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Fischer–Tropsch synthesis on impregnated cobalt-based catalysts:New insights into the effect of impregnation solutions and pH value 被引量:1
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作者 Chuang Xing Peipei Ai +6 位作者 Peipei Zhang Xinhua Gao Ruiqin Yang Noriyuki Yamane Jian Sun Prasert Reubroycharoen Noritatsu Tsubaki 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2016年第6期994-1000,共7页
The Co-based catalysts were prepared with different cobalt acetate solutions. Effects of pH value were studied deeply on Fischer–Tropsch synthesis (FTS) through a semi-batch reactor. Among all impregnation solutions ... The Co-based catalysts were prepared with different cobalt acetate solutions. Effects of pH value were studied deeply on Fischer–Tropsch synthesis (FTS) through a semi-batch reactor. Among all impregnation solutions (water, butanol, amyl alcohol, acetic acid, nitric acid and ammonium nitrate), the catalyst prepared by NH4NO3solution showed the highest catalytic activity due to its small particle size and high reduction degree. However, the catalyst with the smallest particle size derived from water as impregnation solution exhibited low activity as well as high methane selectivity since it was difficult to be reduced and inactive in FTS. According to FT-IR spectra results, the low intensity of absorbed CO on the catalyst prepared from water solution resulted in low FTS activity. Whereas, the high activity of catalysts prepared from NH4NO3solution could be explained by the high intensity of absorbed CO on the catalysts. The cobalt species on the catalysts prepared under lower pH conditions exhibited smaller particle size distribution as well as lower CO conversion than those prepared at higher pH value. © 2016 Science Press 展开更多
关键词 Batch reactors catalyst selectivity catalystS COBALT IMPREGNATION Particle size Particle size analysis pH pH effects
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Fischer-Tropsch Synthesis over Alumina- Supported Cobalt-Based Catalysts: Effect of Support Variables 被引量:1
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作者 Yan Liu Heqin Guo +6 位作者 Litao Jia Zhancheng Ma Yong Xiao Congbiao Chen Ming Xia Bo Hou Debao Li 《Journal of Materials Science and Chemical Engineering》 2014年第12期19-27,共9页
Different kinds of aluminum precursors were obtained from precipitating ammonium bicarbonate, ammonium carbonate, and saturated ammonium bicarbonate, then, boehmite (AlO(OH)), ammonium alumina carbonate hydroxide (AAC... Different kinds of aluminum precursors were obtained from precipitating ammonium bicarbonate, ammonium carbonate, and saturated ammonium bicarbonate, then, boehmite (AlO(OH)), ammonium alumina carbonate hydroxide (AACH) and their mixture were obtained, and then, different kinds of alumina were obtained after calcination. Three catalysts supported on the different alumina were obtained via impregnating cobalt and ruthenium by incipient wetness. The effects of different precipitants on composition of precursors were?studied by XRD, FTIR, and TGA. The property and structure of alumina were studied by XRD and BET. The supported catalysts were studied by characterizations of XRD and H2-TPR, and the catalytic performance for Fischer-Tropsch synthesis (FTS) were evaluated at a fix-bed reactor. The relations among the composition of precursors, the property of alumina and the catalytic performance of supported catalysts were researched thoroughly. 展开更多
关键词 cobalt-based catalysts FISCHER-TROPSCH Synthesis ALUMINA PRECIPITANT
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Nanosized cobalt-based catalyst prepared by supercritical phase condition for Fischer-Tropsch synthesis
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作者 Jingmiao Li Jingchang Zhang Runduo Zhang Weiliang Cao 《Journal of Natural Gas Chemistry》 EI CAS CSCD 2009年第3期325-330,共6页
A series of nanosized Co/Zn/Mn/K composite catalysts for Fischer-Tropsch synthesis (FTS) were prepared by supercritical fluid drying (SCFD) method and common drying (CD) method. The nanosized cobalt-based cataly... A series of nanosized Co/Zn/Mn/K composite catalysts for Fischer-Tropsch synthesis (FTS) were prepared by supercritical fluid drying (SCFD) method and common drying (CD) method. The nanosized cobalt-based catalysts were characterized by XRD, TEM and BET techniques. Their catalytic performances were tested in a slurry-bed reactor under FTS reaction conditions. The drying and crystallization were carried out simultaneously during SCFD, therefore, the catalysts prepared by SCFD method have ideal structure and show the FTS performance superior to the others prepared by CD method. The FTS activity and selectivity were improved via adding Zn, Mn and K promoters, and less CH4 and CO2 as well as higher yield of C5+ products were achieved. The optimal performance of a 92% CO conversion and a 65% C5+ product yield was obtained over a catalyst with the component of Co/Zn/Mn/K = 100/50/10/7. Furthermore, the catalytic performance was studied under the conditions of liquid-phase and supercritical phase slurry-bed, and C5+ product yield were 57.4% and 65.4%, respectively. In summary, better catalytic performance was obtained using the nanosized catalyst prepared by SCFD method under supercritical reaction conditions, resulting in higher conversion of CO, less CO2 byproduct, and higher yield of C5+ products. 展开更多
关键词 nanosized catalyst supercritical combined technique Fischer-Tropsch synthesis supercritical phase liquid fuels
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An Electrocatalytic Strategy for Dehydrogenative[4+2]Cycloaddition over a Cobalt-Based Catalyst 被引量:2
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作者 Xiaomeng Xue Ye Wang +7 位作者 Lina Zhou Ruixiang Ge Jiangrong Yang Xianggui Kong Ming Xu Zhenhua Li Lina Ma Haohong Duan 《Chinese Journal of Chemistry》 SCIE CAS CSCD 2022年第23期2741-2746,共6页
Exploring the anodic reaction to substitute conventional oxygen evolution reaction(OER)for the synthesis of complex pharmaceutical molecules is highly attractive.Here,we report an electrocatalytic strategy for dehydro... Exploring the anodic reaction to substitute conventional oxygen evolution reaction(OER)for the synthesis of complex pharmaceutical molecules is highly attractive.Here,we report an electrocatalytic strategy for dehydrogenative[4+2]cycloaddition of N,N-dialkylanilines with maleimides via dual functionalization of both C(sp3)-H and C(sp2)-H bonds,by using an electrochemically activated cobalt carbonate hydroxide hydrate supported on carbon cloth(CCHH-A/CC),affording various tetrahydroquinolines with high yields.This electrochemical transformation proceeds with high activity and stability,as well as good substrate compatibility.Mechanism study shows thatα-aminoalkyl radical exists in the electrooxidation reaction.This strategy shows significant potential for the synthesis of valuable chemicals by using an electrocatalytic strategy. 展开更多
关键词 CYCLOADDITION C-H activation DEHYDROGENATION Eletrooxidation reactions cobalt-based catalyst
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Electrochemical water oxidation by photo-deposited cobalt-based catalyst on a nano-structured TiO_(2) electrode 被引量:1
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作者 LI Lin SUN LiCheng 《Science China Chemistry》 SCIE EI CAS 2012年第9期1976-1981,共6页
A cobalt-based catalyst was directly photo-deposited on the surface of a widely used n-type nano-structured semiconductor(TiO_(2)).Different thicknesses of the TiO 2 films as well as different time of photo-deposition... A cobalt-based catalyst was directly photo-deposited on the surface of a widely used n-type nano-structured semiconductor(TiO_(2)).Different thicknesses of the TiO 2 films as well as different time of photo-deposition of the Co-based catalyst on TiO_(2) films have been optimized.It was found that the electrode with 3 layers of TiO_(2) film(in 8 m thickness) and 1 hour photo-deposition of the cobalt-based catalyst by light irradiation from a 500 W Xenon lamp gave the highest current density(~5 mA/cm^(2)).Using this cobalt-modified TiO_(2) film as a working electrode in an electrochemical device,highly efficient water oxidation has been demonstrated in a pH 7.0 aqueous solution with low overpotential. 展开更多
关键词 artificial photosynthesis electrochemical water oxidation cobalt-based catalyst photo-deposition water splitting
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Rare Earth Elements(La,Ce,Pr)Modified Co/NC Catalyst for Efficient and Stable Ammonia Decomposition to Hydrogen Production
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作者 ZHU Yi PAN Hongfei 《Journal of Wuhan University of Technology(Materials Science)》 SCIE EI CAS CSCD 2024年第6期1372-1378,共7页
Co/NC catalysts modified with rare earth elements(La,Ce,Pr)were prepared by pyrolysis of rare earth elements doped ZIF-67.The experimental results show that the modification of rare earth elements significantly improv... Co/NC catalysts modified with rare earth elements(La,Ce,Pr)were prepared by pyrolysis of rare earth elements doped ZIF-67.The experimental results show that the modification of rare earth elements significantly improves the ammonia decomposition activity and stability of the Co/NC catalyst.The La-Co/NC catalyst can achieve an 82.3%ammonia decomposition and 18.4 mmol hydrogen production rate at 550℃with a GHSV of 20000 cm^(3)·h^(-1).Furthermore,no obvious performance degradation is observed after 72 hours of reaction for all rare earth elements modified catalysts.It is shown that the modification of rare earth elements significantly improves the surface alkalinity and surface chemical state of the catalyst,and thus improves the ammonia decomposition activity of the catalyst.A new type of high-performance ammonia decomposition Co-based catalyst is proposed,and the promoting effect of rare earth elements on the activity of ammonia decomposition is revealed. 展开更多
关键词 hydrogen carrier hydrogen production ammonia decomposition rare earth elements cobalt-based catalysts
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光学体表成像设备Catalyst的故障维修案例及日常保养方法
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作者 彭旭东 张俞 +1 位作者 何垠波 李光俊 《中国医疗设备》 2024年第4期169-173,180,共6页
本文介绍了光学体表成像设备Catalyst HD的工作原理,以及处理常见的硬件和软件故障的方法,并提供了日常维护保养方法。其中,对于硬件故障,利用Catalyst HD系统的MutilZsn软件来判断Catalyst投影器和摄像头故障,对于软件故障方面,探讨了C... 本文介绍了光学体表成像设备Catalyst HD的工作原理,以及处理常见的硬件和软件故障的方法,并提供了日常维护保养方法。其中,对于硬件故障,利用Catalyst HD系统的MutilZsn软件来判断Catalyst投影器和摄像头故障,对于软件故障方面,探讨了Catalyst HD系统在医用直线加速器上常见的Authorization Pending联锁问题的触发原因。本文为科室更好地开展光学体表引导放疗技术,高效地运用好设备提供参考意见。 展开更多
关键词 光学体表引导放射治疗 catalyst 故障维修 维护保养
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Strong synergy between physical and chemical properties:Insight into optimization of atomically dispersed oxygen reduction catalysts 被引量:4
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作者 Yifan Zhang Linsheng Liu +4 位作者 Yuxuan Li Xueqin Mu Shichun Mu Suli Liu Zhihui Dai 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第4期36-49,共14页
Atomically dispersed catalysts exhibit significant influence on facilitating the sluggish oxygen reduction reaction(ORR)kinetics with high atom economy,owing to remarkable attributes including nearly 100%atomic utiliz... Atomically dispersed catalysts exhibit significant influence on facilitating the sluggish oxygen reduction reaction(ORR)kinetics with high atom economy,owing to remarkable attributes including nearly 100%atomic utilization and exceptional catalytic functionality.Furthermore,accurately controlling atomic physical properties including spin,charge,orbital,and lattice degrees of atomically dispersed catalysts can realize the optimized chemical properties including maximum atom utilization efficiency,homogenous active centers,and satisfactory catalytic performance,but remains elusive.Here,through physical and chemical insight,we review and systematically summarize the strategies to optimize atomically dispersed ORR catalysts including adjusting the atomic coordination environment,adjacent electronic orbital and site density,and the choice of dual-atom sites.Then the emphasis is on the fundamental understanding of the correlation between the physical property and the catalytic behavior for atomically dispersed catalysts.Finally,an overview of the existing challenges and prospects to illustrate the current obstacles and potential opportunities for the advancement of atomically dispersed catalysts in the realm of electrocatalytic reactions is offered. 展开更多
关键词 Atomically dispersed catalysts Coordination environment Electronic orbitals Inter-site distance effect Oxygen reduction reaction
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Catalytic effect in lithium metal batteries: From heterogeneous catalyst to homogenous catalyst 被引量:1
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作者 Haining Fan Xuan-Wen Gao +3 位作者 Hailong Xu Yichun Ding Shi-Xue Dou Wen-Bin Luo 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第3期305-326,I0008,共23页
Lithium metal batteries are regarded as prominent contenders to address the pressing needs owing to the high theoretical capacity.Toward the broader implementation,the primary obstacle lies in the intricate multi-elec... Lithium metal batteries are regarded as prominent contenders to address the pressing needs owing to the high theoretical capacity.Toward the broader implementation,the primary obstacle lies in the intricate multi-electron,multi-step redox reaction associated with sluggish conversion kinetics,subsequently giving rise to a cascade of parasitic issues.In order to smooth reaction kinetics,catalysts are widely introduced to accelerate reaction rate via modulating the energy barrier.Over past decades,a large amount of research has been devoted to the catalyst design and catalytic mechanism exploration,and thus the great progress in electrochemical performance has been realized.Therefore,it is necessary to make a comprehensive review toward key progress in catalyst design and future development pathway.In this review,the basic mechanism of lithium metal batteries is provided along with corresponding advantages and existing challenges detailly described.The main catalysts employed to accelerate cathode reaction with emphasis on their catalytic mechanism are summarized as well.Finally,the rational design and innovative direction toward efficient catalysts are suggested for future application in metal-sulfur/gas battery and beyond.This review is expected to drive and benefit future research on rational catalyst design with multi-parameter synergistic impacts on the activity and stability of next-generation metal battery,thus opening new avenue for sustainable solution to climate change,energy and environmental issues,and the potential industrial economy. 展开更多
关键词 Energy storage and conversion Metal battery Sulfur battery Air battery Catalytic effect Heterogeneous catalyst Homogeneous catalyst
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p-d Orbital Hybridization Engineered Single-Atom Catalyst for Electrocatalytic Ammonia Synthesis 被引量:1
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作者 Jingkun Yu Xue Yong Siyu Lu 《Energy & Environmental Materials》 SCIE EI CAS CSCD 2024年第2期119-125,共7页
The rational design of metal single-atom catalysts(SACs)for electrochemical nitrogen reduction reaction(NRR)is challenging.Two-dimensional metal-organic frameworks(2DMOFs)is a unique class of promising SACs.Up to now,... The rational design of metal single-atom catalysts(SACs)for electrochemical nitrogen reduction reaction(NRR)is challenging.Two-dimensional metal-organic frameworks(2DMOFs)is a unique class of promising SACs.Up to now,the roles of individual metals,coordination atoms,and their synergy effect on the electroanalytic performance remain unclear.Therefore,in this work,a series of 2DMOFs with different metals and coordinating atoms are systematically investigated as electrocatalysts for ammonia synthesis using density functional theory calculations.For a specific metal,a proper metal-intermediate atoms p-d orbital hybridization interaction strength is found to be a key indicator for their NRR catalytic activities.The hybridization interaction strength can be quantitatively described with the p-/d-band center energy difference(Δd-p),which is found to be a sufficient descriptor for both the p-d hybridization strength and the NRR performance.The maximum free energy change(ΔG_(max))andΔd-p have a volcanic relationship with OsC_(4)(Se)_(4)located at the apex of the volcanic curve,showing the best NRR performance.The asymmetrical coordination environment could regulate the band structure subtly in terms of band overlap and positions.This work may shed new light on the application of orbital engineering in electrocatalytic NRR activity and especially promotes the rational design for SACs. 展开更多
关键词 first-principle calculations Nitrogen reduction p-d orbital hybridization single-atom catalysts
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Optimizing high-coordination shell of Co-based single-atom catalysts for efficient ORR and zinc-air batteries 被引量:1
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作者 Yugang Qi Qing Liang +9 位作者 Kexin Song Xinyan Zhou Meiqi Liu Wenwen Li Fuxi Liu Zhou Jiang Xu Zou Zhongjun Chen Wei Zhang Weitao Zheng 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第8期306-314,I0007,共10页
Atom-level modulation of the coordination environment for single-atom catalysts(SACs)is considered as an effective strategy for elevating the catalytic performance.For the MNxsite,breaking the symmetrical geometry and... Atom-level modulation of the coordination environment for single-atom catalysts(SACs)is considered as an effective strategy for elevating the catalytic performance.For the MNxsite,breaking the symmetrical geometry and charge distribution by introducing relatively weak electronegative atoms into the first/second shell is an efficient way,but it remains challenging for elucidating the underlying mechanism of interaction.Herein,a practical strategy was reported to rationally design single cobalt atoms coordinated with both phosphorus and nitrogen atoms in a hierarchically porous carbon derived from metal-organic frameworks.X-ray absorption spectrum reveals that atomically dispersed Co sites are coordinated with four N atoms in the first shell and varying numbers of P atoms in the second shell(denoted as Co-N/P-C).The prepared catalyst exhibits excellent oxygen reduction reaction(ORR)activity as well as zinc-air battery performance.The introduction of P atoms in the Co-SACs weakens the interaction between Co and N,significantly promoting the adsorption process of ^(*)OOH,resulting in the acceleration of reaction kinetics and reduction of thermodynamic barrier,responsible for the increased intrinsic activity.Our discovery provides insights into an ultimate design of single-atom catalysts with adjustable electrocatalytic activities for efficient electrochemical energy conversion. 展开更多
关键词 ELECTROCATALYTIC Oxygen reduction reaction Single atom catalyst Shell coordination optimization
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Single-atom catalysts for the electrochemical reduction of carbon dioxide into hydrocarbons and oxygenates 被引量:1
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作者 Karl Adrian Gandionco Juwon Kim +2 位作者 Lieven Bekaert Annick Hubin Jongwoo Lim 《Carbon Energy》 SCIE EI CAS CSCD 2024年第3期64-117,共54页
The electrochemical reduction of carbon dioxide offers a sound and economically viable technology for the electrification and decarbonization of the chemical and fuel industries.In this technology,an electrocatalytic ... The electrochemical reduction of carbon dioxide offers a sound and economically viable technology for the electrification and decarbonization of the chemical and fuel industries.In this technology,an electrocatalytic material and renewable energy-generated electricity drive the conversion of carbon dioxide into high-value chemicals and carbon-neutral fuels.Over the past few years,single-atom catalysts have been intensively studied as they could provide near-unity atom utilization and unique catalytic performance.Single-atom catalysts have become one of the state-of-the-art catalyst materials for the electrochemical reduction of carbon dioxide into carbon monoxide.However,it remains a challenge for single-atom catalysts to facilitate the efficient conversion of carbon dioxide into products beyond carbon monoxide.In this review,we summarize and present important findings and critical insights from studies on the electrochemical carbon dioxide reduction reaction into hydrocarbons and oxygenates using single-atom catalysts.It is hoped that this review gives a thorough recapitulation and analysis of the science behind the catalysis of carbon dioxide into more reduced products through singleatom catalysts so that it can be a guide for future research and development on catalysts with industry-ready performance for the electrochemical reduction of carbon dioxide into high-value chemicals and carbon-neutral fuels. 展开更多
关键词 ELECTROCATALYSIS electrochemical CO_(2)reduction hydrocarbons OXYGENATES single-atom catalysts
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Boosting Fischer-Tropsch Synthesis via Tuning of N Dopants in TiO_(2)@CN-Supported Ru Catalysts 被引量:1
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作者 Xincheng Li Yunhao Liu +10 位作者 Dejian Zhao Shuaishuai Lyu Jingwei Ye Xiaoshen Li Peipei Wu Ye Tian Yingtian Zhang Tong Ding Song Song Qingpeng Cheng Xingang Li 《Transactions of Tianjin University》 EI CAS 2024年第1期90-102,共13页
Nitrogen(N)-doped carbon materials as metal catalyst supports have attracted signifi cant attention,but the eff ect of N dopants on catalytic performance remains unclear,especially for complex reaction processes such ... Nitrogen(N)-doped carbon materials as metal catalyst supports have attracted signifi cant attention,but the eff ect of N dopants on catalytic performance remains unclear,especially for complex reaction processes such as Fischer-Tropsch synthesis(FTS).Herein,we engineered ruthenium(Ru)FTS catalysts supported on N-doped carbon overlayers on TiO_(2)nanoparticles.By regulating the carbonization temperatures,we successfully controlled the types and contents of N dopants to identify their impacts on metal-support interactions(MSI).Our fi ndings revealed that N dopants establish a favorable surface environment for electron transfer from the support to the Ru species.Moreover,pyridinic N demonstrates the highest electron-donating ability,followed by pyrrolic N and graphitic N.In addition to realizing excellent catalytic stability,strengthening the interaction between Ru sites and N dopants increases the Ru^(0)/Ru^(δ+)ratios to enlarge the active site numbers and surface electron density of Ru species to enhance the strength of adsorbed CO.Consequently,it improves the catalyst’s overall performance,encompassing intrinsic and apparent activities,as well as its ability for carbon chain growth.Accordingly,the as-synthesized Ru/TiO_(2)@CN-700 catalyst with abundant pyridine N dopants exhibits a superhigh C_(5+)time yield of 219.4 mol CO/(mol Ru·h)and C_(5+)selectivity of 85.5%. 展开更多
关键词 Fischer-Tropsch synthesis N-doped carbon materials Ruthenium catalyst Pyridinic N Metal-N interaction
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Cobalt-based multicomponent nanoparticles supported on N-doped graphene as advanced cathodic catalyst for zinc-air batteries 被引量:1
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作者 Shanjing Liu Xiaohan Wan +7 位作者 Yue Sun Shiqi Li Xingmei Guo Ming Li Rui Yin Qinghong Kong Jing Kong Junhao Zhang 《International Journal of Minerals,Metallurgy and Materials》 SCIE EI CAS CSCD 2022年第12期2212-2220,共9页
To improve the efficiency of cathodic oxygen reduction reaction(ORR)in zinc-air batteries(ZABs),an adsorption-complexation-calcination method was proposed to generate cobalt-based multicomponent nanoparticles comprisi... To improve the efficiency of cathodic oxygen reduction reaction(ORR)in zinc-air batteries(ZABs),an adsorption-complexation-calcination method was proposed to generate cobalt-based multicomponent nanoparticles comprising Co,Co_(3)O_(4)and CoN,as well as numerous N heteroatoms,on graphene nanosheets(Co/Co_(3)O_(4)/CoN/NG).The Co/Co_(3)O_(4)/CoN nanoparticles with the size of less than 50 nm are homogeneously dispersed on N-doped graphene(NG)substrate,which greatly improve the catalytic behaviors for ORR.The results show that the half-wave potential is as high as 0.80 V vs.RHE and the limiting current density is 4.60 mA·cm^(−2),which are close to those of commercially available platinum/carbon(Pt/C)catalysts.Applying as cathodic catalyst for ZABs,the battery shows large specific capacity and open circuit voltage of 843.0 mAh∙g^(−1) and 1.41 V,respectively.The excellent performance is attributed to the efficient two-dimensional structure with high accessible surface area and the numerous multiple active sites provided by highly scattered Co/Co_(3)O_(4)/CoN particles and doped nitrogen on the carbon matrix. 展开更多
关键词 adsorption-complexation-calcination cobalt-based multicomponent nanoparticles N-doped graphene oxygen reduction reaction zinc-air batteries
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Cobalt-Based Cocatalysts for Photocatalytic CO_(2)Reduction 被引量:1
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作者 Mengqing Li Lijuan Shen Min-Quan Yang 《Transactions of Tianjin University》 EI CAS 2022年第6期506-532,共27页
Conversion of carbon dioxide(CO_(2))into valuable chemicals and renewable fuels via photocatalysis represents an eco-friendly route to achieve the goal of carbon neutralization.Although various types of semiconductor ... Conversion of carbon dioxide(CO_(2))into valuable chemicals and renewable fuels via photocatalysis represents an eco-friendly route to achieve the goal of carbon neutralization.Although various types of semiconductor materials have been intensively explored,some severe issues,such as rapid charge recombination and sluggish redox reaction kinetics,remain.In this regard,cocatalyst modifi cation by trapping charges and boosting surface reactions is one of the most effi cient strategies to improve the effi ciency of semiconductor photocatalysts.This review focuses on recent advances in CO_(2)photoreduction over costeff ective and earth-abundant cobalt(Co)-based cocatalysts,which are competitive candidates of noble metals for practical applications.First,the functions of Co-based cocatalysts for promoting photocatalytic CO_(2)reduction are briefl y discussed.Then,diff erent kinds of Co-based cocatalysts,including cobalt oxides and hydroxides,cobalt nitrides and phosphides,cobalt sulfi des and selenides,Co single-atom,and Co-based metal–organic frameworks(MOFs),are summarized.The underlying mechanisms of these Co-based cocatalysts for facilitating CO_(2)adsorption–activation,boosting charge separation,and modulating intermediate formation are discussed in detail based on experimental characterizations and density functional theory calculations.In addition,the suppression of the competing hydrogen evolution reaction using Co-based cocatalysts to promote the product selectivity of CO_(2)reduction is highlighted in some selected examples.Finally,the challenges and future perspectives on constructing more effi cient Co-based cocatalysts for practical applications are proposed. 展开更多
关键词 cobalt-based materials COcatalyst Photocatalysis CO_(2)reduction Solar energy conversion
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The regulation of ferrocene-based catalysts on heat transfer in highpressure combustion of ammonium perchlorate/hydroxyl-terminated polybutadiene/aluminum composite propellants 被引量:1
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作者 Jinchao Han Songqi Hu Linlin Liu 《Defence Technology(防务技术)》 SCIE EI CAS CSCD 2024年第5期174-186,共13页
The regulation of the burning rate pressure exponent for the ammonium perchlorate/hydroxylterminated polybutadiene/aluminum(AP/HTPB/Al)composite propellants under high pressures is a crucial step for its application i... The regulation of the burning rate pressure exponent for the ammonium perchlorate/hydroxylterminated polybutadiene/aluminum(AP/HTPB/Al)composite propellants under high pressures is a crucial step for its application in high-pressure solid rocket motors.In this work,the combustion characteristics of AP/HTPB/Al composite propellants containing ferrocene-based catalysts were investigated,including the burning rate,thermal behavior,the local heat transfer,and temperature profile in the range of 7-28 MPa.The results showed that the exponent breaks were still observed in the propellants after the addition of positive catalysts(Ce-Fc-MOF),the burning rate inhibitor((Ferrocenylmethyl)trimethylammonium bromide,Fc Br)and the mixture of Fc Br/catocene(GFP).However,the characteristic pressure has increased,and the exponent decreased from 1.14 to 0.66,0.55,and 0.48 when the addition of Ce-FcMOF,Fc Br and Fc Br/GFP in the propellants.In addition,the temperature in the first decomposition stage was increased by 7.50℃ and 11.40℃ for the AP/Fc Br mixture and the AP/Fc Br/GFP mixture,respectively,compared to the pure AP.On the other hand,the temperature in the second decomposition stage decreased by 48.30℃ and 81.70℃ for AP/Fc Br and AP/Fc Br/GFP mixtures,respectively.It was also found that Fc Br might generate ammonia to cover the AP surface.In this case,a reaction between the methyl in Fc Br and perchloric acid caused more ammonia to appear at the AP surface,resulting in the suppression of ammonia desorption.In addition,the coarse AP particles on the quenched surface were of a concave shape relative to the binder matrix under low and high pressures when the catalysts were added.In the process,the decline at the AP/HTPB interface was only exhibited in the propellant with the addition of Ce-Fc-MOF.The ratio of the gas-phase temperature gradient of the propellants containing catalysts was reduced significantly below and above the characteristic pressure,rather than 3.6 times of the difference in the blank propellant.Overall,the obtained results demonstrated that the pressure exponent could be effectively regulated and controlled by adjusting the propellant local heat and mass transfer under high and low pressures. 展开更多
关键词 AP/HTPB/Al propellants Heat transfer High-pressure combustion Ferrocene-based catalysts Pressure exponent
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High-rate electrochemical H_(2)O_(2) production over multimetallic atom catalysts under acidic–neutral conditions 被引量:1
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作者 Yueyu Tong Jiaxin Liu +5 位作者 Bing-Jian Su Jenh-Yih Juang Feng Hou Lichang Yin Shi Xue Dou Ji Liang 《Carbon Energy》 SCIE EI CAS CSCD 2024年第1期44-62,共19页
Hydrogen peroxide(H_(2)O_(2))production by the electrochemical 2-electron oxygen reduction reaction(2e−ORR)is a promising alternative to the energy-intensive anthraquinone process,and single-atom electrocatalysts show... Hydrogen peroxide(H_(2)O_(2))production by the electrochemical 2-electron oxygen reduction reaction(2e−ORR)is a promising alternative to the energy-intensive anthraquinone process,and single-atom electrocatalysts show the unique capability of high selectivity toward 2e−ORR against the 4e−one.The extremely low surface density of the single-atom sites and the inflexibility in manipulating their geometric/electronic configurations,however,compromise the H_(2)O_(2) yield and impede further performance enhancement.Herein,we construct a family of multiatom catalysts(MACs),on which two or three single atoms are closely coordinated to form high-density active sites that are versatile in their atomic configurations for optimal adsorption of essential*OOH species.Among them,the Cox–Ni MAC presents excellent electrocatalytic performance for 2e−ORR,in terms of its exceptionally high H_(2)O_(2) yield in acidic electrolytes(28.96 mol L^(−1) gcat.^(−1) h^(−1))and high selectivity under acidic to neutral conditions in a wide potential region(>80%,0–0.7 V).Operando X-ray absorption and density functional theory analyses jointly unveil its unique trimetallic Co2NiN8 configuration,which efficiently induces an appropriate Ni–d orbital filling and modulates the*OOH adsorption,together boosting the electrocatalytic 2e−ORR capability.This work thus provides a new MAC strategy for tuning the geometric/electronic structure of active sites for 2e−ORR and other potential electrochemical processes. 展开更多
关键词 hydrogen peroxide production multiatom catalysts operando X-ray adsorption spectrum reaction mechanism tendency structure-property relation
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Bimetallic In_(2)O_(3)/Bi_(2)O_(3) Catalysts Enable Highly Selective CO_(2) Electroreduction to Formate within Ultra-Broad Potential Windows 被引量:1
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作者 Zhongxue Yang Hongzhi Wang +7 位作者 Xinze Bi Xiaojie Tan Yuezhu Zhao Wenhang Wang Yecheng Zou Huai ping Wang Hui Ning Mingbo Wu 《Energy & Environmental Materials》 SCIE EI CAS CSCD 2024年第1期257-264,共8页
CO_(2)electrochemical reduction reaction(CO_(2)RR)to formate is a hopeful pathway for reducing CO_(2)and producing high-value chemicals,which needs highly selective catalysts with ultra-broad potential windows to meet... CO_(2)electrochemical reduction reaction(CO_(2)RR)to formate is a hopeful pathway for reducing CO_(2)and producing high-value chemicals,which needs highly selective catalysts with ultra-broad potential windows to meet the industrial demands.Herein,the nanorod-like bimetallic ln_(2)O_(3)/Bi_(2)O_(3)catalysts were successfully synthesized by pyrolysis of bimetallic InBi-MOF precursors.The abundant oxygen vacancies generated from the lattice mismatch of Bi_(2)O_(3)and ln_(2)O_(3)reduced the activation energy of CO_(2)to*CO_(2)·^(-)and improved the selectivity of*CO_(2)·^(-)to formate simultaneously.Meanwhile,the carbon skeleton derived from the pyrolysis of organic framework of InBi-MOF provided a conductive network to accelerate the electrons transmission.The catalyst exhibited an ultra-broad applied potential window of 1200 mV(from-0.4 to-1.6 V vs RHE),relativistic high Faradaic efficiency of formate(99.92%)and satisfactory stability after 30 h.The in situ FT-IR experiment and DFT calculation verified that the abundant oxygen vacancies on the surface of catalysts can easily absorb CO_(2)molecules,and oxygen vacancy path is dominant pathway.This work provides a convenient method to construct high-performance bimetallic catalysts for the industrial application of CO_(2)RR. 展开更多
关键词 bimetallic catalyst CO_(2)electrochemical reduction reaction FORMATE oxygen vacancy wide potential window
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Current Status and Perspectives of Dual-Atom Catalysts Towards Sustainable Energy Utilization 被引量:1
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作者 Yizhe Li Yajie Li +7 位作者 Hao Sun Liyao Gao Xiangrong Jin Yaping Li Zhi LV Lijun Xu Wen Liu Xiaoming Sun 《Nano-Micro Letters》 SCIE EI CAS CSCD 2024年第7期402-440,共39页
The exploration of sustainable energy utilization requires the imple-mentation of advanced electrochemical devices for efficient energy conversion and storage,which are enabled by the usage of cost-effective,high-perf... The exploration of sustainable energy utilization requires the imple-mentation of advanced electrochemical devices for efficient energy conversion and storage,which are enabled by the usage of cost-effective,high-performance electro-catalysts.Currently,heterogeneous atomically dispersed catalysts are considered as potential candidates for a wide range of applications.Compared to conventional cata-lysts,atomically dispersed metal atoms in carbon-based catalysts have more unsatu-rated coordination sites,quantum size effect,and strong metal-support interactions,resulting in exceptional catalytic activity.Of these,dual-atomic catalysts(DACs)have attracted extensive attention due to the additional synergistic effect between two adja-cent metal atoms.DACs have the advantages of full active site exposure,high selectiv-ity,theoretical 100%atom utilization,and the ability to break the scaling relationship of adsorption free energy on active sites.In this review,we summarize recent research advancement of DACs,which includes(1)the comprehensive understanding of the synergy between atomic pairs;(2)the synthesis of DACs;(3)characterization meth-ods,especially aberration-corrected scanning transmission electron microscopy and synchrotron spectroscopy;and(4)electrochemical energy-related applications.The last part focuses on great potential for the electrochemical catalysis of energy-related small molecules,such as oxygen reduction reaction,CO_(2) reduction reaction,hydrogen evolution reaction,and N_(2) reduction reaction.The future research challenges and opportunities are also raised in prospective section. 展开更多
关键词 Dual-atom catalysts Synergetic effect ELECTROCATALYSIS Oxygen reduction reaction CO_(2)reduction reaction Hydrogen evolution reaction N2 reduction reaction
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In situ formation of multiple catalysts for enhancing the hydrogen storage of MgH_(2) by adding porous Ni_(3)ZnC_(0.7)/Ni loaded carbon nanotubes microspheres 被引量:1
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作者 Bing Zhang Xiubo Xie +6 位作者 Yukun Wang Chuanxin Hou Xueqin Sun Yuping Zhang Xiaoyang Yang Ronghai Yu Wei Du 《Journal of Magnesium and Alloys》 SCIE EI CAS CSCD 2024年第3期1227-1238,共12页
MgH_(2) is considered one of the most promising hydrogen storage materials because of its safety,high efficiency,high hydrogen storage quantity and low cost characteristics.But some shortcomings are still existed:high... MgH_(2) is considered one of the most promising hydrogen storage materials because of its safety,high efficiency,high hydrogen storage quantity and low cost characteristics.But some shortcomings are still existed:high operating temperature and poor hydrogen absorption dynamics,which limit its application.Porous Ni_(3)ZnC_(0.7)/Ni loaded carbon nanotubes microspheres(NZC/Ni@CNT)is prepared by facile filtration and calcination method.Then the different amount of NZC/Ni@CNT(2.5,5.0 and 7.5 wt%)is added to the MgH_(2) by ball milling.Among the three samples with different amount of NZC/Ni@CNT(2.5,5.0 and 7.5 wt%),the MgH_(2)-5 wt%NZC/Ni@CNT composite exhibits the best hydrogen storage performances.After testing,the MgH_(2)-5 wt%NZC/Ni@CNT begins to release hydrogen at around 110℃ and hydrogen absorption capacity reaches 2.34 wt%H_(2) at 80℃ within 60 min.Moreover,the composite can release about 5.36 wt%H_(2) at 300℃.In addition,hydrogen absorption and desorption activation energies of the MgH_(2)-5 wt%NZC/Ni@CNT composite are reduced to 37.28 and 84.22 KJ/mol H_(2),respectively.The in situ generated Mg_(2)NiH_(4)/Mg_(2)Ni can serve as a"hydrogen pump"that plays the main role in providing more activation sites and hydrogen diffusion channels which promotes H_(2) dissociation during hydrogen absorption process.In addition,the evenly dispersed Zn and MgZn2 in Mg and MgH_(2) could provide sites for Mg/MgH_(2) nucleation and hydrogen diffusion channel.This attempt clearly proved that the bimetallic carbide Ni_(3)ZnC_(0.7) is a effective additive for the hydrogen storage performances modification of MgH_(2),and the facile synthesis of the Ni_(3)ZnC_(0.7)/Ni@CNT can provide directions of better designing high performance carbide catalysts for improving MgH_(2). 展开更多
关键词 Mg-based hydrogen storage material Ni_(3)ZnC_(0.7)/Ni@CNT particles Ni loaded carbon nanotubes Multiple catalysts.
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