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Mo_(2)B_(2)O_(2) MBene for Efficient Electrochemical CO Reduction to C_(2) Chemicals:Computational Exploration
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作者 Bikun Zhang Jianwen Jiang 《Energy & Environmental Materials》 SCIE EI CAS CSCD 2024年第6期342-350,共9页
Emerging as a new class of two-dimensional materials with atomically thin layers,MBenes have great potential for many important applications such as energy storage and electrocatalysis.Toward mitigating carbon footpri... Emerging as a new class of two-dimensional materials with atomically thin layers,MBenes have great potential for many important applications such as energy storage and electrocatalysis.Toward mitigating carbon footprint,there has been increasing interest in CO_(2)/CO conversion on MBenes,but mostly focused on C_(1) products.C^(2+) chemicals generally possess higher energy densities and wider applications than C_(1) counterparts.However,C–C coupling is technically challenging because of high energy requirement and currently few catalysts are suited for this process.Here,we explore electrochemical CO reduction reaction to C_(2) chemicals on Mo_(2)B_(2)O_(2) MBene via density-functional theory calculations.Remarkably,the most favorable CO–COH coupling is revealed to be a spontaneous and barrierless process,making Mo_(2)B_(2)O_(2) an efficient catalyst for C–C coupling.Among C_(1) and C_(2) chemicals,ethanol is predicted to be the primary product.Furthermore,by charge and bond analysis,it is unraveled that there exist significantly more unbonded electrons in the C atom of intermediate*COH than other C_(1) intermediates,which is responsible for the facile C–C coupling.From an atomic scale,this work provides microscopic insight into C–C coupling process and suggests Mo_(2)B_(2)O_(2) a promising catalyst for electrochemical CO reduction to C_(2) chemicals. 展开更多
关键词 C_(2) chemicals C-C coupling density-functional theory MBene Mo2B2O2
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Ca_(2)MnO_(4)-layered perovskite modified by NaNO_(3)for chemical-looping oxidative dehydrogenation of ethane to ethylene
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作者 Weixiao Ding Kun Zhao +2 位作者 Shican Jiang Zhen Huang Fang He 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2024年第4期53-64,共12页
Chemical-looping oxidative dehydrogenation(CL-ODH)is a process designed for the conversion of alkanes into olefins through cyclic redox reactions,eliminating the need for gaseous O_(2).In this work,we investigated the... Chemical-looping oxidative dehydrogenation(CL-ODH)is a process designed for the conversion of alkanes into olefins through cyclic redox reactions,eliminating the need for gaseous O_(2).In this work,we investigated the use of Ca_(2)MnO_(4)-layered perovskites modified with NaNO_(3) dopants,serving as redox catalysts(also known as oxygen carriers),for the CL-ODH of ethane within a temperature range of 700-780℃.Our findings revealed that the incorporation of NaNO_(3) as a modifier significantly-nhanced the selectivity for-thylene generation from Ca_(2)MnO_(4).At 750℃and a gas hourly space velocity of 1300 h^(-1),we achieved an-thane conversion up to 68.17%,accompanied by a corresponding-thylene yield of 57.39%.X-ray photoelectron spectroscopy analysis unveiled that the doping NaNO_(3) onto Ca_(2)MnO_(4) not only played a role in reducing the oxidation state of Mn ions but also increased the lattice oxygen content of the redox catalyst.Furthermore,formation of NaNO_(3) shell on the surface of Ca_(2)MnO_(4) led to a reduction in the concentration of manganese sites and modulated the oxygen-releasing behavior in a step-wise manner.This modulation contributed significantly to the enhanced selectivity for ethylene of the NaNO_(3)-doped Ca_(2)MnO_(4) catalyst.These findings provide compelling evidence for the potential of Ca_(2)MnO_(4)-layered perovskites as promising redox catalysts in the context of CL-ODH reactions. 展开更多
关键词 chemical-looping oxidative DEHYDROGENATION ETHANE ETHYLENE NaNO_(3)-doped Ca_(2)MnO_(4)redox catalyst Layered perovskites
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Unraveling the atomic interdiffusion mechanism of NiFe_(2_)O_(4) oxygen carriers during chemical looping CO_(2) conversion
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作者 Da Song Yan Lin +8 位作者 Shiwen Fang Yang Li Kun Zhao Xinfei Chen Zhen Huang Fang He Zengli Zhao Hongyu Huang Fanxing Li 《Carbon Energy》 SCIE EI CAS CSCD 2024年第8期105-121,共17页
By employing metal oxides as oxygen carriers,chemical looping demonstrates its effectiveness in transferring oxygen between reduction and oxidation environments to partially oxidize fuels into syngas and convert CO_(2... By employing metal oxides as oxygen carriers,chemical looping demonstrates its effectiveness in transferring oxygen between reduction and oxidation environments to partially oxidize fuels into syngas and convert CO_(2) into CO.Generally,NiFe_(2_)O_(4) oxygen carriers have demonstrated remarkable efficiency in chemical looping CO_(2) conversion.Nevertheless,the intricate process of atomic migration and evolution within the internal structure of bimetallic oxygen carriers during continuous high‐temperature redox cycling remains unclear.Consequently,the lack of a fundamental understanding of the complex ionic migration and oxygen transfer associated with energy conversion processes hampers the design of high‐performance oxygen carriers.Thus,in this study,we employed in situ characterization techniques and theoretical calculations to investigate the ion migration behavior and structural evolution in the bulk of NiFe_(2_)O_(4) oxygen carriers during H_(2) reduction and CO_(2)/lab air oxidation cycles.We discovered that during the H_(2) reduction step,lattice oxygen rapidly migrates to vacancy layers to replenish consumed active oxygen species,while Ni leaches from the material and migrates to the surface.During the CO_(2) splitting step,Ni migrates toward the core of the bimetallic oxygen carrier,forming Fe–Ni alloys.During the air oxidation step,Fe–Ni migrates outward,creating a hollow structure owing to the Kirkendall effect triggered by the swift transfer of lattice oxygen.The metal atom migration paths depend on the oxygen transfer rates.These discoveries highlight the significance of regulating the release–recovery rate of lattice oxygen to uphold the structures and reactivity of oxygen carriers.This work offers a comprehensive understanding of the oxidation/reduction‐driven atomic interdiffusion behavior of bimetallic oxygen carriers. 展开更多
关键词 chemical looping CO_(2)splitting density functional theory in situ characterization ionic migration
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CO_(2) conversion to solar fuels and chemicals:Opening the new paths
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作者 Gabriele Centi Claudio Ampelli 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第4期680-683,共4页
This future article discusses the new prospects and directions of CO_(2)conversion via the photo-electrocatalytic(PEC)route.The second(2nd)generation solar fuels and chemicals(SFs)are generated directly in PEC systems... This future article discusses the new prospects and directions of CO_(2)conversion via the photo-electrocatalytic(PEC)route.The second(2nd)generation solar fuels and chemicals(SFs)are generated directly in PEC systems via electrons/protons reactions without forming molecular H_(2)as an intermediate,overcoming the thermodynamics limitations and practical issues encountered for electro-fuels produced by multistep thermocatalytic processes(i.e.CO_(2)conversion with H_(2)coming from water electrolysis).A distributed and decentralized production of SFs requires very compact,highly integrated,and intensified technologies.Among the existing reactors of advanced design(based on artificial leaves or photosynthesis),the integrated photovoltaic plus electrocatalytic(PV-EC)device is the only system(demonstrated at large scale)to produce SFs with high solar-to-fuel(STF)efficiency.However,while the literature indicates STF efficiency as the main(and only)measure of process performance,we remark here the need to refer to productivity(in terms of current density)and make tests with reliable flow PEC systems(with electrodes of at least 5–10 cm^(2))to accelerate the scaling-up process.Using approaches that minimize downstream separation costs is also mandatory.Many limitations exist in PEC systems,but most can be overcome by proper electrode and cell engineering,thus going beyond the properties of the electrocatalysts.As examples of current developments,we present the progress of(i)artificial leaf/tree devices for green H_(2)distributed production and(ii)a PEC device producing the same chemicals at both cathode and anode parts without downstream operations for green solvent distributed production.Based on these developments,future directions,such as producing fertilizers and food components from the air,are outlined.The aim is to provide new ideas and research directions from a personal perspective. 展开更多
关键词 Solar fuels Artificial leaf PEC devices PV-EC devices Cell engineering green H_(2) chemicals from theair
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CO_(2)capture costs of chemical looping combustion of biomass:A comparison of natural and synthetic oxygen carrier
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作者 Benjamin Fleiß Juraj Priscak +3 位作者 Martin Hammerschmid Josef Fuchs Stefan Müller Hermann Hofbauer 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第5期296-310,共15页
Chemical looping combustion has the potential to be an efficient and low-cost technology capable of contributing to the reduction of the atmospheric concentration of CO_(2) in order to reach the 1.5/2°C goal and ... Chemical looping combustion has the potential to be an efficient and low-cost technology capable of contributing to the reduction of the atmospheric concentration of CO_(2) in order to reach the 1.5/2°C goal and mitigate climate change.In this process,a metal oxide is used as oxygen carrier in a dual fluidized bed to generate clean CO_(2) via combustion of biomass.Most commonly,natural ores or synthetic materials are used as oxygen carrier whereas both must meet special requirements for the conversion of solid fuels.Synthetic oxygen carriers are characterized by higher reactivity at the expense of higher costs versus the lower-cost natural ores.To determine the viability of both possibilities,a techno-economic comparison of a synthetic material based on manganese,iron,and copper to the natural ore ilmenite was conducted.The synthetic oxygen carrier was characterized and tested in a pilot plant,where high combustion efficiencies up to 98.4%and carbon capture rates up to 98.5%were reached.The techno-economic assessment resulted in CO_(2) capture costs of 75 and 40€/tCO_(2) for the synthetic and natural ore route respectively,whereas a sensitivity analysis showed the high impact of production costs and attrition rates of the synthetic material.The synthetic oxygen carrier could break even with the natural ore in case of lower production costs and attrition rates,which could be reached by adapting the production process and recycling material.By comparison to state-of-the-art technologies,it is demonstrated that both routes are viable and the capture cost of CO_(2) could be reduced by implementing the chemical looping combustion technology. 展开更多
关键词 chemical looping combustion BECCS Techno-economic assessment CO_(2)capture costs Oxygen carrier development Synthetic materials ILMENITE
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Shock-induced chemical reaction characteristics of PTFE-Al-Bi_(2)O_(3)reactive materials
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作者 Chunlan Jiang Rong Hu +2 位作者 Jingbo Zhang Zaicheng Wang Liang Mao 《Defence Technology(防务技术)》 SCIE EI CAS CSCD 2024年第6期1-12,共12页
A ternary system of PTFE/Al/Bi_(2)O_(3)is constructed by incorporating PTFE-based reactive material and thermite for enhancing the energy release of the PTFE-based reactive material.The effects of Bi_(2)O_(3)in the PT... A ternary system of PTFE/Al/Bi_(2)O_(3)is constructed by incorporating PTFE-based reactive material and thermite for enhancing the energy release of the PTFE-based reactive material.The effects of Bi_(2)O_(3)in the PTFE/Al/Bi_(2)O_(3)on both mechanical properties and the energy release were investigated through various tests such as thermogravimetry-differential scanning calorimetry,adiabatic oxygen bomb test and split Hopkinson pressure bar test.The microstructure observed through scanning electron microscope and Xray diffraction results are used to analyze the ignition and reaction mechanism of PTFE/Al/Bi_(2)O_(3).The results indicate that the PTFE/Al/Bi_(2)O_(3)are capable of triggering the exothermic reaction of molten PTFE/Bi_(2)O_(3)and Al/Bi_(2)O_(3)over the PTFE/Al reactive materials,thereby promoting reactions.The excessive aluminum in the ternary system is beneficial for increasing energy release.The ignition of shock-induced chemical reactions in PTFE/Al/Bi_(2)O_(3)is closely related to the material fracture.The dominant mechanism for hot-spot generation under Split Hopkinson Pressure Bar test is the frictional temperature rise at the microcrack after failure. 展开更多
关键词 PTFE/Al/Bi_(2)O_(3) Shock-induced chemical reaction Energy release
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NiO-Doped Fe_(2)O_(3)/MgO Properties for the Chemical Looping Oxidative Dehydrogenation of Ethane
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作者 Liang Hao Chen Junjie +1 位作者 Sun Jie Sun Hui 《China Petroleum Processing & Petrochemical Technology》 SCIE CAS CSCD 2024年第1期27-33,共7页
Ethane chemical looping oxidative dehydrogenation(CL-ODH)to ethylene is a new technology for ethylene preparation.Fe_(2)O_(3)/MgO oxygen carrier was prepared using the co-precipitation method.The influence of added Ni... Ethane chemical looping oxidative dehydrogenation(CL-ODH)to ethylene is a new technology for ethylene preparation.Fe_(2)O_(3)/MgO oxygen carrier was prepared using the co-precipitation method.The influence of added NiO and its different loadings on Fe_(2)O_(3)/MgO were investigated.Then,a series of oxygen carriers were applied in the CL-ODH of the ethane cycle system.Brunauer-Emmett-Teller(BET),X-ray diffractometry(XRD),X-ray photoelection spectroscopy(XPS),and H2-temperature programmed reduction(TPR)were used to characterize the physicochemical properties of these oxygen carriers.It was confirmed that an interaction between NiO and Fe_(2)O_(3) occurred based on the XPS and H2-TPR results.Based on the CL-ODH activity performance tests conducted in a fixed-bed reactor,it was revealed that ethylene selectivity was significantly improved after NiO addition.Fe_(2)O_(3)-10%NiO/MgO showed the best activity performance with 93%ethane conversion and 50%ethylene selectivity at a reaction temperature of 650℃,atmospheric pressure,and space velocity of 7500 mL/(g·h). 展开更多
关键词 chemical looping oxidative dehydrogenation oxygen carrier Fe_(2)O_(3)/MgO NIO
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Melting Flow Analyzation of Radiative Riga Plate Two-Phase Nano-Fluid Across Non-Flatness Plane with Chemical Reaction
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作者 Jupudi Lakshmi Rama Prasad F.Mebarek-Oudina +2 位作者 G.Dharmaiah Putta Babu Rao H.Vaidya 《Frontiers in Heat and Mass Transfer》 EI 2024年第5期1515-1532,共18页
There is a strong relationship between analytical and numerical heat transfers due to thermodynamically anticipated findings,making thermo-dynamical modeling an effective tool for estimating the ideal melting point of... There is a strong relationship between analytical and numerical heat transfers due to thermodynamically anticipated findings,making thermo-dynamical modeling an effective tool for estimating the ideal melting point of heat transfer.Under certain assumptions,the present study builds a mathematical model of melting heat transport nanofluid flow of chemical reactions and joule heating.Nanofluid flow is described by higher-order partial non-linear differential equations.Incorporating suitable similarity transformations and dimensionless parameters converts these controlling partial differential equations into the non-linear ordinary differential equations and resulting system of nonlinear equations is established.Plotted graphic visualizations in MATLAB allow for an indepth analysis of the effects of distinguishing factors on fluid flow.Innovative applications of the findings include electronic cooling,heat transfer,reaction processes,nuclear reactors,micro heat pipes,and other related fields.If the exponential index increases,however,the thermal profile becomes worse.By comparing the current findings to those already published in the literature for this particular example,we find that they are highly congruent,therefore validating the present work.Every one of the numerical findings exhibits asymptotic behavior by meeting the specified boundary conditions. 展开更多
关键词 Non-flat sheet melting surface chemical reaction 2-phase nano fluid
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Uniform deposition of ultra-thin TiO_(2) film on mica substrate by atmospheric pressure chemical vapor deposition: Effect of precursor concentration 被引量:2
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作者 Ming Liu Ying Li +4 位作者 Rui Wang Guoqiang Shao Pengpeng Lv Jun Li Qingshan Zhu 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2023年第8期99-107,共9页
The performance of pearlescent pigment significantly affected by the grain size and the roughness of deposited film. The effect of TiCl_(4) concentration on the initial deposition of TiO_(2) on mica by atmospheric pre... The performance of pearlescent pigment significantly affected by the grain size and the roughness of deposited film. The effect of TiCl_(4) concentration on the initial deposition of TiO_(2) on mica by atmospheric pressure chemical vapor deposition(APCVD) was investigated. The precursor concentration significantly affected the deposition and morphology of TiO_(2) grains assembling the film. The deposition time for fully covering the surface of mica decreased from 120 to 10 s as the TiCl_(4) concentration increased from 0.38%to 2.44%. The grain size increased with the TiCl_(4) concentration. The AFM and TEM analysis demonstrated that the aggregation of TiO_(2) clusters at the initial stage finally result to the agglomeration of fine TiO_(2) grains at high TiCl_(4) concentrations. Following the results, it was suggested that the nucleation density and size was easy to be adjusted when the TiCl_(4) concentration is below 0.90%. 展开更多
关键词 chemical vapor deposition TiO_(2)thin film Nucleation reaction Precursor concentration Pearlescent pigment
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Numerical Simulation of Thermo-Hydro-Mechanical-Chemical Response Caused by CO_(2)Injection into Saline Geological Formations:A Case Study from the Ordos Project,China 被引量:1
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作者 FAN Zejin XU Tianfu +2 位作者 YANG Bo ZHANG Hui ZHU Huixing 《Acta Geologica Sinica(English Edition)》 SCIE CAS CSCD 2023年第3期889-910,共22页
Thermo-hydro-mechanical-chemical(THMC)interactions are prevalent during CO_(2)geological sequestration(CGS).In this study,a sequential coupling THMC numerical simulation program was constructed,which can be used to ex... Thermo-hydro-mechanical-chemical(THMC)interactions are prevalent during CO_(2)geological sequestration(CGS).In this study,a sequential coupling THMC numerical simulation program was constructed,which can be used to explore the following issues of CGS:fluid and heat flow,solute transport;stresses,displacements and rock failures related to geo-mechanical effects;equilibrium and kinetic chemical reactions;chemical damage to mechanical properties of the rock.Then,the coupling program was applied to the Ordos CGS Project to study the formation response under the multifield interaction caused by CO_(2)injection.The simulation results show that the mechanical process dominates the short CO_(2)injection period.Specifically,the formation’s permeability near the injection well increases by 43%,due to the reduction of effective stress,which significantly promotes the lateral migration of CO_(2).When the injection rate exceeds 0.15 million tons per year,the cohesion of the reservoir rock is not enough to resist the shear force inside the rock and rock failure may occur.During the subsequent long-term sequestration period(200 years),the influence of mineral reactions gradually increases.Due to calcite dissolution,the shear modulus of caprock is predicted to decrease by 7.6%,which will to some extent increase the risk of rock failure. 展开更多
关键词 CO_(2) geological sequestration THMC coupling numerical simulation chemical damage
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Surface modification of Cu_(2)O with stabilized Cu^(+) for highly efficient and stable CO_(2) electroreduction to C_(2+) chemicals
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作者 Ziyu Zhou Shuyu Liang +4 位作者 Jiewen Xiao Tianyu Zhang Min Li Wenfu Xie Qiang Wang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2023年第9期277-285,共9页
Copper(Cu)-based materials are known as the most attractive catalysts for electrochemical carbon dioxide reduction reaction(CO_(2)RR),especially the Cu^(+) species(e.g.,Cu_(2)O),which show excellent capability for cat... Copper(Cu)-based materials are known as the most attractive catalysts for electrochemical carbon dioxide reduction reaction(CO_(2)RR),especially the Cu^(+) species(e.g.,Cu_(2)O),which show excellent capability for catalyzing CO_(2) to C_(2+) chemicals because of their unique electronic structure.However,the active Cu^(+) species are prone to be reduced to metallic Cu under an electroreduction environment,thus resulting in fast deactivation and poor selectivity.Here,we developed an advanced surface modification strategy to maintain the active Cu^(+) species via assembling a protective layer of metal-organic framework(copper benzenetricarboxylate,CuBTC) on the surface of Cu_(2)O octahedron(Cu_(2)O@CuBTC).It's encouraging to see that the Cu_(2)O@CuBTC heterostructure outperforms the bare Cu_(2)O octahedron in catalyzing CO_(2) to C_(2+) chemicals and dramatically enhances the ratio of C_(2)H_(4)/CH_(4) products.A systematic study reveals that the introduced CuBTC shell plays a critical role in maintaining the active Cu^(+) species in Cu_(2)O@CuBTC heterostructure under reductive conditions.This work offers a practical strategy for improving the catalytic performance of CO_(2)RR over copper oxides and also establishes a route to maintain the state of valence-sensitive catalysts. 展开更多
关键词 CO_(2)RR Copper Oxide Metal-organic Framework Core-shell Structure C_(2+)chemicals
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Controllable growth of wafer-scale PdS and PdS_(2) nanofilms via chemical vapor deposition combined with an electron beam evaporation technique
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作者 Hui Gao Hongyi Zhou +6 位作者 Yulong Hao Guoliang Zhou Huan Zhou Fenglin Gao Jinbiao Xiao Pinghua Tang Guolin Hao 《Journal of Semiconductors》 EI CAS CSCD 2023年第12期64-71,共8页
Palladium(Pd)-based sulfides have triggered extensive interest due to their unique properties and potential applications in the fields of electronics and optoelectronics.However,the synthesis of large-scale uniform Pd... Palladium(Pd)-based sulfides have triggered extensive interest due to their unique properties and potential applications in the fields of electronics and optoelectronics.However,the synthesis of large-scale uniform PdS and PdS_(2)nanofilms(NFs)remains an enormous challenge.In this work,2-inch wafer-scale PdS and PdS_(2) NFs with excellent stability can be controllably prepared via chemical vapor deposition combined with electron beam evaporation technique.The thickness of the pre-deposited Pd film and the sulfurization temperature are critical for the precise synthesis of PdS and PdS_(2) NFs.A corresponding growth mechanism has been proposed based on our experimental results and Gibbs free energy calculations.The electrical transport properties of PdS and PdS_(2) NFs were explored by conductive atomic force microscopy.Our findings have achieved the controllable growth of PdS and PdS_(2) NFs,which may provide a pathway to facilitate PdS and PdS_(2) based applications for next-generation high performance optoelectronic devices. 展开更多
关键词 PDS PdS_(2) NANOFILMS controllable growth chemical vapor deposition electron beam evaporation
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Chemical bonding of perovskite LaFeO_(3) with Li_(1.2)Mn_(0.6)Ni_(0.2)O_(2) to moderate anion redox for achieving high cycling stability
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作者 Xin Zhang Chaochao Fu +5 位作者 Dong Luo Xiaoqing Liu Qiao Wang Baoyun Li Guangshe Li Liping Li 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2023年第4期330-339,共10页
Oxygen anion redox reaction provides a high theoretical capacity for Li-rich manganese-based cathodes.However,irreversible surface oxygen release often results in further oxygen loss and exacerbates the decomposition ... Oxygen anion redox reaction provides a high theoretical capacity for Li-rich manganese-based cathodes.However,irreversible surface oxygen release often results in further oxygen loss and exacerbates the decomposition of the electrolyte,which could reduce the capacity contribution from the anionic redox and produce more acidic substances to corrode the surface of the material.In this paper,the surface oxygen release is suppressed by moderating oxygen anion redox activity via constructing chemical bonds between M(M=Fe and La)in LaFeO_(3)and surface oxygen anions of Li_(1.2)Mn_(0.6)Ni_(0.2)O_(2).The constructed interface layer stabilizes the surface lattice oxygen and retards the electrolyte from being attacked by the nucleophilic oxygen generated in the process of oxygen release,as evidenced by Differential Electrochemical Mass Spectrometry(DEMS)and X-ray Photoelectron Spectroscopy(XPS)detections.Moreover,in the charge and discharge process,the formed FeF_(3),located at the cathode electrolyte interfacial layer,is conducive to the stability of the cathode surface.The modified Li_(1.2)Mn_(0.6)Ni_(0.2)O_(2)electrode with 3 wt%LaFeO_(13)exhibits a high specific capacity of 189.5 mA h g-at 1C(200 mA g^(-1))after 150 cycles with capacity retentions of 96.6%,and 112.6 mA h g^(-1)(84.7%)at 5C after 200 cycles higher than the pristine sample.This study provides a rational design chemical bonding method to suppress the oxygen release from the cathode surface and enhance cyclic stability. 展开更多
关键词 Lithium battery Li_(1.2)Mn_(0.6)Ni_(0.2)O_(2) Oxygen release Interface chemical bond Electrolyte decomposition
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5%Ag掺杂对MNO_(2)纳米棒和海胆微球形貌及其甲苯氧化性能的影响
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作者 鲁美娟 方汉孙 +4 位作者 黄华军 李丹萍 吴玮玲 屈小路 喻成龙 《环境工程技术学报》 CAS CSCD 北大核心 2024年第4期1239-1246,共8页
采用水热法制备了MNO_(2)纳米棒和海胆微球,并原位掺杂5%Ag制备了Mn-Ag复合氧化物,利用SEM、XRD、BET、Raman等表征技术对其结构进行表征,并考察不同催化剂对甲苯的去除性能。结果表明:(NH_(4))_(2)S_(2)O_(8)的掺入量会对MNO_(2)的形... 采用水热法制备了MNO_(2)纳米棒和海胆微球,并原位掺杂5%Ag制备了Mn-Ag复合氧化物,利用SEM、XRD、BET、Raman等表征技术对其结构进行表征,并考察不同催化剂对甲苯的去除性能。结果表明:(NH_(4))_(2)S_(2)O_(8)的掺入量会对MNO_(2)的形貌产生影响,当其掺入量为2.28 g时,形成MNO_(2)纳米棒,当其掺入量为6.84 g时,形成MNO_(2)海胆微球;MNO_(2)纳米棒掺杂5%的Ag后,形貌未发生变化,但当MNO_(2)海胆微球掺杂5%Ag时,表面的纳米线较MNO_(2)海胆微球有所增长,且出现了缠绕现象,形成了空心鸟巢状结构;5%Ag掺杂后,对MNO_(2)纳米棒和MNO_(2)海胆微球的晶型未产生影响,均为α-MNO_(2),但5%Ag-MNO_(2)纳米棒出现了Mn2O_(3)的衍射峰;MNO_(2)海胆微球较MNO_(2)纳米棒的比表面积、孔径和孔容均增大,且Ag的掺杂进一步提高了MNO_(2)海胆微球的比表面积、孔径和孔容;MNO_(2)海胆微球比MNO_(2)纳米棒具有更好的甲苯去除性能,且5%Ag掺杂后,MNO_(2)海胆微球对甲苯的去除性能达到最好。 展开更多
关键词 MNO_(2)纳米棒 MNO_(2)海胆微球 AG掺杂 形貌影响 甲苯去除
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La_(1-x)Ce_(x)MnO_(3)-Ba/Al_(2)O_(3)催化剂对NO选择性生成NH_(3)的影响
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作者 宋崇林 郑庆贺 +3 位作者 吕誉 崔立峰 李云强 吕刚 《天津大学学报(自然科学与工程技术版)》 EI CAS CSCD 北大核心 2024年第10期1053-1061,共9页
为了实现碳中和目标,降低内燃机碳排放,稀薄燃烧技术成为了当前重要的研究方向.该技术不仅能提高发动机燃油热效率,还能有效降低CO_(2)排放.但是稀薄燃烧往往会伴随着大量氮氧化物的产生,为了解决该问题,采用LNT-SCR耦合的NO_(x)净化技... 为了实现碳中和目标,降低内燃机碳排放,稀薄燃烧技术成为了当前重要的研究方向.该技术不仅能提高发动机燃油热效率,还能有效降低CO_(2)排放.但是稀薄燃烧往往会伴随着大量氮氧化物的产生,为了解决该问题,采用LNT-SCR耦合的NO_(x)净化技术,此时LNT的作用是将排气中部分NO_(x)转化为NH_(3),为下游的SCR提供还原剂.基于此,制备了LNT催化剂,研究催化剂对NO选择性生成NH_(3)的影响.采用溶胶-凝胶法制备了La_(1-x)Ce_(x)MnO_(3)系列钙钛矿氧化物,并通过分步浸渍法得到了La_(1-x)Ce_(x)MnO_(3)-Ba/Al_(2)O_(3)负载型催化剂.利用XRD、H_(2)-TPR、NO-TPD等表征手段研究了钙钛矿氧化物的晶相结构,以及负载型催化剂的还原特性、NO_(x)吸附-脱附性能等物化性质,并且通过H_(2)选择性催化还原NO实验探究了催化剂掺杂Ce对NO转化成NH_(3)的影响.结果表明,Ce掺杂催化剂具有良好的NH_(3)产物选择性,并且显著提高了NO转化率.温度是NO转化和NH_(3)产物选择性生成的决定性因素,而H_(2)和NO体积比是NO转化和NH_(3)产物选择性生成的关键性因素.其中,La_(0.95)Ce_(0.05)MnO_(3)-Ba/Al_(2)O_(3)在低温下催化活性表现最佳,在350℃、H_(2)和NO体积比为5.0时NH_(3)产物选择性为65%,NO转化率为100%.此外,所制备的La_(1-x)Ce_(x)MnO_(3)都形成了钙钛矿型结构,而且Ce掺杂催化剂的大部分Ce离子可以进入到LaMnO_(3)结构中.在催化剂适量掺杂Ce后,H_(2)消耗总面积增大、还原峰的峰值温度降低,表明掺杂Ce改善了催化剂的还原特性;同时NO吸附和脱附面积增大,表明Ce掺杂改变了催化剂的NO_(x)吸附-脱附性能. 展开更多
关键词 La_(1-x)Ce_(x)MnO_(3)-Ba/Al_(2)O_(3)催化剂 H_(2)选择性催化还原NO NH_(3)产物选择性 NO转化率 晶相结构 还原特性 NO_(x)吸附-脱附
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MnO_(2)/碳气凝胶复合电极材料的制备及其电化学性能
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作者 夏傲 陈军 +2 位作者 李佳萌 于博涛 谈国强 《陕西科技大学学报》 北大核心 2024年第6期126-133,共8页
采用溶胶-凝胶法,利用可溶性淀粉制备碳气凝胶基体,并通过水热反应将MnO_(2)纳米结构在碳气凝胶(CA)表面原位生长,制得了MnO_(2)/CA复合电极材料,并对该复合材料进行了结构和形貌表征以及电化学性能测试.结果显示,MnO_(2)/CA复合材料相... 采用溶胶-凝胶法,利用可溶性淀粉制备碳气凝胶基体,并通过水热反应将MnO_(2)纳米结构在碳气凝胶(CA)表面原位生长,制得了MnO_(2)/CA复合电极材料,并对该复合材料进行了结构和形貌表征以及电化学性能测试.结果显示,MnO_(2)/CA复合材料相比于纯相的MnO_(2)有着更好的电化学性能.样品M15CA(原料中KMnO 4与CA以15∶1的质量比复合得到的样品)在1 A/g的电流密度下比电容可达202 F/g,电流密度从1 A/g增加至10 A/g时比电容保持率为77.4%,在10 A/g下经过10000次循环后比电容保持率为88.6%.复合材料性能的提升主要归因于CA高的导电性,其与MnO_(2)复合后电极的转移电阻显著降低.另外,CA的三维多孔网络结构有效防止了MnO_(2)的团聚,使得电极材料与电解液更加充分接触、反应活性位点增多. 展开更多
关键词 超级电容器 MnO_(2) 碳气凝胶 电极材料 复合材料
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多孔MnO_(2)-Fe_(3)O_(4)壳聚糖微球用于增强类Fenton降解染料废水的研究
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作者 王东钢 汪志敏 《现代化工》 CAS CSCD 北大核心 2024年第S02期215-222,共8页
将壳聚糖与金属盐混合溶液滴入碱性溶液中,采用一步法制备了金属壳聚糖微球(MnO_(2)-Fe_(3)O_(4)/CS),并用于刚果红(CR)的类Fenton降解。结果表明,与单金属壳聚糖微球(MnO_(2)/CS、Fe_(3)O_(4)/CS)相比,MnO_(2)-Fe_(3)O_(4)/CS具有更好... 将壳聚糖与金属盐混合溶液滴入碱性溶液中,采用一步法制备了金属壳聚糖微球(MnO_(2)-Fe_(3)O_(4)/CS),并用于刚果红(CR)的类Fenton降解。结果表明,与单金属壳聚糖微球(MnO_(2)/CS、Fe_(3)O_(4)/CS)相比,MnO_(2)-Fe_(3)O_(4)/CS具有更好的催化活性;在最佳条件下(50 mg/L CR,pH=7,0.9 mol/L H_(2)O_(2),2.0 g/L催化剂,60 min),CR的去除率达到100%。MnO_(2)-Fe_(3)O_(4)/CS的高活性归因于其较大的比表面积和孔体积,特殊多孔结构有利于反应物的吸附/扩散和活性位点的暴露;Mn-Fe双金属之间的协同作用促进了电子传递,有效提高了催化活性。金属壳聚糖微球可以很容易地从反应体系中收集,重复使用5次后仍然保持较高催化活性(88.2%)。 展开更多
关键词 类Fenton催化 壳聚糖 刚果红 二氧化锰 四氧化三铁
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溶胶凝胶法铈锆锰基脱硝催化剂制备及性能
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作者 李渊 王旭超 谭小耀 《天津工业大学学报》 CAS 北大核心 2024年第3期23-31,共9页
为了提高铈锆基脱硝催化剂的低温脱硝性能,采用溶胶凝胶法和溶胶凝胶法+浸渍法制备了一系列铈锆锰基脱硝催化剂,通过XRD、XPS、N_(2)-吸附脱附、NH_(3)-TPD、H_(2)-TPR、SEM/EDS等手段对催化剂进行了表征,对催化剂的脱硝性能进行了评价... 为了提高铈锆基脱硝催化剂的低温脱硝性能,采用溶胶凝胶法和溶胶凝胶法+浸渍法制备了一系列铈锆锰基脱硝催化剂,通过XRD、XPS、N_(2)-吸附脱附、NH_(3)-TPD、H_(2)-TPR、SEM/EDS等手段对催化剂进行了表征,对催化剂的脱硝性能进行了评价。结果表明:在100~350℃温度范围内,空速为220000 h^(-1)的条件下,采用溶胶凝胶法制备的CZM-0.2催化剂展现出最好的低温脱硝性能;CZM-0.2催化剂优异的低温脱硝性能主要与其较好的Mn分散度、较高的Mn^(4+)含量、较强的低温还原性能(MnO_(x)的逐步还原)和较多的弱酸位点有关。 展开更多
关键词 NH3-SCR 铈锆锰基脱硝催化剂 溶胶凝胶 掺杂改性
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水系铵离子电池β-MnO_(2)正极材料的制备及性能研究
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作者 刘扬 陈晗 +1 位作者 向凯雄 周伟 《湖南工业大学学报》 2024年第1期78-83,共6页
通过简单的水热法合成了隧道型β-MnO_(2)正极材料并应用于水系铵离子电池,并采用1 mol/L(NH4)2SO4水系电解液,在窗口电压为0~1.6 V范围内,测试其电化学性能。实验结果表明:β-MnO_(2)正极材料在0.1A/g电流密度下表现出109.8 mAh/g放电... 通过简单的水热法合成了隧道型β-MnO_(2)正极材料并应用于水系铵离子电池,并采用1 mol/L(NH4)2SO4水系电解液,在窗口电压为0~1.6 V范围内,测试其电化学性能。实验结果表明:β-MnO_(2)正极材料在0.1A/g电流密度下表现出109.8 mAh/g放电比容量,经过140次循环后,其放电比容量仍有101.9 mAh/g,容量保留率为92.8%,库伦效率接近100%,具有优异的循环稳定性能。同时还具有优异的倍率性能,β-MnO_(2)纳米棒正极材料即使在1.0 A/g大电流密度下仍有78.7 mAh/g。此外,通过非原位FTIR、XPS测试探索了其储铵机理,结果表明铵根离子具有良好的可逆性。 展开更多
关键词 水系铵离子电池 β-MnO_(2) 正极材料 水热法
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准东煤分步和直接化学链燃烧特性
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作者 亚力昆江·吐尔逊 高志伟 +5 位作者 代正华 钟梅 靳立军 李建 刘洋 魏博 《洁净煤技术》 CAS CSCD 北大核心 2024年第6期16-26,共11页
化学链燃烧作为高效的低碳排放燃烧技术,在提高燃料利用率和减少CO_(2)排放方面显示出其独特优势。采用Fe_(2)O_(3)/Al_(2)O_(3)载氧体,利用两段式固定床反应器开展了准东煤直接和分步化学链燃烧试验,探究了载氧体反应前后理化特性。发... 化学链燃烧作为高效的低碳排放燃烧技术,在提高燃料利用率和减少CO_(2)排放方面显示出其独特优势。采用Fe_(2)O_(3)/Al_(2)O_(3)载氧体,利用两段式固定床反应器开展了准东煤直接和分步化学链燃烧试验,探究了载氧体反应前后理化特性。发现准东煤热解挥发分化学链燃烧碳转化率和CO_(2)选择性随温度和载氧体与煤质量比(OC/C)增加而升高。OC/C和温度升高提高半焦化学链燃烧碳转化率,但降低CO_(2)选择性。相比煤直接化学链燃烧,在相同条件,分步化学链燃烧CO_(2)选择性大幅提高、碳转化率有所降低。反应温度800℃,分步化学链燃烧CO_(2)选择性达89.51%,相比直接化学链燃烧提升了29.18%。反应温度950℃,分步化学链燃烧碳转化率在60.40%,比直接化学链燃烧降低6.78%。与半焦反应后载氧体还原程度高于与煤热解挥发分反应后载氧体,半焦与载氧体的反应是煤化学链燃烧的限制因素之一。本研究为实现准东煤低碳清洁燃烧提供重要理论依据和技术支撑。 展开更多
关键词 化学链燃烧 载氧体 煤热解挥发分 半焦 CO_(2)选择性
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