-Mo S_(2)@Co S_(2).was reported The optimal CSC-Mo S_(2)@Co S_(2)-24 possessed good dualfunctional electrocatalytic activity(hydrogen evolution(HER),10 m A·cm^(-2)@241.5 m V and oxygen evolution(OER),10 m A·cm^(-2)@350 m V).Especially,CSC-Mo S_(2)@CoS_(2)-24 exhibited an extremely high mass activity for HER,and only required an overpotential of~550 m V when reaching a large current density of 1422 m A·mg^(-1),which was20.6-fold that of the bulk CoS_(2)(69 m A·mg^(-1)),as well as exhibiting stability of up to 100 h.The good electrocatalytic performance was attributed to the nuclear-shell heterostructure of Mo S_(2)@CoS_(2)hybrid could bring critical synergies,improving efficient mass transfer and electron transfer processes between Co S_(2)and Mo S_(2),which collaboratively promoted the electrocatalytic kinetics.It is foreseeable that the method proposed in this work will have guiding value for the preparation of dual-functional electrocatalysts with multi-interface heterostructures by assembling layered sulfides on cubic sulfides.
基金The China Postdoctoral Science Foundation(2019M661072)the Basic Research Program of Liaoning Education Department(2017J080)the National Natural Science Foundation of China(31771926)funded this study.
文摘There is no study on food-derived peptide with both anticoagulant and angiotensin I-converting enzyme inhibitory (ACEI) activities yet. In this work, the anticoagulant and ACEI activities of the casein hydrolysates released by pepsin digestion were evaluated for the first time to the best of our knowledge. Results indicated that the casein hydrolysate exhibited potent anticoagulant activity by prolonging the thrombin time (TT) and the activated partial thromboplastin time (APTT). Compared with control samples, at 10 mg/mL, the TT and APTT of casein hydrolysate were 186.0 % ± 6.6 % and 163.5 % ± 7.4 %, respectively. The casein hydrolysate also showed a strong ACEI activity with an IC50 value of 1.775 mg/mL. The components of the bioactive casein hydrolysate were analyzed by nanoscale liquid chromatography quadrupole time-of-flight tandem mass spectrometry (NanoLC-Q-TOF-MS/MS). Total of 115 peptides were identified, among which 34, 9, 55 and 17 peptides were derived from α_(s1-), α_(s2-), β-, and κ-casein, respectively. The results of PeptideRanker and PepSite 2 analysis showed that 6 peptides (FRQFYQL, NENLLRF, NPWDQVKR, PVVVPPFLQ, PVRGPFPIIV, and ARHPHPHLSF) have both ACEI and anticoagulant activities by binding to the active sites of ACE and thrombin. This study indicated that casein is a potential functional food supplement that can be used for medical purposes.
基金supported by the funding from the Strategy Priority Research Program of Chinese Academy of Science (Grant No. XDA17020404)DICP&QIBEBT (DICP&QIBEBT UN201702)+8 种基金R&D Projects in Key Areas of Guangdong Province (2019B090908001)Science and Technology Innovation Foundation of Dalian (2018J11CY020)Defense Industrial Technology Development Program (JCKY2018130C107)National Natural Science Foundation of China (Grants 51872283)Liao Ning Revitalization Talents Program (Grant XLYC1807153)Natural Science Foundation of Liaoning Province (Grant 20180510038)DICP (DICP ZZBS201708, DICP ZZBS201802)DNL Cooperation FundCAS (DNL180310, DNL180308, DNL201912, and DNL201915)。
文摘Developing sulfur cathodes with high catalytic activity on accelerating the sluggish redox kinetics of lithium polysulfides(Li PSs) and unveiling their mechanisms are pivotal for advanced lithium–sulfur(Li–S)batteries. Herein, MoS2 is verified to reduce the Gibbs free energy for rate-limiting step of sulfur reduction and the dissociation energy of lithium sulfide(Li2 S) for the first time employing theoretical calculations. The Mo S2 nanosheets coated on mesoporous hollow carbon spheres(MHCS) are then reasonably designed as a sulfur host for high-capacity and long-life Li–S battery, in which MHCS can guarantee the high sulfur loading and fast electron/ion transfer. It is revealed that the shuttle effect is efficiently inhibited because of the boosted conversion of Li PSs. As a result, the coin cell based on the MHCS@Mo S2-S cathode exhibits stable cycling performance maintaining 735.7 mAh g^(-1) after 500 cycles at 1.0 C. More importantly, the pouch cell employing the MHCS@Mo S2-S cathodes achieves high specific capacity of1353.2 m Ah g^(-1) and prominent cycle stability that remaining 960.0 m Ah g^(-1) with extraordinary capacity retention of 79.8% at 0.1 C after 170 cycles. Therefore, this work paves a new avenue for developing practical high specific energy and long-life pouch-type Li–S batteries.
基金financially supported by the National Natural Science Foundation of China(Nos.52371081,U2106226)the Key Research and Development Program of Shandong province(No.2020CXGC010703)the Foundation of Key Laboratory of National Defense Science and Technology(No.JS220406).
文摘Although extremely challenging,it is highly desirable to develop self-healing materials that exhibit high efficiency under environmental conditions for marine protection applications.In this work,polyurethane elastomers with hydrogen bond and dimethylglyoxime-urethane(DOU)coordination complex were combined with in-situ dual-functional BiOI@Bi_(2)S_(3) to synthesize high-efficiency photothermal cyclic self-healing antibacterial coating.The photothermal efficiency of BiOI@Bi_(2)S_(3) is improved by 38% through interfacial regulation.BiOI@Bi_(2)S_(3)/PU rapidly rises by 50.2℃ within 300 s under near-infrared(NIR)light,which can trigger the hydrogen bond of polyurethane coating and recover the barrier properties of the coating through self-healing.Density functional theory was used to simulate and analyze the generation of multiple electron transfer paths after the vulcanization of BiOI,which improves the interfacial mobility of photogenerated carriers and generates more heat.Importantly,molecular dynamics verified the self-healing mechanism of hydrogen bond and the photothermal lifting mechanism of the coating.After 5th scratches and self-healing cycle tests,the coating has a self-healing efficiency of more than 80%,which can ensure the self-healing and anticorrosion protection performance of the coating for multiple cycles.The photocatalytic and photothermal properties of BiOI@Bi_(2)S_(3) enhance the antibacterial rate of the coating up to 99%.This work provides heuristic perspectives for the design of coatings with anti-corrosion,antibacterial and self-healing properties.
基金This work was financially supported by the Australian Research Council(ARC)Discovery Projects(DP210103266 and DPI 701048343)the Griffith University Ph.D.Scholarships.
文摘Binders could play crucial or even decisive roles in the fabrication of low-cost, stable and high-capacity electrodes. This is especially the case for the silicon (Si) anodes and sulfur (S) cathodes that undergo large volume change and active material loss in lithium-ion batteries during prolonged cycles. Herein, a hydrophilic polymer poly(methyl vinyl ether-alt-maleic acid) (PMVEMA) was explored as a dual-functional aqueous binder for the preparation of high-performance silicon anode and sulfur cathode. Benefiting from the dual functions of PMVEMA, i.e., the excellent dispersion ability and strong binding forces, the as-prepared electrodes exhibit improved capacity, rate capability and long-term cycling performance. In particular, the as-prepared Si electrode delivers a high initial discharge capacity of 1346.5 mAh g^(−1) at a high rate of 8.4 A/g and maintains 834.5 mAh g^(−1) after 300 cycles at 4.2 A/g, while the as-prepared S cathode exhibits enhanced cycling performance with high remaining discharge capacities of 663.4 mAh g^(−1) after 100 cycles at 0.2 C and 487.07 mAh g^(−1) after 300 cycles at 1 C, respectively. These encouraging results suggest that PMVEMA could be a universal binder to facilitate the green manufacture of both anode and cathode for high-capacity energy storage systems.
基金financially supported by the National Natural Science Foundation of China(51974368,51774333)the Hunan Provincial Natural Science Foundation of China(2020JJ2048)。
文摘High-nickel single-crystal layered oxide material has become the most promising cathode material for electric vehicle power battery due to its high energy density.However,this material still suffers from structural degradation during cycling and especially the severe interfacial reactions at elevated temperatures that exacerbate irreversible capacity loss.Here,a simple strategy was used to construct a dualfunction Li_(1.5)Al_(0.5)Ge_(1.5)P_(3)O_(12)(LAGP)protective layer on the surface of the high-nickel single-crystal(SC)cathode material,leading to SC@LAGP material.The strong Al-O bonding effectively inhibits the release of lattice oxygen(O)at elevated temperatures,which is supported by the positive formation energy of O vacancy from first-principal calculations.Besides,theoretical calculations demonstrate that the appropriate amount of Al doping accelerates the electron and Li^(+)transport,and thus reduces the kinetic barriers.In addition,the LAGP protective layer alleviates the stress accumulation during cycling and effectively reduces the erosion of materials from the electrolyte decomposition at elevated temperatures.The obtained SC@LAGP cathode material demonstrates much enhanced cycling stability even at high voltage(4.6 V)and elevated temperature(55℃),with a high capacity retention of 91.3%after 100 cycles.This work reports a simple dual-function coating strategy that simultaneously stabilizes the structure and interface of the single-crystal cathode material,which can be applied to design other cathode materials.
基金support from the National Natural Science Foundation of China(Nos.21773314,21821003 and 21890382)the Guangdong Natural Science Funds for Distinguished Young Scholar(No.2019B151502017)。
文摘Photocatalytic dual-functional reaction under visible light irradiation represents a sustainable development strategy.In detail,H2production coupled with benzylamine oxidation can remarkably lower the cost by replacing sacrificial agents.In this work,Cd S quantum dots(Cd S QDs)were successfully loaded onto the surface of a porphyrinic metal-organic framework(Pd-PCN-222)by the electrostatic selfassembly at room temperature.The consequent Pd-PCN-222/CdS heterojunction composites displayed superb photocatalytic activity under visible light irradiation,achieving a H2production and benzylamine oxidation rate of 5069 and 3717μmol g^(-1)h^(-1)with>99%selectivity in 3 h.There is no noticeable loss of catalytic capability during three successive runs.Mechanistic studies by in situ electron spin resonance and X-ray photoelectron spectroscopy disclosed that CdS QDs injected photoexcited electrons to Pd-PCN-222 and then Zr6clusters under visible-light irradiation,and thus Cd S QDs and Zr6clusters behave as the photocatalytic oxidation and reduction centers,respectively.
