The characteristics of the energy structure of rich coal,less oil and less gas,coupling with a high external dependence on oil and natural gas and the emphasis on the efficient and clean utilisation of coal,have broug...The characteristics of the energy structure of rich coal,less oil and less gas,coupling with a high external dependence on oil and natural gas and the emphasis on the efficient and clean utilisation of coal,have brought opportunities for coal chemical industry.However,with the large-scale popularisation of coal gasification technology,the production and resulting storage of coal gasification slag continue to increase,which not only result in serious environmental pollution and a waste of terrestrial resources,but also seriously affect the sustainable development of coal chemical enterprises.Hence,the treatment of coal gasification slag is extremely important.In this paper,the production,composition,morphology,particle size structure and water holding characteristics of coal gasification slag are introduced,and the methods of carbon ash separation of gasification slag,both domestically and abroad,are summarised.In addition,the paper also summarises the research progress on gasification slag in building materials,ecological restoration,residual carbon utilisation and other high-value utilisation,and ultimately puts forward the idea of the comprehensive utilisation of gasification slag.For large-scale consumption to solve the environmental problems of enterprises and achieve high-value utilisation to increase the economic benefits of enterprises,it is urgent to zealously design a reasonable and comprehensive utilisation technologies with simple operational processes,strong adaptability and economic benefits.展开更多
Active non-noble metal catalysts plays a decisive role for water electrolysis,however,the rational design and development of cost-efficient electrocatalysts with Pt/IrO2-like activity is still a challenging task.Herei...Active non-noble metal catalysts plays a decisive role for water electrolysis,however,the rational design and development of cost-efficient electrocatalysts with Pt/IrO2-like activity is still a challenging task.Herein,a facile one-step electrodeposition route in deep eutectic solvents(DESs) is developed for morphology-controllable synthesis of cobalt oxide/phosphate-carbon nano hybrids on nickel foam(CoPO@C/NF).A series of CoPO@C/NF nanostructures including cubes,octahedrons,microspheres and nanoflowers are synthesized,which show promising electrocatalytic properties toward oxygen and hydrogen evolution reactions(OER/HER).Such surface self-organized microstructure with accessible active sites make a significant contribution to the enhanced electrochemical activity,and hybridizing cobalt oxide with cobalt pyrophosphates and carbon can result in enhanced OER performance through synergistic catalysis.Among all nanostructures,the obtained microspherical CoPO@C/NF-3 catalyst exhibits excellent catalytic activities for OER and HER in 1.0 M KOH,affording an anodic current density of 10 mA cm^(-2) at overpotentials of 293 mV for OER and 93 mV for HER,with good long-time stability.This work offers a practical route for engineering the high-performance electrocatalysts towards efficient energy conversion and storage devices.展开更多
The crystallization has significant influence on fluidity of slag and slag discharge of entrained-flow-bed(EFB) gasifier. The crystallization characteristics and fluidity of five synthetic slags with different MgO/CaO...The crystallization has significant influence on fluidity of slag and slag discharge of entrained-flow-bed(EFB) gasifier. The crystallization characteristics and fluidity of five synthetic slags with different MgO/CaO ratios prepared on the basis of the range of oxide contents of Zhundong coal ash were investigated in this study. The results show that with the MgO/CaO ratio increase, the initial crystallization temperature increases, and the main temperature range of crystallization ratio growth moves to higher temperature range gradually which causes Tp25(Tp25is the temperature corresponding to the viscosity of 25 Pa·s)to increase. Mg-rich crystals are formed preferentially than Ca-rich crystals when adding the same amount of MgO and CaO during cooling. The effective slagging operating temperature range decrease from 217 ℃ for the slag with a 0:4 MgO/CaO ratio to 44 ℃ for the slag with a 4:0 MgO/CaO ratio with the MgO/CaO ratio increase. The slags with 2:2 and 1:3 MgO/CaO ratios show similar effective slagging operating temperature range, Tp25and the temperature corresponding to the viscosity of 2 Pa·s.However, compared with the slag with a 1:3 MgO/CaO ratio, the crystallization ratio and rate of slag with a 2:2 MgO/CaO ratio are lower within lower temperature range(1300–1200 ℃), causing its lower critical viscosity temperature and wider actual operating temperature range. Of the five slags, the widest effective slagging operating temperature range and the lowest Tp25of the slag with a 0:4 MgO/CaO ratio due to its low crystallization ratio, and wider actual operating temperature range of the slag with a 2:2 MgO/CaO ratio make the two slags suitable for slag discharge of EFB gasifier.展开更多
The present study aims to investigate the physico-chemical structural evolution characteristics of char structure of CO_(2) atmosphere torrefaction pretreated sludge with Yangchangwan bituminous coal(YC)during co-gasi...The present study aims to investigate the physico-chemical structural evolution characteristics of char structure of CO_(2) atmosphere torrefaction pretreated sludge with Yangchangwan bituminous coal(YC)during co-gasification.The co-gasification reactivity of torrefied sludge and YC was measured using a thermogravimetric analyzer.The co-gasification reactivity of torrefied sludge with YC was thoroughly explored in depth by in situ heating stage microscope coupled with traditional characterization means of char sample(Scanning electron microscope,nitrogen adsorption analyzer,laser Raman spectroscopy).The results show that the gasification reaction rate of sludge treated under CO_(2) atmosphere and coal blended char was better than other char samples at 1100–1200℃.The torrefied sludge under CO_(2) atmosphere promoted its thermal decomposition to the maximum extent,so that it eventually was transformed into a large number of small broken particles.The specific surface area and ID1/IG ratio of blended char of torrefied sludge under CO_(2) atmosphere and YC were 1.70 and 1.07 times higher than that of YC,respectively.The in situ technique revealed that YC char with the addition of torrefied sludge undergo gasification by shrinking core modes and the presence of obvious ash melting flow phenomenon.It was more obvious than that of YC.展开更多
The recovery and utilization of carbon dioxide(CO_(2))is the key to achieve the targets of peak carbon dioxide emissions and carbon neutrality.The Na-CO_(2)battery made with cheap alkali metal sodium and greenhouse ga...The recovery and utilization of carbon dioxide(CO_(2))is the key to achieve the targets of peak carbon dioxide emissions and carbon neutrality.The Na-CO_(2)battery made with cheap alkali metal sodium and greenhouse gas CO_(2)is an effective strategy to consume CO_(2)and store clean renewable energy.However,the liquid electrolyte volatilization in the open battery system and inevitable dendrite growth restrict the application of Na-CO_(2)batteries.In this work,magnesium-doped Na_(3)Zr_(2)Si_(2)PO_(12)(NZSP)was studied as a solid electrolyte for solid-state Na-CO_(2)batteries.The ionic conductivity of Na_(3.2)Zr_(1.9)Mg_(0.1)Si_(2)PO_(12)reaches 1.16 mS cm^(−1)at room temperature by replacing Zr ions in Na_(3.2)Zr_(1.9)Mg_(0.1)Si_(2)PO_(12)with Mg ions,and the structural changes are analyzed by neutron powder diffraction.The composite electrolyte consisting of highly conductive Na_(3.2)Zr_(1.9)Mg_(0.1)Si_(2)PO_(12)and high processability poly(vinylidene fluoride-co-hexafluoropropylene)(PVDF-HFP)is utilized for the first time to assemble a solid-state Na-CO_(2)battery.The cell shows a full discharge capacity of 7720 mAh g^(−1)at 200 mA g^(−1).The middle gap voltage is lower than 2 V after 120 cycles at 200 mA g^(−1)and at a cut-off capacity of 500 mAh g^(−1).This work demonstrates a promising strategy to design high-performance solid-state Na-CO_(2)batteries.展开更多
Designing efficient and long-lasting non-metal electrocatalysts is an urgent task for addressing the issue of kinetic hysteresis in electrochemical oxidation reactions.The bimetallic hydroxides,catalyzing the oxygen e...Designing efficient and long-lasting non-metal electrocatalysts is an urgent task for addressing the issue of kinetic hysteresis in electrochemical oxidation reactions.The bimetallic hydroxides,catalyzing the oxygen evolution reaction(OER),have significant research potential because hydroxide reconstruction to generate an active phase is a remarkable advantage.Herein,the complete reconstruction of ultrathin CoNi(OH)_(2) nanosheets was achieved by embedding Ag nanoparticles into the hydroxide to induce a spontaneous redox reaction(SRR),forming heterojunction Ag@CoNi(OH)_(2) for bifunctional hydrolysis.Theoretical calculations and in situ Raman and ex situ characterizations revealed that the inductive effect of the Ag cation redistributed the charge to promote phase transformation to highly activate Ag-modified hydroxides.The Co-Ni dual sites in Co/NiOOH serve as novel active sites for optimizing the intermediates,thereby weakening the barrier formed by OOH^*.Ag@CoNi(OH)_(2) required a potential of 1.55 V to drive water splitting at a current density of 10 mA cm^(-2),with nearly 98.6% Faraday efficiency.Through ion induction and triggering of electron regulation in the OER via the synergistic action of the heterogeneous interface and surface reconstruction,this strategic design can overcome the limited capacity of bimetallic hydroxides and bridge the gap between the basic theory and industrialization of water decomposition.展开更多
In this work,the coal samples from Hongshiwan(HSW)mining area,Ningxia,northwest of China,are characterized by using several modern materials characterization techniques,such as proximate and ultimate analyses,solid st...In this work,the coal samples from Hongshiwan(HSW)mining area,Ningxia,northwest of China,are characterized by using several modern materials characterization techniques,such as proximate and ultimate analyses,solid state 13C nuclear magnetic resonance(13C NMR),X-ray photoelectron spectroscopy and Fourier transform infrared spectroscopy(FT-IR).Then the key information about elements,valence,and chemical bonding for coal molecular structural construction is obtained.The results reveal that the main structure of HSW coal has 75.96%aromatic skeleton in mass.The ratio of aromatic bridge carbon to aromatic peripheral carbon of HSW coal is 0.315,indicating more naphthalene than benzene and anthracene in coal structures.Oxygen predominantly presents in the forms of ether(C–O),carbonyl(C=O)and carboxyl(–COO).Nitrogen presents in the forms of both pyridine and pyrrole.Methyl(–CH_(3))group is predominant in cyclic and aliphatic hydrocarbons.Based on obtained structural information and the approaches of average molecular structure,the single molecular formula of HSW coal is defined as C_(221)H_(148)O_(28)N_(2),with a molecular weight of 3142.32.Also,the 2D and 3D molecular model of HSW coal are built with computeraided modeling.The model is optimized and further verified by FT-IR and^(13)C NMR spectra simulation with quantum chemical calculations.Besides,a more complicated structure of complex model for HSW coal containing 10 single-molecules is also obtained.Therefore,molecular structure of HSW coal has been comprehensively depicted and understood at atomic level from both experimental and quantum chemical approaches in the current work.展开更多
Coal ash melting characteristics has a direct impact on the smooth operation of entrained gasifier.Mineral conversion of coal ash is very significant to be investigated,because the mineral can affect the melting tempe...Coal ash melting characteristics has a direct impact on the smooth operation of entrained gasifier.Mineral conversion of coal ash is very significant to be investigated,because the mineral can affect the melting temperature and viscosity under high temperature conditions.In this paper,the effects of different Al2O3/CaO on the mineral conversion,melting temperature and viscosity of Ningdong coal ash are studied by the combination of experiment and simulation.The trend of melting temperature decreases firstly and rises with increasing Al_(2)O_(3)/CaO.The ashmelting point reached to the lowestwhen the ratio is 1.23.XRD and Factsage software are used to analyze crystallization behavior of samples.The results showthat the content of anorthite,albite and corundumincreases and subsequently decreases,while the content of mullite decreases firstly and then rises with increasing Al_(2)O_(3)/CaO.High content with CaO can contribute to form albite and anorthite of low-melting.Besides,high content with Al_(2)O_(3) can tend to produce mullite of high-melting.The results of experimental and simulation are basically the same,which lays a foundation for the melting characteristics of Ningdong coal ash and can provide technical support for the smooth operation of the entrained-gasifier.展开更多
Metal–organic frameworks(MOFs)and layered double hydroxides(LDHs)have been considered to be one of the most promising and worthy hot spot materials to develop advanced catalysts for effi cient hydrogen evolution due ...Metal–organic frameworks(MOFs)and layered double hydroxides(LDHs)have been considered to be one of the most promising and worthy hot spot materials to develop advanced catalysts for effi cient hydrogen evolution due to their prominent characteristics,including unique structures,environmentally friendly nature,high redox activities,and homogeneously eff ective utilization of transition metal atoms.In this work,the delicate S-scheme heterojunction photocatalyst,CoAl LDH@Ni-MOF-74,was rationally designed and successfully constructed by coupling Ni-MOF-74 with CoAl LDH based on their peculiar structure,excellent electronic properties,and opposite surface potential for enhancing hydrogen generation activity under visible light irradiation.The CoAl LDH nanolayers evenly and dispersedly load on the surface of Ni-MOF-74.The CoAl LDH@Ni-MOF-74 exhibited higher photocatalytic hydrogen evolution activity compared with Ni-MOF-74 and CoAl LDH alone,mainly because the formation of the CoAl LDH@Ni-MOF-74 S-scheme heterojunction accelerated the recombination of several electrons(from conduction band(CB)of Ni-MOF-74)and holes(from valence band(VB)of CoAl LDH)and prevented the recombination of other electrons(from CB of CoAl LDH)and holes(from VB of Ni-MOF-74).展开更多
Chemical looping combustion(CLC)is an energy conversion technology with high efficiency and inherent separation of CO_(2).The existence of sulfur in coal may affect the CO_(2) purity and the performance of oxygen carr...Chemical looping combustion(CLC)is an energy conversion technology with high efficiency and inherent separation of CO_(2).The existence of sulfur in coal may affect the CO_(2) purity and the performance of oxygen carrier due to the interactions between sulfur contaminants and oxygen carrier.The migration of sulfur in Beisu coal during the in-situ gasification chemical looping combustion(i G-CLC)process using two oxygen carriers(iron ore and Cu O/Si O_(2))was investigated respectively.The thermodynamic analysis results showed the formation of metal sulfides was thermodynamically favored at low temperatures and low oxygen excess coefficients,while they were obviously inhibited and the production of SO_(2) was significantly promoted with an increase in temperature and oxygen excess coefficient.Moreover,part of sulfur was captured and fixed in the forms of alkali/alkaline earth metal sulfate due to the high amount of alkali/alkaline earth metal oxides in the coal ash or/and oxygen carrier.The experimental results showed that the sulfur in coal mainly released in the form of SO_(2),and the sulfur conversion efficiency(XS)in the reduction stage were 51.04%and 48.24%when using iron ore and Cu O/Si O_(2) respectively.The existence of metal sulfides was observed in the reduced oxygen carriers.The values of XSin the reoxidation process reached 3.80%and 7.64%when using iron ore and Cu O/Si O_(2) respectively.The residue and accumulation of sulfur were also found on the surfaces of two oxygen carriers.展开更多
In this study,the effect of ash removal on Shenfu bituminous coal was investigated.The coal was pretreated by hydrofluoric acid(HF)pickling,and the raw/pretreated coal chars were prepared at 900°C in a fixed bed ...In this study,the effect of ash removal on Shenfu bituminous coal was investigated.The coal was pretreated by hydrofluoric acid(HF)pickling,and the raw/pretreated coal chars were prepared at 900°C in a fixed bed reactor.The structure of coal and char were detected by Fourier transform infrared(FTIR)and Raman spectroscopy.The reactivity was tested in a thermogravimetric analyzer,including coal pyrolysis and char gasification.The reaction kinetics was analyzed through the Coats–Redfern method,master plots,the model-free and model-fitting method.The results show that the HF pickling can remove silicon from coal efficiently,and the macromolecular framework of coal is quite stable according to FTIR.The Raman parameters imply some carbonaceous structure on coal surface changed.For slow pyrolysis of coal,the effect of heating rate is considered.The changes of pyrolysis characteristics and kinetics are insignificant.For char gasification,the reactivity under isothermal and non-isothermal condition are discussed with an emphasis in different residence time of devolatilization process.In kinetic control region(low temperature),the activation energy(Ea)is very close(about 240 kJ/mol)for all chars.With the temperature increases,the reactivity of raw coal char is more easily suffered by diffusion.The random pore model is more suitable for the ash-free coal char,and the char with long residence time has a larger value of structural parameterψand smaller value of pre-exponential factor A.The Ea calculated by model-fitting and model-free method were in good agreement.展开更多
Due to the high salt content of coal chemical wastewater,pipeline fouling often occurs during wastewater treatment.Fouling will cause the diameter of the pipe to shrink or even block,which is not conducive to the safe...Due to the high salt content of coal chemical wastewater,pipeline fouling often occurs during wastewater treatment.Fouling will cause the diameter of the pipe to shrink or even block,which is not conducive to the safe and stable operation of the wastewater treatment process.In this paper,the experimental device was designed by using FLUENT software and the fouling deposition mechanisms at different flow velocities and different positions in a 90 deg bend were studied.The experimental results show that when the flow velocity is between 0.2 m·s^(-1) and 0.3 m·s^(-1),the thickness of fouling layer was positively correlated with the flow velocity;when the flow velocity is equal to 0.4 m·s^(-1),the formation of fouling is the most serious;when the flow velocity is between 0.4 m·s^(-1) and 0.7 m·s^(-1),the thickness of fouling layer was negative correlation with the flow velocity;with the increase of inlet velocity,the time for sediment point to develop into sediment surface is shortened.The fouling layer is easy to fall off because of the large shear force on the wall surface of the inner bend of the 90°elbow,so the density of sediment at this position is high.展开更多
Chemical looping gasification(CLG) of Ningdong coal by using Fe_(2) O_(3) as the oxygen carriers(OCs) was studied,and the gasification characteristics were obtained.A computation fluid dynamics(CFD) model based on Eul...Chemical looping gasification(CLG) of Ningdong coal by using Fe_(2) O_(3) as the oxygen carriers(OCs) was studied,and the gasification characteristics were obtained.A computation fluid dynamics(CFD) model based on Eulerian--Lagrangian multiphase framework was established,and a numerical simulation the coal chemical looping gasification processes in fuel reactor(FR) was investigated.In addition,the heterogeneous reactions,homogeneous reactions and Fe_(2) O_(3) oxygen carriers' reduction reactions were considered in the gasification process.The characteristics of gas flow and gasification in the FR were analyzed and it was found that the experiment results were consistent with the simulation values.The results show that when the O/C mole rate was 0.5:1,the gasification temperature was 900℃ and the water vapor volume flow rate was 2.2 ml·min^(-1),the mole fraction of syngas reached a maximum value of the experimental result and simulation value were 71.5% and 70.2%,respectively.When the O/C mole rate was 0.5:1,the gasification temperature was 900℃,and the water vapor volume flow was 1.8 ml·min^(-1);the gasification efficiency reached the maximum value was 62.2%,and the maximum carbon conversion rate was 84.0%.展开更多
The present study aims to explore the physico-chemical structure evolution characteristic during Yangchangwan bituminous coal(YCW)gasification in the presence of iron-based waste catalyst(IWC).The catalytic gasificati...The present study aims to explore the physico-chemical structure evolution characteristic during Yangchangwan bituminous coal(YCW)gasification in the presence of iron-based waste catalyst(IWC).The catalytic gasification reactivity of YCW was measured by thermogravimetric analyzer.Scanning electron microscope–energy dispersive system,nitrogen adsorption analyzer and laser Raman spectroscopy were employed to analyze the char physico-chemical properties.The results show that the optimal IWC loading ratio was 5 wt%at 1000°C.The distribution of IWC on char was uneven and Fe catalyst concentrated on the surface of some chars.The specific surface area of YCW gasified semi-char decreased significantly with the increase of gasification time.i.e.,the specific surface area reduced from 382 m2/g(0 min)to 192 m2/g(3 min),meanwhile,the number of micropores and mesopores decreased sharply at the late gasification stage.The carbon microcrystalline structure of YCW gasified semi-char was gradually destroyed with the increase of gasification time,and the microcrystalline structure with small size was gradually generated,resulting in the decreasing order degree of carbon microcrystalline structure.IWC can catalyze YCW gasification which could provide theoretical guidance for industrial solid waste recycling.展开更多
Coal,one of the fossil fuels which is burned for heat,contributes a quarter of the world’s primary energy and two-fifths of its electricity.According to the World Energy Model(WEM)provided by the International Energy...Coal,one of the fossil fuels which is burned for heat,contributes a quarter of the world’s primary energy and two-fifths of its electricity.According to the World Energy Model(WEM)provided by the International Energy Agency(IEA),the total primary energy demand from coal reached 3750 Mtoe in 2017,and its growth rate will decrease a lot in the future 10–20 years.Nevertheless,coal will remain as the main primary energy in the next few decades.展开更多
The slag composition corresponding to different coals varies significantly,which directly affects the operation of industrial entrained-flow gasifier and the service life of refractory bricks.In this study,the corrosi...The slag composition corresponding to different coals varies significantly,which directly affects the operation of industrial entrained-flow gasifier and the service life of refractory bricks.In this study,the corrosion resistance of several typical coal slags for gasification on high chromia refractory bricks was comparatively investigated by static laboratory crucible tests and thermodynamic simulations.The results demonstrated that the corrosion degree of high chromia refractory bricks by different coal slags was high-Ca/Na slag>high-Fe slag>high-Si/Al slag.The surface structure of the refractory was relatively flat after corrosion by high-Si/Al slag,and the primary corrosion reaction was the partial dissolution of the matrix by the slag.High-Fe slag was prone to the precipitation of iron phases as well as the formation of(Mg,Fe)(Al,Cr)_(2)O_(4)composite spinel layer at the slag/refractory interface.The high-Ca/Na slag was susceptible to react with the refractory to yield a low melting point phase,which led to the destruction of the matrix structure of the refractory and an isolated distribution of particles.In addition,the monoclinic ZrO_(2) in the refractory reacted with CaO in the slag to formed calcium zirconate,which loosened its phase toughening effect,was the primary factor that aggravated the refractory corrosion.展开更多
Catalytic hydrogenation of CO_(2) using renewable hydrogen not only reduces greenhouse gas emissions,but also provides industrial chemicals.Herein,a Co-Fe bimetallic catalyst was developed by a facile reactive ball-mi...Catalytic hydrogenation of CO_(2) using renewable hydrogen not only reduces greenhouse gas emissions,but also provides industrial chemicals.Herein,a Co-Fe bimetallic catalyst was developed by a facile reactive ball-milling method for highly active and selective hydrogenation of CO_(2) to value-added hydrocarbons.When reacted at 320℃,1.0 MPa and 9600 mL h^(-1) g_(cat)^(-1),the selectivity to light olefin(C_(2)^(=)-C_(4)^(=)) and C_(5)+ species achieves 57.3% and 22.3%,respectively,at a CO_(2) co nversion of 31.4%,which is superior to previous Fe-based catalysts.The CO_(2) activation can be promoted by the CoFe phase formed by reactive ball milling of the Fe-Co_(3)O_(4) mixture,and the in-situ Co_(2)C and Fe_(5)C_(2) formed during hydrogenation are beneficial for the C-C coupling reaction.The initial C-C coupling is related to the combination of CO species with the surface carbon of Fe/Co carbides,and the sustained C-C coupling is maintained by self-recovery of defective carbides.This new strategy contributes to the development of efficient catalysts for the hydrogenation of CO_(2) to value-added hydrocarbons.展开更多
Flexoelectric effect, referring to the strain gradient induced polarization, widely exists in dielectric materials, but its molecular dynamics has not been studied so much so far. In this work, the radial distribution...Flexoelectric effect, referring to the strain gradient induced polarization, widely exists in dielectric materials, but its molecular dynamics has not been studied so much so far. In this work, the radial distribution function of BaTiO_(3) and the phase transition temperatures have been investigated, and the results show that the core-shell potential model is effective and the structure of BaTiO_(3) is stable in a temperature range of 10 K–150 K. Molecular dynamics simulated hysteresis loops of BaTiO_(3) show that anisotropy can play an important role in the coercive field. Based on the rational simulation process,the effects of cantilever beam bent angle and fixed length on the polarization are analyzed. It is found that the small bent angle of the curved cantilever beam can give a proportional relationship with a fixed end length and a non-linear relationship is presented when the bent angle is much larger. The prediction of flexoelectric coefficient in BaTiO_(3) is 18.5 nC/m. This work provides a computational framework for the study of flexoelectric effect by using molecular dynamics.展开更多
With the rise of aqueous multivalent rechargeable batteries,inorganic-organic hybrid cathodes have attracted more and more attention due to the complement of each other’s advantages.Herein,a strategy of designing hyb...With the rise of aqueous multivalent rechargeable batteries,inorganic-organic hybrid cathodes have attracted more and more attention due to the complement of each other’s advantages.Herein,a strategy of designing hybrid cathode is adopted for high efficient aqueous zinc-ion batteries(AZIBs).Methylene blue(MB)intercalated vanadium oxide(HVO-MB)was synthesized through sol-gel and ion exchange method.Compared with other organic-inorganic intercalation cathode,not only can the MB intercalation enlarge the HVO interlayer spacing to improve ion mobility,but also provide coordination reactions with the Zn^(2+)to enhance the intrinsic electrochemical reaction kinetics of the hybrid electrode.As a key component for the cathode of AZIBs,HVO-MB contributes a specific capacity of 418 mA h g^(-1) at 0.1 A g^(-1),high rate capability(243 mA h g^(-1) at 5 A g^(-1))and extraordinary stability(88%of capacity retention after 2000cycles at a high current density of 5 A g^(-1))in 3 M Zn(CF_(3)SO_(3))_(2) aqueous electrolyte.The electrochemical kinetics reveals HVO-MB characterized with large pseudocapacitance charge storage behavior due to the fast ion migration provided by the coordination reaction and expanded interlayer distance.Furthermore,a mixed energy storage mechanism involving Zn^(2+)insertion and coordination reaction is confirmed by various ex-situ characterization.Thus,this work opens up a new path for constructing the high performance cathode of AZIBs through organic-inorganic hybridization.展开更多
Water-splitting reactions such as the hydrogen evolution reaction(HER)and the oxygen evolution reaction(OER)typically require expensive noble metal-based electrocatalysts.This has motivated researchers to develop nove...Water-splitting reactions such as the hydrogen evolution reaction(HER)and the oxygen evolution reaction(OER)typically require expensive noble metal-based electrocatalysts.This has motivated researchers to develop novel,cost-effective electrocatalytic systems.In this study,a new multicomponent nanocomposite was assembled by combining functionalized multiwalled carbon nanotubes,a Cu-based metal–organic framework(MOF)(HKUST-1 or HK),and a sulfidized NiMn-layered double hydroxide(NiMn-S).The resulting nanocomposite,abbreviated as MW/HK/NiMn-S,features a unique architecture,high porosity,numerous electroactive Cu/Ni/Mn sites,fast charge transfer,excellent structural stability,and conductivity.At a current density of 10 mA cm-2,this dual-function electrocatalyst shows remarkable performance,with ultralow overpotential values of 163 mV(OER)or 73 mV(HER),as well as low Tafel slopes(57 and 75 mV dec-1,respectively).Additionally,its high turnover frequency values(4.43 s-1 for OER;3.96 s-1 for HER)are significantly superior to those of standard noble metal-based Pt/C and IrO2 systems.The synergistic effect of the nanocomposite's different components is responsible for its enhanced electrocatalytic performance.A density functional theory study revealed that the multi-interface and multicomponent heterostructure contribute to increased electrical conductivity and decreased energy barrier,resulting in superior electrocatalytic HER/OER activity.This study presents a novel vision for designing advanced electrocatalysts with superior performance in water splitting.Various composites have been utilized in water-splitting applications.This study investigates the use of the MW/HK/NiMn-S electrocatalyst for water splitting for the first time to indicate the synergistic effect between carbon-based materials along with layered double hydroxide compounds and porous compounds of MOF.The unique features of each component in this composite can be an interesting topic in the field of water splitting.展开更多
基金financially supported by the National Key Research and Development Program of China(2019YFC1904302)Foundation of State Key Laboratory of High-efficiency Utilisation of Coal and Green Chemical Engineering(2021-K81)the Technology of Coal-to-liquids Research Institute of National Energy Group([2020]010)。
文摘The characteristics of the energy structure of rich coal,less oil and less gas,coupling with a high external dependence on oil and natural gas and the emphasis on the efficient and clean utilisation of coal,have brought opportunities for coal chemical industry.However,with the large-scale popularisation of coal gasification technology,the production and resulting storage of coal gasification slag continue to increase,which not only result in serious environmental pollution and a waste of terrestrial resources,but also seriously affect the sustainable development of coal chemical enterprises.Hence,the treatment of coal gasification slag is extremely important.In this paper,the production,composition,morphology,particle size structure and water holding characteristics of coal gasification slag are introduced,and the methods of carbon ash separation of gasification slag,both domestically and abroad,are summarised.In addition,the paper also summarises the research progress on gasification slag in building materials,ecological restoration,residual carbon utilisation and other high-value utilisation,and ultimately puts forward the idea of the comprehensive utilisation of gasification slag.For large-scale consumption to solve the environmental problems of enterprises and achieve high-value utilisation to increase the economic benefits of enterprises,it is urgent to zealously design a reasonable and comprehensive utilisation technologies with simple operational processes,strong adaptability and economic benefits.
基金supported by the National Natural Science Foundation of China (21421001, 21875118)the Natural Science Foundation of Xinjiang Autonomous Region (2016D01A009)+1 种基金the 111 project (B12015)the Foundation of State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering (2020-KF-22)。
文摘Active non-noble metal catalysts plays a decisive role for water electrolysis,however,the rational design and development of cost-efficient electrocatalysts with Pt/IrO2-like activity is still a challenging task.Herein,a facile one-step electrodeposition route in deep eutectic solvents(DESs) is developed for morphology-controllable synthesis of cobalt oxide/phosphate-carbon nano hybrids on nickel foam(CoPO@C/NF).A series of CoPO@C/NF nanostructures including cubes,octahedrons,microspheres and nanoflowers are synthesized,which show promising electrocatalytic properties toward oxygen and hydrogen evolution reactions(OER/HER).Such surface self-organized microstructure with accessible active sites make a significant contribution to the enhanced electrochemical activity,and hybridizing cobalt oxide with cobalt pyrophosphates and carbon can result in enhanced OER performance through synergistic catalysis.Among all nanostructures,the obtained microspherical CoPO@C/NF-3 catalyst exhibits excellent catalytic activities for OER and HER in 1.0 M KOH,affording an anodic current density of 10 mA cm^(-2) at overpotentials of 293 mV for OER and 93 mV for HER,with good long-time stability.This work offers a practical route for engineering the high-performance electrocatalysts towards efficient energy conversion and storage devices.
基金supported by the National Natural Science Foundation of China(21878082).
文摘The crystallization has significant influence on fluidity of slag and slag discharge of entrained-flow-bed(EFB) gasifier. The crystallization characteristics and fluidity of five synthetic slags with different MgO/CaO ratios prepared on the basis of the range of oxide contents of Zhundong coal ash were investigated in this study. The results show that with the MgO/CaO ratio increase, the initial crystallization temperature increases, and the main temperature range of crystallization ratio growth moves to higher temperature range gradually which causes Tp25(Tp25is the temperature corresponding to the viscosity of 25 Pa·s)to increase. Mg-rich crystals are formed preferentially than Ca-rich crystals when adding the same amount of MgO and CaO during cooling. The effective slagging operating temperature range decrease from 217 ℃ for the slag with a 0:4 MgO/CaO ratio to 44 ℃ for the slag with a 4:0 MgO/CaO ratio with the MgO/CaO ratio increase. The slags with 2:2 and 1:3 MgO/CaO ratios show similar effective slagging operating temperature range, Tp25and the temperature corresponding to the viscosity of 2 Pa·s.However, compared with the slag with a 1:3 MgO/CaO ratio, the crystallization ratio and rate of slag with a 2:2 MgO/CaO ratio are lower within lower temperature range(1300–1200 ℃), causing its lower critical viscosity temperature and wider actual operating temperature range. Of the five slags, the widest effective slagging operating temperature range and the lowest Tp25of the slag with a 0:4 MgO/CaO ratio due to its low crystallization ratio, and wider actual operating temperature range of the slag with a 2:2 MgO/CaO ratio make the two slags suitable for slag discharge of EFB gasifier.
基金supported by the Scientific Research Fund Project of Yunnan Provincial Department of Education(2022J0756)the National Natural Science Foundation of China(32260321,21968024).
文摘The present study aims to investigate the physico-chemical structural evolution characteristics of char structure of CO_(2) atmosphere torrefaction pretreated sludge with Yangchangwan bituminous coal(YC)during co-gasification.The co-gasification reactivity of torrefied sludge and YC was measured using a thermogravimetric analyzer.The co-gasification reactivity of torrefied sludge with YC was thoroughly explored in depth by in situ heating stage microscope coupled with traditional characterization means of char sample(Scanning electron microscope,nitrogen adsorption analyzer,laser Raman spectroscopy).The results show that the gasification reaction rate of sludge treated under CO_(2) atmosphere and coal blended char was better than other char samples at 1100–1200℃.The torrefied sludge under CO_(2) atmosphere promoted its thermal decomposition to the maximum extent,so that it eventually was transformed into a large number of small broken particles.The specific surface area and ID1/IG ratio of blended char of torrefied sludge under CO_(2) atmosphere and YC were 1.70 and 1.07 times higher than that of YC,respectively.The in situ technique revealed that YC char with the addition of torrefied sludge undergo gasification by shrinking core modes and the presence of obvious ash melting flow phenomenon.It was more obvious than that of YC.
基金supported by Foundation of State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering(Grant No.2022-K15)China University of Mining&Technology(Beijing),Beijing National Laboratory for Condensed Matter Physics,and the National Natural Science Foundation of China(No.51672029 and 51372271)the Spanish Ministry of Science,Innovation to the project MAT2017-84496-R.CAL acknowledges ANPCyT,UNSL for financial support(projects PICT2017-1842,PROICO 2-2016),Argentine.
文摘The recovery and utilization of carbon dioxide(CO_(2))is the key to achieve the targets of peak carbon dioxide emissions and carbon neutrality.The Na-CO_(2)battery made with cheap alkali metal sodium and greenhouse gas CO_(2)is an effective strategy to consume CO_(2)and store clean renewable energy.However,the liquid electrolyte volatilization in the open battery system and inevitable dendrite growth restrict the application of Na-CO_(2)batteries.In this work,magnesium-doped Na_(3)Zr_(2)Si_(2)PO_(12)(NZSP)was studied as a solid electrolyte for solid-state Na-CO_(2)batteries.The ionic conductivity of Na_(3.2)Zr_(1.9)Mg_(0.1)Si_(2)PO_(12)reaches 1.16 mS cm^(−1)at room temperature by replacing Zr ions in Na_(3.2)Zr_(1.9)Mg_(0.1)Si_(2)PO_(12)with Mg ions,and the structural changes are analyzed by neutron powder diffraction.The composite electrolyte consisting of highly conductive Na_(3.2)Zr_(1.9)Mg_(0.1)Si_(2)PO_(12)and high processability poly(vinylidene fluoride-co-hexafluoropropylene)(PVDF-HFP)is utilized for the first time to assemble a solid-state Na-CO_(2)battery.The cell shows a full discharge capacity of 7720 mAh g^(−1)at 200 mA g^(−1).The middle gap voltage is lower than 2 V after 120 cycles at 200 mA g^(−1)and at a cut-off capacity of 500 mAh g^(−1).This work demonstrates a promising strategy to design high-performance solid-state Na-CO_(2)batteries.
基金supported by the Inner Mongolia R&D Program Plan(2021ZD0042,2021EEDSCXSFQZD006)the National Natural Science Foundation of China(21902123)the Natural Science Basic Research Program of Shaanxi(2023-JC-ZD-22)。
文摘Designing efficient and long-lasting non-metal electrocatalysts is an urgent task for addressing the issue of kinetic hysteresis in electrochemical oxidation reactions.The bimetallic hydroxides,catalyzing the oxygen evolution reaction(OER),have significant research potential because hydroxide reconstruction to generate an active phase is a remarkable advantage.Herein,the complete reconstruction of ultrathin CoNi(OH)_(2) nanosheets was achieved by embedding Ag nanoparticles into the hydroxide to induce a spontaneous redox reaction(SRR),forming heterojunction Ag@CoNi(OH)_(2) for bifunctional hydrolysis.Theoretical calculations and in situ Raman and ex situ characterizations revealed that the inductive effect of the Ag cation redistributed the charge to promote phase transformation to highly activate Ag-modified hydroxides.The Co-Ni dual sites in Co/NiOOH serve as novel active sites for optimizing the intermediates,thereby weakening the barrier formed by OOH^*.Ag@CoNi(OH)_(2) required a potential of 1.55 V to drive water splitting at a current density of 10 mA cm^(-2),with nearly 98.6% Faraday efficiency.Through ion induction and triggering of electron regulation in the OER via the synergistic action of the heterogeneous interface and surface reconstruction,this strategic design can overcome the limited capacity of bimetallic hydroxides and bridge the gap between the basic theory and industrialization of water decomposition.
基金by Ningxia Higher Educational Program for Excellent Youth(No.NGY2016064).H.Bai also thanks the financial supports from Key R&D Projects of Ningxia(No.2018BCE01002)National Academic Subjects Construction Project of Ningxia(Chemical Engineering and Technology,NXYLXK2017A04).
文摘In this work,the coal samples from Hongshiwan(HSW)mining area,Ningxia,northwest of China,are characterized by using several modern materials characterization techniques,such as proximate and ultimate analyses,solid state 13C nuclear magnetic resonance(13C NMR),X-ray photoelectron spectroscopy and Fourier transform infrared spectroscopy(FT-IR).Then the key information about elements,valence,and chemical bonding for coal molecular structural construction is obtained.The results reveal that the main structure of HSW coal has 75.96%aromatic skeleton in mass.The ratio of aromatic bridge carbon to aromatic peripheral carbon of HSW coal is 0.315,indicating more naphthalene than benzene and anthracene in coal structures.Oxygen predominantly presents in the forms of ether(C–O),carbonyl(C=O)and carboxyl(–COO).Nitrogen presents in the forms of both pyridine and pyrrole.Methyl(–CH_(3))group is predominant in cyclic and aliphatic hydrocarbons.Based on obtained structural information and the approaches of average molecular structure,the single molecular formula of HSW coal is defined as C_(221)H_(148)O_(28)N_(2),with a molecular weight of 3142.32.Also,the 2D and 3D molecular model of HSW coal are built with computeraided modeling.The model is optimized and further verified by FT-IR and^(13)C NMR spectra simulation with quantum chemical calculations.Besides,a more complicated structure of complex model for HSW coal containing 10 single-molecules is also obtained.Therefore,molecular structure of HSW coal has been comprehensively depicted and understood at atomic level from both experimental and quantum chemical approaches in the current work.
基金supported by the Key Research and Development Program of Ningxia(2018BCE01004)Natural Science Foundation of Ningxia(2018AAC03013)Discipline Project of Ningxia(NXYLXK2017A04).
文摘Coal ash melting characteristics has a direct impact on the smooth operation of entrained gasifier.Mineral conversion of coal ash is very significant to be investigated,because the mineral can affect the melting temperature and viscosity under high temperature conditions.In this paper,the effects of different Al2O3/CaO on the mineral conversion,melting temperature and viscosity of Ningdong coal ash are studied by the combination of experiment and simulation.The trend of melting temperature decreases firstly and rises with increasing Al_(2)O_(3)/CaO.The ashmelting point reached to the lowestwhen the ratio is 1.23.XRD and Factsage software are used to analyze crystallization behavior of samples.The results showthat the content of anorthite,albite and corundumincreases and subsequently decreases,while the content of mullite decreases firstly and then rises with increasing Al_(2)O_(3)/CaO.High content with CaO can contribute to form albite and anorthite of low-melting.Besides,high content with Al_(2)O_(3) can tend to produce mullite of high-melting.The results of experimental and simulation are basically the same,which lays a foundation for the melting characteristics of Ningdong coal ash and can provide technical support for the smooth operation of the entrained-gasifier.
基金This work was financially supported by the Natural Science Foundation of the Ningxia Hui Autonomous Region(No.2020AAC02026).
文摘Metal–organic frameworks(MOFs)and layered double hydroxides(LDHs)have been considered to be one of the most promising and worthy hot spot materials to develop advanced catalysts for effi cient hydrogen evolution due to their prominent characteristics,including unique structures,environmentally friendly nature,high redox activities,and homogeneously eff ective utilization of transition metal atoms.In this work,the delicate S-scheme heterojunction photocatalyst,CoAl LDH@Ni-MOF-74,was rationally designed and successfully constructed by coupling Ni-MOF-74 with CoAl LDH based on their peculiar structure,excellent electronic properties,and opposite surface potential for enhancing hydrogen generation activity under visible light irradiation.The CoAl LDH nanolayers evenly and dispersedly load on the surface of Ni-MOF-74.The CoAl LDH@Ni-MOF-74 exhibited higher photocatalytic hydrogen evolution activity compared with Ni-MOF-74 and CoAl LDH alone,mainly because the formation of the CoAl LDH@Ni-MOF-74 S-scheme heterojunction accelerated the recombination of several electrons(from conduction band(CB)of Ni-MOF-74)and holes(from valence band(VB)of CoAl LDH)and prevented the recombination of other electrons(from CB of CoAl LDH)and holes(from VB of Ni-MOF-74).
基金supported by the National Natural Science Foundation of China(51606087)Start-Up Foundation of Jiangsu University(15JDG157)Foundation of State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering(2020-KF-07)。
文摘Chemical looping combustion(CLC)is an energy conversion technology with high efficiency and inherent separation of CO_(2).The existence of sulfur in coal may affect the CO_(2) purity and the performance of oxygen carrier due to the interactions between sulfur contaminants and oxygen carrier.The migration of sulfur in Beisu coal during the in-situ gasification chemical looping combustion(i G-CLC)process using two oxygen carriers(iron ore and Cu O/Si O_(2))was investigated respectively.The thermodynamic analysis results showed the formation of metal sulfides was thermodynamically favored at low temperatures and low oxygen excess coefficients,while they were obviously inhibited and the production of SO_(2) was significantly promoted with an increase in temperature and oxygen excess coefficient.Moreover,part of sulfur was captured and fixed in the forms of alkali/alkaline earth metal sulfate due to the high amount of alkali/alkaline earth metal oxides in the coal ash or/and oxygen carrier.The experimental results showed that the sulfur in coal mainly released in the form of SO_(2),and the sulfur conversion efficiency(XS)in the reduction stage were 51.04%and 48.24%when using iron ore and Cu O/Si O_(2) respectively.The existence of metal sulfides was observed in the reduced oxygen carriers.The values of XSin the reoxidation process reached 3.80%and 7.64%when using iron ore and Cu O/Si O_(2) respectively.The residue and accumulation of sulfur were also found on the surfaces of two oxygen carriers.
基金This work was supported by National Key R&D Program of China(2017YFB0602601)National Natural Science Foundation of China(21878093).
文摘In this study,the effect of ash removal on Shenfu bituminous coal was investigated.The coal was pretreated by hydrofluoric acid(HF)pickling,and the raw/pretreated coal chars were prepared at 900°C in a fixed bed reactor.The structure of coal and char were detected by Fourier transform infrared(FTIR)and Raman spectroscopy.The reactivity was tested in a thermogravimetric analyzer,including coal pyrolysis and char gasification.The reaction kinetics was analyzed through the Coats–Redfern method,master plots,the model-free and model-fitting method.The results show that the HF pickling can remove silicon from coal efficiently,and the macromolecular framework of coal is quite stable according to FTIR.The Raman parameters imply some carbonaceous structure on coal surface changed.For slow pyrolysis of coal,the effect of heating rate is considered.The changes of pyrolysis characteristics and kinetics are insignificant.For char gasification,the reactivity under isothermal and non-isothermal condition are discussed with an emphasis in different residence time of devolatilization process.In kinetic control region(low temperature),the activation energy(Ea)is very close(about 240 kJ/mol)for all chars.With the temperature increases,the reactivity of raw coal char is more easily suffered by diffusion.The random pore model is more suitable for the ash-free coal char,and the char with long residence time has a larger value of structural parameterψand smaller value of pre-exponential factor A.The Ea calculated by model-fitting and model-free method were in good agreement.
基金financially supported by the Natural Science Foundation of Ningxia Hui Autonomous Region(2020AAC03025)Undergraduate Training Programs for Innovation(2019107490001)+1 种基金East-West Cooperation Project of Ningxia Key R&D Plan(2017BY064)National First-rate Discipline Construction Project of Ningxia(NXYLXK2017A04)。
文摘Due to the high salt content of coal chemical wastewater,pipeline fouling often occurs during wastewater treatment.Fouling will cause the diameter of the pipe to shrink or even block,which is not conducive to the safe and stable operation of the wastewater treatment process.In this paper,the experimental device was designed by using FLUENT software and the fouling deposition mechanisms at different flow velocities and different positions in a 90 deg bend were studied.The experimental results show that when the flow velocity is between 0.2 m·s^(-1) and 0.3 m·s^(-1),the thickness of fouling layer was positively correlated with the flow velocity;when the flow velocity is equal to 0.4 m·s^(-1),the formation of fouling is the most serious;when the flow velocity is between 0.4 m·s^(-1) and 0.7 m·s^(-1),the thickness of fouling layer was negative correlation with the flow velocity;with the increase of inlet velocity,the time for sediment point to develop into sediment surface is shortened.The fouling layer is easy to fall off because of the large shear force on the wall surface of the inner bend of the 90°elbow,so the density of sediment at this position is high.
基金supported by the Key Research and Development Program of Ningxia (2018 BCE01002)the Discipline Project of Ningxia (NXYLXK2017A04)。
文摘Chemical looping gasification(CLG) of Ningdong coal by using Fe_(2) O_(3) as the oxygen carriers(OCs) was studied,and the gasification characteristics were obtained.A computation fluid dynamics(CFD) model based on Eulerian--Lagrangian multiphase framework was established,and a numerical simulation the coal chemical looping gasification processes in fuel reactor(FR) was investigated.In addition,the heterogeneous reactions,homogeneous reactions and Fe_(2) O_(3) oxygen carriers' reduction reactions were considered in the gasification process.The characteristics of gas flow and gasification in the FR were analyzed and it was found that the experiment results were consistent with the simulation values.The results show that when the O/C mole rate was 0.5:1,the gasification temperature was 900℃ and the water vapor volume flow rate was 2.2 ml·min^(-1),the mole fraction of syngas reached a maximum value of the experimental result and simulation value were 71.5% and 70.2%,respectively.When the O/C mole rate was 0.5:1,the gasification temperature was 900℃,and the water vapor volume flow was 1.8 ml·min^(-1);the gasification efficiency reached the maximum value was 62.2%,and the maximum carbon conversion rate was 84.0%.
基金The present work was supported by the National Natural Science Foundation of China (21968024)the Project of Key Research Plan of Ningxia (2019BCH01001)The authors also gratefully thank Professor Junzhuo Fang for his help in taking SEM–EDS photos.
文摘The present study aims to explore the physico-chemical structure evolution characteristic during Yangchangwan bituminous coal(YCW)gasification in the presence of iron-based waste catalyst(IWC).The catalytic gasification reactivity of YCW was measured by thermogravimetric analyzer.Scanning electron microscope–energy dispersive system,nitrogen adsorption analyzer and laser Raman spectroscopy were employed to analyze the char physico-chemical properties.The results show that the optimal IWC loading ratio was 5 wt%at 1000°C.The distribution of IWC on char was uneven and Fe catalyst concentrated on the surface of some chars.The specific surface area of YCW gasified semi-char decreased significantly with the increase of gasification time.i.e.,the specific surface area reduced from 382 m2/g(0 min)to 192 m2/g(3 min),meanwhile,the number of micropores and mesopores decreased sharply at the late gasification stage.The carbon microcrystalline structure of YCW gasified semi-char was gradually destroyed with the increase of gasification time,and the microcrystalline structure with small size was gradually generated,resulting in the decreasing order degree of carbon microcrystalline structure.IWC can catalyze YCW gasification which could provide theoretical guidance for industrial solid waste recycling.
文摘Coal,one of the fossil fuels which is burned for heat,contributes a quarter of the world’s primary energy and two-fifths of its electricity.According to the World Energy Model(WEM)provided by the International Energy Agency(IEA),the total primary energy demand from coal reached 3750 Mtoe in 2017,and its growth rate will decrease a lot in the future 10–20 years.Nevertheless,coal will remain as the main primary energy in the next few decades.
基金financial support from the Joint Funds of the National Natural Science Foundation of China(U21A20318).
文摘The slag composition corresponding to different coals varies significantly,which directly affects the operation of industrial entrained-flow gasifier and the service life of refractory bricks.In this study,the corrosion resistance of several typical coal slags for gasification on high chromia refractory bricks was comparatively investigated by static laboratory crucible tests and thermodynamic simulations.The results demonstrated that the corrosion degree of high chromia refractory bricks by different coal slags was high-Ca/Na slag>high-Fe slag>high-Si/Al slag.The surface structure of the refractory was relatively flat after corrosion by high-Si/Al slag,and the primary corrosion reaction was the partial dissolution of the matrix by the slag.High-Fe slag was prone to the precipitation of iron phases as well as the formation of(Mg,Fe)(Al,Cr)_(2)O_(4)composite spinel layer at the slag/refractory interface.The high-Ca/Na slag was susceptible to react with the refractory to yield a low melting point phase,which led to the destruction of the matrix structure of the refractory and an isolated distribution of particles.In addition,the monoclinic ZrO_(2) in the refractory reacted with CaO in the slag to formed calcium zirconate,which loosened its phase toughening effect,was the primary factor that aggravated the refractory corrosion.
基金supported by the National Natural Science Foundation of China (22008098, 21978156, 42002040)the Program for Innovative Research Team (in Science and Technology) in University of Henan Province (21IRTSTHN004)+1 种基金the Program for Science & Technology Innovation Talents in Universities of Henan Province (22HASTIT008)the Foundation of State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering (2022-K34)。
文摘Catalytic hydrogenation of CO_(2) using renewable hydrogen not only reduces greenhouse gas emissions,but also provides industrial chemicals.Herein,a Co-Fe bimetallic catalyst was developed by a facile reactive ball-milling method for highly active and selective hydrogenation of CO_(2) to value-added hydrocarbons.When reacted at 320℃,1.0 MPa and 9600 mL h^(-1) g_(cat)^(-1),the selectivity to light olefin(C_(2)^(=)-C_(4)^(=)) and C_(5)+ species achieves 57.3% and 22.3%,respectively,at a CO_(2) co nversion of 31.4%,which is superior to previous Fe-based catalysts.The CO_(2) activation can be promoted by the CoFe phase formed by reactive ball milling of the Fe-Co_(3)O_(4) mixture,and the in-situ Co_(2)C and Fe_(5)C_(2) formed during hydrogenation are beneficial for the C-C coupling reaction.The initial C-C coupling is related to the combination of CO species with the surface carbon of Fe/Co carbides,and the sustained C-C coupling is maintained by self-recovery of defective carbides.This new strategy contributes to the development of efficient catalysts for the hydrogenation of CO_(2) to value-added hydrocarbons.
基金Project supported by the Natural Science Funds of Ningxia,China (Grant No.ZR1221)the National Natural Science Foundation of China (Grant No.11964027)。
文摘Flexoelectric effect, referring to the strain gradient induced polarization, widely exists in dielectric materials, but its molecular dynamics has not been studied so much so far. In this work, the radial distribution function of BaTiO_(3) and the phase transition temperatures have been investigated, and the results show that the core-shell potential model is effective and the structure of BaTiO_(3) is stable in a temperature range of 10 K–150 K. Molecular dynamics simulated hysteresis loops of BaTiO_(3) show that anisotropy can play an important role in the coercive field. Based on the rational simulation process,the effects of cantilever beam bent angle and fixed length on the polarization are analyzed. It is found that the small bent angle of the curved cantilever beam can give a proportional relationship with a fixed end length and a non-linear relationship is presented when the bent angle is much larger. The prediction of flexoelectric coefficient in BaTiO_(3) is 18.5 nC/m. This work provides a computational framework for the study of flexoelectric effect by using molecular dynamics.
基金supported by the National Natural Science Foundation of China(21965027 and 22065030)the Natural Science Foundation of Ningxia Province(2022AAC03109)the National First-rate Discipline Construction Project of Ningxia:Chemical Engineering and Technology(NXY-LXK2017A04)。
文摘With the rise of aqueous multivalent rechargeable batteries,inorganic-organic hybrid cathodes have attracted more and more attention due to the complement of each other’s advantages.Herein,a strategy of designing hybrid cathode is adopted for high efficient aqueous zinc-ion batteries(AZIBs).Methylene blue(MB)intercalated vanadium oxide(HVO-MB)was synthesized through sol-gel and ion exchange method.Compared with other organic-inorganic intercalation cathode,not only can the MB intercalation enlarge the HVO interlayer spacing to improve ion mobility,but also provide coordination reactions with the Zn^(2+)to enhance the intrinsic electrochemical reaction kinetics of the hybrid electrode.As a key component for the cathode of AZIBs,HVO-MB contributes a specific capacity of 418 mA h g^(-1) at 0.1 A g^(-1),high rate capability(243 mA h g^(-1) at 5 A g^(-1))and extraordinary stability(88%of capacity retention after 2000cycles at a high current density of 5 A g^(-1))in 3 M Zn(CF_(3)SO_(3))_(2) aqueous electrolyte.The electrochemical kinetics reveals HVO-MB characterized with large pseudocapacitance charge storage behavior due to the fast ion migration provided by the coordination reaction and expanded interlayer distance.Furthermore,a mixed energy storage mechanism involving Zn^(2+)insertion and coordination reaction is confirmed by various ex-situ characterization.Thus,this work opens up a new path for constructing the high performance cathode of AZIBs through organic-inorganic hybridization.
基金Iran National Science Foundation(INSF)under project No.4025105the Foundation of State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering(Grant No.2022-K31)+1 种基金the Zhejiang Province Key Research and Development Project(2023 C01191)Alexander M.Kirillov acknowledges the Foundation for Science and Technology(LISBOA-01-0145-FEDER-029697,PTDC/QUIQIN/3898/2020,LA/P/0056/2020,UIDB/00100/2020).
文摘Water-splitting reactions such as the hydrogen evolution reaction(HER)and the oxygen evolution reaction(OER)typically require expensive noble metal-based electrocatalysts.This has motivated researchers to develop novel,cost-effective electrocatalytic systems.In this study,a new multicomponent nanocomposite was assembled by combining functionalized multiwalled carbon nanotubes,a Cu-based metal–organic framework(MOF)(HKUST-1 or HK),and a sulfidized NiMn-layered double hydroxide(NiMn-S).The resulting nanocomposite,abbreviated as MW/HK/NiMn-S,features a unique architecture,high porosity,numerous electroactive Cu/Ni/Mn sites,fast charge transfer,excellent structural stability,and conductivity.At a current density of 10 mA cm-2,this dual-function electrocatalyst shows remarkable performance,with ultralow overpotential values of 163 mV(OER)or 73 mV(HER),as well as low Tafel slopes(57 and 75 mV dec-1,respectively).Additionally,its high turnover frequency values(4.43 s-1 for OER;3.96 s-1 for HER)are significantly superior to those of standard noble metal-based Pt/C and IrO2 systems.The synergistic effect of the nanocomposite's different components is responsible for its enhanced electrocatalytic performance.A density functional theory study revealed that the multi-interface and multicomponent heterostructure contribute to increased electrical conductivity and decreased energy barrier,resulting in superior electrocatalytic HER/OER activity.This study presents a novel vision for designing advanced electrocatalysts with superior performance in water splitting.Various composites have been utilized in water-splitting applications.This study investigates the use of the MW/HK/NiMn-S electrocatalyst for water splitting for the first time to indicate the synergistic effect between carbon-based materials along with layered double hydroxide compounds and porous compounds of MOF.The unique features of each component in this composite can be an interesting topic in the field of water splitting.