In this work,we open an avenue toward rational design of potential efficient catalysts for sustainable ammonia synthesis through composition engineering strategy by exploiting the synergistic effects among the active ...In this work,we open an avenue toward rational design of potential efficient catalysts for sustainable ammonia synthesis through composition engineering strategy by exploiting the synergistic effects among the active sites as exemplified by diatomic metals anchored graphdiyne via the combination of hierarchical high-throughput screening,first-principles calculations,and molecular dynamics simulations.Totally 43 highly efficient catalysts feature ultralow onset potentials(|U_(onset)|≤0.40 V)with Rh-Hf and Rh-Ta showing negligible onset potentials of 0 and-0.04 V,respectively.Extremely high catalytic activities of Rh-Hf and Rh-Ta can be ascribed to the synergistic effects.When forming heteronuclears,the combinations of relatively weak(such as Rh)and relatively strong(such as Hf or Ta)components usually lead to the optimal strengths of adsorption Gibbs free energies of reaction intermediates.The origin can be ascribed to the mediate d-band centers of Rh-Hf and Rh-Ta,which lead to the optimal adsorption strengths of intermediates,thereby bringing the high catalytic activities.Our work provides a new and general strategy toward the architecture of highly efficient catalysts not only for electrocatalytic nitrogen reduction reaction(eNRR)but also for other important reactions.We expect that our work will boost both experimental and theoretical efforts in this direction.展开更多
As a promising material in the aircraft industry,2A97 Al-Cu-Li alloy exhibits high corrosion susceptibility that may limit its application.In the present work,to illustrate the influences of precipitate and grain-stor...As a promising material in the aircraft industry,2A97 Al-Cu-Li alloy exhibits high corrosion susceptibility that may limit its application.In the present work,to illustrate the influences of precipitate and grain-stored energy on localized corrosion evolution in 2A97 Al-Cu-Li alloy,cold working and artificial aging were carried out to produce 2A97 Al-Cu-Li alloys under different thermomechanical conditions.Quasi-in-situ analysis,traditional immersion test and electrochemical measurement were then conducted to examine the corrosion behavior of 2A97 alloys.It is revealed that precipitate significantly affects Cu enrichment at corrosion fronts,which determines corrosion susceptibility of alloys,whereas grain-stored energy distribution is closely associated with localized corrosion propagation.It is also indicated that quasi-in-situ analysis exhibits a consistent corrosion evolution with traditional immersion tests,which is regarded as a proper method to explore localized corrosion mechanisms by providing local microstructural information with enhanced time and spatial resolutions.展开更多
The severe dependence of traditional phase change materials(PCMs)on the temperature-response and lattice deficiencies in versatility cannot satisfy demand for using such materials in complex application scenarios.Here...The severe dependence of traditional phase change materials(PCMs)on the temperature-response and lattice deficiencies in versatility cannot satisfy demand for using such materials in complex application scenarios.Here,we introduced metal ions to induce the self-assembly of MXene nanosheets and achieve their ordered arrangement by combining suction filtration and rapid freezing.Subsequently,a series of MXene/K^(+)/paraffin wax(PW)phase change composites(PCCs)were obtained via vacuum impregnation in molten PW.The prepared MXene-based PCCs showed versatile applications from macroscale technologies,successfully transforming solar,electric,and magnetic energy into thermal energy stored as latent heat in the PCCs.Moreover,due to the absence of binder in the MXene-based aerogel,MK3@PW exhibits a prime solar-thermal conversion efficiency(98.4%).Notably,MK3@PW can further convert the collected heat energy into electric energy through thermoelectric equipment and realize favorable solar-thermal-electric conversion(producing 206 mV of voltage with light radiation intensity of 200 mw cm^(−2)).An excellent Joule heat performance(reaching 105℃with an input voltage of 2.5 V)and responsive magnetic-thermal conversion behavior(a charging time of 11.8 s can achieve a thermal insulation effect of 285 s)for contactless thermotherapy were also demonstrated by the MK3@PW.Specifically,as a result of the ordered arrangement of MXene nanosheet self-assembly induced by potassium ions,MK3@PW PCC exhibits a higher electromagnetic shielding efficiency value(57.7 dB)than pure MXene aerogel/PW PCC(29.8 dB)with the same MXene mass.This work presents an opportunity for the multi-scene response and practical application of PCMs that satisfy demand of next-generation multifunctional PCCs.展开更多
The integration of interfacial solar steam generation and photocatalytic degradation technology has pro-vided a promising platform to simultaneously produce freshwater and degrade pollutants.However,con-structing low-...The integration of interfacial solar steam generation and photocatalytic degradation technology has pro-vided a promising platform to simultaneously produce freshwater and degrade pollutants.However,con-structing low-cost,multi-functional evaporators for treating Cr(Ⅵ)-polluted water remains challenging,and the synergistic mechanism on Cr(Ⅵ)reduction is fuzzy.Herein,we propose the combined strategy of ball milling and solution mixing for the sustainable production of Bi-MOF microrod from waste poly(ethylene terephthalate),and construct Bi-MOF-based solar evaporators for simultaneous photo-Fenton Cr(Ⅵ)reduction and freshwater production.Firstly,the evaporator comprised of Bi-MOF microrod and graphene nanosheet possesses high light absorption,efficient photothermal conversion,and good hydro-philic property.Attributing to the advantages,the hybrid evaporator exhibits the evaporation rate of 2.16 kg m^(-2) h^(-1) and evaporation efficiency of 87.5%under 1 kW m^(-2) of irradiation.When integrating with photo-Fenton reaction,the Cr(Ⅵ)reduction efficiency is 91.3%,along with the reaction kinetics of 0.0548 min^(-1),surpassing many advanced catalysts.In the outdoor freshwater production and Cr(Ⅵ)reduction,the daily accumulative water yield is 5.17 kg m^(-2) h^(-1),and the Cr(Ⅵ)reduction efficiency is 99.9%.Furthermore,we prove that the localization effect derived from the interfacial solar-driven evap-oration enhances H_(2)O_(2) activation for the photo-Fenton reduction of Cr(Ⅵ).Based on the result of density functional theory,Bi-MOF microrod provides rich active centers for H_(2)O_(2) activation to produce active sites such as e-or-O_(2).This study not only proposes a new strategy to construct multi-functional solar evaporators for freshwater production and catalytic reduction of pollutants,but also advances the chem-ical upcycling of waste polyesters.展开更多
Urea is widely used as fertilizer and is a key substance supporting global food production. However, the traditional industrial synthesis of urea faces the challenges with high energy consumption and serious environme...Urea is widely used as fertilizer and is a key substance supporting global food production. However, the traditional industrial synthesis of urea faces the challenges with high energy consumption and serious environmental problems. With the increasing global demand for environmental protection and sustainable development, it is much necessary to develop novel and clean methods for the synthesis of urea.Electrocatalysis provides an efficient and renewable synthesis route that can directly produce urea at room temperature and atmospheric pressure by the coupling of CO_(2) and nitrogenous molecules. In this review, we summarized the most recent advances in electrochemical synthesis of urea via CAN coupling systematically, focusing on the coupling of CO_(2) and different nitrogen sources. And the associated coupling mechanism, catalysts optimization, and electrolyzer design are well discussed. Moreover, the challenges and future directions for electrocatalytic CAN coupling are prospected. This review will provide timely and valuable guidance for others and attract more interests to promote the development of electrochemical synthesis of urea or other valuable chemicals containing CAN bond.展开更多
Molecular copper catalysts serve as exemplary models for correlating the structure-reaction-mechanism relationship in the electrochemical CO_(2) reduction(eCO_(2)R),owing to their adaptable environments surrounding th...Molecular copper catalysts serve as exemplary models for correlating the structure-reaction-mechanism relationship in the electrochemical CO_(2) reduction(eCO_(2)R),owing to their adaptable environments surrounding the copper metal centres.This investigation,employing density functional theory calculations,focuses on a novel family of binuclear Cu molecular catalysts.The modulation of their coordination configuration through the introduction of organic groups aims to assess their efficacy in converting CO_(2) to C_(2)products.Our findings highlight the crucial role of chemical valence state in shaping the characteristics of binuclear Cu catalysts,consequently influencing the eCO_(2)R behaviour,Notably,the Cu(Ⅱ)Cu(Ⅱ)macrocycle catalyst exhibits enhanced suppression of the hydrogen evolution reaction(HER),facilitating proton trans fer and the eCO_(2)R process.Fu rthermore,we explo re the impact of diverse electro n-withdrawing and electron-donating groups coordinated to the macrocycle(R=-F,-H,and-OCH_3)on the electron distribution in the molecular catalysts.Strategic placement of-OCH_3 groups in the macrocycles leads to a favourable oxidation state of the Cu centres and subsequent C-C coupling to form C_(2) products.This research provides fundamental insights into the design and optimization of binuclear Cu molecular catalysts for the electrochemical conversion of CO_(2) to value-added C_(2) products.展开更多
The high-nickel layered cathodes Li[Ni_(x)Co_(y)Mn_(1-x-y)]O_(2)(x≥0.8)with high specific capacity and long cycle life are considered as prospective cathodes for lithium-ion batteries.However,the microcrack formation...The high-nickel layered cathodes Li[Ni_(x)Co_(y)Mn_(1-x-y)]O_(2)(x≥0.8)with high specific capacity and long cycle life are considered as prospective cathodes for lithium-ion batteries.However,the microcrack formation and poor structural stability give rise to inferior rate performance and undesirable cycling life.Herein,we propose a dual modification strategy combining primary particle structure design and element doping to modify Li[Ni_(0.95)Co_(0.025)Mn_(0.025)]O_(2) cathode by tungsten and fluorine co-doped(W-F-NCM95).The doping of W can convert the microstructure of primary particles to the unique rod-like shape,which is beneficial to enhance the reversibility of phase transition and alleviate the generation of microcracks.F doping is conducive to alleviating the surface side reactions.Thus,due to the synergistic effect of W,F codoping,the obtained W-F-NCM95 cathodes deliver a high initial capacity of 236.1 mA h g^(-1) at 0.1 C and superior capacity retention of 88.7%over 100 cycles at 0.5 C.Moreover,the capacity still maintains73.8%after 500 cycles at 0.5 C and the texture of primary particle is intact.This work provides an available strategy by W and F co-doping to enhance the electrochemistry performance of high-nickel cathodes for practical application.展开更多
Graphene oxide(GO)is regarded as a promising candidate to construct solar absorbers for addressing freshwater crisis,but the easy delamination of GO in water poses a critical challenge for practical solar desalination...Graphene oxide(GO)is regarded as a promising candidate to construct solar absorbers for addressing freshwater crisis,but the easy delamination of GO in water poses a critical challenge for practical solar desalination.Herein,we improve the stability of GO membranes by a self-crosslinking poly(ionic liquid)(PIL)in a mild condition,which crosslinks neighbouring GO nanosheets without blemishing the hydrophilic structure of GO.By further adding carbon nanotubes(CNTs),the sandwiched GO/CNT@PIL(GCP)membrane displays a good stability in pH=1 or 13 solution even for 270 days.The molecular dynamics simulation results indicate that the generation of water nanofluidics in nanochannels of GO nanosheets remarkably reduces the water evaporation enthalpy in GCP membrane,compared to bulk water.Consequently,the GCP membrane exhibits a high evaporation rate(1.87 kg m^(-2)h^(-1))and displays stable evaporation rates for 14 h under 1 kW m^(-2)irradiation.The GCP membrane additionally works very well when using different water sources(e.g.,dye-polluted water)or even strong acidic solution(pH=1)or basic solution(pH=13).More importantly,through bundling pluralities of GCP membrane,an efficient solar desalination device is developed to produce drinkable water from seawater.The average daily drinkable water amount in sunny day is 10.1 kg m^(-2),which meets with the daily drinkable water needs of five adults.The high evaporation rate,long-time durability and good scalability make the GCP membrane an outstanding candidate for practical solar seawater desalination.展开更多
Enhancing the stability of Pt-based electrocatalysts for the sluggish cathodic oxygen reduction reaction(ORR)is critical for proton exchange membrane fuel cells(PEMFCs).Herein,high-entropy intermetallic(HEI)L1_(2)-Pt(...Enhancing the stability of Pt-based electrocatalysts for the sluggish cathodic oxygen reduction reaction(ORR)is critical for proton exchange membrane fuel cells(PEMFCs).Herein,high-entropy intermetallic(HEI)L1_(2)-Pt(FeCoNiCuZn)3is designed for durable ORR catalysis.Benefiting from the unique HEI structure and the enhanced intermetallic phase stability,Pt(FeCoNiCuZn)3/C nanoparticles demonstrate significantly improved stability over Pt/C and PtCu_(3)/C catalysts.The Pt(FeCoNiCuZn)3/C exhibits a negligible decay of the half-wave potential during 30,000 potential cycles from 0.6 to 1.0 V,whereas Pt/C and PtCu_(3)/C are negatively shifted by 46 and 36 m V,respectively.Even after 10,000 cycles at potential up to 1.5 V,the mass activity of Pt(FeCoNiCuZn)3/C still shows~70%retention.As evidenced by the structural characterizations,the HEI structure of Pt(FeCoNiCuZn)3/C is well maintained,while PtCu_(3)/C nanoparticles undergo severe Cu leaching and particle growth.In addition,when assembled Pt(FeCoNiCuZn)3/C as the cathode in high-temperature PEMFC of 160℃,the H_(2)-O_(2)fuel cell delivers almost no degradation even after operating for 150 h,demonstrating the potential for fuel cell applications.This work provides a facile design strategy for the development of high-performance ultrastable electrocatalysts.展开更多
High-energy lithium-sulfur batteries(LSBs)have experienced relentless development over the past decade with discernible improvements in electrochemical performance.However,a scrutinization of the cell operation condit...High-energy lithium-sulfur batteries(LSBs)have experienced relentless development over the past decade with discernible improvements in electrochemical performance.However,a scrutinization of the cell operation conditions reveals a huge gap between the demands for practical batteries and those in the literature.Low sulfur loading,a high electrolyte/sulfur(E/S)ratio and excess anodes for lab-scale LSBs significantly offset their high-energy merit.To approach practical LSBs,high loading and lean electrolyte parameters are needed,which involve budding challenges of slow charge transfer,polysulfide precipitation and severe shuttle effects.To track these obstacles,the exploration of electrocatalysts to immobilize polysulfides and accelerate Li-S redox kinetics has been widely reported.Herein,this review aims to survey state-of-the-art catalytic materials for practical LSBs with emphasis on elucidating the correlation among catalyst design strategies,material structures and electrochemical performance.We also statistically evaluate the state-of-the-art catalyst-modified LSBs to identify the remaining discrepancy between the current advancements and the real-world requirements.In closing,we put forward our proposal for a catalytic material study to help realize practical LSBs.展开更多
The electrocatalytic water splitting technology can generate highpurity hydrogen without emitting carbon dioxide,which is in favor of relieving environmental pollution and energy crisis and achieving carbon neutrality...The electrocatalytic water splitting technology can generate highpurity hydrogen without emitting carbon dioxide,which is in favor of relieving environmental pollution and energy crisis and achieving carbon neutrality.Electrocatalysts can effectively reduce the reaction energy barrier and increase the reaction efficiency.Facet engineering is considered as a promising strategy in controlling the ratio of desired crystal planes on the surface.Owing to the anisotropy,crystal planes with different orientations usually feature facet-dependent physical and chemical properties,leading to differences in the adsorption energies of oxygen or hydrogen intermediates,and thus exhibit varied electrocatalytic activity toward hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).In this review,a brief introduction of the basic concepts,fundamental understanding of the reaction mechanisms as well as key evaluating parameters for both HER and OER are provided.The formation mechanisms of the crystal facets are comprehensively overviewed aiming to give scientific theory guides to realize dominant crystal planes.Subsequently,three strategies of selective capping agent,selective etching agent,and coordination modulation to tune crystal planes are comprehensively summarized.Then,we present an overview of significant contributions of facet-engineered catalysts toward HER,OER,and overall water splitting.In particular,we highlight that density functional theory calculations play an indispensable role in unveiling the structure–activity correlation between the crystal plane and catalytic activity.Finally,the remaining challenges in facet-engineered catalysts for HER and OER are provided and future prospects for designing advanced facet-engineered electrocatalysts are discussed.展开更多
Thiol-ene click reaction is an intriguing strategy for preparing polymer electrolytes due to its high activity,atom economy and less side reaction.However,the explosive reaction rate and the use of non-electrolytic am...Thiol-ene click reaction is an intriguing strategy for preparing polymer electrolytes due to its high activity,atom economy and less side reaction.However,the explosive reaction rate and the use of non-electrolytic amine catalyst hamper its application in in-situ batteries.Herein,a nitrogen-containing eutectic solution is designed as both the catalyst of the thiol-ene reaction and the plasticizer to in-situ synthesize the gel polymer electrolytes,realizing a mild in-situ gelation process and the preparation of high-performance gel electrolytes.The obtained gel polymer electrolytes exhibit a high ionic conductivity of 4×10^(−4)S cm^(−1)and lithium-ion transference number(t_(Li)^(+))of 0.51 at 60°C.The as-assembled Li/LiFePO_(4)(LFP)cell delivers a high initial discharge capacity of 155.9 mAh g^(-1),and a favorable cycling stability with the capacity retention of 82%after 800 cycles at 1 C is also obtained.In addition,this eutectic solution significantly improves the rate performance of the LFP cell with high specific capacity of 141.5 and 126.8 mAh g^(-1)at 5 C and 10 C,respectively,and the cell can steadily work at various charge–discharge rate for 200 cycles.This powerful and efficient strategy may provide a novel way for in-situ preparing gel polymer electrolytes with desirable comprehensive performances.展开更多
It is recently suggested that air-formed film plays an important role in controlling corrosion resistance of Mg-Li alloys. However, the structure of the air-formed film and its effect on corrosion resistance of Mg-Li ...It is recently suggested that air-formed film plays an important role in controlling corrosion resistance of Mg-Li alloys. However, the structure of the air-formed film and its effect on corrosion resistance of Mg-Li alloys has not been fully understood. Firstly, the air-formed films formed on α and β phases in a dual-phase LZ91 Mg-Li alloy after exposure to laboratory air for up to 48 h have been examined by SEM under the assistance of ultramicrotomy. Then, the effect of the air-formed film on surface potential and, consequently, corrosion/oxidation behavior of the alloy has been investigated. Finally, in order to exclude the influence from α phase, the structure of the air-formed film on β phase and its effect on corrosion/oxidation behavior of Mg-Li alloys have been studied based on a single-phase LA141 Mg-Li alloy. The results show that the air-formed film is thin and negligible on α phase but thick on β phase after prolonged exposure to laboratory air. The thick air-formed film on β phase has a multilayer structure with an inner layer consisting of Mg O/Mg(OH)_(2) and outer layer consisting of Li_(2)CO_(3), which greatly elevates the surface potential of β phase in air. Both LZ91 and LA141 Mg-Li alloys firstly undergo uniform corrosion and then filiform corrosion when immersed in Na Cl solution and the pre-existed air-formed film on β-Li phase can retard the occurrence of filiform corrosion in the alloys.展开更多
In the present study,the distribution of Ag in the coating formed on Mg-Ag alloy by plasma electrolytic oxidation(PEO)and its ionic release kinetics when exposed to a 0.9 wt.%Na Cl solution at 37℃have been investigat...In the present study,the distribution of Ag in the coating formed on Mg-Ag alloy by plasma electrolytic oxidation(PEO)and its ionic release kinetics when exposed to a 0.9 wt.%Na Cl solution at 37℃have been investigated.Both metallic Ag and Ag oxide particles with~5 to~40 nm in diameters were observed in the PEO coating.Further,an Ag-enriched layer of~20 nm in thickness at the substrate/coating interface was also observed.The PEO coating on the Mg-Ag alloy not only increases its corrosion resistance with the corrosion current density decreasing by up to 3 orders of magnitude from 8.04×10^(-3)to 4.03×10^(-6)A/cm^(2),but also controls the release of Ag+to the level that is sufficient for anti-infective efficacy without causing cytotoxicity to mammal cells.展开更多
Harvesting solar energy in an effective manner for steam and electricity generation is a promising technique to simultaneously cope with the energy and water crises.However,the construction of efficient and easy scale...Harvesting solar energy in an effective manner for steam and electricity generation is a promising technique to simultaneously cope with the energy and water crises.However,the construction of efficient and easy scale-up photothermal materials for steam and electricity cogeneration remains challenging.Herein,we report a facile and cost-effective strategy to prepare MnO_(2)-decorated cotton cloth(MCx).The wide adsorption spectrum and excellent photothermal conversion ability of the in situ-formed MnO_(2)nanoparticles make the MCx to be advanced photothermal materials.Consequently,the hybrid device integrated with MCx as the photothermal layer and the thermoelectric(TE)module for electricity power conversion exhibits an extremely high evaporation rate of 2.24 kg m^(−2)h^(−1)under 1 kW m^(−2)irradiation,which is ranked among the most powerful solar evaporators.More importantly,during solar evaporation,the hybrid device produces an open-circuit voltage of 0.3 V and a power output of 1.6 W m^(−2)under 3 Sun irradiation,and outperforms most of the previously reported solar-driven electricity generation devices.Therefore,the integrated device with synergistic solar-thermal utilization opens up a green way toward simultaneous solar vapor and electric power generation in remote and resource-constrained areas.展开更多
We report a new facile light-induced strategy to disperse micron-sized aggregated bulk covalent organic frameworks(COFs)into isolated COFs nanoparticles.This was achieved by a series of metal-coordinated COFs,namely C...We report a new facile light-induced strategy to disperse micron-sized aggregated bulk covalent organic frameworks(COFs)into isolated COFs nanoparticles.This was achieved by a series of metal-coordinated COFs,namely COF-909-Cu,-Co or-Fe,where for the first time the diffusio-phoretic propulsion was utilized to design COF-based micro/nanomotors.The mechanism studies revealed that the metal ions decorated in the COF-909 backbone could promote the separation of electron and holes and trigger the production of sufficient ionic and reactive oxygen species under visible light irradiation.In this way,strong light-induced self-diffusiophoretic effect is achieved,resulting in good dispersion of COFs.Among them,COF-909-Fe showed the highest dispersion performance,along with a drastic decrease in particle size from 5μm to500 nm,within only 30 min light irradiation,which is inaccessible by using traditional magnetic stirring or ultrasonication methods.More importantly,benefiting from the outstanding dispersion efficiency,COF-909-Fe micro/nanomotors were demonstrated to be efficient in photocatalytic degradation of tetracycline,about 8 times faster than using traditional magnetic stirring method.This work opens up a new avenue to prepare isolated nanosized COFs in a high-fast,simple,and green manner.展开更多
Aromatization of methanol over co-impregnated La/Zn/HZSM-5 zeolite catalyst was studied.The selectivity of aromatics and BTX(benzene,toluene,and xylene)reached 64.0%and 56.6%,respectively,using La/Zn/HZSM-5 at 437...Aromatization of methanol over co-impregnated La/Zn/HZSM-5 zeolite catalyst was studied.The selectivity of aromatics and BTX(benzene,toluene,and xylene)reached 64.0%and 56.6%,respectively,using La/Zn/HZSM-5 at 437°C,0.1 MPa and methanol WHSV(weight hourly space velocity)=0.8 h-1.Catalytic results showed that the La species was a very good promoter,increased selectivity of aromatics,and prolonged the catalyst lifetime on stream.The effects of the SiO2/Al2O3 ratio in zeolite,Zn and La loading,WHSV,reaction temperature, water content in the feed and H2 pretreatment of catalysts on the catalytic performance were studied in detail. Characterizations of the catalysts by thermogravimetric analysis(TGA),NH3-TPD(temperature programmed desorption),SEM(scanning electron micrograph),N2 adsorption-desorption,XRD(X-ray diffraction)and XRF (X-ray fluorescence),were carried out to understand the structure and discuss the aromatization performance of La/Zn/HZSM-5 zeolite catalyst.展开更多
The hierarchical mesoporous Zn/ZSM-5 zeolite catalyst was prepared by NaOH treatment and Zn impregnation, and its application in the conversion of methanol to gasoline (MTG) was studied. N2 adsorption-desorption res...The hierarchical mesoporous Zn/ZSM-5 zeolite catalyst was prepared by NaOH treatment and Zn impregnation, and its application in the conversion of methanol to gasoline (MTG) was studied. N2 adsorption-desorption results showed that the mesopores with sizes of 2-20 nm in HZ5/0.3AT was formed by 0.3 M NaOH alkali treatment. The zeolite samples after modification were also characterized by XRF, AAS, XRD, SEM and NH3-TPD methods. Zn impregnated catalyst Zn/HZ5/0.3AT exhibited dramatic improvements in catalytic lifetime and liquid hydrocarbons yield. The selectivity of aromatic hydrocarbons was also improved after Zn impregnation. It is suggested that the mesopores of Zn/HZ5/0.3AT enhanced the synergetic effect of Zn species and acid sites and the capability to coke tolerance, which were confirmed by the results of catalytic test and TGA analysis, respectively.展开更多
In this study,an acid-induced assembly strategy for a rutile TiO2 photocatalyst was proposed on the basis of the treatment of lamellar protonated titanate with a concentrated HNO3 solution.Nitrate groups were successf...In this study,an acid-induced assembly strategy for a rutile TiO2 photocatalyst was proposed on the basis of the treatment of lamellar protonated titanate with a concentrated HNO3 solution.Nitrate groups were successfully grafted onto a TiO2 surface and induced the assembly of rutile TiO2 nanorods into uniform spindle-like nanobundles.The resulting TiO2 product achieved a photocatalytic hydrogen evolution rate of 402.4μmol h^?1,which is 3.1 times higher than that of Degussa P25-TiO2.It was demonstrated that nitrate group grafting caused the rutile TiO2 surface to become negatively charged,which is favorable for trapping positive protons and improving charge carrier separation,thereby enhancing photocatalytic hydrogen production.Additionally,surface charges were crucial to structural stability based on electrostatic repulsion.This study not only developed a facile surface modification strategy for fabricating efficient H2 production photocatalysts but also identified an influence mechanism of inorganic acids different from that reported in the literature.展开更多
Developing robust oxygen electrocatalyst with high-performance is very significant for practical rechargeable Zn-air battery.We report herein the preparation of three-dimensional continuous nanocarbon network composed...Developing robust oxygen electrocatalyst with high-performance is very significant for practical rechargeable Zn-air battery.We report herein the preparation of three-dimensional continuous nanocarbon network composed of interconnected nitrogen-doped carbon nanotubes and its application as oxygen electrocatalysis in rechargeable Zn-air battery.Except the excellent electrochemical bifunctionality,this carbon nanotube matrix also delivers an impressive battery performance.Specifically,an opencircuit voltage of 1.50 V as well as a high power density of 220 m W cm^(-2) with remarkable cycling stability for 1600 h is achieved in the rechargeable Zn-air battery.The study not only provides an efficient bifunctional oxygen electrocatalyst but more importantly may pave significant concepts in designing robust electrode for long-life rechargeable Zn-air battery and other energy technologies.展开更多
基金support from the National Natural Science Foundation of China(22073033,21873032,21673087,21903032)startup fund(2006013118 and 3004013105)from Huazhong University of Science and Technology+1 种基金the Fundamental Research Funds for the Central Universities(2019kfyRCPY116)the Innovation and Talent Recruitment Base of New Energy Chemistry and Device(B21003)
文摘In this work,we open an avenue toward rational design of potential efficient catalysts for sustainable ammonia synthesis through composition engineering strategy by exploiting the synergistic effects among the active sites as exemplified by diatomic metals anchored graphdiyne via the combination of hierarchical high-throughput screening,first-principles calculations,and molecular dynamics simulations.Totally 43 highly efficient catalysts feature ultralow onset potentials(|U_(onset)|≤0.40 V)with Rh-Hf and Rh-Ta showing negligible onset potentials of 0 and-0.04 V,respectively.Extremely high catalytic activities of Rh-Hf and Rh-Ta can be ascribed to the synergistic effects.When forming heteronuclears,the combinations of relatively weak(such as Rh)and relatively strong(such as Hf or Ta)components usually lead to the optimal strengths of adsorption Gibbs free energies of reaction intermediates.The origin can be ascribed to the mediate d-band centers of Rh-Hf and Rh-Ta,which lead to the optimal adsorption strengths of intermediates,thereby bringing the high catalytic activities.Our work provides a new and general strategy toward the architecture of highly efficient catalysts not only for electrocatalytic nitrogen reduction reaction(eNRR)but also for other important reactions.We expect that our work will boost both experimental and theoretical efforts in this direction.
基金supports from the National Natural Science Foundation of China(Nos.52371065,52001128)the Hubei Provincial Natural Science Foundation of China(No.2023AFB637)。
文摘As a promising material in the aircraft industry,2A97 Al-Cu-Li alloy exhibits high corrosion susceptibility that may limit its application.In the present work,to illustrate the influences of precipitate and grain-stored energy on localized corrosion evolution in 2A97 Al-Cu-Li alloy,cold working and artificial aging were carried out to produce 2A97 Al-Cu-Li alloys under different thermomechanical conditions.Quasi-in-situ analysis,traditional immersion test and electrochemical measurement were then conducted to examine the corrosion behavior of 2A97 alloys.It is revealed that precipitate significantly affects Cu enrichment at corrosion fronts,which determines corrosion susceptibility of alloys,whereas grain-stored energy distribution is closely associated with localized corrosion propagation.It is also indicated that quasi-in-situ analysis exhibits a consistent corrosion evolution with traditional immersion tests,which is regarded as a proper method to explore localized corrosion mechanisms by providing local microstructural information with enhanced time and spatial resolutions.
基金the National Natural Science Foundation of China[grant numbers 52203038,52173036 and 52073107]the National Key Technology R&D Program of China[grant number 2022YFC3901904,2022YFC3901903,and 2020YFB1709301]the Central University Basic Research Fund of China[grant number 2021XXJS035].
文摘The severe dependence of traditional phase change materials(PCMs)on the temperature-response and lattice deficiencies in versatility cannot satisfy demand for using such materials in complex application scenarios.Here,we introduced metal ions to induce the self-assembly of MXene nanosheets and achieve their ordered arrangement by combining suction filtration and rapid freezing.Subsequently,a series of MXene/K^(+)/paraffin wax(PW)phase change composites(PCCs)were obtained via vacuum impregnation in molten PW.The prepared MXene-based PCCs showed versatile applications from macroscale technologies,successfully transforming solar,electric,and magnetic energy into thermal energy stored as latent heat in the PCCs.Moreover,due to the absence of binder in the MXene-based aerogel,MK3@PW exhibits a prime solar-thermal conversion efficiency(98.4%).Notably,MK3@PW can further convert the collected heat energy into electric energy through thermoelectric equipment and realize favorable solar-thermal-electric conversion(producing 206 mV of voltage with light radiation intensity of 200 mw cm^(−2)).An excellent Joule heat performance(reaching 105℃with an input voltage of 2.5 V)and responsive magnetic-thermal conversion behavior(a charging time of 11.8 s can achieve a thermal insulation effect of 285 s)for contactless thermotherapy were also demonstrated by the MK3@PW.Specifically,as a result of the ordered arrangement of MXene nanosheet self-assembly induced by potassium ions,MK3@PW PCC exhibits a higher electromagnetic shielding efficiency value(57.7 dB)than pure MXene aerogel/PW PCC(29.8 dB)with the same MXene mass.This work presents an opportunity for the multi-scene response and practical application of PCMs that satisfy demand of next-generation multifunctional PCCs.
基金supported by the National Natural Science Foundation of China(52373099)the Innovation and Talent Recruitment Base of New Energy Chemistry and Device(B21003)。
文摘The integration of interfacial solar steam generation and photocatalytic degradation technology has pro-vided a promising platform to simultaneously produce freshwater and degrade pollutants.However,con-structing low-cost,multi-functional evaporators for treating Cr(Ⅵ)-polluted water remains challenging,and the synergistic mechanism on Cr(Ⅵ)reduction is fuzzy.Herein,we propose the combined strategy of ball milling and solution mixing for the sustainable production of Bi-MOF microrod from waste poly(ethylene terephthalate),and construct Bi-MOF-based solar evaporators for simultaneous photo-Fenton Cr(Ⅵ)reduction and freshwater production.Firstly,the evaporator comprised of Bi-MOF microrod and graphene nanosheet possesses high light absorption,efficient photothermal conversion,and good hydro-philic property.Attributing to the advantages,the hybrid evaporator exhibits the evaporation rate of 2.16 kg m^(-2) h^(-1) and evaporation efficiency of 87.5%under 1 kW m^(-2) of irradiation.When integrating with photo-Fenton reaction,the Cr(Ⅵ)reduction efficiency is 91.3%,along with the reaction kinetics of 0.0548 min^(-1),surpassing many advanced catalysts.In the outdoor freshwater production and Cr(Ⅵ)reduction,the daily accumulative water yield is 5.17 kg m^(-2) h^(-1),and the Cr(Ⅵ)reduction efficiency is 99.9%.Furthermore,we prove that the localization effect derived from the interfacial solar-driven evap-oration enhances H_(2)O_(2) activation for the photo-Fenton reduction of Cr(Ⅵ).Based on the result of density functional theory,Bi-MOF microrod provides rich active centers for H_(2)O_(2) activation to produce active sites such as e-or-O_(2).This study not only proposes a new strategy to construct multi-functional solar evaporators for freshwater production and catalytic reduction of pollutants,but also advances the chem-ical upcycling of waste polyesters.
基金National Natural Science Foundation of China (No. 22202065, 22075092 and U21A20500)。
文摘Urea is widely used as fertilizer and is a key substance supporting global food production. However, the traditional industrial synthesis of urea faces the challenges with high energy consumption and serious environmental problems. With the increasing global demand for environmental protection and sustainable development, it is much necessary to develop novel and clean methods for the synthesis of urea.Electrocatalysis provides an efficient and renewable synthesis route that can directly produce urea at room temperature and atmospheric pressure by the coupling of CO_(2) and nitrogenous molecules. In this review, we summarized the most recent advances in electrochemical synthesis of urea via CAN coupling systematically, focusing on the coupling of CO_(2) and different nitrogen sources. And the associated coupling mechanism, catalysts optimization, and electrolyzer design are well discussed. Moreover, the challenges and future directions for electrocatalytic CAN coupling are prospected. This review will provide timely and valuable guidance for others and attract more interests to promote the development of electrochemical synthesis of urea or other valuable chemicals containing CAN bond.
基金the HUST-QMUL Strategic Partnership Research Funding(No.2022-HUST-QMUL-SPRF-03),which funded the project“Design of Binuclear Copper Electrocatalysts for CO_(2) Conversion from First Principles”the China Scholarship Council for financial support。
文摘Molecular copper catalysts serve as exemplary models for correlating the structure-reaction-mechanism relationship in the electrochemical CO_(2) reduction(eCO_(2)R),owing to their adaptable environments surrounding the copper metal centres.This investigation,employing density functional theory calculations,focuses on a novel family of binuclear Cu molecular catalysts.The modulation of their coordination configuration through the introduction of organic groups aims to assess their efficacy in converting CO_(2) to C_(2)products.Our findings highlight the crucial role of chemical valence state in shaping the characteristics of binuclear Cu catalysts,consequently influencing the eCO_(2)R behaviour,Notably,the Cu(Ⅱ)Cu(Ⅱ)macrocycle catalyst exhibits enhanced suppression of the hydrogen evolution reaction(HER),facilitating proton trans fer and the eCO_(2)R process.Fu rthermore,we explo re the impact of diverse electro n-withdrawing and electron-donating groups coordinated to the macrocycle(R=-F,-H,and-OCH_3)on the electron distribution in the molecular catalysts.Strategic placement of-OCH_3 groups in the macrocycles leads to a favourable oxidation state of the Cu centres and subsequent C-C coupling to form C_(2) products.This research provides fundamental insights into the design and optimization of binuclear Cu molecular catalysts for the electrochemical conversion of CO_(2) to value-added C_(2) products.
基金supported by the National Key R&D Program of China(2018YFB0905600)。
文摘The high-nickel layered cathodes Li[Ni_(x)Co_(y)Mn_(1-x-y)]O_(2)(x≥0.8)with high specific capacity and long cycle life are considered as prospective cathodes for lithium-ion batteries.However,the microcrack formation and poor structural stability give rise to inferior rate performance and undesirable cycling life.Herein,we propose a dual modification strategy combining primary particle structure design and element doping to modify Li[Ni_(0.95)Co_(0.025)Mn_(0.025)]O_(2) cathode by tungsten and fluorine co-doped(W-F-NCM95).The doping of W can convert the microstructure of primary particles to the unique rod-like shape,which is beneficial to enhance the reversibility of phase transition and alleviate the generation of microcracks.F doping is conducive to alleviating the surface side reactions.Thus,due to the synergistic effect of W,F codoping,the obtained W-F-NCM95 cathodes deliver a high initial capacity of 236.1 mA h g^(-1) at 0.1 C and superior capacity retention of 88.7%over 100 cycles at 0.5 C.Moreover,the capacity still maintains73.8%after 500 cycles at 0.5 C and the texture of primary particle is intact.This work provides an available strategy by W and F co-doping to enhance the electrochemistry performance of high-nickel cathodes for practical application.
基金the financial support of the National Key R&D Program of China(No.2019YFC1806000)the Huazhong University of Science and Technology(No.3004013118)+2 种基金support from the National Natural Science Foundation of China(No.51903099)Huazhong University of Science and Technology(No.3004013134)the 100 Talents Program of the Hubei Provincial Government.Z.D.thanks the Postdoctoral Science Foundation of China(No.0106013063).
文摘Graphene oxide(GO)is regarded as a promising candidate to construct solar absorbers for addressing freshwater crisis,but the easy delamination of GO in water poses a critical challenge for practical solar desalination.Herein,we improve the stability of GO membranes by a self-crosslinking poly(ionic liquid)(PIL)in a mild condition,which crosslinks neighbouring GO nanosheets without blemishing the hydrophilic structure of GO.By further adding carbon nanotubes(CNTs),the sandwiched GO/CNT@PIL(GCP)membrane displays a good stability in pH=1 or 13 solution even for 270 days.The molecular dynamics simulation results indicate that the generation of water nanofluidics in nanochannels of GO nanosheets remarkably reduces the water evaporation enthalpy in GCP membrane,compared to bulk water.Consequently,the GCP membrane exhibits a high evaporation rate(1.87 kg m^(-2)h^(-1))and displays stable evaporation rates for 14 h under 1 kW m^(-2)irradiation.The GCP membrane additionally works very well when using different water sources(e.g.,dye-polluted water)or even strong acidic solution(pH=1)or basic solution(pH=13).More importantly,through bundling pluralities of GCP membrane,an efficient solar desalination device is developed to produce drinkable water from seawater.The average daily drinkable water amount in sunny day is 10.1 kg m^(-2),which meets with the daily drinkable water needs of five adults.The high evaporation rate,long-time durability and good scalability make the GCP membrane an outstanding candidate for practical solar seawater desalination.
基金supported by the National Natural Science Foundation(22279036)the Innovation and Talent Recruitment Base of New Energy Chemistry and Device(B21003)。
文摘Enhancing the stability of Pt-based electrocatalysts for the sluggish cathodic oxygen reduction reaction(ORR)is critical for proton exchange membrane fuel cells(PEMFCs).Herein,high-entropy intermetallic(HEI)L1_(2)-Pt(FeCoNiCuZn)3is designed for durable ORR catalysis.Benefiting from the unique HEI structure and the enhanced intermetallic phase stability,Pt(FeCoNiCuZn)3/C nanoparticles demonstrate significantly improved stability over Pt/C and PtCu_(3)/C catalysts.The Pt(FeCoNiCuZn)3/C exhibits a negligible decay of the half-wave potential during 30,000 potential cycles from 0.6 to 1.0 V,whereas Pt/C and PtCu_(3)/C are negatively shifted by 46 and 36 m V,respectively.Even after 10,000 cycles at potential up to 1.5 V,the mass activity of Pt(FeCoNiCuZn)3/C still shows~70%retention.As evidenced by the structural characterizations,the HEI structure of Pt(FeCoNiCuZn)3/C is well maintained,while PtCu_(3)/C nanoparticles undergo severe Cu leaching and particle growth.In addition,when assembled Pt(FeCoNiCuZn)3/C as the cathode in high-temperature PEMFC of 160℃,the H_(2)-O_(2)fuel cell delivers almost no degradation even after operating for 150 h,demonstrating the potential for fuel cell applications.This work provides a facile design strategy for the development of high-performance ultrastable electrocatalysts.
基金supported by grants from the Research Grants Council of the Hong Kong Special Administrative Region,China(Poly U25216121,Poly U15303219)the National Natural Science Foundation of China for Young Scholar(52102310)the Research Committee of the Hong Kong Polytechnic University(A-PB1 M,1-BBXK,1-CD4 M,and G-UAMV)。
文摘High-energy lithium-sulfur batteries(LSBs)have experienced relentless development over the past decade with discernible improvements in electrochemical performance.However,a scrutinization of the cell operation conditions reveals a huge gap between the demands for practical batteries and those in the literature.Low sulfur loading,a high electrolyte/sulfur(E/S)ratio and excess anodes for lab-scale LSBs significantly offset their high-energy merit.To approach practical LSBs,high loading and lean electrolyte parameters are needed,which involve budding challenges of slow charge transfer,polysulfide precipitation and severe shuttle effects.To track these obstacles,the exploration of electrocatalysts to immobilize polysulfides and accelerate Li-S redox kinetics has been widely reported.Herein,this review aims to survey state-of-the-art catalytic materials for practical LSBs with emphasis on elucidating the correlation among catalyst design strategies,material structures and electrochemical performance.We also statistically evaluate the state-of-the-art catalyst-modified LSBs to identify the remaining discrepancy between the current advancements and the real-world requirements.In closing,we put forward our proposal for a catalytic material study to help realize practical LSBs.
基金support from the National Natural Science Foundation of China(No.22005147)Dr.You acknowledges the financial support from the National Key Research and Development Program of China(2021YFA1600800)+1 种基金the Innovation and Talent Recruitment Base of New Energy Chemistry and Device(B21003)the Open Research Fund of Key Laboratory of Material Chemistry for Energy Conversion and Storage(HUST),Ministry of Education(2021JYBKF03).
文摘The electrocatalytic water splitting technology can generate highpurity hydrogen without emitting carbon dioxide,which is in favor of relieving environmental pollution and energy crisis and achieving carbon neutrality.Electrocatalysts can effectively reduce the reaction energy barrier and increase the reaction efficiency.Facet engineering is considered as a promising strategy in controlling the ratio of desired crystal planes on the surface.Owing to the anisotropy,crystal planes with different orientations usually feature facet-dependent physical and chemical properties,leading to differences in the adsorption energies of oxygen or hydrogen intermediates,and thus exhibit varied electrocatalytic activity toward hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).In this review,a brief introduction of the basic concepts,fundamental understanding of the reaction mechanisms as well as key evaluating parameters for both HER and OER are provided.The formation mechanisms of the crystal facets are comprehensively overviewed aiming to give scientific theory guides to realize dominant crystal planes.Subsequently,three strategies of selective capping agent,selective etching agent,and coordination modulation to tune crystal planes are comprehensively summarized.Then,we present an overview of significant contributions of facet-engineered catalysts toward HER,OER,and overall water splitting.In particular,we highlight that density functional theory calculations play an indispensable role in unveiling the structure–activity correlation between the crystal plane and catalytic activity.Finally,the remaining challenges in facet-engineered catalysts for HER and OER are provided and future prospects for designing advanced facet-engineered electrocatalysts are discussed.
基金the National Natural Science Foundation of China(Grant no.51973073)the Fel owship of China Postdoctoral Science Foundation(2021M701303)the analytical and testing assistance from the Analysis and Testing Center of HUST for support of this work
文摘Thiol-ene click reaction is an intriguing strategy for preparing polymer electrolytes due to its high activity,atom economy and less side reaction.However,the explosive reaction rate and the use of non-electrolytic amine catalyst hamper its application in in-situ batteries.Herein,a nitrogen-containing eutectic solution is designed as both the catalyst of the thiol-ene reaction and the plasticizer to in-situ synthesize the gel polymer electrolytes,realizing a mild in-situ gelation process and the preparation of high-performance gel electrolytes.The obtained gel polymer electrolytes exhibit a high ionic conductivity of 4×10^(−4)S cm^(−1)and lithium-ion transference number(t_(Li)^(+))of 0.51 at 60°C.The as-assembled Li/LiFePO_(4)(LFP)cell delivers a high initial discharge capacity of 155.9 mAh g^(-1),and a favorable cycling stability with the capacity retention of 82%after 800 cycles at 1 C is also obtained.In addition,this eutectic solution significantly improves the rate performance of the LFP cell with high specific capacity of 141.5 and 126.8 mAh g^(-1)at 5 C and 10 C,respectively,and the cell can steadily work at various charge–discharge rate for 200 cycles.This powerful and efficient strategy may provide a novel way for in-situ preparing gel polymer electrolytes with desirable comprehensive performances.
基金gratefully acknowledge Chongqing Talent Plan: Leading Talents in Innovation and Entrepreneurship (CQYC201903051)University Innovation Research Group of Chongqing (CXQT20023)Natural Science Foundation of Chongqing (cstc2021ycjh-bgzxm0184)。
文摘It is recently suggested that air-formed film plays an important role in controlling corrosion resistance of Mg-Li alloys. However, the structure of the air-formed film and its effect on corrosion resistance of Mg-Li alloys has not been fully understood. Firstly, the air-formed films formed on α and β phases in a dual-phase LZ91 Mg-Li alloy after exposure to laboratory air for up to 48 h have been examined by SEM under the assistance of ultramicrotomy. Then, the effect of the air-formed film on surface potential and, consequently, corrosion/oxidation behavior of the alloy has been investigated. Finally, in order to exclude the influence from α phase, the structure of the air-formed film on β phase and its effect on corrosion/oxidation behavior of Mg-Li alloys have been studied based on a single-phase LA141 Mg-Li alloy. The results show that the air-formed film is thin and negligible on α phase but thick on β phase after prolonged exposure to laboratory air. The thick air-formed film on β phase has a multilayer structure with an inner layer consisting of Mg O/Mg(OH)_(2) and outer layer consisting of Li_(2)CO_(3), which greatly elevates the surface potential of β phase in air. Both LZ91 and LA141 Mg-Li alloys firstly undergo uniform corrosion and then filiform corrosion when immersed in Na Cl solution and the pre-existed air-formed film on β-Li phase can retard the occurrence of filiform corrosion in the alloys.
基金the financial support from the Hubei Provincial Natural Science Foundation of China(No.2020CFB295)the National Natural Science Foundation of China(No.52001128)+1 种基金the Innovative Foundation of Huazhong University of Science and Technology(No.2021JYCXJJ023)the Innovation and Talent Recruitment Base of New Energy Chemistry and Device(No.B21003)。
文摘In the present study,the distribution of Ag in the coating formed on Mg-Ag alloy by plasma electrolytic oxidation(PEO)and its ionic release kinetics when exposed to a 0.9 wt.%Na Cl solution at 37℃have been investigated.Both metallic Ag and Ag oxide particles with~5 to~40 nm in diameters were observed in the PEO coating.Further,an Ag-enriched layer of~20 nm in thickness at the substrate/coating interface was also observed.The PEO coating on the Mg-Ag alloy not only increases its corrosion resistance with the corrosion current density decreasing by up to 3 orders of magnitude from 8.04×10^(-3)to 4.03×10^(-6)A/cm^(2),but also controls the release of Ag+to the level that is sufficient for anti-infective efficacy without causing cytotoxicity to mammal cells.
基金supported by Huazhong University of Science and Technology(No.2021XXJS036,3004013134)National Natural Science Foundation of China(No.51903099,22102059)+1 种基金the National Key Technology R&D Program of China(No.2020YFB1709301,2020YFB1709304,2021YFC2101705)the Innovation and Talent Recruitment Base of New Energy Chemistry and Device(No.B21003)。
文摘Harvesting solar energy in an effective manner for steam and electricity generation is a promising technique to simultaneously cope with the energy and water crises.However,the construction of efficient and easy scale-up photothermal materials for steam and electricity cogeneration remains challenging.Herein,we report a facile and cost-effective strategy to prepare MnO_(2)-decorated cotton cloth(MCx).The wide adsorption spectrum and excellent photothermal conversion ability of the in situ-formed MnO_(2)nanoparticles make the MCx to be advanced photothermal materials.Consequently,the hybrid device integrated with MCx as the photothermal layer and the thermoelectric(TE)module for electricity power conversion exhibits an extremely high evaporation rate of 2.24 kg m^(−2)h^(−1)under 1 kW m^(−2)irradiation,which is ranked among the most powerful solar evaporators.More importantly,during solar evaporation,the hybrid device produces an open-circuit voltage of 0.3 V and a power output of 1.6 W m^(−2)under 3 Sun irradiation,and outperforms most of the previously reported solar-driven electricity generation devices.Therefore,the integrated device with synergistic solar-thermal utilization opens up a green way toward simultaneous solar vapor and electric power generation in remote and resource-constrained areas.
基金supported by Huazhong University of Science and Technology(No.2021XXJS036,3004013134)National Natural Science Foundation of China(No.51903099,82002879,22102059)+2 种基金the Innovation and Talent Recruitment Base of New Energy Chemistry and Device(No.B21003)China Postdoctoral Science Foundation(2021M692475,2021T140524,XJ2021037)support from the 100 Talents Program of the Hubei Provincial Government。
文摘We report a new facile light-induced strategy to disperse micron-sized aggregated bulk covalent organic frameworks(COFs)into isolated COFs nanoparticles.This was achieved by a series of metal-coordinated COFs,namely COF-909-Cu,-Co or-Fe,where for the first time the diffusio-phoretic propulsion was utilized to design COF-based micro/nanomotors.The mechanism studies revealed that the metal ions decorated in the COF-909 backbone could promote the separation of electron and holes and trigger the production of sufficient ionic and reactive oxygen species under visible light irradiation.In this way,strong light-induced self-diffusiophoretic effect is achieved,resulting in good dispersion of COFs.Among them,COF-909-Fe showed the highest dispersion performance,along with a drastic decrease in particle size from 5μm to500 nm,within only 30 min light irradiation,which is inaccessible by using traditional magnetic stirring or ultrasonication methods.More importantly,benefiting from the outstanding dispersion efficiency,COF-909-Fe micro/nanomotors were demonstrated to be efficient in photocatalytic degradation of tetracycline,about 8 times faster than using traditional magnetic stirring method.This work opens up a new avenue to prepare isolated nanosized COFs in a high-fast,simple,and green manner.
基金Supported by the Fundamental Research Funds for the Central Universities,HUST(Z2009008)the National Natural Science Foundation of China(20973068)
文摘Aromatization of methanol over co-impregnated La/Zn/HZSM-5 zeolite catalyst was studied.The selectivity of aromatics and BTX(benzene,toluene,and xylene)reached 64.0%and 56.6%,respectively,using La/Zn/HZSM-5 at 437°C,0.1 MPa and methanol WHSV(weight hourly space velocity)=0.8 h-1.Catalytic results showed that the La species was a very good promoter,increased selectivity of aromatics,and prolonged the catalyst lifetime on stream.The effects of the SiO2/Al2O3 ratio in zeolite,Zn and La loading,WHSV,reaction temperature, water content in the feed and H2 pretreatment of catalysts on the catalytic performance were studied in detail. Characterizations of the catalysts by thermogravimetric analysis(TGA),NH3-TPD(temperature programmed desorption),SEM(scanning electron micrograph),N2 adsorption-desorption,XRD(X-ray diffraction)and XRF (X-ray fluorescence),were carried out to understand the structure and discuss the aromatization performance of La/Zn/HZSM-5 zeolite catalyst.
基金supported by the Fundamental Research Funds for the Central Universities, HUST (No. Z2009008)the National Natural Science Foundation of China (No. 20973068)
文摘The hierarchical mesoporous Zn/ZSM-5 zeolite catalyst was prepared by NaOH treatment and Zn impregnation, and its application in the conversion of methanol to gasoline (MTG) was studied. N2 adsorption-desorption results showed that the mesopores with sizes of 2-20 nm in HZ5/0.3AT was formed by 0.3 M NaOH alkali treatment. The zeolite samples after modification were also characterized by XRF, AAS, XRD, SEM and NH3-TPD methods. Zn impregnated catalyst Zn/HZ5/0.3AT exhibited dramatic improvements in catalytic lifetime and liquid hydrocarbons yield. The selectivity of aromatic hydrocarbons was also improved after Zn impregnation. It is suggested that the mesopores of Zn/HZ5/0.3AT enhanced the synergetic effect of Zn species and acid sites and the capability to coke tolerance, which were confirmed by the results of catalytic test and TGA analysis, respectively.
基金supported by the National Natural Science Foundation of China (21771070, 21571071)the Fundamental Research Funds for the Central Universities (2018KFYYXJJ120, 2019KFYRCPY104)~~
文摘In this study,an acid-induced assembly strategy for a rutile TiO2 photocatalyst was proposed on the basis of the treatment of lamellar protonated titanate with a concentrated HNO3 solution.Nitrate groups were successfully grafted onto a TiO2 surface and induced the assembly of rutile TiO2 nanorods into uniform spindle-like nanobundles.The resulting TiO2 product achieved a photocatalytic hydrogen evolution rate of 402.4μmol h^?1,which is 3.1 times higher than that of Degussa P25-TiO2.It was demonstrated that nitrate group grafting caused the rutile TiO2 surface to become negatively charged,which is favorable for trapping positive protons and improving charge carrier separation,thereby enhancing photocatalytic hydrogen production.Additionally,surface charges were crucial to structural stability based on electrostatic repulsion.This study not only developed a facile surface modification strategy for fabricating efficient H2 production photocatalysts but also identified an influence mechanism of inorganic acids different from that reported in the literature.
基金financially supported by the National Natural Science Foundation of China(21802048,21805103,21805104)the Fundamental Research Funds for the Central Universities(2018KFYXKJC044,2018KFYYXJJ121,2017KFXKJC002,2017KFYXJJ164)the National 1000 Young Talents Program of China。
文摘Developing robust oxygen electrocatalyst with high-performance is very significant for practical rechargeable Zn-air battery.We report herein the preparation of three-dimensional continuous nanocarbon network composed of interconnected nitrogen-doped carbon nanotubes and its application as oxygen electrocatalysis in rechargeable Zn-air battery.Except the excellent electrochemical bifunctionality,this carbon nanotube matrix also delivers an impressive battery performance.Specifically,an opencircuit voltage of 1.50 V as well as a high power density of 220 m W cm^(-2) with remarkable cycling stability for 1600 h is achieved in the rechargeable Zn-air battery.The study not only provides an efficient bifunctional oxygen electrocatalyst but more importantly may pave significant concepts in designing robust electrode for long-life rechargeable Zn-air battery and other energy technologies.