A multi-dimensional conductive heterojunction structure,composited by TiO2,SnO2,and Ti3C2TX MXene,is facilely designed and applied as electron transport layer in efficient and stable planar perovskite solar cells.Base...A multi-dimensional conductive heterojunction structure,composited by TiO2,SnO2,and Ti3C2TX MXene,is facilely designed and applied as electron transport layer in efficient and stable planar perovskite solar cells.Based on an oxygen vacancy scramble effect,the zero-dimensional anatase TiO2 quantum dots,surrounding on two-dimensional conductive Ti3C2TX sheets,are in situ rooted on three-dimensional SnO2 nanoparticles,constructing nanoscale TiO2/SnO2 heterojunctions.The fabrication is implemented in a controlled lowtemperature anneal method in air and then in N2 atmospheres.With the optimal MXene content,the optical property,the crystallinity of perovskite layer,and internal interfaces are all facilitated,contributing more amount of carrier with effective and rapid transferring in device.The champion power conversion efficiency of resultant perovskite solar cells achieves 19.14%,yet that of counterpart is just 16.83%.In addition,it can also maintain almost 85%of its initial performance for more than 45 days in 30–40%humidity air;comparatively,the counterpart declines to just below 75%of its initial performance.展开更多
The efficiency and stability of catalysts for photocatalytic hydrogen evolution(PHE)are largely governed by the charge transfer behaviors across the heterojunction interfaces.In this study,CuO,a typical semiconductor ...The efficiency and stability of catalysts for photocatalytic hydrogen evolution(PHE)are largely governed by the charge transfer behaviors across the heterojunction interfaces.In this study,CuO,a typical semiconductor featuring a broad spectral absorption range,is successfully employed as the electron acceptor to combine with CdS for constructing a S-scheme heterojunction.The optimized photocatalyst(CdSCuO2∶1)delivers an exceptional hydrogen evolution rate of 18.89 mmol/(g·h),4.15-fold higher compared with bare CdS.X-ray photoelectron spectroscopy(XPS)and ultraviolet-visible diffuse reflection absorption spectroscopy(UV-vis DRS)confirmed the S-scheme band structure of the composites.Moreover,the surface photovoltage(SPV)and electron paramagnetic resonance(EPR)indicated that the photogenerated electrons and photogenerated holes of CdS-CuO2∶1 were respectively transferred to the conduction band(CB)of CdS with a higher reduction potential and the valence band(VB)of CuO with a higher oxidation potential under illumination,as expected for the S-scheme mechanism.Density-functional-theory calculations of the electron density difference(EDD)disclose an interfacial electric field oriented from CdS to CuO.This built-in field suppresses charge recombination and accelerates carrier migration,rationalizing the markedly enhanced PHE activity.This study offers a novel strategy for designing S-scheme heterojunctions with high light harvesting and charge utilization toward sustainable solar-tohydrogen conversion.展开更多
Lithium-sulfur(Li-S)batteries require efficient catalysts to accelerate polysulfide conversion and mitigate the shuttle effect.However,the rational design of catalysts remains challenging due to the lack of a systemat...Lithium-sulfur(Li-S)batteries require efficient catalysts to accelerate polysulfide conversion and mitigate the shuttle effect.However,the rational design of catalysts remains challenging due to the lack of a systematic strategy that rationally optimizes electronic structures and mesoscale transport properties.In this work,we propose an autogenously transformed CoWO_(4)/WO_(2) heterojunction catalyst,integrating a strong polysulfide-adsorbing intercalation catalyst with a metallic-phase promoter for enhanced activity.CoWO_(4) effectively captures polysulfides,while the CoWO_(4)/WO_(2) interface facilitates their S-S bond activation on heterogenous catalytic sites.Benefiting from its directional intercalation channels,CoWO_(4) not only serves as a dynamic Li-ion reservoir but also provides continuous and direct pathways for rapid Li-ion transport.Such synergistic interactions across the heterojunction interfaces enhance the catalytic activity of the composite.As a result,the CoWO_(4)/WO_(2) heterostructure demonstrates significantly enhanced catalytic performance,delivering a high capacity of 1262 mAh g^(−1) at 0.1 C.Furthermore,its rate capability and high sulfur loading performance are markedly improved,surpassing the limitations of its single-component counterparts.This study provides new insights into the catalytic mechanisms governing Li-S chemistry and offers a promising strategy for the rational design of high-performance Li-S battery catalysts.展开更多
Photo-assisted lithium–sulfur batteries(PALSBs)offer an eco-friendly solution to address the issue of sluggish reaction kinetics of conventional LSBs.However,designing an efficient photoelectrode for practical implem...Photo-assisted lithium–sulfur batteries(PALSBs)offer an eco-friendly solution to address the issue of sluggish reaction kinetics of conventional LSBs.However,designing an efficient photoelectrode for practical implementation remains a significant challenge.Herein,we construct a free-standing polymer–inorganic hybrid photoelectrode with a direct Z-scheme heterostructure to develop high-efficiency PALSBs.Specifically,polypyrrole(PPy)is in situ vapor-phase polymerized on the surface of N-doped TiO_(2) nanorods supported on carbon cloth(N-TiO_(2)/CC),thereby forming a well-defined p–n heterojunction.This architecture efficiently facilitates the carrier separation of photo-generated electron–hole pairs and significantly enhances carrier transport by creating a built-in electric field.Thus,the PPy@N-TiO_(2)/CC can simultaneously act as a photocatalyst and an electrocatalyst to accelerate the reduction and evolution of sulfur,enabling ultrafast sulfur redox dynamics,as convincingly validated by both theoretical simulations and experimental results.Consequently,the PPy@N-TiO_(2)/CC PALSB achieves a high discharge capacity of 1653 mAh g−1,reaching 98.7%of the theoretical value.Furthermore,5 h of photo-charging without external voltage enables the PALSB to deliver a discharge capacity of 333 mAh g−1,achieving dual-mode energy harvesting capabilities.This work successfully integrates solar energy conversion and storage within a rechargeable battery system,providing a promising strategy for sustainable energy storage technologies.展开更多
Drug-resistant bacteria,using their dense cell membranes as strong barrier,significantly reduce the efficacy of conventional antibacterial treatments.Phototriggered 2D catalytic nanomaterials have emerged as promising...Drug-resistant bacteria,using their dense cell membranes as strong barrier,significantly reduce the efficacy of conventional antibacterial treatments.Phototriggered 2D catalytic nanomaterials have emerged as promising candidates against drug-resistant bacteria by inducing membrane mechanical damage and generating reactive oxygen species(ROS).However,the practical antibacterial efficacy of typical 2D graphitic carbon nitride(g-C_(3)N_(4))is severely limited due to the low ROS production.Herein,we report an interfacial band-engineered lamellar heterojunctions(MnCN LHJs)through in situ Mn_(2)O_(3)growth on g-C_(3)N_(4).The charges generated in g-C_(3)N_(4)are stabilized by Mn_(2)O_(3),minimizing electron-hole recombination and boosting ROS production.Meanwhile,the photocatalytic effect of MnCN LHJs works synergistically with photothermal effects of Mn_(2)O_(3)to induce a robust“melee attack”against drug-resistant bacteria.High-resolution synchrotron radiation X-ray tomography directly visualized that MnCN LHJs possessed bacterial trapping capabilities,revealing their ability to induce mechanical damage to bacteria membrane for the first time.Additionally,MnCN LHJs can deplete endogenous glutathione,thereby enhancing ROS generation and weakening the bacterial antioxidant defense system.These combined effects achieve a remarkable bactericidal rate exceeding 98% against methicillin-resistant Staphylococcus aureus(MRSA).Notably,MnCN LHJs demonstrate prolonged retention at wound sites,helping to reduce inflammation and promote angiogenesis in infected wounds.This work not only advances interfacial band engineering approach to enhance the photocatalytic performance of g-C_(3)N_(4)but also underscores the significance of nanomaterial-bacteria interaction in design of next-generation antibacterial materials.展开更多
The exploration of efficient photocatalytic materials for CO_(2)conversion into hydrocarbon energy fuel is of paramount significance.However,problems,such as rapid charge recombination,low quantum efficiency,and poor ...The exploration of efficient photocatalytic materials for CO_(2)conversion into hydrocarbon energy fuel is of paramount significance.However,problems,such as rapid charge recombination,low quantum efficiency,and poor product selectivity,still limit the efficiency of photocatalytic CO_(2)reduction.Here,this study reports a Sscheme heterostructure of MnFe_(2)O_(4)/Bi_(2)WO_(6),formed by loading MnFe_(2)O_(4)nanoparticles onto Bi_(2)WO_(6) microflowers with oxygen-rich vacancies,enabling photocatalytic CO_(2)reduction.Notably,the developed MnFe_(2)O_(4)/Bi_(2)WO_(6) heterostructure improved the photocatalytic CO_(2)reduction ability,achieving a maximum CO generation rate of 32.7μmol·h^(-1)·g^(-1),which is 3.7 and 14.3 times higher than that of Bi_(2)WO_(6) and MnFe_(2)O_(4),respectively.Additionally,the CO production mechanism by CO_(2)photocatalytic reduction was proposed based on detailed characterization and density functional theory(DFT)calculation.The findings of this study suggest that introducing oxygen vacancies and constructing heterojunctions can significantly improve the photocatalytic CO_(2)reduction performance of Bi_(2)WO_(6).展开更多
Heterostructure engineering has emerged as a promising strategy to enhance the electrochemical CO_(2)reduction reaction(CO_(2)RR)by optimizing interfacial electron transfer.Herein,we report a novel octahedral SnS_(2)/...Heterostructure engineering has emerged as a promising strategy to enhance the electrochemical CO_(2)reduction reaction(CO_(2)RR)by optimizing interfacial electron transfer.Herein,we report a novel octahedral SnS_(2)/SnO_(2)heterojunction catalyst synthesized via an ion-exchange vulcanization method,which achieves exceptional activity and selectivity for CO_(2)-toformate conversion.Through in-situ Raman spectroscopy,ex-situ X-ray diffraction(XRD),and X-ray photoelectron spectroscopy(XPS),we demonstrate that the octahedral SnS_(2)/SnO_(2)heterojunction dynamically restructures into a sulfur-doped Sn/SnO_(2)(Sn(S)/SnO_(2))heterostructure under operating conditions.Density functional theory(DFT)calculations reveal that the Sn(S)/SnO_(2)interface facilitates electron transfer from SnO_(2)to metallic Sn(S),generating a built-in electric field that stabilizes Sn^(4+)in SnO_(2)and accelerates proton-coupled electron transfer to*OCHO intermediates.Consequently,the catalyst achieves a formate Faradaic efficiency exceeding 90% over a broad potential window(-0.6 to -1.0 V vs.reversible hydrogen electrode(RHE))with a high partial current density of -280 mA·cm^(-2),surpassing most reported Sn-based catalysts.This work elucidates the structural dynamics and interfacial enhancement mechanisms of heterojunction catalysts,offering a rational design principle for advanced CO_(2)RR electrocatalysts.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
S-scheme heterostructure photocatalysts utilize the synergistic and superposition effects of materials,ef-fectively separating electrons and holes,maintaining strong redox capacity,and addressing issues en-countered b...S-scheme heterostructure photocatalysts utilize the synergistic and superposition effects of materials,ef-fectively separating electrons and holes,maintaining strong redox capacity,and addressing issues en-countered by current photocatalytic reactions.This review explores the origins and unique benefits of S-scheme heterojunctions.Specifically,we summarized and discussed the effects of different dimensions of semiconductors constituting S-scheme heterojunctions and the similarities and differences in elec-tron transfer processes when constructing heterojunctions.Additionally,we analyzed several methods for proving the formation of S-scheme heterojunctions and the electron transfer process,both directly and indirectly.Finally,we review the applications of S-scheme heterojunctions in various fields of photo-catalysis,including photocatalytic water splitting,pollution degradation,CO_(2) reduction and other related photocatalytic applications.Our hope is that this review will provide an essential reference for the devel-opment and application of S-scheme heterojunction photocatalysis.展开更多
In the quest for effective solutions to address Environ.Pollut.and meet the escalating energy demands,heterojunction photocatalysts have emerged as a captivating and versatile technology.These photocatalysts have garn...In the quest for effective solutions to address Environ.Pollut.and meet the escalating energy demands,heterojunction photocatalysts have emerged as a captivating and versatile technology.These photocatalysts have garnered significant interest due to their wideranging applications,including wastewater treatment,air purification,CO_(2) capture,and hydrogen generation via water splitting.This technique harnesses the power of semiconductors,which are activated under light illumination,providing the necessary energy for catalytic reactions.With visible light constituting a substantial portion(46%)of the solar spectrum,the development of visible-light-driven semiconductors has become imperative.Heterojunction photocatalysts offer a promising strategy to overcome the limitations associated with activating semiconductors under visible light.In this comprehensive review,we present the recent advancements in the field of photocatalytic degradation of contaminants across diverse media,as well as the remarkable progress made in renewable energy production.Moreover,we delve into the crucial role played by various operating parameters in influencing the photocatalytic performance of heterojunction systems.Finally,we address emerging challenges and propose novel perspectives to provide valuable insights for future advancements in this dynamic research domain.By unraveling the potential of heterojunction photocatalysts,this reviewcontributes to the broader understanding of their applications and paves the way for exciting avenues of exploration and innovation.展开更多
It is very appealing that 5-hydroxymethylfurfural(HMF)is electrocatalytical oxidized as 2,5-furandicarboxylic acid(FDCA)linking to non-classical cathodic hydrogen(H_(2))production.However,the electrocatalysts for elec...It is very appealing that 5-hydroxymethylfurfural(HMF)is electrocatalytical oxidized as 2,5-furandicarboxylic acid(FDCA)linking to non-classical cathodic hydrogen(H_(2))production.However,the electrocatalysts for electrocatalytic HMF oxidative reaction(e-HMFOR)have been facing low Faradaic efficiency(FE)and high water splitting voltage.Herein,we propose a strategy of the NiSeO_(3)@(CoSeO_(3))_(4)heterojunction by constructing a Co-Ni paired site,where the Co site is in charge of adsorbing for HMF while the electrons are transferred to the Ni site,thus giving the NiSeO_(3)@(CoSeO_(3))_(4)heterojunction superior electrocata lytic performances for e-HMFOR and water splitting.By optimizing conditions,the NiSeO_(3)@(CoSeO_(3))_(4)heterojunction has high conversion of 99.7%,high selectivity of 99.9%,and high FE of 98.4%at 1.3 V,as well as low cell voltage of 1.31 V at 10 mA cm^(-2)in 1 M KOH+0.1 M HMF.This study offers a potential insight for e-HMFOR to high value-added FDCA coupling water splitting to produce H_(2)in an economical manner.展开更多
A composite anti-disturbance predictive control strategy employing a Multi-dimensional Taylor Network(MTN)is presented for unmanned systems subject to time-delay and multi-source disturbances.First,the multi-source di...A composite anti-disturbance predictive control strategy employing a Multi-dimensional Taylor Network(MTN)is presented for unmanned systems subject to time-delay and multi-source disturbances.First,the multi-source disturbances are addressed according to their specific characteristics as follows:(A)an MTN data-driven model,which is used for uncertainty description,is designed accompanied with the mechanism model to represent the unmanned systems;(B)an adaptive MTN filter is used to remove the influence of the internal disturbance;(C)an MTN disturbance observer is constructed to estimate and compensate for the influence of the external disturbance;(D)the Extended Kalman Filter(EKF)algorithm is utilized as the learning mechanism for MTNs.Second,to address the time-delay effect,a recursiveτstep-ahead MTN predictive model is designed utilizing recursive technology,aiming to mitigate the impact of time-delay,and the EKF algorithm is employed as its learning mechanism.Then,the MTN predictive control law is designed based on the quadratic performance index.By implementing the proposed composite controller to unmanned systems,simultaneous feedforward compensation and feedback suppression to the multi-source disturbances are conducted.Finally,the convergence of the MTN and the stability of the closed-loop system are established utilizing the Lyapunov theorem.Two exemplary applications of unmanned systems involving unmanned vehicle and rigid spacecraft are presented to validate the effectiveness of the proposed approach.展开更多
The rapid recombination of photogenerated carriers poses a significant limitation on the use of CdS quantum dots(QDs)in photocatalysis.Herein,the construction of a novel S-scheme heterojunction between cubic-phase CdS...The rapid recombination of photogenerated carriers poses a significant limitation on the use of CdS quantum dots(QDs)in photocatalysis.Herein,the construction of a novel S-scheme heterojunction between cubic-phase CdS QDs and hollow nanotube In_(2)O_(3)is successfully achieved using an electrostatic self-assembly method.Under visible light irradiation,all CdS-In_(2)O_(3)composites exhibit higher hydrogen evolution efficiency compared to pure CdS QDs.Notably,the photocatalytic H_(2)evolution rate of the optimal CdS-7%In_(2)O_(3)composite is determined to be 2258.59μmol g^(−1)h^(−1),approximately 12.3 times higher than that of pure CdS.The cyclic test indicates that the CdS-In_(2)O_(3)composite maintains considerable activity even after 5 cycles,indicating its excellent stability.In situ X-ray photoelectron spectroscopy and density functional theory calculations confirm that carrier migration in CdS-In_(2)O_(3)composites adheres to a typical S-scheme heterojunction mechanism.Additionally,a series of characterizations demonstrate that the formation of S-scheme heterojunctions between In_(2)O_(3)and CdS inhibits charge recombination and accelerates the separation and migration of photogenerated carriers in the CdS QDs,thus achieving enhanced photocatalytic performance.This work elucidates the pivotal role of S-scheme heterojunctions in photocatalytic H_(2)production and offers novel insights into the construction of effective composite photocatalysts.展开更多
The goal of photocatalytic CO_(2)reduction is to obtain a single energy-bearing product with high efficiency and stability.Consequently,constructing highly selective photocatalysts with enhanced surface and optoelectr...The goal of photocatalytic CO_(2)reduction is to obtain a single energy-bearing product with high efficiency and stability.Consequently,constructing highly selective photocatalysts with enhanced surface and optoelectronic properties is crucial for achieving this objective.Here,we have developed a simple one-pot vulcanization method to synthesize a MIL-68(In)-derived Cd In_(2)S_(4)/In_(2)S_(3)heterojunction that exhibited stable and high selectivity.Multiple characterizations of the Cd In_(2)S_(4)/In_(2)S_(3)heterojunction revealed a hierarchical tubular structure with numerous surface reactive sites,a high visible-light utilization rate(λ<600 nm),efficient charge separation,and a prolonged charge-carrier lifetime.Moreover,an S-scheme charge transfer mechanism,based on the interleaved band between the two components,improved the reduction capability of the electrons.Benefiting from the compositional and structural synergy,the yield CO by Cd In_(2)S_(4)/In_(2)S_(3)-250(CI-250)reached 135.62μmol·g^(-1)·h^(-1),which was 49.32 times and 32.88 times higher than that of In_(2)S_(3)and Cd In_(2)S_(4),respectively.The Cd In_(2)S_(4)/In_(2)S_(3)heterojunction exhibited a quantum efficiency of 4.23%with a CO selectivity of 71%.Four cycle tests confirmed the good stability and recyclability of the CI-250.This work provides a new approach for designing and preparing high-performance hollow MOFsbased photocatalysts for scalable and sustainable CO_(2)reduction.展开更多
BiVO_(4)porous spheres modified by ZnO were designed and synthesized using a facile two-step method.The resulting ZnO/BiVO_(4)composite catalysts have shown remarkable efficiency as piezoelectric catalysts for degradi...BiVO_(4)porous spheres modified by ZnO were designed and synthesized using a facile two-step method.The resulting ZnO/BiVO_(4)composite catalysts have shown remarkable efficiency as piezoelectric catalysts for degrading Rhodamine B(RhB)unde mechanical vibrations,they exhibit superior activity compared to pure ZnO.The 40wt%ZnO/BiVO_(4)heterojunction composite displayed the highest activity,along with good stability and recyclability.The enhanced piezoelectric catalytic activity can be attributed to the form ation of an I-scheme heterojunction structure,which can effectively inhibit the electron-hole recombination.Furthermore,hole(h+)and superoxide radical(·O_(2)^(-))are proved to be the primary active species.Therefore,ZnO/BiVO_(4)stands as an efficient and stable piezoelectric catalyst with broad potential application in the field of environmental water pollution treatment.展开更多
There is limited research reported on the multiple loss mechanism of electromagnetic waves(EMW)and the development of interface models.Dielectric loss and magnetic loss,as the two primary attenuation mechanisms in EMW...There is limited research reported on the multiple loss mechanism of electromagnetic waves(EMW)and the development of interface models.Dielectric loss and magnetic loss,as the two primary attenuation mechanisms in EMW absorbers,still pose challenges,especially in elucidating the correlation between composition,morphology,interface,and performance.Here,we construct 3D hierarchical porous conducting network structures and Schottky heterojunctions(MoNi_(4)@NC-NiFe_(2)O_(4)@NC)with a high density of defects,using trimetallic NiMoFe-MOFs.Synergistic enhancement of the dielectric and magnetic losses is realized through manipulation of the defects,interfaces,phase engineering,and magnetic resonance.In particular,the even dispersion of magnetic MoNi_(4) and NiFe_(2)O_(4)nanoparticles(NPs)within the carbon matrix triggers the creation of multiple heterogeneous interfaces.These inseparable interfaces,along with oxygen vacancies,play a role in enhancing dielectric polarization,while the closely spaced interactions among magnetic units contribute to magnetic loss.After optimizing the interfacial structure,NiFe_(2)O_(4)/MoNi_(4)-NC exhibits remarkable EMW absorption properties.A reflection loss(RL)value of-67.91 dB can be achieved at an ultra-thin thickness of 1.95 mm,and the effective absorption bandwidth(EAB,RL≤-10 dB)is as high as 5.76 GHz.Furthermore,we conducted radar scattering cross-section(RCS)simulations using computer simulation technology(CST)software,which revealed that NiFe_(2)O_(4)/MoNi_(4)-NC exhibits an RCS reduction value of 39.1 dB m^(2).Hence,this work provides comprehensive guidance for the construction of Schottky heterojunctions for lightweight EMW absorbers from a mechanistic point of view.展开更多
Fenton method combined with light to accelerate the production of free radicals from H2O2 can achieve more efficient pollutant degradation.In this paper,a novel BiOI/FeWO4 S-scheme heterojunction photocatalyst was obt...Fenton method combined with light to accelerate the production of free radicals from H2O2 can achieve more efficient pollutant degradation.In this paper,a novel BiOI/FeWO4 S-scheme heterojunction photocatalyst was obtained by in situ synthesis,which can activate H2O2 and degrade the organic pollutant OFC(ofloxacin)under visible light.The S-scheme charge transfer mechanism was confirmed by XPS spectroscopy,in situ KPFM and theoretical calculation.The photogenerated electrons were transferred from FeWO4 to BiOI driven by the built-in electric field and band bending,which inhibited carrier recombination and facilitated the activation of H2O2.The BiFe-5/Vis/H2O2 system degraded OFC up to 96.4%in 60 min.This study provides new systematic insights into the activation of H2O2 by S-scheme heterojunctions,which is of great significance for the treatment of antibiotic wastewater.展开更多
Coatings of marine equipment inevitably suffer from physical or chemical damage in service,together with biofouling from microbial attachment,leading to a shorter service life of them.Herein,a multi-functional corrosi...Coatings of marine equipment inevitably suffer from physical or chemical damage in service,together with biofouling from microbial attachment,leading to a shorter service life of them.Herein,a multi-functional corrosion-resistant coating with efficient photothermal self-healing and anti-biofouling per-formance was designed by using CuO/g-C_(3)N_(4)(CuO/CN)S-scheme heterojunction filler in combination with polydimethylsiloxane(PDMS)as the coating matrix for achieving the effective protection of Q235 steel.The results of the electrochemical impedance spectroscopy(EIS)experiments indicate that the CuO/CN/PDMS composite coatings possessed excellent corrosion resistance,in which the impedance ra-dius of optimal CuO/CN-1/PDMS composite coating could still remain 3.49×10^(9)Ωcm^(2)after 60 d of immersion in seawater under sunlight irradiation.Meanwhile,the as-prepared CuO/CN/PDMS compos-ite coating not only can be rapidly heated up under the Xenon lamp illumination to achieve complete self-repair of scratches within 45 min,but also exhibited excellent antimicrobial effects in the antifouling experiments.This study opens a new avenue for the development of g-C_(3)N_(4)-based multifunctional coat-ings and provides guidance for the development of the next generation of intelligent protective coatings.展开更多
Composite solid electrolytes(CSEs)are considered among the most promising candidates for solid-state batteries.However,their practical application is hindered by low ionic conductivity and a limited lithium-ion transf...Composite solid electrolytes(CSEs)are considered among the most promising candidates for solid-state batteries.However,their practical application is hindered by low ionic conductivity and a limited lithium-ion transference number,primarily owing to the insufficient mobility of Li+.In this work,we design a heterojunc-tion nanoparticle composed of bimetallic zeolitic imidazolate frameworks(ZIFs)coupled with amorphous tita-nium oxide(TiO_(2)@Zn/Co–ZIF)as a filler to fabricate a composite solid-state electrolyte(PVZT).The amor-phous TiO_(2) coating facilitates salt dissociation through Lewis acid–base interactions with the anions of the lithium salt.Meanwhile,the Zn/Co–ZIF framework not only provides additional selective pathways for Li+transport but also effectively restricts anion migration through its confined pore size.The synergistic effect results in a high room-temperature ionic conductivity(8.8×10^(-4) S·cm^(-1))and a lithium-ion transference number of 0.47 for PVZT.A symmetrical cell using PVZT demonstrates stable Li+deposition/stripping for over 1100 h at a current density of 0.1 mA·cm^(-2).Additionally,a LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)/Li full cell using PVZT retains 75.0%of its capacity after 1200 cycles at a 2 C rate.This work offers valuable insights into the design of func-tional fillers for CSEs with highly efficient ion transport.展开更多
S-scheme heterojunctions have gained widespread application in photocatalytic reactions due to their dis-tinctive carrier transport mechanism and remarkable redox capabilities.However,a significant challenge persists ...S-scheme heterojunctions have gained widespread application in photocatalytic reactions due to their dis-tinctive carrier transport mechanism and remarkable redox capabilities.However,a significant challenge persists in extending carrier lifetimes while simultaneously enhancing light absorption,both of which are essential for optimizing photocatalytic activity.Herein,we report the solvothermal synthesis of ul-trathin CdS nanosheets grown in situ on two-dimensional(2D)Ni-MOF to construct 2D/2D S-scheme heterojunctions.Comprehensive characterizations reveal that the incorporation of Ni-MOF(metal-organic framework)with ligand-to-metal charge transfer(LMCT)states not only broadens optical absorption but also significantly prolongs carrier lifetimes.This synergistic enhancement,coupled with the S-scheme charge transport mechanism,enables the composite to function as a bifunctional catalyst for photocat-alytic hydrogen production and simultaneous benzylamine coupling.The optimal system demonstrates an impressive hydrogen evolution rate of 8.5 mmol g^(-1) h^(-1) and an N-benzylidenebenzylamine yield of 4.6 mmol g^(-1) h^(-1) without requiring a cocatalyst.This work underscores the potential of integrating MOFs with LMCT states into S-scheme heterojunctions to enhance interfacial charge transfer,offering valuable insights for the design of S-scheme heterojunctions for artificial photosynthesis and related fields.展开更多
基金supported by the Science & Technology Project of Anhui Province (16030701091)the Natural Science Research Project of Anhui Provincial Education Department (KJ2019A0030)+2 种基金the Support Project of Outstanding Young Talents in Anhui Provincial Universities (gxyqZD2018006)the National Natural Science Foundation of China(11704002, 31701323)the Anhui Provincial Natural Science Foundation (1908085QF251,1808085MF185)
文摘A multi-dimensional conductive heterojunction structure,composited by TiO2,SnO2,and Ti3C2TX MXene,is facilely designed and applied as electron transport layer in efficient and stable planar perovskite solar cells.Based on an oxygen vacancy scramble effect,the zero-dimensional anatase TiO2 quantum dots,surrounding on two-dimensional conductive Ti3C2TX sheets,are in situ rooted on three-dimensional SnO2 nanoparticles,constructing nanoscale TiO2/SnO2 heterojunctions.The fabrication is implemented in a controlled lowtemperature anneal method in air and then in N2 atmospheres.With the optimal MXene content,the optical property,the crystallinity of perovskite layer,and internal interfaces are all facilitated,contributing more amount of carrier with effective and rapid transferring in device.The champion power conversion efficiency of resultant perovskite solar cells achieves 19.14%,yet that of counterpart is just 16.83%.In addition,it can also maintain almost 85%of its initial performance for more than 45 days in 30–40%humidity air;comparatively,the counterpart declines to just below 75%of its initial performance.
文摘The efficiency and stability of catalysts for photocatalytic hydrogen evolution(PHE)are largely governed by the charge transfer behaviors across the heterojunction interfaces.In this study,CuO,a typical semiconductor featuring a broad spectral absorption range,is successfully employed as the electron acceptor to combine with CdS for constructing a S-scheme heterojunction.The optimized photocatalyst(CdSCuO2∶1)delivers an exceptional hydrogen evolution rate of 18.89 mmol/(g·h),4.15-fold higher compared with bare CdS.X-ray photoelectron spectroscopy(XPS)and ultraviolet-visible diffuse reflection absorption spectroscopy(UV-vis DRS)confirmed the S-scheme band structure of the composites.Moreover,the surface photovoltage(SPV)and electron paramagnetic resonance(EPR)indicated that the photogenerated electrons and photogenerated holes of CdS-CuO2∶1 were respectively transferred to the conduction band(CB)of CdS with a higher reduction potential and the valence band(VB)of CuO with a higher oxidation potential under illumination,as expected for the S-scheme mechanism.Density-functional-theory calculations of the electron density difference(EDD)disclose an interfacial electric field oriented from CdS to CuO.This built-in field suppresses charge recombination and accelerates carrier migration,rationalizing the markedly enhanced PHE activity.This study offers a novel strategy for designing S-scheme heterojunctions with high light harvesting and charge utilization toward sustainable solar-tohydrogen conversion.
基金support of the National Natural Science Foundation of China(22075131 and 22078265)the Shaanxi Fundamental Science Research Project for Mathematics and Physics under Grants(No.22JSZ005)the State-Key Laboratory of Multiphase Complex Systems(No.MPCS-2021-A).
文摘Lithium-sulfur(Li-S)batteries require efficient catalysts to accelerate polysulfide conversion and mitigate the shuttle effect.However,the rational design of catalysts remains challenging due to the lack of a systematic strategy that rationally optimizes electronic structures and mesoscale transport properties.In this work,we propose an autogenously transformed CoWO_(4)/WO_(2) heterojunction catalyst,integrating a strong polysulfide-adsorbing intercalation catalyst with a metallic-phase promoter for enhanced activity.CoWO_(4) effectively captures polysulfides,while the CoWO_(4)/WO_(2) interface facilitates their S-S bond activation on heterogenous catalytic sites.Benefiting from its directional intercalation channels,CoWO_(4) not only serves as a dynamic Li-ion reservoir but also provides continuous and direct pathways for rapid Li-ion transport.Such synergistic interactions across the heterojunction interfaces enhance the catalytic activity of the composite.As a result,the CoWO_(4)/WO_(2) heterostructure demonstrates significantly enhanced catalytic performance,delivering a high capacity of 1262 mAh g^(−1) at 0.1 C.Furthermore,its rate capability and high sulfur loading performance are markedly improved,surpassing the limitations of its single-component counterparts.This study provides new insights into the catalytic mechanisms governing Li-S chemistry and offers a promising strategy for the rational design of high-performance Li-S battery catalysts.
基金financial support from the National Natural Science Foundation of China(22109127)the Chinese Postdoctoral Science Foundation(2021M702666),+1 种基金he Research Fund of the State Key Laboratory of Solidification Processing(NPU),China(Grant No.2023-TS-02)financial support from the Youth Project of"Shaanxi High-level Talents Introduction Plan"and the Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education)are also sincerely appreciated.
文摘Photo-assisted lithium–sulfur batteries(PALSBs)offer an eco-friendly solution to address the issue of sluggish reaction kinetics of conventional LSBs.However,designing an efficient photoelectrode for practical implementation remains a significant challenge.Herein,we construct a free-standing polymer–inorganic hybrid photoelectrode with a direct Z-scheme heterostructure to develop high-efficiency PALSBs.Specifically,polypyrrole(PPy)is in situ vapor-phase polymerized on the surface of N-doped TiO_(2) nanorods supported on carbon cloth(N-TiO_(2)/CC),thereby forming a well-defined p–n heterojunction.This architecture efficiently facilitates the carrier separation of photo-generated electron–hole pairs and significantly enhances carrier transport by creating a built-in electric field.Thus,the PPy@N-TiO_(2)/CC can simultaneously act as a photocatalyst and an electrocatalyst to accelerate the reduction and evolution of sulfur,enabling ultrafast sulfur redox dynamics,as convincingly validated by both theoretical simulations and experimental results.Consequently,the PPy@N-TiO_(2)/CC PALSB achieves a high discharge capacity of 1653 mAh g−1,reaching 98.7%of the theoretical value.Furthermore,5 h of photo-charging without external voltage enables the PALSB to deliver a discharge capacity of 333 mAh g−1,achieving dual-mode energy harvesting capabilities.This work successfully integrates solar energy conversion and storage within a rechargeable battery system,providing a promising strategy for sustainable energy storage technologies.
基金financially supported by the National Basic Research Program of China(Nos.2022YFA1603701,2024YFC2310502,and 2024YFC2310503)the National Natural Science Foundation of China(Nos.22422403,82341044,and 22027810)+1 种基金the New Cornerstone Science Foundation(No.NCI202318)the Basic Science Center Project of the National Natural Science Foundation of China(No.22388101).
文摘Drug-resistant bacteria,using their dense cell membranes as strong barrier,significantly reduce the efficacy of conventional antibacterial treatments.Phototriggered 2D catalytic nanomaterials have emerged as promising candidates against drug-resistant bacteria by inducing membrane mechanical damage and generating reactive oxygen species(ROS).However,the practical antibacterial efficacy of typical 2D graphitic carbon nitride(g-C_(3)N_(4))is severely limited due to the low ROS production.Herein,we report an interfacial band-engineered lamellar heterojunctions(MnCN LHJs)through in situ Mn_(2)O_(3)growth on g-C_(3)N_(4).The charges generated in g-C_(3)N_(4)are stabilized by Mn_(2)O_(3),minimizing electron-hole recombination and boosting ROS production.Meanwhile,the photocatalytic effect of MnCN LHJs works synergistically with photothermal effects of Mn_(2)O_(3)to induce a robust“melee attack”against drug-resistant bacteria.High-resolution synchrotron radiation X-ray tomography directly visualized that MnCN LHJs possessed bacterial trapping capabilities,revealing their ability to induce mechanical damage to bacteria membrane for the first time.Additionally,MnCN LHJs can deplete endogenous glutathione,thereby enhancing ROS generation and weakening the bacterial antioxidant defense system.These combined effects achieve a remarkable bactericidal rate exceeding 98% against methicillin-resistant Staphylococcus aureus(MRSA).Notably,MnCN LHJs demonstrate prolonged retention at wound sites,helping to reduce inflammation and promote angiogenesis in infected wounds.This work not only advances interfacial band engineering approach to enhance the photocatalytic performance of g-C_(3)N_(4)but also underscores the significance of nanomaterial-bacteria interaction in design of next-generation antibacterial materials.
基金supported by the National Natural Science Foundation of China(No.11974152)the Liaoning Provincial Natural Science Foundation Program,the Doctoral Research Initiation Project(No.2024-BS-003)the Liaoning University 2024 Basic Research Projects in Science and Technology(No.LJ212410140026).
文摘The exploration of efficient photocatalytic materials for CO_(2)conversion into hydrocarbon energy fuel is of paramount significance.However,problems,such as rapid charge recombination,low quantum efficiency,and poor product selectivity,still limit the efficiency of photocatalytic CO_(2)reduction.Here,this study reports a Sscheme heterostructure of MnFe_(2)O_(4)/Bi_(2)WO_(6),formed by loading MnFe_(2)O_(4)nanoparticles onto Bi_(2)WO_(6) microflowers with oxygen-rich vacancies,enabling photocatalytic CO_(2)reduction.Notably,the developed MnFe_(2)O_(4)/Bi_(2)WO_(6) heterostructure improved the photocatalytic CO_(2)reduction ability,achieving a maximum CO generation rate of 32.7μmol·h^(-1)·g^(-1),which is 3.7 and 14.3 times higher than that of Bi_(2)WO_(6) and MnFe_(2)O_(4),respectively.Additionally,the CO production mechanism by CO_(2)photocatalytic reduction was proposed based on detailed characterization and density functional theory(DFT)calculation.The findings of this study suggest that introducing oxygen vacancies and constructing heterojunctions can significantly improve the photocatalytic CO_(2)reduction performance of Bi_(2)WO_(6).
基金the Natural Science Foundation of Jiangsu Province(No.BK20253049)the Science and Technology Program of Xuzhou(No.KC25028)+3 种基金the Basic Science(Natural Science)Research Project of Higher Education Institutions in Jiangsu Province(No.25KJB430013)the Natural Science Foundation of the Jiangsu Higher Education Institutions of China(No.24KJA150003)the National Natural Science Foundation of China(No.22271122)the Xuzhou Key Research and Development Program(Social Development)(No.KC23298).
文摘Heterostructure engineering has emerged as a promising strategy to enhance the electrochemical CO_(2)reduction reaction(CO_(2)RR)by optimizing interfacial electron transfer.Herein,we report a novel octahedral SnS_(2)/SnO_(2)heterojunction catalyst synthesized via an ion-exchange vulcanization method,which achieves exceptional activity and selectivity for CO_(2)-toformate conversion.Through in-situ Raman spectroscopy,ex-situ X-ray diffraction(XRD),and X-ray photoelectron spectroscopy(XPS),we demonstrate that the octahedral SnS_(2)/SnO_(2)heterojunction dynamically restructures into a sulfur-doped Sn/SnO_(2)(Sn(S)/SnO_(2))heterostructure under operating conditions.Density functional theory(DFT)calculations reveal that the Sn(S)/SnO_(2)interface facilitates electron transfer from SnO_(2)to metallic Sn(S),generating a built-in electric field that stabilizes Sn^(4+)in SnO_(2)and accelerates proton-coupled electron transfer to*OCHO intermediates.Consequently,the catalyst achieves a formate Faradaic efficiency exceeding 90% over a broad potential window(-0.6 to -1.0 V vs.reversible hydrogen electrode(RHE))with a high partial current density of -280 mA·cm^(-2),surpassing most reported Sn-based catalysts.This work elucidates the structural dynamics and interfacial enhancement mechanisms of heterojunction catalysts,offering a rational design principle for advanced CO_(2)RR electrocatalysts.
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the National Natu-ral Science Foundation of China(Nos.22108133,51972180,and 41907315)the Science,Education and Industry Integration of Basic Research Projects of Qilu University of Technology(No.2022PY062)the Youth Innovation Team Development Plan of Universities in Shandong Province(No.2021KJ056).
文摘S-scheme heterostructure photocatalysts utilize the synergistic and superposition effects of materials,ef-fectively separating electrons and holes,maintaining strong redox capacity,and addressing issues en-countered by current photocatalytic reactions.This review explores the origins and unique benefits of S-scheme heterojunctions.Specifically,we summarized and discussed the effects of different dimensions of semiconductors constituting S-scheme heterojunctions and the similarities and differences in elec-tron transfer processes when constructing heterojunctions.Additionally,we analyzed several methods for proving the formation of S-scheme heterojunctions and the electron transfer process,both directly and indirectly.Finally,we review the applications of S-scheme heterojunctions in various fields of photo-catalysis,including photocatalytic water splitting,pollution degradation,CO_(2) reduction and other related photocatalytic applications.Our hope is that this review will provide an essential reference for the devel-opment and application of S-scheme heterojunction photocatalysis.
基金supported by the National Natural Science Foundation of China (Nos.52072152 and 51802126)Jiangsu University Jinshan Professor Fund,Jiangsu Specially-Appointed Professor Fund,the Open Fund from Guangxi Key Laboratory of Electrochemical Energy Materials,Zhenjiang“Jinshan Talents”Project 2021,China PostDoctoral Science Foundation (No.2022M721372)+1 种基金the“Doctor of Entrepreneurship and Innovation”in Jiangsu Province (No.JSSCBS20221197)the Postgraduate Research&Practice Innovation Program of Jiangsu Province (No.KYCX22_3645).
文摘In the quest for effective solutions to address Environ.Pollut.and meet the escalating energy demands,heterojunction photocatalysts have emerged as a captivating and versatile technology.These photocatalysts have garnered significant interest due to their wideranging applications,including wastewater treatment,air purification,CO_(2) capture,and hydrogen generation via water splitting.This technique harnesses the power of semiconductors,which are activated under light illumination,providing the necessary energy for catalytic reactions.With visible light constituting a substantial portion(46%)of the solar spectrum,the development of visible-light-driven semiconductors has become imperative.Heterojunction photocatalysts offer a promising strategy to overcome the limitations associated with activating semiconductors under visible light.In this comprehensive review,we present the recent advancements in the field of photocatalytic degradation of contaminants across diverse media,as well as the remarkable progress made in renewable energy production.Moreover,we delve into the crucial role played by various operating parameters in influencing the photocatalytic performance of heterojunction systems.Finally,we address emerging challenges and propose novel perspectives to provide valuable insights for future advancements in this dynamic research domain.By unraveling the potential of heterojunction photocatalysts,this reviewcontributes to the broader understanding of their applications and paves the way for exciting avenues of exploration and innovation.
基金supported by the National Natural Science Foundation of China(22302019)the Changzhou Sci&Tech Program(CJ20220214).
文摘It is very appealing that 5-hydroxymethylfurfural(HMF)is electrocatalytical oxidized as 2,5-furandicarboxylic acid(FDCA)linking to non-classical cathodic hydrogen(H_(2))production.However,the electrocatalysts for electrocatalytic HMF oxidative reaction(e-HMFOR)have been facing low Faradaic efficiency(FE)and high water splitting voltage.Herein,we propose a strategy of the NiSeO_(3)@(CoSeO_(3))_(4)heterojunction by constructing a Co-Ni paired site,where the Co site is in charge of adsorbing for HMF while the electrons are transferred to the Ni site,thus giving the NiSeO_(3)@(CoSeO_(3))_(4)heterojunction superior electrocata lytic performances for e-HMFOR and water splitting.By optimizing conditions,the NiSeO_(3)@(CoSeO_(3))_(4)heterojunction has high conversion of 99.7%,high selectivity of 99.9%,and high FE of 98.4%at 1.3 V,as well as low cell voltage of 1.31 V at 10 mA cm^(-2)in 1 M KOH+0.1 M HMF.This study offers a potential insight for e-HMFOR to high value-added FDCA coupling water splitting to produce H_(2)in an economical manner.
基金co-supported by the National Key R&D Program of China(No.2023YFB4704400)the Zhejiang Provincial Natural Science Foundation of China(No.LQ24F030012)the National Natural Science Foundation of China General Project(No.62373033)。
文摘A composite anti-disturbance predictive control strategy employing a Multi-dimensional Taylor Network(MTN)is presented for unmanned systems subject to time-delay and multi-source disturbances.First,the multi-source disturbances are addressed according to their specific characteristics as follows:(A)an MTN data-driven model,which is used for uncertainty description,is designed accompanied with the mechanism model to represent the unmanned systems;(B)an adaptive MTN filter is used to remove the influence of the internal disturbance;(C)an MTN disturbance observer is constructed to estimate and compensate for the influence of the external disturbance;(D)the Extended Kalman Filter(EKF)algorithm is utilized as the learning mechanism for MTNs.Second,to address the time-delay effect,a recursiveτstep-ahead MTN predictive model is designed utilizing recursive technology,aiming to mitigate the impact of time-delay,and the EKF algorithm is employed as its learning mechanism.Then,the MTN predictive control law is designed based on the quadratic performance index.By implementing the proposed composite controller to unmanned systems,simultaneous feedforward compensation and feedback suppression to the multi-source disturbances are conducted.Finally,the convergence of the MTN and the stability of the closed-loop system are established utilizing the Lyapunov theorem.Two exemplary applications of unmanned systems involving unmanned vehicle and rigid spacecraft are presented to validate the effectiveness of the proposed approach.
文摘The rapid recombination of photogenerated carriers poses a significant limitation on the use of CdS quantum dots(QDs)in photocatalysis.Herein,the construction of a novel S-scheme heterojunction between cubic-phase CdS QDs and hollow nanotube In_(2)O_(3)is successfully achieved using an electrostatic self-assembly method.Under visible light irradiation,all CdS-In_(2)O_(3)composites exhibit higher hydrogen evolution efficiency compared to pure CdS QDs.Notably,the photocatalytic H_(2)evolution rate of the optimal CdS-7%In_(2)O_(3)composite is determined to be 2258.59μmol g^(−1)h^(−1),approximately 12.3 times higher than that of pure CdS.The cyclic test indicates that the CdS-In_(2)O_(3)composite maintains considerable activity even after 5 cycles,indicating its excellent stability.In situ X-ray photoelectron spectroscopy and density functional theory calculations confirm that carrier migration in CdS-In_(2)O_(3)composites adheres to a typical S-scheme heterojunction mechanism.Additionally,a series of characterizations demonstrate that the formation of S-scheme heterojunctions between In_(2)O_(3)and CdS inhibits charge recombination and accelerates the separation and migration of photogenerated carriers in the CdS QDs,thus achieving enhanced photocatalytic performance.This work elucidates the pivotal role of S-scheme heterojunctions in photocatalytic H_(2)production and offers novel insights into the construction of effective composite photocatalysts.
基金financially supported by the Program for the Development of Science and Technology of Jilin Province(Nos.20240601047RC and YDZJ202201ZYTS629)Hainan Province Science and Technology Special Fund(No.ZDYF2022SHFZ090)+1 种基金the National Natural Science Foundation(Nos.22466017 and 22061014)the specific research fund of the Innovation Platform for Academicians of Hainan Province。
文摘The goal of photocatalytic CO_(2)reduction is to obtain a single energy-bearing product with high efficiency and stability.Consequently,constructing highly selective photocatalysts with enhanced surface and optoelectronic properties is crucial for achieving this objective.Here,we have developed a simple one-pot vulcanization method to synthesize a MIL-68(In)-derived Cd In_(2)S_(4)/In_(2)S_(3)heterojunction that exhibited stable and high selectivity.Multiple characterizations of the Cd In_(2)S_(4)/In_(2)S_(3)heterojunction revealed a hierarchical tubular structure with numerous surface reactive sites,a high visible-light utilization rate(λ<600 nm),efficient charge separation,and a prolonged charge-carrier lifetime.Moreover,an S-scheme charge transfer mechanism,based on the interleaved band between the two components,improved the reduction capability of the electrons.Benefiting from the compositional and structural synergy,the yield CO by Cd In_(2)S_(4)/In_(2)S_(3)-250(CI-250)reached 135.62μmol·g^(-1)·h^(-1),which was 49.32 times and 32.88 times higher than that of In_(2)S_(3)and Cd In_(2)S_(4),respectively.The Cd In_(2)S_(4)/In_(2)S_(3)heterojunction exhibited a quantum efficiency of 4.23%with a CO selectivity of 71%.Four cycle tests confirmed the good stability and recyclability of the CI-250.This work provides a new approach for designing and preparing high-performance hollow MOFsbased photocatalysts for scalable and sustainable CO_(2)reduction.
基金financially supported by the National Natural Science Foundation of China(No.22272151)Public Welfare Technology Application Research Project of Jinhua City,China(No.2023-4-022)。
文摘BiVO_(4)porous spheres modified by ZnO were designed and synthesized using a facile two-step method.The resulting ZnO/BiVO_(4)composite catalysts have shown remarkable efficiency as piezoelectric catalysts for degrading Rhodamine B(RhB)unde mechanical vibrations,they exhibit superior activity compared to pure ZnO.The 40wt%ZnO/BiVO_(4)heterojunction composite displayed the highest activity,along with good stability and recyclability.The enhanced piezoelectric catalytic activity can be attributed to the form ation of an I-scheme heterojunction structure,which can effectively inhibit the electron-hole recombination.Furthermore,hole(h+)and superoxide radical(·O_(2)^(-))are proved to be the primary active species.Therefore,ZnO/BiVO_(4)stands as an efficient and stable piezoelectric catalyst with broad potential application in the field of environmental water pollution treatment.
基金supported by the National Natural Science Foundation of China(No.22269010)the Jiangxi Provincial Natural Science Foundation(No.20224BAB214021).
文摘There is limited research reported on the multiple loss mechanism of electromagnetic waves(EMW)and the development of interface models.Dielectric loss and magnetic loss,as the two primary attenuation mechanisms in EMW absorbers,still pose challenges,especially in elucidating the correlation between composition,morphology,interface,and performance.Here,we construct 3D hierarchical porous conducting network structures and Schottky heterojunctions(MoNi_(4)@NC-NiFe_(2)O_(4)@NC)with a high density of defects,using trimetallic NiMoFe-MOFs.Synergistic enhancement of the dielectric and magnetic losses is realized through manipulation of the defects,interfaces,phase engineering,and magnetic resonance.In particular,the even dispersion of magnetic MoNi_(4) and NiFe_(2)O_(4)nanoparticles(NPs)within the carbon matrix triggers the creation of multiple heterogeneous interfaces.These inseparable interfaces,along with oxygen vacancies,play a role in enhancing dielectric polarization,while the closely spaced interactions among magnetic units contribute to magnetic loss.After optimizing the interfacial structure,NiFe_(2)O_(4)/MoNi_(4)-NC exhibits remarkable EMW absorption properties.A reflection loss(RL)value of-67.91 dB can be achieved at an ultra-thin thickness of 1.95 mm,and the effective absorption bandwidth(EAB,RL≤-10 dB)is as high as 5.76 GHz.Furthermore,we conducted radar scattering cross-section(RCS)simulations using computer simulation technology(CST)software,which revealed that NiFe_(2)O_(4)/MoNi_(4)-NC exhibits an RCS reduction value of 39.1 dB m^(2).Hence,this work provides comprehensive guidance for the construction of Schottky heterojunctions for lightweight EMW absorbers from a mechanistic point of view.
基金supported by the National Key Research and Development Program of China(2020YFD1100501)Thanks zkec(www.zjkec.cc)for XRD.
文摘Fenton method combined with light to accelerate the production of free radicals from H2O2 can achieve more efficient pollutant degradation.In this paper,a novel BiOI/FeWO4 S-scheme heterojunction photocatalyst was obtained by in situ synthesis,which can activate H2O2 and degrade the organic pollutant OFC(ofloxacin)under visible light.The S-scheme charge transfer mechanism was confirmed by XPS spectroscopy,in situ KPFM and theoretical calculation.The photogenerated electrons were transferred from FeWO4 to BiOI driven by the built-in electric field and band bending,which inhibited carrier recombination and facilitated the activation of H2O2.The BiFe-5/Vis/H2O2 system degraded OFC up to 96.4%in 60 min.This study provides new systematic insights into the activation of H2O2 by S-scheme heterojunctions,which is of great significance for the treatment of antibiotic wastewater.
基金supported by the National Natural Science Foundation of China(Nos.22006057 and 21906072)the China Postdoctoral Science Foundation(No.2023M743178)+2 种基金the Jiangsu Province Industry-University-Research Cooperation Project(No.BY20231482)the Open Fund of the Key Laboratory of Solar Cell electrode Materials in China Petroleum,Chemical Industry(No.2024A093)the Key Laboratory of Functional Inorganic Mate-rial Chemistry(Heilongjiang University),Ministry of Education and Postgraduate Research&Practice Innovation Program of Jiangsu Province(China)(No.SJCX24_2481).
文摘Coatings of marine equipment inevitably suffer from physical or chemical damage in service,together with biofouling from microbial attachment,leading to a shorter service life of them.Herein,a multi-functional corrosion-resistant coating with efficient photothermal self-healing and anti-biofouling per-formance was designed by using CuO/g-C_(3)N_(4)(CuO/CN)S-scheme heterojunction filler in combination with polydimethylsiloxane(PDMS)as the coating matrix for achieving the effective protection of Q235 steel.The results of the electrochemical impedance spectroscopy(EIS)experiments indicate that the CuO/CN/PDMS composite coatings possessed excellent corrosion resistance,in which the impedance ra-dius of optimal CuO/CN-1/PDMS composite coating could still remain 3.49×10^(9)Ωcm^(2)after 60 d of immersion in seawater under sunlight irradiation.Meanwhile,the as-prepared CuO/CN/PDMS compos-ite coating not only can be rapidly heated up under the Xenon lamp illumination to achieve complete self-repair of scratches within 45 min,but also exhibited excellent antimicrobial effects in the antifouling experiments.This study opens a new avenue for the development of g-C_(3)N_(4)-based multifunctional coat-ings and provides guidance for the development of the next generation of intelligent protective coatings.
基金supported by National Science Fund for Distinguished Young Scholars(Grant No.52325206)National Key Research and Development Program of China(Grant No.2021YFF0500600)+3 种基金National Natural Science Foundation of China(Grant Nos.U2001220 and 52203298)Shenzhen Technical Plan Project(Grant Nos.RCJC20200714114436091,JCYJ20220530143012027,JCYJ20220818101003008,and JCYJ20220818101003007)Tsinghua Shenzhen International Graduate School-Shenzhen Pengrui Young Faculty Program of Shenzhen Pengrui Foundation(Grant No.SZPR2023006)Shenzhen Science and Technology Program(Grant No.WDZC20231126160733001).
文摘Composite solid electrolytes(CSEs)are considered among the most promising candidates for solid-state batteries.However,their practical application is hindered by low ionic conductivity and a limited lithium-ion transference number,primarily owing to the insufficient mobility of Li+.In this work,we design a heterojunc-tion nanoparticle composed of bimetallic zeolitic imidazolate frameworks(ZIFs)coupled with amorphous tita-nium oxide(TiO_(2)@Zn/Co–ZIF)as a filler to fabricate a composite solid-state electrolyte(PVZT).The amor-phous TiO_(2) coating facilitates salt dissociation through Lewis acid–base interactions with the anions of the lithium salt.Meanwhile,the Zn/Co–ZIF framework not only provides additional selective pathways for Li+transport but also effectively restricts anion migration through its confined pore size.The synergistic effect results in a high room-temperature ionic conductivity(8.8×10^(-4) S·cm^(-1))and a lithium-ion transference number of 0.47 for PVZT.A symmetrical cell using PVZT demonstrates stable Li+deposition/stripping for over 1100 h at a current density of 0.1 mA·cm^(-2).Additionally,a LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)/Li full cell using PVZT retains 75.0%of its capacity after 1200 cycles at a 2 C rate.This work offers valuable insights into the design of func-tional fillers for CSEs with highly efficient ion transport.
基金financially supported by the National Key Re-search and Development Program of China(Nos.2022YFB3803600 and 2022YFE0115900)the National Natural Science Foundation of China(Nos.U24A2071,22278324,22238009,22361142704,22202187,and U23A20102)+1 种基金the National Science Foundation of Hubei Province of China(No.2022CFA001)Key R&D Program Projects in Hubei Province(No.2023BAB113).
文摘S-scheme heterojunctions have gained widespread application in photocatalytic reactions due to their dis-tinctive carrier transport mechanism and remarkable redox capabilities.However,a significant challenge persists in extending carrier lifetimes while simultaneously enhancing light absorption,both of which are essential for optimizing photocatalytic activity.Herein,we report the solvothermal synthesis of ul-trathin CdS nanosheets grown in situ on two-dimensional(2D)Ni-MOF to construct 2D/2D S-scheme heterojunctions.Comprehensive characterizations reveal that the incorporation of Ni-MOF(metal-organic framework)with ligand-to-metal charge transfer(LMCT)states not only broadens optical absorption but also significantly prolongs carrier lifetimes.This synergistic enhancement,coupled with the S-scheme charge transport mechanism,enables the composite to function as a bifunctional catalyst for photocat-alytic hydrogen production and simultaneous benzylamine coupling.The optimal system demonstrates an impressive hydrogen evolution rate of 8.5 mmol g^(-1) h^(-1) and an N-benzylidenebenzylamine yield of 4.6 mmol g^(-1) h^(-1) without requiring a cocatalyst.This work underscores the potential of integrating MOFs with LMCT states into S-scheme heterojunctions to enhance interfacial charge transfer,offering valuable insights for the design of S-scheme heterojunctions for artificial photosynthesis and related fields.
