Cobalt nickel bimetallic oxides(NiCo_(2)O_(4))have received numerous attentions in terms of their controllable morphology,high temperature,corrosion resistance and strong electromagnetic wave(EMW)absorption capability...Cobalt nickel bimetallic oxides(NiCo_(2)O_(4))have received numerous attentions in terms of their controllable morphology,high temperature,corrosion resistance and strong electromagnetic wave(EMW)absorption capability.However,broadening the absorption bandwidth is still a huge challenge for NiCo_(2)O_(4)-based absorbers.Herein,the unique NiCo_(2)O_(4)@C core-shell microcubes with hollow structures were fabricated via a facile sacrificial template strategy.The concentration of oxygen vacancies and morphologies of the three-dimensional(3D)cubic hollow core-shell NiCo_(2)O_(4)@C framework were effectively optimized by adjusting the calcination temperature.The specially designed 3D framework structure facilitated the multiple reflections of incident electromagnetic waves and provided rich interfaces between multiple components,generating significant interfacial polarization losses.Dipole polarizations induced by oxygen vacancies could further enhance the attenuation ability for the incident EM waves.The optimized NiCo_(2)O_(4)@C hollow microcubes exhibit superior EMW absorption capability with minimum RL(RLmin)of-84.45 dB at 8.4 GHz for the thickness of 3.0 mm.Moreover,ultrabroad effective absorption bandwidth(EAB)as large as 12.48 GHz(5.52-18 GHz)is obtained.This work is believed to illuminate the path to synthesis of high-performance cobalt nickel bimetallic oxides for EMW absorbers with excellent EMW absorption capability,especially in broadening effective absorption bandwidth.展开更多
Intermetallic complexes of rare-earth and 3d transition metals with core-shell structures are commonly employed as microwave absorbing materials due to their high saturation magnetizations and natural resonance in GHz...Intermetallic complexes of rare-earth and 3d transition metals with core-shell structures are commonly employed as microwave absorbing materials due to their high saturation magnetizations and natural resonance in GHz. Hence, we synthesized Y_2Co_(17)alloy via the co-precipitation reduction-diffusion technique, then coated the Y_2Co_(17)magnetic powders with SiO_(2)to create Y_2Co_(17)@SiO_(2) core-shell structures. The formation of Y_2Co_(17)@SiO_(2)/polyurethane(PU) at various volume fractions and their magnetic, electromagnetic properties were investigated using x-ray diffraction, scanning electron microscopy, energy dispersive spectroscopy, and vector network analyzer. The microwave absorption characteristics of Y_2Co_(17)@SiO_(2)/PU were also investigated at various volume fractions. We not only investigate the zero-reflection conditions of the samples with different volume fractions, but also show that every absorber has a strong reflection loss value(RL ≤-65.00 d B) and excellent microwave absorption properties with an average RL of Y_2Co_(17)@SiO_(2)/PU being below-10 d B at 8 GHz–18 GHz under different thicknesses, showing that the enhancement of microwave absorption performance arises from the balance between permeability and permittivity of absorber.展开更多
CoFe_(2)O_(4)has been widely used for electromagnetic wave absorption owing to its high Snoek limit,high anisotropy,and suitable saturation magnetization;however,its inherent shortcomings,including low dielectric loss...CoFe_(2)O_(4)has been widely used for electromagnetic wave absorption owing to its high Snoek limit,high anisotropy,and suitable saturation magnetization;however,its inherent shortcomings,including low dielectric loss,high density,and magnetic agglomeration,limit its application as an ideal absorbent.This study investigated a microstructure regulation strategy to mitigate the inherent disadvantages of pristine CoFe_(2)O_(4)synthesized via a sol–gel auto-combustion method.A series of CoFe_(2)O_(4)foams(S0.5,S1.0,and S1.5,corresponding to foams with citric acid(CA)-to-Fe(NO_(3))_(3)·9H_(2)O molar ratios of 0.5,1.0,and 1.5,respectively)with two-dimensional(2D)curved surfaces were obtained through the adjustment of CA-to-Fe^(3+)ratio,and the electromagnetic parameters were adjusted through morphology regulation.Owing to the appropriate impedance matching and conductance loss provided by moderate complex permittivity,the effective absorption bandwidth(EAB)of S0.5 was as high as 7.3 GHz,exceeding those of most CoFe_(2)O_(4)-based absorbents.Moreover,the EAB of S1.5 reached 5.0 GHz(8.9–13.9 GHz),covering most of the X band,owing to the intense polarization provided by lattice defects and the heterogeneous interface.The three-dimensional(3D)foam structure circumvented the high density and magnetic agglomeration issues of CoFe_(2)O_(4)nanoparticles,and the good conductivity of 2D curved surfaces could effectively elevate the complex permittivity to ameliorate the dielectric loss of pure CoFe_(2)O_(4).This study provides a novel idea for the theoretical design and practical production of lightweight and broadband pure ferrites.展开更多
Energy supply dominated by fossil energy has been and remains the main cause of carbon dioxide emissions,the major greenhouse gas leading to the current grave climate change challenges.Many technical pathways have bee...Energy supply dominated by fossil energy has been and remains the main cause of carbon dioxide emissions,the major greenhouse gas leading to the current grave climate change challenges.Many technical pathways have been proposed to address the challenges.Carbon capture and utilization(CCU) represents one of the approaches and thermochemical CO_(2) splitting driven by thermal energy is a subset of the CCU,which converts the captured CO_(2) into CO and makes it possible to achieve closed-loop carbon recirculation.Redox-active catalysts are among the most critical components of the thermochemical splitting cycles and perovskites are regarded as the most promising catalysts.Here we review the latest advancements in thermochemical cycles based on perovskites,covering thermodynamic principles,material modifications,reaction kinetics,oxygen pressure control,circular strategies,and demonstrations to provide a comprehensive overview of the topical area.Thermochemical cycles based on such materials require the consideration of trade-off between cost and efficiency,which is related to actual material used,operation mode,oxygen removal,and heat recovery.Lots of efforts have been made towards improving reaction rates,conversion efficiency and cycling stability,materials related research has been lacking-a key aspect affecting the performance across all above aspects.Double perovskites and composite perovskites arise recently as a potentially promising addition to material candidates.For such materials,more effective oxygen removal would be needed to enhance the overall efficiency,for which thermochemical or electrochemical oxygen pumps could contribute to efficient oxygen removal as well as serve as means for inert gas regeneration.The integration of thermochemical CO_(2) splitting process with downstream fuel production and other processes could reduce costs and increase efficiency of the technology.This represents one of the directions for the future research.展开更多
The development of earth-abundant electrocatalysts with high performance for electrochemical CO_(2)reduction(ECR)is of great significance.Cu-based catalysts have been widely investigated for ECR due to their unique ab...The development of earth-abundant electrocatalysts with high performance for electrochemical CO_(2)reduction(ECR)is of great significance.Cu-based catalysts have been widely investigated for ECR due to their unique ability to generate various carbonaceous products,but directing selectivity toward one certain product and identifying the real active sites during ECR are still full of challenge.Here,after the incorporation of CdO into CuO,the Cu_(0.5)Cd_(0.5)-O catalyst achieves a 10.3-fold enhancement for CO selectivity in comparison with CuO,and a CO faradic efficiency nearly 90%with a current density around20 mA cm^(-2)could maintain at least 60 h.Interestingly,a wide CO/H_(2)ratio(0.07-10)is reached on Cu_(x)Cd_(1-x)-O catalysts by varying the Cu/Cd ratio,demonstrating the potential of syngas production using such catalysts.The results of ex situ XRD,XPS,and in situ Raman reveal that the real active sites of Cu_(0.5)Cd_(0.5)-O catalysts for CO production during ECR reaction are the reconstructed mixed phases of CuCd alloy and CdCO_(3).In situ FTIR and theoretical calculations further implicate the presence of Cd related species promotes the CO desorption and inhibits the H_(2)evolution,thus leading to an enhanced CO generation.展开更多
The poor electrochemical performance of all-solid-state batteries(ASSBs),which is assemblied by Ni-rich cathode and poly(ethylene oxide)(PEO)-based electrolytes,can be attributed to unstable cathodic interface and poo...The poor electrochemical performance of all-solid-state batteries(ASSBs),which is assemblied by Ni-rich cathode and poly(ethylene oxide)(PEO)-based electrolytes,can be attributed to unstable cathodic interface and poor crystal structure stability of Ni-rich cathode.Several coating strategies are previously employed to enhance the stability of the cathodic interface and crystal structure for Ni-rich cathode.However,these methods can hardly achieve simplicity and high efficiency simultaneously.In this work,polyacrylic acid(PAA)replaced traditional PVDF as a binder for cathode,which can achieve a uniform PAA-Li(LixPAA(0<x≤1))coating layer on the surface of single-crystal LiNi_(0.83)Co_(0.12)Mn_(0.05)O_(2)(SC-NCM83)due to H^(+)/Li^(+)exchange reaction during the initial charging-discharging process.The formation of PAA-Li coating layer on cathode can promote interfacial Li^(+)transport and enhance the stability of the cathodic interface.Furthermore,the partially-protonated surface of SC-NCM83 casued by H^(+)/Li^(+)exchange reaction can restrict Ni ions transport to enhance the crystal structure stability.The proposed SC-NCM83-PAA exhibits superior cycling performance with a retention of 92%compared with that(57.3%)of SC-NCM83-polyvinylidene difluoride(PVDF)after 200 cycles.This work provides a practical strategy to construct high-performance cathodes for ASSBs.展开更多
PEG (Polyethylene glycol average molecular weight 300) is used as absorbent of NO2. The absorption efficiency is found to reach up to 97%. The absorbing product, PEG NO2, can be used to cleave benzyl ethers mildly and...PEG (Polyethylene glycol average molecular weight 300) is used as absorbent of NO2. The absorption efficiency is found to reach up to 97%. The absorbing product, PEG NO2, can be used to cleave benzyl ethers mildly and selectively to benzaldehyde and corresponding fatty alcohols, showing that PEG is a valuable oxidizing agent of benzyl ethers. As a carrier of NO2.PEG can be recovered and utilized repeatedly after the oxidation.展开更多
Graphitic carbon nitride(g-C_(3)N_(4))has attracted great interest in photocatalysis and photoelectrocatalysis.However,their poor hydrophilicity poses a great challenge for their applications in aqueous environment.He...Graphitic carbon nitride(g-C_(3)N_(4))has attracted great interest in photocatalysis and photoelectrocatalysis.However,their poor hydrophilicity poses a great challenge for their applications in aqueous environment.Here,we demonstrate synthesis of a hydrophilic bi-functional hierarchical architecture by the assembly of B-doped g-C_(3)N_(4)nanoplatelets.Such hierarchical B-doped g-C_(3)N_(4)material enables full utilization of their highly enhanced visible light absorption and photogenerated carrier separation in aqueous medium,leading to an excellent photocatalytic H_(2)O_(2)production rate of 4240.3μM g^(-1)h^(-1),2.84,2.64 and 2.13 times higher than that of the bulk g-C_(3)N_(4),g-C_(3)N_(4)nanoplatelets and bulk B doped g-C_(3)N_(4),respectively.Photoanodes based on these hierarchical architectures can generate an unprecedented photocurrent density of 1.72 m A cm^(-2)at 1.23 V under AM 1.5 G illumination for photoelectrochemical water splitting.This work makes a fundamental improvement towards large-scale exploitation of highly active,hydrophilic and stable metal-free g-C_(3)N_(4)photocatalysts for various practical applications.展开更多
CO_(2)capture with a low energy consumption is of important application significance for reducing CO_(2)emission.The phase-change absorbent developed in recent years shows its potential for low-energy CO_(2)capture.Th...CO_(2)capture with a low energy consumption is of important application significance for reducing CO_(2)emission.The phase-change absorbent developed in recent years shows its potential for low-energy CO_(2)capture.The unclear phase-splitting rule hinders the efficient development of CO_(2)phase-change absorbents.To predict phase-splitting behaviors of mono/poly-amine-organic solvent-water system with various concentrations,a quasi-activity coefficient was developed based on Debye&Mc Aulay equation and some Density function theory descriptors.Six models based on Debye&Mc Aulay equation were developed with different ion radius,descriptors or poly-amine-CO_(2)products.The phase-splitting boundary was drawn on the model with the best predictability.This quasi-activity coefficient would provide guidance for the phase-splitting systems development,especially for polyamines.展开更多
A novel nanocomposite of Ni nanoparticles loaded on Mg-doped Al_(2)O_(3)(Ni/Mg-Al_(2)O_(3))was prepared.By photothermocatalytic CO_(2) reduction with methane(CRM)merely using focused UV-vis-IR illumination on Ni/Mg-Al...A novel nanocomposite of Ni nanoparticles loaded on Mg-doped Al_(2)O_(3)(Ni/Mg-Al_(2)O_(3))was prepared.By photothermocatalytic CO_(2) reduction with methane(CRM)merely using focused UV-vis-IR illumination on Ni/Mg-Al_(2)O_(3),high production rates of H_(2)(r_(H2),69.71 mmol min^(−1) g^(−1))and CO(rCO,74.57 mmol min^(−1) g^(−1))and an extremely large light-to-fuel efficiency(η,32.9%)are acquired.High rH2 and rCO(51.07 and 59.66 mmol min^(−1) g^(−1))and a largeη(32.5%)are acquired even by using focusedλ>560 nm vis-IR illumination.Ni/Mg-Al_(2)O_(3) shows good durability for photothermocatalytic CRM due to the side reaction of carbon deposition being enormously inhibited in comparison with a reference catalyst of Ni nanoparticles loaded on Al_(2)O_(3).The enormous carbon deposition inhibition is ascribed to the presence of a fence of CO_(2) molecules(strongly adsorbed on Mg-doped Al_(2)O_(3))around Ni nanoparticles,which block the polymerization and growth of carbon species to nanofibers by promoting the oxidation of carbon species formed by CH_(4) dissociation.The high photothermocatalytic activity of Ni/Mg-Al_(2)O_(3) arises from efficient light-driven thermocatalytic CRM.A photoactivation is found to considerably raise the photothermocatalytic activity of Ni/Mg-Al_(2)O_(3) because of the apparent activation energy(Ea)being substantially decreased upon focused illumination.The Ea reduction is associated with the rate-determining steps of CRM(e.g.,CH_(4) dissociation and the oxidation of carbon species)being accelerated upon focused illumination.展开更多
The continuous and excessive emission of CO_(2)into the atmosphere presents a pressing challenge for global sustainable development.In response,researchers have been devoting significant efforts to develop methods for...The continuous and excessive emission of CO_(2)into the atmosphere presents a pressing challenge for global sustainable development.In response,researchers have been devoting significant efforts to develop methods for converting CO_(2)into valuable chemicals and fuels.These conversions have the potential to establish a closed artificial carbon cycle and provide an alternative resource to depleting fossil fuels.Among the various conversion routes,thermochemical CO_(2)reduction stands out as a promising candidate for industrialization.Within the realm of heterogeneous catalysis,single atom catalysts(SACs)have garnered significant attention.The utilization of SACs offers tremendous potential for enhancing catalytic performance.To achieve optimal activity and selectivity of SACs in CO_(2)thermochemical reduction reactions,a comprehensive understanding of key factors such as single atom metal-support interactions,chemical coordination,and accessibility of active sites is crucial.Despite extensive research in this field,the atomic-scale reaction mechanisms in different chemical environments remain largely unexplored.While SACs have been found successful applications in electrochemical and photochemical CO_(2)reduction reactions,their implementation in thermochemical CO_(2)reduction encounters challenges due to the sintering and/or agglomeration effects that occur at elevated temperatures.In this review,we present a unique approach that combines theoretical understanding with experimental strategies to guide researchers in the design of controlled and thermally stable SACs.By elucidating the underlying principles,we aim to enable the creation of SACs that exhibit stable and efficient catalytic activity for thermochemical CO_(2)reduction reactions.Subsequently,we provide a comprehensive overview of recent literature on noble metal-and transition metal-based SACs for thermochemical CO_(2)reduction.The current review is focused on certain CO_(2)-derived products involving one step reduction only for simplicity and for better understanding the SACs enhancement mechanism.We emphasize various synthesis methods employed and highlight the catalytic activity of these SACs.Finally,we delve into the perspectives and challenges associated with SACs in the context of thermochemical CO_(2)reduction reactions,providing valuable insights for future research endeavor.Through this review,we aim to contribute to the advancement of SACs in the field of thermochemical CO_(2)reduction,shedding light on their potential as effective catalysts and addressing the challenges that need to be overcome for their successful implementation as paradigm shift in catalysis.展开更多
The efficient utilization of photocatalytic technology is essential for clean energy.Bismuth-based multimetal oxides(Bi_(2)WO_(6),Bi_(2)MoO_(6),BiVO_(4)and Bi_(4)Ti_(3)O_(12))have aroused widespread attention as a vis...The efficient utilization of photocatalytic technology is essential for clean energy.Bismuth-based multimetal oxides(Bi_(2)WO_(6),Bi_(2)MoO_(6),BiVO_(4)and Bi_(4)Ti_(3)O_(12))have aroused widespread attention as a visible light responsive photocatalyst for hydrogen evolution due to their low cost,nontoxicity,modifiable morphology,and outstanding optical and chemical properties.Nevertheless,the photocatalytic activities of pure materials are unsatisfactory because of their relative small specific surface area,poor quantum yield,and the rapid recombination of photogenerated carriers.Therefore,some modification strategies,including morphological control,semiconductor combination,doping,and defect engineering,have been systematically studied to enhance photocatalytic H_(2)evolution activity in the past few years.Herein,we summarize the recent research progress on bismuth-based photocatalysts,pointing out the prospects,opportunities and challenges of bismuth-based photocatalysts.Eventually,we aims to put forward valuable suggestions for designing of bismuth-based photocatalysts applied in hydrogen production on the premise of consolidating the existing theoretical basis of photocatalysis.展开更多
In recent years, interest in hydrogen as a fuel has sharply increased in the field of alternative and green energy due to its high energy capability and zero-emission behaviour. As a result, research in the developmen...In recent years, interest in hydrogen as a fuel has sharply increased in the field of alternative and green energy due to its high energy capability and zero-emission behaviour. As a result, research in the development of new highly efficient methods for producing high-purity hydrogen is relevant. This paper presents, for the first time, the test results of an electrochemical cell with a proton-conducting La_(0.9)Sr_(0.1)ScO_(3-δ) electrolyte and symmetrical Sr_(1.95)Fe_(1.4)Ni_(0.1)Mo_(0.5)O_(6-δ)+ La_(0.9)Sr_(0.1)Sc_(0.9)Co_(0.1)O_(3-δ) electrodes as a hybrid setup for electricity generation in proton ceramic fuel cell mode, for hydrogen separation from H_(2)+ Ar mixture and the production of high-purity hydrogen from methane with simultaneous CO_(2) utilization.It was found that this electrochemical cell generates high flow rates of hydrogen during its separation through a proton-conducting membrane from H_(2)+ Ar mixture, about 500 cm^(3)h^(-1)cm^(-2)at a current density of 0.6 A cm^(-2)as well as about 370 cm^(3) h^(-1)cm^(-2)at a current density of 0.5 A cm^(-2) from CH_(4)+ CO_(2) mixture at 800 ℃ which shows that these cells are promising for hydrogen production.展开更多
Photocatalytic methane(CH_(4))production wherein CO_(2)is reduced to CH_(4) by utilizing solar radiation energy is gaining research and industrial focus because of its environmental-friendly notion.It offers twofold a...Photocatalytic methane(CH_(4))production wherein CO_(2)is reduced to CH_(4) by utilizing solar radiation energy is gaining research and industrial focus because of its environmental-friendly notion.It offers twofold advantages:reduction in CO_(2)emission and production of artificial natural gas(methane)at the same time.In this paper,comparative energy,economic and environmental assessment of such photocatalytic methane production has been carried out between Japan and Malaysian conditions.Assumptions on the photocatalytic methane production plant and estimation of energy production,CO_(2)emission reduction,and economic indicators are made based on previous research and existing technologies.Energy analysis shows that Malaysia has a higher potential for energy production and CO_(2)emission reduction than Japan.Economic analysis reveals that the feasible reaction efficiencies of the plant in Japan and Malaysia are 8%.The slightly higher conversion efficiency in Malaysia is due to the energy price and CO_(2)tax.For the implementation of the photocatalytic methane production plant,the high energy price and CO_(2)tax will work as a driving force.展开更多
Electrochemical transformation emerges as an important solution to sustainable energy conversion and chemical production.Conventional electrolytic systems usually operate under galvanostatic or potentiostatic conditio...Electrochemical transformation emerges as an important solution to sustainable energy conversion and chemical production.Conventional electrolytic systems usually operate under galvanostatic or potentiostatic conditions that sometimes result in unsatisfactory efficiencies or selectivities.Pulse electrolysis by pulsating and programming the potentials/currents can feature unique tunability to the electrodeelectrolyte interface properties that can give rise to drastically different electrochemical behaviors compared to the steady-state counterparts.Although invented almost 100 years ago,pulse electrolysis has received little attention over the period,but has recently attracted a revived focus toward the energyefficient electrolysis.This review will summarize the history and recent efforts of pulse electrolysis in three categories:water electrolysis,CO_(2)electrolysis and other electrolysis.In each section,the advantage of pulse electrolysis over steady-state electrolysis will be discussed in detail,giving a comprehensive overview of the pulse effect on the electrolytic systems.Finally,we will provide our vision of future directions in pulse electrolysis based on previous works.展开更多
Quantifying the gross and net production is an essential component of carbon cycling and marine ecosystem studies.Triple oxygen isotope measurements and the O_(2)/Ar ratio are powerful indices in quantifying the gross...Quantifying the gross and net production is an essential component of carbon cycling and marine ecosystem studies.Triple oxygen isotope measurements and the O_(2)/Ar ratio are powerful indices in quantifying the gross primary production and net community production of the mixed layer zone,respectively.Although there is a substantial advantage in refining the gas exchange term and water column vertical mixing calibration,application of mixed layer depth history to the gas exchange term and its contribution to reducing indices error are unclear.Therefore,two cruises were conducted in the slope regions of the northern South China Sea in October 2014(autumn)and June 2015(spring).Discrete water samples at Station L07 in the upper 150 m depth were collected for the determination ofδ^(17)0,δ^(18)O,and the O_(2)/Ar ratio of dissolved gases.Gross oxygen production(GOP)was estimated using the triple oxygen isotopes of the dissolved O_(2),and net oxygen production(NOP)was calculated using O_(2)/Ar ratio and O_(2)concentration.The vertical mixing effect in NOP was calibrated via a N_(2)O based approach.GOP for autumn and spring was(169±23)mmol/(m^(2)·d)(by O_(2))and(189±26)mmol/(m^(2)·d)(by O_(2)),respectively.While NOP was 1.5 mmol/(m^(2)·d)(by O_(2))in autumn and 8.2 mmol/(m^(2)·d)(by O_(2))in spring.Application of mixed layer depth history in the gas flux parametrization reduced up to 9.5%error in the GOP and NOP estimations.A comparison with an independent O_(2)budget calculation in the diel observation indicated a26%overestimation in the current GOP,likely due to the vertical mixing effect.Both GOP and NOP in June were higher than those in October.Potential explanations for this include the occurrence of an eddy process in June,which may have exerted a submesoscale upwelling at the sampling station,and also the markedly higher terrestrial impact in June.展开更多
Coal fly ash(FA),a valuable industrial solid residue generated from coal combustion,is composed of various metal oxides and has a high thermal stability.Given that the coal-based energy will continue to account for a ...Coal fly ash(FA),a valuable industrial solid residue generated from coal combustion,is composed of various metal oxides and has a high thermal stability.Given that the coal-based energy will continue to account for a significant portion of global electricity generation in the coming years,the lack of effective management strategies exacerbates the threat of FA wastes to the surrounding environment and human health.For a sustainable development,green and renewable hydrogen economy and CO_(2)capture efforts provide appealing opportunities to valorize FA as catalysts and/or sorbents due to their appealing physicochemical properties.Hydrogen applications along with carbon neutrality are potential strategies to mitigate climate change crisis,but high processing costs(catalysts/sorbents)are challenging to realize this purpose.In this context,the utilization of FA not only enhances industrial competitiveness(by reducing manufacturing costs),but also provides ecologically friendly approaches to minimizing this solid waste.This state-of-the-art review highlights a wide-ranging outlook on the valorization of FA as catalysts and sorbents for hydrogen-rich gas production via conventional/intensified processes(CO_(2)/H_(2)O reforming,ammonia decomposition,hydride hydrolysis).The fundamental physicochemical characterizations and hazards/utilization of FA,which significantly affect the FA's utilization in various fields,are first introduced.The influence of several factors(like FA types and catalysis/sorption operation conditions)on the activity performance of FA-based materials is then discussed in detail.This critical review aims to open the window to further innovative ideas regarding the application of different FA residues in other catalytic and sorption processes.展开更多
基金This work was supported by Natural Science Foundation of Shandong Province(ZR2022ME089)National Natural Science Foundation of China(52207249)Yantai Basic Research Project(2022JCYJ04).
文摘Cobalt nickel bimetallic oxides(NiCo_(2)O_(4))have received numerous attentions in terms of their controllable morphology,high temperature,corrosion resistance and strong electromagnetic wave(EMW)absorption capability.However,broadening the absorption bandwidth is still a huge challenge for NiCo_(2)O_(4)-based absorbers.Herein,the unique NiCo_(2)O_(4)@C core-shell microcubes with hollow structures were fabricated via a facile sacrificial template strategy.The concentration of oxygen vacancies and morphologies of the three-dimensional(3D)cubic hollow core-shell NiCo_(2)O_(4)@C framework were effectively optimized by adjusting the calcination temperature.The specially designed 3D framework structure facilitated the multiple reflections of incident electromagnetic waves and provided rich interfaces between multiple components,generating significant interfacial polarization losses.Dipole polarizations induced by oxygen vacancies could further enhance the attenuation ability for the incident EM waves.The optimized NiCo_(2)O_(4)@C hollow microcubes exhibit superior EMW absorption capability with minimum RL(RLmin)of-84.45 dB at 8.4 GHz for the thickness of 3.0 mm.Moreover,ultrabroad effective absorption bandwidth(EAB)as large as 12.48 GHz(5.52-18 GHz)is obtained.This work is believed to illuminate the path to synthesis of high-performance cobalt nickel bimetallic oxides for EMW absorbers with excellent EMW absorption capability,especially in broadening effective absorption bandwidth.
基金the National Key Research and Development Program of China (Grant No. 2021YFB3501302)the National Natural Science Foundation of China (Grant No. 51731001)the Fund from the State Key Laboratory of Baiyunobo Rare Earth Resource Researches and Comprehensive Utilization’s Key Research and Development Projects。
文摘Intermetallic complexes of rare-earth and 3d transition metals with core-shell structures are commonly employed as microwave absorbing materials due to their high saturation magnetizations and natural resonance in GHz. Hence, we synthesized Y_2Co_(17)alloy via the co-precipitation reduction-diffusion technique, then coated the Y_2Co_(17)magnetic powders with SiO_(2)to create Y_2Co_(17)@SiO_(2) core-shell structures. The formation of Y_2Co_(17)@SiO_(2)/polyurethane(PU) at various volume fractions and their magnetic, electromagnetic properties were investigated using x-ray diffraction, scanning electron microscopy, energy dispersive spectroscopy, and vector network analyzer. The microwave absorption characteristics of Y_2Co_(17)@SiO_(2)/PU were also investigated at various volume fractions. We not only investigate the zero-reflection conditions of the samples with different volume fractions, but also show that every absorber has a strong reflection loss value(RL ≤-65.00 d B) and excellent microwave absorption properties with an average RL of Y_2Co_(17)@SiO_(2)/PU being below-10 d B at 8 GHz–18 GHz under different thicknesses, showing that the enhancement of microwave absorption performance arises from the balance between permeability and permittivity of absorber.
基金supported by the National Natural Science Foundation of China (Nos.22004106 and 51872238)。
文摘CoFe_(2)O_(4)has been widely used for electromagnetic wave absorption owing to its high Snoek limit,high anisotropy,and suitable saturation magnetization;however,its inherent shortcomings,including low dielectric loss,high density,and magnetic agglomeration,limit its application as an ideal absorbent.This study investigated a microstructure regulation strategy to mitigate the inherent disadvantages of pristine CoFe_(2)O_(4)synthesized via a sol–gel auto-combustion method.A series of CoFe_(2)O_(4)foams(S0.5,S1.0,and S1.5,corresponding to foams with citric acid(CA)-to-Fe(NO_(3))_(3)·9H_(2)O molar ratios of 0.5,1.0,and 1.5,respectively)with two-dimensional(2D)curved surfaces were obtained through the adjustment of CA-to-Fe^(3+)ratio,and the electromagnetic parameters were adjusted through morphology regulation.Owing to the appropriate impedance matching and conductance loss provided by moderate complex permittivity,the effective absorption bandwidth(EAB)of S0.5 was as high as 7.3 GHz,exceeding those of most CoFe_(2)O_(4)-based absorbents.Moreover,the EAB of S1.5 reached 5.0 GHz(8.9–13.9 GHz),covering most of the X band,owing to the intense polarization provided by lattice defects and the heterogeneous interface.The three-dimensional(3D)foam structure circumvented the high density and magnetic agglomeration issues of CoFe_(2)O_(4)nanoparticles,and the good conductivity of 2D curved surfaces could effectively elevate the complex permittivity to ameliorate the dielectric loss of pure CoFe_(2)O_(4).This study provides a novel idea for the theoretical design and practical production of lightweight and broadband pure ferrites.
文摘Energy supply dominated by fossil energy has been and remains the main cause of carbon dioxide emissions,the major greenhouse gas leading to the current grave climate change challenges.Many technical pathways have been proposed to address the challenges.Carbon capture and utilization(CCU) represents one of the approaches and thermochemical CO_(2) splitting driven by thermal energy is a subset of the CCU,which converts the captured CO_(2) into CO and makes it possible to achieve closed-loop carbon recirculation.Redox-active catalysts are among the most critical components of the thermochemical splitting cycles and perovskites are regarded as the most promising catalysts.Here we review the latest advancements in thermochemical cycles based on perovskites,covering thermodynamic principles,material modifications,reaction kinetics,oxygen pressure control,circular strategies,and demonstrations to provide a comprehensive overview of the topical area.Thermochemical cycles based on such materials require the consideration of trade-off between cost and efficiency,which is related to actual material used,operation mode,oxygen removal,and heat recovery.Lots of efforts have been made towards improving reaction rates,conversion efficiency and cycling stability,materials related research has been lacking-a key aspect affecting the performance across all above aspects.Double perovskites and composite perovskites arise recently as a potentially promising addition to material candidates.For such materials,more effective oxygen removal would be needed to enhance the overall efficiency,for which thermochemical or electrochemical oxygen pumps could contribute to efficient oxygen removal as well as serve as means for inert gas regeneration.The integration of thermochemical CO_(2) splitting process with downstream fuel production and other processes could reduce costs and increase efficiency of the technology.This represents one of the directions for the future research.
基金financially supported by the National Natural Science Foundation of China with grant number of 22172082 and 21978137。
文摘The development of earth-abundant electrocatalysts with high performance for electrochemical CO_(2)reduction(ECR)is of great significance.Cu-based catalysts have been widely investigated for ECR due to their unique ability to generate various carbonaceous products,but directing selectivity toward one certain product and identifying the real active sites during ECR are still full of challenge.Here,after the incorporation of CdO into CuO,the Cu_(0.5)Cd_(0.5)-O catalyst achieves a 10.3-fold enhancement for CO selectivity in comparison with CuO,and a CO faradic efficiency nearly 90%with a current density around20 mA cm^(-2)could maintain at least 60 h.Interestingly,a wide CO/H_(2)ratio(0.07-10)is reached on Cu_(x)Cd_(1-x)-O catalysts by varying the Cu/Cd ratio,demonstrating the potential of syngas production using such catalysts.The results of ex situ XRD,XPS,and in situ Raman reveal that the real active sites of Cu_(0.5)Cd_(0.5)-O catalysts for CO production during ECR reaction are the reconstructed mixed phases of CuCd alloy and CdCO_(3).In situ FTIR and theoretical calculations further implicate the presence of Cd related species promotes the CO desorption and inhibits the H_(2)evolution,thus leading to an enhanced CO generation.
基金the financial support from the National Natural Science Foundation of China(Nos.52034011 and 52204328)the Science and Technology Innovation Program of Hunan Province(2023RC305)the Changsha Municipal Natural Science Foundation(kq2202085)。
文摘The poor electrochemical performance of all-solid-state batteries(ASSBs),which is assemblied by Ni-rich cathode and poly(ethylene oxide)(PEO)-based electrolytes,can be attributed to unstable cathodic interface and poor crystal structure stability of Ni-rich cathode.Several coating strategies are previously employed to enhance the stability of the cathodic interface and crystal structure for Ni-rich cathode.However,these methods can hardly achieve simplicity and high efficiency simultaneously.In this work,polyacrylic acid(PAA)replaced traditional PVDF as a binder for cathode,which can achieve a uniform PAA-Li(LixPAA(0<x≤1))coating layer on the surface of single-crystal LiNi_(0.83)Co_(0.12)Mn_(0.05)O_(2)(SC-NCM83)due to H^(+)/Li^(+)exchange reaction during the initial charging-discharging process.The formation of PAA-Li coating layer on cathode can promote interfacial Li^(+)transport and enhance the stability of the cathodic interface.Furthermore,the partially-protonated surface of SC-NCM83 casued by H^(+)/Li^(+)exchange reaction can restrict Ni ions transport to enhance the crystal structure stability.The proposed SC-NCM83-PAA exhibits superior cycling performance with a retention of 92%compared with that(57.3%)of SC-NCM83-polyvinylidene difluoride(PVDF)after 200 cycles.This work provides a practical strategy to construct high-performance cathodes for ASSBs.
文摘PEG (Polyethylene glycol average molecular weight 300) is used as absorbent of NO2. The absorption efficiency is found to reach up to 97%. The absorbing product, PEG NO2, can be used to cleave benzyl ethers mildly and selectively to benzaldehyde and corresponding fatty alcohols, showing that PEG is a valuable oxidizing agent of benzyl ethers. As a carrier of NO2.PEG can be recovered and utilized repeatedly after the oxidation.
基金financially supported by the National Natural Science Foundation of China(U1663225)the Changjiang Scholar Program of Chinese Ministry of Education(IRT15R52)the program of Introducing Talents of Discipline to Universities-Plan 111(B20002)of Ministry of Science and Technology and the Ministry of Education of China and the project “Depollut Air”of Interreg V France-WallonieVlaanderen。
文摘Graphitic carbon nitride(g-C_(3)N_(4))has attracted great interest in photocatalysis and photoelectrocatalysis.However,their poor hydrophilicity poses a great challenge for their applications in aqueous environment.Here,we demonstrate synthesis of a hydrophilic bi-functional hierarchical architecture by the assembly of B-doped g-C_(3)N_(4)nanoplatelets.Such hierarchical B-doped g-C_(3)N_(4)material enables full utilization of their highly enhanced visible light absorption and photogenerated carrier separation in aqueous medium,leading to an excellent photocatalytic H_(2)O_(2)production rate of 4240.3μM g^(-1)h^(-1),2.84,2.64 and 2.13 times higher than that of the bulk g-C_(3)N_(4),g-C_(3)N_(4)nanoplatelets and bulk B doped g-C_(3)N_(4),respectively.Photoanodes based on these hierarchical architectures can generate an unprecedented photocurrent density of 1.72 m A cm^(-2)at 1.23 V under AM 1.5 G illumination for photoelectrochemical water splitting.This work makes a fundamental improvement towards large-scale exploitation of highly active,hydrophilic and stable metal-free g-C_(3)N_(4)photocatalysts for various practical applications.
基金financial support from National Natural Science Foundation of China(21878190)China Petrochemical Corporation(419033-1)the Engineering Experimental Teaching Center,School of Chemical Engineering,Sichuan University for the Nuclear Magnetic Resonance(NMR,JNM-ECZ400S/L1,JEOL Ltd.)support and the compute server support。
文摘CO_(2)capture with a low energy consumption is of important application significance for reducing CO_(2)emission.The phase-change absorbent developed in recent years shows its potential for low-energy CO_(2)capture.The unclear phase-splitting rule hinders the efficient development of CO_(2)phase-change absorbents.To predict phase-splitting behaviors of mono/poly-amine-organic solvent-water system with various concentrations,a quasi-activity coefficient was developed based on Debye&Mc Aulay equation and some Density function theory descriptors.Six models based on Debye&Mc Aulay equation were developed with different ion radius,descriptors or poly-amine-CO_(2)products.The phase-splitting boundary was drawn on the model with the best predictability.This quasi-activity coefficient would provide guidance for the phase-splitting systems development,especially for polyamines.
基金supported by National Natural Science Foundation of China(21972109,21673168)DFT calculations were conducted at the Shanghai Supercomputer Center(SSC),China.
文摘A novel nanocomposite of Ni nanoparticles loaded on Mg-doped Al_(2)O_(3)(Ni/Mg-Al_(2)O_(3))was prepared.By photothermocatalytic CO_(2) reduction with methane(CRM)merely using focused UV-vis-IR illumination on Ni/Mg-Al_(2)O_(3),high production rates of H_(2)(r_(H2),69.71 mmol min^(−1) g^(−1))and CO(rCO,74.57 mmol min^(−1) g^(−1))and an extremely large light-to-fuel efficiency(η,32.9%)are acquired.High rH2 and rCO(51.07 and 59.66 mmol min^(−1) g^(−1))and a largeη(32.5%)are acquired even by using focusedλ>560 nm vis-IR illumination.Ni/Mg-Al_(2)O_(3) shows good durability for photothermocatalytic CRM due to the side reaction of carbon deposition being enormously inhibited in comparison with a reference catalyst of Ni nanoparticles loaded on Al_(2)O_(3).The enormous carbon deposition inhibition is ascribed to the presence of a fence of CO_(2) molecules(strongly adsorbed on Mg-doped Al_(2)O_(3))around Ni nanoparticles,which block the polymerization and growth of carbon species to nanofibers by promoting the oxidation of carbon species formed by CH_(4) dissociation.The high photothermocatalytic activity of Ni/Mg-Al_(2)O_(3) arises from efficient light-driven thermocatalytic CRM.A photoactivation is found to considerably raise the photothermocatalytic activity of Ni/Mg-Al_(2)O_(3) because of the apparent activation energy(Ea)being substantially decreased upon focused illumination.The Ea reduction is associated with the rate-determining steps of CRM(e.g.,CH_(4) dissociation and the oxidation of carbon species)being accelerated upon focused illumination.
基金support by Khalifa University through CIRA-2020-077 and RC2-2018-024 grants。
文摘The continuous and excessive emission of CO_(2)into the atmosphere presents a pressing challenge for global sustainable development.In response,researchers have been devoting significant efforts to develop methods for converting CO_(2)into valuable chemicals and fuels.These conversions have the potential to establish a closed artificial carbon cycle and provide an alternative resource to depleting fossil fuels.Among the various conversion routes,thermochemical CO_(2)reduction stands out as a promising candidate for industrialization.Within the realm of heterogeneous catalysis,single atom catalysts(SACs)have garnered significant attention.The utilization of SACs offers tremendous potential for enhancing catalytic performance.To achieve optimal activity and selectivity of SACs in CO_(2)thermochemical reduction reactions,a comprehensive understanding of key factors such as single atom metal-support interactions,chemical coordination,and accessibility of active sites is crucial.Despite extensive research in this field,the atomic-scale reaction mechanisms in different chemical environments remain largely unexplored.While SACs have been found successful applications in electrochemical and photochemical CO_(2)reduction reactions,their implementation in thermochemical CO_(2)reduction encounters challenges due to the sintering and/or agglomeration effects that occur at elevated temperatures.In this review,we present a unique approach that combines theoretical understanding with experimental strategies to guide researchers in the design of controlled and thermally stable SACs.By elucidating the underlying principles,we aim to enable the creation of SACs that exhibit stable and efficient catalytic activity for thermochemical CO_(2)reduction reactions.Subsequently,we provide a comprehensive overview of recent literature on noble metal-and transition metal-based SACs for thermochemical CO_(2)reduction.The current review is focused on certain CO_(2)-derived products involving one step reduction only for simplicity and for better understanding the SACs enhancement mechanism.We emphasize various synthesis methods employed and highlight the catalytic activity of these SACs.Finally,we delve into the perspectives and challenges associated with SACs in the context of thermochemical CO_(2)reduction reactions,providing valuable insights for future research endeavor.Through this review,we aim to contribute to the advancement of SACs in the field of thermochemical CO_(2)reduction,shedding light on their potential as effective catalysts and addressing the challenges that need to be overcome for their successful implementation as paradigm shift in catalysis.
基金This research was supported by National Natural Science Foundation of China(21706132 and 21976093)Jiangsu Provincial Specially Appointed Professors Foundation,The Startup Foundation for Introducing Talent of NUIST.
文摘The efficient utilization of photocatalytic technology is essential for clean energy.Bismuth-based multimetal oxides(Bi_(2)WO_(6),Bi_(2)MoO_(6),BiVO_(4)and Bi_(4)Ti_(3)O_(12))have aroused widespread attention as a visible light responsive photocatalyst for hydrogen evolution due to their low cost,nontoxicity,modifiable morphology,and outstanding optical and chemical properties.Nevertheless,the photocatalytic activities of pure materials are unsatisfactory because of their relative small specific surface area,poor quantum yield,and the rapid recombination of photogenerated carriers.Therefore,some modification strategies,including morphological control,semiconductor combination,doping,and defect engineering,have been systematically studied to enhance photocatalytic H_(2)evolution activity in the past few years.Herein,we summarize the recent research progress on bismuth-based photocatalysts,pointing out the prospects,opportunities and challenges of bismuth-based photocatalysts.Eventually,we aims to put forward valuable suggestions for designing of bismuth-based photocatalysts applied in hydrogen production on the premise of consolidating the existing theoretical basis of photocatalysis.
文摘In recent years, interest in hydrogen as a fuel has sharply increased in the field of alternative and green energy due to its high energy capability and zero-emission behaviour. As a result, research in the development of new highly efficient methods for producing high-purity hydrogen is relevant. This paper presents, for the first time, the test results of an electrochemical cell with a proton-conducting La_(0.9)Sr_(0.1)ScO_(3-δ) electrolyte and symmetrical Sr_(1.95)Fe_(1.4)Ni_(0.1)Mo_(0.5)O_(6-δ)+ La_(0.9)Sr_(0.1)Sc_(0.9)Co_(0.1)O_(3-δ) electrodes as a hybrid setup for electricity generation in proton ceramic fuel cell mode, for hydrogen separation from H_(2)+ Ar mixture and the production of high-purity hydrogen from methane with simultaneous CO_(2) utilization.It was found that this electrochemical cell generates high flow rates of hydrogen during its separation through a proton-conducting membrane from H_(2)+ Ar mixture, about 500 cm^(3)h^(-1)cm^(-2)at a current density of 0.6 A cm^(-2)as well as about 370 cm^(3) h^(-1)cm^(-2)at a current density of 0.5 A cm^(-2) from CH_(4)+ CO_(2) mixture at 800 ℃ which shows that these cells are promising for hydrogen production.
基金the support from the Kyoto University and University of Malaya double degree programme to carry out this research
文摘Photocatalytic methane(CH_(4))production wherein CO_(2)is reduced to CH_(4) by utilizing solar radiation energy is gaining research and industrial focus because of its environmental-friendly notion.It offers twofold advantages:reduction in CO_(2)emission and production of artificial natural gas(methane)at the same time.In this paper,comparative energy,economic and environmental assessment of such photocatalytic methane production has been carried out between Japan and Malaysian conditions.Assumptions on the photocatalytic methane production plant and estimation of energy production,CO_(2)emission reduction,and economic indicators are made based on previous research and existing technologies.Energy analysis shows that Malaysia has a higher potential for energy production and CO_(2)emission reduction than Japan.Economic analysis reveals that the feasible reaction efficiencies of the plant in Japan and Malaysia are 8%.The slightly higher conversion efficiency in Malaysia is due to the energy price and CO_(2)tax.For the implementation of the photocatalytic methane production plant,the high energy price and CO_(2)tax will work as a driving force.
基金supports from the National Key R&D program of China(2019YFC1604602)supports from the National Key Basic Research Program of China(2019YFC1906700)the National Natural Science Foundation of China(21876049,51878643)。
文摘Electrochemical transformation emerges as an important solution to sustainable energy conversion and chemical production.Conventional electrolytic systems usually operate under galvanostatic or potentiostatic conditions that sometimes result in unsatisfactory efficiencies or selectivities.Pulse electrolysis by pulsating and programming the potentials/currents can feature unique tunability to the electrodeelectrolyte interface properties that can give rise to drastically different electrochemical behaviors compared to the steady-state counterparts.Although invented almost 100 years ago,pulse electrolysis has received little attention over the period,but has recently attracted a revived focus toward the energyefficient electrolysis.This review will summarize the history and recent efforts of pulse electrolysis in three categories:water electrolysis,CO_(2)electrolysis and other electrolysis.In each section,the advantage of pulse electrolysis over steady-state electrolysis will be discussed in detail,giving a comprehensive overview of the pulse effect on the electrolytic systems.Finally,we will provide our vision of future directions in pulse electrolysis based on previous works.
基金The National Key Research and Development Programs of China of the Ministry of Science and Technology under contract Nos 2020YFA0608301,2014CB441503the National Natural Science Foundation of China under contract Nos 41976042,41776122+1 种基金the Fundamental Research Funds for the Central Universitiesthe Taishan Scholars Program of Shandong Province,China。
文摘Quantifying the gross and net production is an essential component of carbon cycling and marine ecosystem studies.Triple oxygen isotope measurements and the O_(2)/Ar ratio are powerful indices in quantifying the gross primary production and net community production of the mixed layer zone,respectively.Although there is a substantial advantage in refining the gas exchange term and water column vertical mixing calibration,application of mixed layer depth history to the gas exchange term and its contribution to reducing indices error are unclear.Therefore,two cruises were conducted in the slope regions of the northern South China Sea in October 2014(autumn)and June 2015(spring).Discrete water samples at Station L07 in the upper 150 m depth were collected for the determination ofδ^(17)0,δ^(18)O,and the O_(2)/Ar ratio of dissolved gases.Gross oxygen production(GOP)was estimated using the triple oxygen isotopes of the dissolved O_(2),and net oxygen production(NOP)was calculated using O_(2)/Ar ratio and O_(2)concentration.The vertical mixing effect in NOP was calibrated via a N_(2)O based approach.GOP for autumn and spring was(169±23)mmol/(m^(2)·d)(by O_(2))and(189±26)mmol/(m^(2)·d)(by O_(2)),respectively.While NOP was 1.5 mmol/(m^(2)·d)(by O_(2))in autumn and 8.2 mmol/(m^(2)·d)(by O_(2))in spring.Application of mixed layer depth history in the gas flux parametrization reduced up to 9.5%error in the GOP and NOP estimations.A comparison with an independent O_(2)budget calculation in the diel observation indicated a26%overestimation in the current GOP,likely due to the vertical mixing effect.Both GOP and NOP in June were higher than those in October.Potential explanations for this include the occurrence of an eddy process in June,which may have exerted a submesoscale upwelling at the sampling station,and also the markedly higher terrestrial impact in June.
基金supported by the Natural Sciences and Engineering Research Council of Canada(NSERC)the China Scholarship Council(CSC,201708130079)。
文摘Coal fly ash(FA),a valuable industrial solid residue generated from coal combustion,is composed of various metal oxides and has a high thermal stability.Given that the coal-based energy will continue to account for a significant portion of global electricity generation in the coming years,the lack of effective management strategies exacerbates the threat of FA wastes to the surrounding environment and human health.For a sustainable development,green and renewable hydrogen economy and CO_(2)capture efforts provide appealing opportunities to valorize FA as catalysts and/or sorbents due to their appealing physicochemical properties.Hydrogen applications along with carbon neutrality are potential strategies to mitigate climate change crisis,but high processing costs(catalysts/sorbents)are challenging to realize this purpose.In this context,the utilization of FA not only enhances industrial competitiveness(by reducing manufacturing costs),but also provides ecologically friendly approaches to minimizing this solid waste.This state-of-the-art review highlights a wide-ranging outlook on the valorization of FA as catalysts and sorbents for hydrogen-rich gas production via conventional/intensified processes(CO_(2)/H_(2)O reforming,ammonia decomposition,hydride hydrolysis).The fundamental physicochemical characterizations and hazards/utilization of FA,which significantly affect the FA's utilization in various fields,are first introduced.The influence of several factors(like FA types and catalysis/sorption operation conditions)on the activity performance of FA-based materials is then discussed in detail.This critical review aims to open the window to further innovative ideas regarding the application of different FA residues in other catalytic and sorption processes.