CO_(2)-Induced Modulation of Si-O Bonds for Low Temperature Plastic Deformation of Amorphous Silica Nanoparticles with Enhanced Photoluminescence

Modulation of Si-O bonds under mild conditions has been a challenging issue in the field of material science,which is critical to manufacture highperformance silica-based optical and photonic devices.Herein,we introduce a nondestructive technique to achieve Si-O bond rearrangement,leading to plastic deformation and photoluminescence enhancement of amorphous silica nanoparticles using supercritical carbon dioxides in EtOH/H_(2)O solution under mild temperature.Specifically,plastic deformation is achieved by treating hollow mesoporous silica nanospheres using supercritical CO_(2)at 40°C under 20 MPa.Experimental and theoretical studies revealed the critical role of supercritical CO_(2)in the plastic deformation process,which can be intercalated into the hollow mesoporous silica nanospheres with anisotropic stresses and induces the rearrangement of Si-O bonds and transformation of ring structures.This work suggests a novel approach to engineer high-performance nano-silica glass components for numerous optical and photonic devices under mild condition.

Electro-assisted photocatalytic reduction of CO_(2) in ambient air using Ag/TNTAs at the gas-solid interface

The direct conversion of atmospheric CO_(2) into fuel via photocatalysis exhibits significant practical application value in advancing the carbon cycle.In this study,we established an electro-assisted photocatalytic system with dual compartments and interfaces,and coated Ag nanoparticles on the titanium nanotube arrays(TNTAs)by polydopamine modification.In the absence of sacrificial agent and alkali absorption liquid conditions,the stable,efficient and highly selective conversion of CO_(2) to CO at the gas-solid interface in ambient air was realized by photoelectric synergy.Specifically,with the assistance of potential,the CO formation rates reached 194.9μmol h^(−1) m^(−2) and 103.9μmol h^(−1) m^(−2) under ultraviolet and visible light irradiation,respectively;the corresponding CO_(2) conversion rates in ambient air were 30%and 16%,respectively.The excellent catalytic effect is mainly attributed to the formation of P–N heterojunction during the catalytic process and the surface plasmon resonance effect.Additionally,the introduction of solid agar electrolytes effectively inhibits the hydrogen evolution reaction and improves the electron utilization rate.This system promotes the development of photocatalytic technology for practical applications and provides new insights and support for the carbon cycle.

Carbon Doping Triggered Efficient Electrochemical Hydrogen Evolution of Cross-Linked Porous Ru-MoO_(2) Via Solid-Phase Reaction Strategy

The defect-free structure of Mo-based materials is a“double-edged sword”,which endows the material with excellent stability,but limits its chemical versatility and application in electrochemical hydrogen evolution reaction(HER).Carbon doping engineering is an attractive strategy to effectively improve the performance of Mo-based catalyst and maintain their stability.Herein,we report a cross-linked porous carbon-doped MoO_(2)(C–MoO_(2))-based catalyst Ru/C–MoO_(2) for electrochemical HER,which is prepared by the convenient redox solid-phase reaction(SPR)of porous RuO_(2)/Mo_(2)C composite precursor.Theoretical studies reveal that due to the presence of carbon atoms,the electronic structure of C–MoO_(2) has been properly adjusted,and the loaded small Ru nanoparticles provide a fast water dissociation rate and moderate H adsorption strength.In electrochemical studies under a pH-universal environment,Ru/C–MoO_(2) electrocatalyst exhibits a low overpotential at a current density of 10 mA cm^(-2) and has a low Tafel slope.Meanwhile,Ru/C-MoO_(2) has excellent stability for more than 100 h at an initial current density of 100 mA cm^(-2).

A universal multifunctional dual cation doping strategy towards stabilized ultra-high nickel cobalt-free lithium layered oxide cathode

Ultra-high nickel cobalt-free lithium layered oxides are promising cathode material for lithium-ion batteries(LIBs)because of their relatively high capacity and low cost.Nevertheless,the high nickel content would induce bulk structure degradation and interfacial environment deterioration,and the absence of Co element reduces the lithium diffusion kinetics,severely limiting the performance liberation of this kind of cathodes.Herein,a multifunctional Ti/Zr dual cation co-doping strategy has been employed to improve the lithium storage performance of LiNi_(0.9)Mn_(0.1)O_(2)(NM91)cathode.On the one hand,the Ti/Zr co-doping weakens the Li^(+)/Ni^(2+)mixing through magnetic interactions due to the inexistence of unpaired electrons for Ti^(4+)and Zr^(4+),increasing the lithium diffusion rate and suppressing the harmful coexistence of H1 and H2 phases.On the other hand,they enhance the lattice oxygen stability because of the strong Ti-O and Zr-O bonds,inhibiting the undesired H3 phase transition and lattice oxygen loss,improving the bulk structure and cathode-electrolyte interface stability.As a result,the Ti/Zr co-doped NM91(NMTZ)exhibits a 91.2%capacity retention rate after 100 cycles,while that of NM91 is only82.9%.Also,the NMTZ displays better rate performance than NM91 with output capacities of 115 and93 mA h g^(-1)at a high current density of 5 C,respectively.Moreover,the designed NMTZ could enable the full battery to deliver an energy density up to 263 W h kg^(-1),making the ultra-high nickel cobaltfree lithium layered oxide cathode closer to practical applications.

Cation-Anion Redox Active Organic Complex for High Performance Aqueous Zinc Ion Battery

Organic redox compounds are attractive cathode materials in aqueous zinc-ion batteries owing to their low cost,environmental friendliness,multiple-electron-transfer reactions,and resource sustainability.However,the realized energy density is constrained by the limited capacity and low voltage.Herein,copper-tetracyanoquinodimethane(CuTCNQ),an organic charge-transfer complex is evaluated as a zinc-ion battery cathode owing to the good electron acceptation ability in the cyano groups that improves the voltage output.Through electrochemical activation,electrolyte optimization,and adoption of graphene-based separator,CuTCNQ-based aqueous zinc-ion batteries deliver much improved rate performance and cycling stability with anti-self-discharge properties.The structural evolution of CuTCNQ during discharge/charge are investigated by ex situ Fourier transform infra-red(FT-IR)spectra,ex situ X-ray photoelectron spectroscopy(XPS),and in situ ultraviolet visible spectroscopy(UV-vis),revealing reversible redox reactions in both cuprous cations(Cu^(+))and organic anions(TCNQ^(x-1)),thus delivering a high voltage output of 1.0 V and excellent discharge capacity of 158 mAh g^(-1).The remarkable electrochemical performance in Zn//CuTCNQ is ascribed to the strong inductive effect of cyano groups in CuTCNQ that elevated the voltage output and the graphene-modified separator that inhibited CuTCNQ dissolution and shuttle effect in aqueous electrolytes.

Supramolecular Macrocycle Regulated Single-Atom MoS_(2)@Co Catalysts for Enhanced Oxygen Evolution Reaction

The development of active water oxidation catalysts for water splitting has stimulated considerable interest.Herein,the design and building of single atom Co sites using a supramolecular tailoring strategy are reported,that is,the introduction of pillar[4]arene[1]quinone(P4A1Q)permits mononuclear Co species stereoelectronically assembled on MoS_(2)matrix to construct an atomically dispersed MoS_(2)@Co catalyst with modulated local electronic structure,definite chemical environment and enhanced oxygen evolution reaction performance.Theoretical calculations indicate that immsobilized single-Co sites exhibit an optimized adsorption capability of oxygen-containing intermediates,endowing the catalyst an excellent electrocatalytic oxygen evolution reaction activity,with a low overpotential of 370 mV at 10 mA cm^(-2)and a small Tafel slope of 90 mV dec^(-1).The extendable potential of this strategy to other electrocatalysts such as MoS_(2)@Ni and MoS_(2)@Zn,and other applications such as the hydrogen evolution reaction was also demonstrated.This study affords new insights into the rational design of single metal atom systems with enhanced electrocatalytic performance.

Spent graphite regeneration:Exploring diverse repairing manners with impurities-catalyzing effect towards high performance and low energy consumption

Spent battery recycling has received considerable attention because of its economic and environmental potential.A large amount of retired graphite has been produced as the main electrode material,accompanied by a detailed exploration of the repair mechanism.However,they still suffer from unclear repair mechanisms and physicochemical evolution.In this study,spent graphite was repaired employing three methodologies:pickling-sintering,pyrogenic-recovery,and high-temperature sintering.Owing to the catalytic effect of the metal-based impurities and temperature control,the as-obtained samples displayed an ordered transformation,including the interlayer distance,crystalline degree,and grain size.As anodes of lithium ions batteries,the capacity of repaired samples reached up to 310 mA h g^(-1)above after 300loops at 1.0 C,similar to that of commercial graphite.Meanwhile,benefitting from the effective assembly of carbon atoms in internal structure of graphite at>1400℃,their initial coulombic efficiency were>87%.Even at 2.0 C,the capacity of samples remained approximately 244 mA h g^(-1)after 500 cycles.Detailed electrochemical and kinetic analyses revealed that a low temperature enhanced the isotropy,thereby enhancing the rate properties.Further,economic and environmental analyses revealed that the revenue obtained through suitable pyrogenic-recovering manners was approximately the largest value(5500$t^(-1)).Thus,this study is expected to clarify the in-depth effect of different repair methods on the traits of graphite,while offering all-round evaluations of repaired graphite.

Two-Dimensional Materials for Highly Efficient and Stable Perovskite Solar Cells

Perovskite solar cells(PSCs)offer low costs and high power conversion efficiency.However,the lack of long-term stability,primarily stemming from the interfacial defects and the sus-ceptible metal electrodes,hinders their practical application.In the past few years,two-dimensional(2D)materials(e.g.,graphene and its derivatives,transitional metal dichalcogenides,MXenes,and black phosphorus)have been identified as a promising solution to solving these problems because of their dangling bond-free surfaces,layer-dependent electronic band structures,tunable functional groups,and inherent compactness.Here,recent progress of 2D material toward efficient and stable PSCs is summarized,including its role as both interface materials and electrodes.We discuss their beneficial effects on perovskite growth,energy level alignment,defect passivation,as well as blocking external stimulus.In particular,the unique properties of 2D materials to form van der Waals heterojunction at the bottom interface are emphasized.Finally,perspectives on the further development of PSCs using 2D materials are provided,such as designing high-quality van der Waals heterojunction,enhancing the uniformity and coverage of 2D nanosheets,and developing new 2D materials-based electrodes.

A novel strategy of lithium recycling from spent lithium-ion batteries using imidazolium ionic liquid

In light of the increasing demand for environmental protection and energy conservation,the recovery of highly valuable metals,such as Li,Co,and Ni,from spent lithium-ion batteries(LIBs)has attracted widespread attention.Most conventional recycling strategies,however,suffer from a lack of lithium recycling,although they display high efficiency in the recovery of Co and Ni.In this work,we report an efficient extraction process of lithium from the spent LIBs by using a functional imidazolium ionic liquid.The extraction efficiency can be reached to 92.5%after a three-stage extraction,while the extraction efficiency of Ni-Co-Mn is less than 4.0%.The new process shows a high selectivity of lithium ion.FTIR spectroscopy and ultraviolet are utilized to characterize the variations in the functional groups during extraction to reveal that the possible extraction mechanism is cation exchange.The results of this work provide an effective and sustainable strategy of lithium recycling from spent LIBs.

Gradually modulating the three parts of D-π-A type polymers for high-performance organic solar cells

Organic solar cells(OSCs)have received great attention for the prominent advantage of low-cost,light-weight and potential for fabricating flexible and semi-transparent device via roll-to-roll printing toward making better use of inexhaustible renewable clean energy during the past years[1-4].

The Main Progress of Perovskite Solar Cells in 2020-2021

Perovskite solar cells(PSCs)emerging as a promising photovoltaic technology with high efficiency and low manufacturing cost have attracted the attention from all over the world.Both the efficiency and stability of PSCs have increased steadily in recent years,and the research on reducing lead leakage and developing eco-friendly lead-free perovskites pushes forward the commercialization of PSCs step by step.This review summarizes the main progress of PSCs in 2020 and 2021 from the aspects of efficiency,stability,perovskite-based tandem devices,and lead-free PSCs.Moreover,a brief discussion on the development of PSC modules and its challenges toward practical application is provided.

Gradual chlorination at different positions of D-π-A copolymers based on benzodithiophene and isoindigo for organic solar cells

Isoindigo(IID)has been widely used as strong acceptor unit(A)to construct narrow bandgap polymers in organic field effect transistors(OFETs)and organic solar cells(OSCs).Combing with IID,we chose benzodithiophene(BDT)as the donor unit(D)and thieno[3,2-b]thiophene(TT)as theπbridge to construct a new type of D-π-A polymer PE70.Based on PE70,we adopt the chlorination strategy to fine-tune photoelectric characteristics and film morphology,and then developed PE74 and PE75.By blending with non-fullerene acceptor(NFA)Y6,device based on PE74 with chloride substitution on the BDT unit showed increasing photovoltaic performance.In addition,further chlorine substitution on the IID(PE75)would greatly reduce the non-radiative voltage loss(ΔV3),and the distorted molecular conformation also took responsible for the excessive recombination.As results,PE74:Y6-based device achieves a power conversion efficiency(PCE)of 11.06%with open-circuit voltage(VOC)of 0.76 V,which are higher than those of PE70:Y6(PCE of 10.40%and VOC of 0.72 V)and PE75:Y6-based device(PCE of 6.24%and VOC of 0.84 V).This work demonstrates the regularity of the photovoltaic performance caused by chlorination strategy in polymer in the non-fullerene OSC devices,which provide important insights into highperformance photovoltaic materials.

Tuning the optoelectronic properties of vinylene linked perylenediimide dimer by ring annulation at the inside or outside bay positions for fullerene-free organic solar cells

Among various perylenediimide(PDI)-based small molecular non-fullerene acceptors(NFAs),PDI dimer can effectively avoid the excessive aggregation of single PDI and improve the photovoltaic performance.However,the twist of perylene core in PDI dimer will destroy the effective conjugation.Thus,ring annulation of PDI dimer is a feasible method to balance the film quality and electron transport,but the systematic study has attracted few attentions.Herein,we choose a simple vinylene linked PDI dimer,V-PDI2,and then conduct further studies on the structure-property-performance relationship of four kinds of derived fused-PDI dimers,namely V-TDI2,V-FDI2,V-PDIS2 and V-PDISe2 respectively.The former two are incorporated thianaphthene and benzofuran at the inside bay positions,and the latter two are fused thiophene and selenophene at the outside bay positions,respectively.Theoretical calculations reveal the inside-and outside-fused structures largely affect the skeleton configuration,the former two tend to be planar structure and the latter two maintain the distorted backbone.The photovoltaic characterizations show that the inside-fused PDI dimers offer high open circuit voltage(VOC),while the outside-fused PDI dimers afford large short-circuit current density(JSC).This variation tendency results from the reasonably tunable energy levels,light absorption,molecular crystallinity and film morphology.As a result,PBDB-T:V-PDISe2 device exhibits the highest power conversion efficiency(PCE)of 6.51%,and PBDB-T:VFDI2 device realizes the highest VOC of 1.00 V.This contribution indicates that annulation of PDI dimers in outside or inside bay regions is a feasible method to modulate the properties of PDI-based non-fullerene acceptors.

Novel closed-cycle reaction mode for totally green production of Cu_(1.8)Se nanoparticles based on laser-generated Se colloidal solution

Non-stoichiometric copper selenide(Cu_(2-x)Se,x=0.18~0.25)nanomaterials have attracted extensive attentions due to their excellent thermoelectric,optoelectronic and photocatalytic performances.However,efficient production of Cu_(2-x)Se nanoparticles(NPs)through a green and convenient way is still hindered by the inevitable non-environmentally friendly operations in common chemical synthesis.Herein,we initially reveal the coexistence of seleninic acid content and elemental selenium(Se)NPs in pulsed laser-generated Se colloidal solution.Consequently,we put forward firstly a closedcycle reaction mode for totally green production of Cu_(1.8)Se NPs to exclude traditional requirements of high temperature and toxic precursors by using Se colloidal solution.In such closed-cycle reaction,seleninic acid works as the initiator to oxidize copper sheet to release cuprous ions which can catalyze the disproportion of Se NPs to form Se O_(3)^(2-)and Se^(2-)ions and further produce Cu_(2-x)Se NPs,and the by-product SeO_(3)^(2-)ions promote subsequent formation of cuprous from the excessive Cu sheet.In experiments,the adequate copper(Cu)sheet was simply dipped into such Se colloidal solution at 70℃,and then the stream of Cu_(1.8)SeNPs could be produced until the exhaustion of selenium source.The conversion rate of Se element reaches to more than 75%when the size of Se NPs in weakly acidic colloidal solution is limited between 1 nm and 50 nm.The laser irradiation duration shows negative correlation with the size of Se NPs and unobvious impact to the p H of the solution which both are essential to the high yield of Cu_(1.8)SeNPs.Before Cu sheet is exhausted,Se colloidal solution can be successively added without influences to the product quality and the Se conversion rate.Such green methodology positively showcases a brand-new and potential strategy for mass production of Cu_(2-x)Se nanomaterials.

Multifunctional Perovskite Photodetectors: From Molecular-Scale Crystal Structure Design to Micro/Nano-scale Morphology Manipulation

Multifunctional photodetectors boost the development of traditional optical communication technology and emerging artificial intelligence fields, such as robotics and autonomous driving. However, the current implementation of multifunctional detectors is based on the physical combination of optical lenses, gratings, and multiple photodetectors, the large size and its complex structure hinder the miniaturization, lightweight, and integration of devices. In contrast, perovskite materials have achieved remarkable progress in the field of multifunctional photodetectors due to their diverse crystal structures, simple morphology manipulation, and excellent optoelectronic properties. In this review, we first overview the crystal structures and morphology manipulation techniques of perovskite materials and then summarize the working mechanism and performance parameters of multifunctional photodetectors. Furthermore, the fabrication strategies of multifunctional perovskite photodetectors and their advancements are highlighted, including polarized light detection, spectral detection, angle-sensing detection, and selfpowered detection. Finally, the existing problems of multifunctional detectors and the perspectives of their future development are presented.

Laminar Composite Solid Electrolyte with Poly(Ethylene Oxide)-Threaded Metal-Organic Framework Nanosheets for High-Performance All-Solid-State Lithium Battery

Developing laminar composite solid electrolyte with ultrathin thickness and continuous conduction channels in vertical direction holds great promise for all-solid-state lithium batteries.Herein,a thin,laminar solid electrolyte is synthesized by filtrating–NH 2 functionalized metal-organic framework nanosheets and then being threaded with poly(ethylene oxide)chains induced by the hydrogen-bonding interaction from–NH_(2) groups.It is demonstrated that the threaded poly(ethylene oxide)chains lock the adjacent metal-organic framework nanosheets,giving highly enhanced structural stability(Young’s modulus,1.3 GPa)to 7.5-μm-thick laminar composite solid electrolyte.Importantly,these poly(ethylene oxide)chains with stretching structure serve as continuous conduction pathways along the chains in pores.It makes the non-conduction laminar metal-organic framework electrolyte highly conductive:3.97×10^(−5) S cm^(−1) at 25℃,which is even over 25 times higher than that of pure poly(ethylene oxide)electrolyte.The assembled lithium cell,thus,acquires superior cycling stability,initial discharge capacity(148 mAh g^(−1) at 0.5 C and 60℃),and retention(94% after 150 cycles).Besides,the pore size of nanosheet is tailored(24.5–40.9˚A)to evaluate the mechanisms of chain conformation and ion transport in confined space.It shows that the confined pore only with proper size could facilitate the stretching of poly(ethylene oxide)chains,and meanwhile inhibit their disorder degree.Specifically,the pore size of 33.8˚A shows optimized confinement effect with trans-poly(ethylene oxide)and cis-poly(ethylene oxide)conformation,which offers great significance in ion conduction.Our design of poly(ethylene oxide)-threaded architecture provides a platform and paves a way to the rational design of next-generation high-performance porous electrolytes.

Unveiling the surface-interface properties of perovskite crystals and pivotal regulation strategies

Metal-halide perovskite solar cells have garnered significant research attention in the last decade due to their exceptional photovoltaic performance and potential for commercialization.Despite achieving remarkable power conversion efficiency of up to 26.1%,a substantial discrepancy persists when compared to the theoretical Shockley-Queisser(SQ)limit.One of the most serious challenges facing perovskite solar cells is the energy loss incurred during photovoltaic conversion,which affects the SQ limits and stability of the device.More significant than the energy loss occurring in the bulk phase of the perovskite is the energy loss occurring at the surface-interface.Here,we provide a systematic overview of the physical and chemical properties of the surface-interface.Firstly,we delve into the underlying mechanism causing the energy deficit and structural degradation at the surface-interface,aiming to enhance the understanding of carrier transport processes and structural chemical reactivity.Furthermore,we systematically summarized the primary modulating pathways,including surface reconstruction,dimensional construction,and electric-field regulation.Finally,we propose directions for future research to advance the efficiency of perovskite solar cells towards the radiative limit and their widespread commercial application.

Epigenetic silencing of BEND4,a novel DNA damage repair gene,is a synthetic lethal marker for ATM inhibitor in pancreatic cancer

Synthetic lethality is a novel model for cancer therapy.To understand the function and mechanism of BEN domain-containing protein 4(BEND4)in pancreatic cancer,eight cell lines and a total of 492 cases of pancreatic neoplasia samples were included in this study.Methylation-specific polymerase chain reaction,CRISPR/Cas9,immunoprecipitation assay,comet assay,and xenograft mouse model were used.BEND4 is a new member of the BEN domain family.The expression of BEND4 is regulated by promoter region methylation.It is methylated in 58.1%(176/303)of pancreatic ductal adenocarcinoma(PDAC),33.3%(14/42)of intraductal papillary mucinous neoplasm,31.0%(13/42)of pancreatic neuroendocrine tumor,14.3%(3/21)of mucinous cystic neoplasm,4.3%(2/47)of solid pseudopapillary neoplasm,and 2.7%(1/37)of serous cystic neoplasm.BEND4 methylation is significantly associated with late-onset PDAC(>50 years,P<0.01)and tumor differentiation(P<0.0001),and methylation of BEND4 is an independent poor prognostic marker(P<0.01)in PDAC.Furthermore,BEND4 plays tumor-suppressive roles in vitro and in vivo.Mechanistically,BEND4 involves non-homologous end joining signaling by interacting with Ku80 and promotes DNA damage repair.Loss of BEND4 increased the sensitivity of PDAC cells to ATM inhibitor.Collectively,the present study revealed an uncharacterized tumor suppressor BEND4 and indicated that methylation of BEND4 may serve as a potential synthetic lethal marker for ATM inhibitor in PDAC treatment.

Optimizing electronic structure of Mo_(2)TiC_(2)T_(x) MXene through Nb doping for enhanced electrochemical performance

MXene is a promising electrode material for both high volumetric capacitance and high-rate performance in supercapacitors.However,the current study has mainly focused on the monometallic element Ti_(3)C_(2)T_(x) MXene until now,while the bimetallic and multimetallic MXene have received comparatively less attention.In this work,we demonstrate that the electronic structure of the Mo_(2)TiC_(2)T_(x) MXene could be regulated by fine-tuning the content of doped Nb atoms.The enhanced electron cloud density of surface–O termination and the electron spin of the Mo atoms in the Mo_(2)TiC_(2)T_(x) MXene,leads to the boost of electric double-layer capacitor(EDLC)and improvement of pseudocapacitance.As a consequence,the electrochemical performance of Nb-doped Mo_(2)TiC_(2)T_(x) MXene(Nb-0.3-MXene)demonstrates a capacitance of 398 F·cm^(−3),roughly doubling that of the pristine Mo_(2)TiC_(2)T_(x) MXene electrode at 197 F·cm^(−3) in the 3 M H_(2)SO_(4) electrolyte.At the same time,the Nb-0.3-MXene could even maintain a capacitance of 82.75% at 200 mV·s−1,with high cyclic stability for 19,000 cycles at 10 A·g−1.Additionally,Nb-0.3-MXene-based hybrid supercapacitors deliver a remarkable volumetric energy density of 48.1 W·h·L^(−1)at 230.7 W·L^(−1),and 34.4 W·h·L^(−1)at a high power density of 82.6 kW·L^(−1).There exists a balance between the volumetric capacitance and rate performance with different ratios of Nb atoms in the Nb-doped MXene due to the strong interaction between the Nb-doped MXene and the intercalated protons.Therefore,optimizing the electronic structure of MXene through heteroatom doping is of great potential for enhanced supercapacitor performance.

Catalytic degradation of chlorinated volatile organic compounds(CVOCs)over Ce-Mn-Ti composite oxide catalysts

Developing industrially moldable catalysts with harmonized redox performance and acidity is of great significance for the efficient disposal of chlorinated volatile organic compounds(CVOCs)in actual exhaust gasses.Here,commercial TiO_(2),typically used for molding catalysts,was chosen as the carrier to fabricate a series of Ce_(0.02)Mn_(0-0.24)TiO_(x) materials with different Mn doping ratios and employed for chlorobenzene(CB)destruction.The introduction of Mn remarkedly facilitated the synergistic effect of each element via the electron transfer processes:Ce^(3+)+Mn^(4+/3+)■Ce^(4+)+Mn^(3+/2+)and Mn^(4+/3+)+Ti^(4+)■Mn^(3+/2+)+Ti^(3+).These synergistic interactions in Ce_(0.02)Mn_(0.04-0.24)TiO_(x),especially Ce_(0.02)Mn_(0.16)TiO_(x),significantly elevated the active oxygen species,oxygen vacancies and redox properties,endowing the superior catalytic oxidation of CB.When the Mn doping amount increased to 0.24,a separate Mn_(3)O_(4) phase appeared,which in turn might weaken the synergistic effect.Furthermore,the acidity of Ce_(0.02)Mn_(0.04-0.24)TiO_(x) was decreased with the Mn doping,regulating the balance of redox property and acidity.Notably,Ce_(0.02)Mn_(0.16)TiO_(x) featured relatively abundant B-acid sites.Its coordinating redox ability and moderate acidity promoted the deep oxidation of CB and RCOOH-intermediates,as well as the rapid desorption of Cl species,thus obtaining sustainable reactivity.In comparison,CeTiO_(x) owned the strongest acidity,however,its poor redox property was not sufficient for the timely oxidative decomposition of the easier adsorbed CB,resulting in its rapid deactivation.This finding provides a promising strategy for the construction of efficient commercial molding catalysts to decompose the industrial-scale CVOCs.