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Enhanced stability of nitrogen-doped carbon-supported palladium catalyst for oxidative carbonylation of phenol
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作者 Xiaojing Liu Ruohan Zhao +4 位作者 Hao Zhao Zhimiao Wang Fang Li Wei Xue Yanji Wang 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2024年第1期19-28,共10页
Enhancing the stability of supported noble metal catalysts emerges is a major challenge in both science and industry.Herein,a heterogeneous Pd catalyst(Pd/NCF)was prepared by supporting Pd ultrafine metal nanoparticle... Enhancing the stability of supported noble metal catalysts emerges is a major challenge in both science and industry.Herein,a heterogeneous Pd catalyst(Pd/NCF)was prepared by supporting Pd ultrafine metal nanoparticles(NPs)on nitrogen-doped carbon;synthesized by using F127 as a stabilizer,as well as chitosan as a carbon and nitrogen source.The Pd/NCF catalyst was efficient and recyclable for oxidative carbonylation of phenol to diphenyl carbonate,exhibiting higher stability than Pd/NC prepared without F127 addition.The hydrogen bond between chitosan(CTS)and F127 was enhanced by F127,which anchored the N in the free amino group,increasing the N content of the carbon material and ensuring that the support could provide sufficient N sites for the deposition of Pd NPs.This process helped to improve metal dispersion.The increased metal-support interaction,which limits the leaching and coarsening of Pd NPs,improves the stability of the Pd/NCF catalyst.Furthermore,density functional theory calculations indicated that pyridine N stabilized the Pd^(2+)species,significantly inhibiting the loss of Pd^(2+)in Pd/NCF during the reaction process.This work provides a promising avenue towards enhancing the stability of nitrogen-doped carbon-supported metal catalysts. 展开更多
关键词 Supported Pd catalyst N-doped carbon Amphiphilic triblock copolymer Pyridinic nitrogen STABILITY
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Engineering single-atom Mn on nitrogen-doped carbon to regulate lithium-peroxide reaction kinetics for rechargeable lithium-oxygen batteries
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作者 Yaling Huang Yong Liu +3 位作者 Yang Liu Chenyang Zhang Wenzhang Li Jie Li 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2024年第7期199-207,共9页
Precision engineering of catalytic sites to guide more favorable pathways for Li_(2)O_(2) nucleation and decom-position represents an enticing kinetic strategy for mitigating overpotential,enhancing discharge capac-it... Precision engineering of catalytic sites to guide more favorable pathways for Li_(2)O_(2) nucleation and decom-position represents an enticing kinetic strategy for mitigating overpotential,enhancing discharge capac-ity,and improving recycling stability of Li-O_(2) batteries.In this work,we employ metal-organic frameworks(MOFs)derivation and ion substitution strategies to construct atomically dispersed Mn-N_(4) moieties on hierarchical porous nitrogen-doped carbon(Mn SAs-NC)with the aim of reducing the over-potential and improving the cycling stability of Li-O_(2) batteries.The porous structure provides more chan-nels for mass transfer and exposes more highly active sites for electrocatalytic reactions,thus promoting the formation and decomposition of Li_(2)O_(2).The Li-O_(2) batteries with Mn SAs-NC cathode achieve lower overpotential,higher specific capacity(14290 mA h g^(-1) at 100 mAg^(-1)),and superior cycle stability(>100 cycles at 200 mA g^(-1))compared with the Mn NPs-NC and NC.Density functional theory(DFT)cal-culations reveal that the construction of Mn-N_(4) moiety tunes the charge distribution of the pyridinic N-rich vacancy and balances the affinity of the intermediates(LiO_(2) and Li_(2)O_(2)).The initial nucleation of Li_(2)O_(2) on Mn SAs-NC favors the O_(2)-→LiO_(2)→Li_(2)O_(2) surface-adsorption pathway,which mitigates the overpoten-tials of the oxygen reduction(ORR)and oxygen evolution reaction(OER).As a result,Mn SAs-NC with Mn-N_(4) moiety effectively facilitates the Li_(2)O_(2) nucleation and enables its reversible decomposition.This work establishes a methodology for constructing carbon-based electrocatalysts with high activity and selectivity for Li-O_(2)batteries. 展开更多
关键词 Single-atom Mn MOFs-oriented architecture Rechargeable Li-O_(2)battery N-doped carbon Density functional theory calculation
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PtZn nanoparticles supported on porous nitrogen-doped carbon nanofibers as highly stable electrocatalysts for oxygen reduction reaction
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作者 Lei Zhao Jinxia Jiang +6 位作者 Shuhao Xiao Zhao Li Junjie Wang Xinxin Wei Qingquan Kong Jun Song Chen Rui Wu 《Nano Materials Science》 EI CAS CSCD 2023年第3期329-334,共6页
The oxygen reduction reaction(ORR)electrocatalytic activity of Pt-based catalysts can be significantly improved by supporting Pt and its alloy nanoparticles(NPs)on a porous carbon support with large surface area.Howev... The oxygen reduction reaction(ORR)electrocatalytic activity of Pt-based catalysts can be significantly improved by supporting Pt and its alloy nanoparticles(NPs)on a porous carbon support with large surface area.However,such catalysts are often obtained by constructing porous carbon support followed by depositing Pt and its alloy NPs inside the pores,in which the migration and agglomeration of Pt NPs are inevitable under harsh operating conditions owing to the relatively weak interaction between NPs and carbon support.Here we develop a facile electrospinning strategy to in-situ prepare small-sized PtZn NPs supported on porous nitrogen-doped carbon nanofibers.Electrochemical results demonstrate that the as-prepared PtZn alloy catalyst exhibits excellent initial ORR activity with a half-wave potential(E_(1/2))of 0.911 V versus reversible hydrogen electrode(vs.RHE)and enhanced durability with only decreasing 11 mV after 30,000 potential cycles,compared to a more significant drop of 24 mV in E_(1/2)of Pt/C catalysts(after 10,000 potential cycling).Such a desirable performance is ascribed to the created triple-phase reaction boundary assisted by the evaporation of Zn and strengthened interaction between nanoparticles and the carbon support,inhibiting the migration and aggregation of NPs during the ORR. 展开更多
关键词 PtZn alloy Porous nitrogen-doped carbon nanofibers ELECTROSPINNING Oxygen reduction reaction
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Unraveling the Role of Nitrogen-Doped Carbon Nanowires Incorporated with MnO_(2)Nanosheets as High Performance Cathode for Zinc-Ion Batteries 被引量:1
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作者 Xiaohui Li Qiancheng Zhou +5 位作者 Ze Yang Xing Zhou Dan Qiu Huajun Qiu Xintang Huang Ying Yu 《Energy & Environmental Materials》 SCIE EI CAS CSCD 2023年第3期205-213,共9页
Manganese-based cathode materials are considered as a promising candidate for rechargeable aqueous zinc-ion batteries(ZIBs).Suffering from poor conductive and limited structure tolerance,various carbon matrix,especial... Manganese-based cathode materials are considered as a promising candidate for rechargeable aqueous zinc-ion batteries(ZIBs).Suffering from poor conductive and limited structure tolerance,various carbon matrix,especially N-doped carbon,were employed to incorporate with MnO_(2)for greatly promoted electrochemical performances.However,the related underlying mechanism is still unknown,which is unfavorable to guide the design of high performance electrode.Herein,by incorporating layered MnO_(2)with N-doped carbon nanowires,a free-standing cathode with hierarchical core-shell structure(denoted as MnO_(2)@NC)is prepared.Benefiting from the N-doped carbon and rational architecture,the MnO_(2)@NC electrode shows an enhanced specific capacity(325 mAh g^(−1)at 0.1 A g^(−1))and rate performance(90 mAh g^(−1)at 2 A g^(−1)),as well as improved cycling stability.Furthermore,the performance improvement mechanism of MnO_(2)incorporated by N-doped carbon is investigated by X-ray photoelectron spectroscopy(XPS),Raman spectrums and density functional theory(DFT)calculation.The N atom elongates the Mn-O bond and reduces the valence of Mn^(4+)ion in MnO_(2)crystal by delocalizing its electron clouds.Thus,the electrostatic repulsion will be weakened when Zn^(2+)/H^(+)insert into the host MnO_(2)lattices,which is profitable to more cation insertion and faster ion transfer kinetics for higher capacity and rate capability.This work elucidates a fundamental understanding of the functions of N-doped carbon in composite materials and shed light on a practical pathway to optimize other electrode materials. 展开更多
关键词 core-shell nanostructure MnO_(2)nanosheets N-doped carbon Zn ion batteries
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Bimetallic AgNi nanoparticles anchored onto MOF-derived nitrogen-doped carbon nanostrips for efficient hydrogen evolution
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作者 Dandan Chen Cheng Han +6 位作者 Qiuhong Sun Junyang Ding Qi Huang Ting-Ting Li Yue Hu Jinjie Qian Shaoming Huang 《Green Energy & Environment》 SCIE EI CSCD 2023年第1期258-266,共9页
Hydrogen energy has long been recognized as a clean alternative to conventional fossil fuels,which can be applied in a wide range of transportation and power generation applications.The rational design and engineering... Hydrogen energy has long been recognized as a clean alternative to conventional fossil fuels,which can be applied in a wide range of transportation and power generation applications.The rational design and engineering of high-performance and robust catalysts for hydrogen evolution reaction(HER)shows not a great significance but a challenge for efficient electrochemical water splitting.Herein,a new type of Nibased Ni-ABDC precursor has been obtained,which leads to the formation of N-doped porous carbon nanomaterials uniformly coated with wellproportioned bimetallic AgNi alloys via a stepwise strategy.To their credit,all samples of AgNi/NC-X are structurally calcined from the pristine AgNi-ABDC-X by tuning the different concentration of AgNO3,which means all of them maintain the vermicelli-like morphology compared with Ni-ABDC.The series of AgNi/NC-X materials can be regarded as effective electrocatalysts for HER both in acidic and alkaline media,but an acid-leaching phenomenon is observed.Among them,the as-prepared AgNi/NC-2 exhibits a low overpotential of 103 mV at the current density of 10 mA cm^(-2)and decent durability with a high retention rate of 90.9%after 10 h in 1.0 mol L^(-1)KOH electrolyte.The compelling HER properties of AgNi/NC-2 can be attributed to the synergistic effect between the hierarchical carbon materials,partial N-doping and abundant AgNi alloys.Meanwhile,this study provides a practicable method for the development of efficient HER electrocatalysts for energy applications,which can be conveniently prepared through the reasonable introduction of active components in the crystalline inorganic-organic precursors.©2021 Institute of Process Engineering,Chinese Academy of Sciences.Publishing services by Elsevier B.V.on behalf of KeAi Communications Co.,Ltd.This is an open access article under the CC BY-NC-ND license(http://creativecommons.org/licenses/by-nc-nd/4.0/). 展开更多
关键词 Metal-organic framework carbon nanomaterial AgNi alloy Hydrogen evolution ELECTROCATALYSIS
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Electrocatalytic hydrogen peroxide formation on mesoporous non-metal nitrogen-doped carbon catalyst 被引量:6
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作者 Frédéric Hasché Mehtap Oezaslan +1 位作者 Peter Strasser Tim-Patrick Fellinger 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2016年第2期249-255,共7页
Direct electrochemical formation of hydrogen peroxide(H2O2) from pure O2 and H2on cheap metal-free earth abundant catalysts has emerged as the highest atom-efficient and environmentally friendly reaction pathway and... Direct electrochemical formation of hydrogen peroxide(H2O2) from pure O2 and H2on cheap metal-free earth abundant catalysts has emerged as the highest atom-efficient and environmentally friendly reaction pathway and is therefore of great interest from an academic and industrial point of view. Very recently,novel metal-free mesoporous nitrogen-doped carbon catalysts have attracted large attention due to the unique reactivity and selectivity for the electrochemical hydrogen peroxide formation [1–3]. In this work,we provide deeper insights into the electrocatalytic activity, selectivity and durability of novel metal-free mesoporous nitrogen-doped carbon catalyst for the peroxide formation with a particular emphasis on the influence of experimental reaction parameters such as p H value and electrode potential for three different electrolytes. We used two independent approaches for the investigation of electrochemical hydrogen peroxide formation, namely rotating ring-disk electrode(RRDE) technique and photometric UV–VIS technique. Our electrochemical and photometric results clearly revealed a considerable peroxide formation activity as well as high catalyst durability for the metal-free nitrogen-doped carbon catalyst material in both acidic as well as neutral medium at the same electrode potential under ambient temperature and pressure. In addition, the obtained electrochemical reactivity and selectivity indicate that the mechanisms for the electrochemical formation and decomposition of peroxide are strongly dependent on the p H value and electrode potential. 展开更多
关键词 Electrochemical hydrogen peroxide FORMATION SELECTIVITY Mesoporous nitrogen-doped carbon Green synthesis ELECTROCATALYSIS Metal-free catalysis
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Hierarchically porous nitrogen-doped carbon as cathode for lithium–sulfur batteries 被引量:9
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作者 Rui Wu Siguo Chen +5 位作者 Jianghai Deng Xun Huang Yujie Song Ruiyi Gan Xiaoju Wan Zidong Wei 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2018年第6期1661-1667,共7页
Porous nitrogen-doped carbon is an especially promising material energy storage due to its excellentconductivity, stable physicochemical properties, easy processability, controllable porosity and low price.Herein, we ... Porous nitrogen-doped carbon is an especially promising material energy storage due to its excellentconductivity, stable physicochemical properties, easy processability, controllable porosity and low price.Herein, we reported a novel well-designed hierarchically porous nitrogen-doped carbon (HPNC) via acombination of salt template (ZnC12) and hard template (SiO2) as sulfur host for lithium-sulfur batter-ies. The low-melting ZnC12 is boiled off and leaves behind micropores and small size mesopores duringpyrolysis process, while the silica spheres are removed by acid leaching to generate interconnected 3Dnetwork of macropores. The HPNC-S electrode exhibits an initial specific capacity of 1355 mAh g^-l at 0.IC (IC= 1675 mAh g^-1 ), a high-rate capability of 623 mAh g-l at 2 C, and a small decay of 0.13% per cycleover 300 cycles at 0.2 C. This excellent rate capability and remarkable long-term cyclability of the HPNC-Selectrode are attributed to its hierarchical porous structures for confining the soluble lithium polysulfideas well as the nitrogen doping for high absorbability of lithium polysulfide. 展开更多
关键词 Hierarchically porous structure nitrogen-doped carbon Lithium-sulfur batteries
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Nitrogen-doped carbon nanotube encapsulating cobalt nanoparticles towards efficient oxygen reduction for zinc–air battery 被引量:4
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作者 Haihua Wu Xiaole Jiang +5 位作者 Yifan Ye Chengcheng Yan Songhai Xie Shu Miao Guoxiong Wang Xinhe Bao 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2017年第6期1181-1186,共6页
Nitrogen-doped carbon materials encapsulating 3 d transition metals are promising alternatives to replace noble metal Pt catalysts for efficiently catalyzing the oxygen reduction reaction(ORR). Herein, we use cobalt s... Nitrogen-doped carbon materials encapsulating 3 d transition metals are promising alternatives to replace noble metal Pt catalysts for efficiently catalyzing the oxygen reduction reaction(ORR). Herein, we use cobalt substituted perfluorosulfonic acid/polytetrafluoroethylene copolymer and dicyandiamide as the pyrolysis precursor to synthesize nitrogen-doped carbon nanotube(N–CNT) encapsulating cobalt nanoparticles hybrid material. The carbon layers and specific surface area of N–CNT have a critical role to the ORR performance due to the exposed active sites, determined by the mass ratio of the two precursors. The optimum hybrid material exhibits high ORR activity and stability, as well as excellent performance and durability in zinc–air battery. 展开更多
关键词 nitrogen-doped carbon nanotube Perfluorosulfonic Acid/polytetrafluoroethylene copolymer Cobalt substitution Oxygen reduction reaction Zinc–air battery
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Novel Co_3O_4 Nanoparticles/Nitrogen-Doped Carbon Composites with Extraordinary Catalytic Activity for Oxygen Evolution Reaction(OER) 被引量:4
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作者 Xiaobing Yang Juan Chen +4 位作者 Yuqing Chen Pingjing Feng Huixian Lai Jintang Li Xuetao Luo 《Nano-Micro Letters》 SCIE EI CAS 2018年第1期137-147,共11页
Herein, Co_3O_4 nanoparticles/nitrogen-doped carbon(Co_3O_4/NPC) composites with different structures were prepared via a facile method. Structure control was achieved by the rational morphology design of ZIF-67 precu... Herein, Co_3O_4 nanoparticles/nitrogen-doped carbon(Co_3O_4/NPC) composites with different structures were prepared via a facile method. Structure control was achieved by the rational morphology design of ZIF-67 precursors, which were then pyrolyzed in air to obtain Co_3O_4/NPC composites. When applied as catalysts for the oxygen evolution reaction(OER), the M-Co_3O_4/NPC composites derived from the flower-like ZIF-67 showedsuperior catalytic activities than those derived from the rhombic dodecahedron and hollow spherical ZIF-67. The former M-Co_3O_4/NPC composite displayed a small overpotential of 0.3 V, low onset potential of 1.41 V, small Tafel slope of 83 m V dec^(-1), and a desirable stability.(94.7% OER activity was retained after 10 h.) The excellent performance of the flower-like M-Co_3O_4/NPC composite in the OER was attributed to its favorable structure. 展开更多
关键词 Co3O4 nanoparticles nitrogen-doped carbon ZIF-67 CATALYTIC Oxygen evolution reaction(OER)
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Nitrogen-doped carbon encapsulated in mesoporous TiO2 nanotubes for fast capacitive sodium storage 被引量:2
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作者 Baosong Li Shoaib Anwer +3 位作者 Xinhua Huang Shaohong Luo Jing Fu Kin Liao 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2021年第4期202-210,共9页
Controllable synthesis of insertion-type anode materials with beneficial micro-and nanostructures is a promising approach for the synthesis of sodium-ion storage devices with high-reactivity and excellent electrochemi... Controllable synthesis of insertion-type anode materials with beneficial micro-and nanostructures is a promising approach for the synthesis of sodium-ion storage devices with high-reactivity and excellent electrochemical performance.In this study,we developed a sacrificial-templating route to synthesize TiO_(2)@N-doped carbon nanotubes(TiO_(2)@NC-NTs)with excellent electrochemical performance.The asprepared mesoporous TiO_(2)@NC-NTs with tiny nanocrystals of anatase TiO_(2) wrapped in N-doped carbon layers showed a well-defined tube structure with a large specific surface area of 198 m^(2) g^(-1) and a large pore size of~5 nm.The TiO_(2)@NC-NTs delivered high reversible capacities of 158 m A h g^(-1) at 2 C(1 C=335 m A g^(-1))for 2200 cycles and 146 m A h g^(-1) at 5 C for 4000 cycles,as well as an ultrahigh rate capability of up to 40 C with a capacity of 98 m A h g^(-1).Even at a high current density of 10 C,a capacity of 138 m A h g^(-1) could be delivered over 10,000 cycles.Thus,the synthesis of mesoporous TiO_(2)@NC-NTs was demonstrated to be an efficient approach for developing electrode materials with high sodium storage and long cycle life. 展开更多
关键词 TiO2 nanotubes MoO3 template nitrogen-doped carbon ANODE Sodium-ion battery
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Nitrogen-Doped Carbon Nanotube-Supported Pd Catalyst for Improved Electrocatalytic Performance toward Ethanol Electrooxidation 被引量:2
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作者 Ying Wei Xinyuan Zhang +4 位作者 Zhiyong Luo Dian Tang Changxin Chen Teng Zhang Zailai Xie 《Nano-Micro Letters》 SCIE EI CAS 2017年第3期43-51,共9页
In this study, hydrothermal carbonization(HTC)was applied for surface functionalization of carbon nanotubes(CNTs) in the presence of glucose and urea. The HTC process allowed the deposition of thin nitrogen-doped carb... In this study, hydrothermal carbonization(HTC)was applied for surface functionalization of carbon nanotubes(CNTs) in the presence of glucose and urea. The HTC process allowed the deposition of thin nitrogen-doped carbon layers on the surface of the CNTs. By controlling the ratio of glucose to urea, nitrogen contents of up to 1.7 wt%were achieved. The nitrogen-doped carbon nanotube-supported Pd catalysts exhibited superior electrochemical activity for ethanol oxidation relative to the pristine CNTs.Importantly, a 1.5-fold increase in the specific activity was observed for the Pd/HTC-N1.67%CNTs relative to the catalyst without nitrogen doping(Pd/HTC-CNTs). Furtherexperiments indicated that the introduction of nitrogen species on the surface of the CNTs improved the Pd(0)loading and increased the binding energy. 展开更多
关键词 Direct alcohol fuel cells Hydrothermal carbonization nitrogen-doped carbon nanotubes Pdbased catalyst Ethanol electrocatalyst
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A correlation between structural changes in a Ni-Cu catalyst during decomposition of ethylene/ammonia mixture and properties of nitrogen-doped carbon nanofibers 被引量:1
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作者 O. Yu. Podyacheva A. N. Shmakov +4 位作者 A. I. Boronin L. S. Kibis S. V. Koscheev E. Yu. Gerasimov Z. R. Ismagilov 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2013年第2期270-278,共9页
Changes of a 65Ni25Cu10A1203 catalyst consisting of Ni-enriched and Cu-enriched alloys were investigated in the bulk and on the surface during the growth of nitrogen-doped carbon nanofibers (N-CNFs) by decomposition... Changes of a 65Ni25Cu10A1203 catalyst consisting of Ni-enriched and Cu-enriched alloys were investigated in the bulk and on the surface during the growth of nitrogen-doped carbon nanofibers (N-CNFs) by decomposition of a 50%C2I-I4/50%NH3 mixture using in situ X-ray diffraction (XRD) analysis, ex situ X-ray photoelectron spectroscopy (XPS) and transmission electron microscopy (TEM) techniques. It was shown that N-CNF growth at 450-650 ℃is accompanied by dissolution of carbon and nitrogen in the Ni-enriched alloy, whereas Cu-enriched alloy remains inactive. A correlation between nickel and copper surface concentrations and properties of N-CNFs in relation to the nitrogen content was found. It was demonstrated that phase composition of the catalyst during N-CNF growth determines the type of N-CNFs structure. 展开更多
关键词 carbon nanofibers nitrogen-doped carbon nanofibers XRD in situ XPS CATALYST
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Robust copper nanocrystal/nitrogen-doped carbon monoliths as carbon monoxide-resistant electrodes for methanol oxidation reaction 被引量:1
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作者 Fei Chen Na Wu +4 位作者 Meixu Zhai Xue Zhang Ruihong Guo Tuoping Hu Mingming Ma 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2021年第7期247-255,共9页
Noble metal-based electrocatalysts present high activities for methanol oxidation reaction(MOR),but are limited by their high cost,low stability and poor resistance to carbon monoxide(CO) poisoning.The development of ... Noble metal-based electrocatalysts present high activities for methanol oxidation reaction(MOR),but are limited by their high cost,low stability and poor resistance to carbon monoxide(CO) poisoning.The development of active and stable non-noble metal electrocatalysts for MOR is desired,but remains a challenge.Herein,we report a simple strategy to make copper nanocrystal/nitrogen-doped carbon(Cu/N-C)monoliths,which can serve as active and robust electrodes for MOR.Copper nanocrystals were electrochemically deposited onto a conductive polyaniline hydrogel and calcined to form Cu/N-C monolith,where the active copper nanocrystals are protected by nitrogen-doped carbon.Owing to their extremely high electrical conductivity(1.25 × 10^(5) S cm^(-1)) and mechanical robustness,these Cu/N-C monoliths can be directly used as electrodes for MOR,without using substrates or additives.The optimal Cu/N-C(FT)@500 monolith shows a high MOR activity of 189 mA cm^(-2) at 0.6 V vs.SCE in alkaline methanol solution,superior to most of reported Cu-based MOR catalysts.Cu/N-C(FT)@500 also presents a better stability than Pt/C catalyst in the long-term MOR test at high current densities.Upon carbon monoxide(CO) poisoning,Cu/N-C(FT)@500 retains 96% of its MOR activity,far exceeding the performance of Pt/C catalyst(61% retention).Owing to its facile synthesis,outstanding activity,high stability and mechanical robustness,Cu/N-C(FT)@500 monolith is promising as a low-cost,efficient and CO-resistant electrocatalyst for MOR. 展开更多
关键词 Copper nanocrystal Methanol oxidation reaction Non-noble metal-based electrocatalysts Poison-resistant electrocatalysts nitrogen-doped carbon
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Ultrafine VN nanodots induced generation of abundant cobalt single-atom active sites on nitrogen-doped carbon nanotube for efficient hydrogen evolution 被引量:1
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作者 Yan Cheng Juhui Gong +7 位作者 Bo Cao Xuan Xu Peng Jing Shien-Ping Feng Rui Cheng Baocang Liu Rui Gao Jun Zhang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2022年第5期646-657,共12页
Development of highly active and stable non-noble electrocatalysts with well-defined nanostructures is crucial for efficient hydrogen evolution reaction(HER). Herein, a novel three-dimensional(3D) selfsupported electr... Development of highly active and stable non-noble electrocatalysts with well-defined nanostructures is crucial for efficient hydrogen evolution reaction(HER). Herein, a novel three-dimensional(3D) selfsupported electrode consists of vanadium nitride(VN) nanodots and Co nanoparticles co-embedded and highly active single Co atoms anchored in N-doped carbon nanotubes supported on carbon cloth(VN-Co@CoSAs-NCNTs/CC) is fabricated via a one-step in situ nanoconfined pyrolysis strategy, which shows remarkable enhanced HER electrocatalytic activity in acidic medium. During pyrolysis, the formed VN nanodots induce the generation of atomic Co Nxsites in NCNTs, contributing to superior electrocatalytic activity. Experimental and density functional theory(DFT) calculation results reveal that the electrode has multiple accessible active sites, fast reaction kinetics, low charge/mass transfer resistances,high conductivity, as well as downshifted d-band center with a thermodynamically favorable hydrogen adsorption free energy(△G_(H·)), all of which greatly boost the HER performance. As a result, the VNCo@CoSAs-NCNTs/CC electrode displays superb catalytic performance toward HER with a low overpotential of 29 mV at 10 mA cm^(-2) in acidic medium, which could maintain for at least 60 h of stable performance. This work opens a facile avenue to explore low-cost, high performance, but inexpensive metals/nitrogen-doped carbon composite electrocatalysts for HER. 展开更多
关键词 Single cobalt atoms nitrogen-doped carbon nanotubes Vanadium nitride nanodots Cobalt nanoparticles Hydrogen evolution reaction
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Pre-fixing defects in carbon framework for revealing the active sites of oxygen reduction reaction at nitrogen-doped carbon nanotubes 被引量:1
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作者 Bing Huang Kun Hou +2 位作者 Yang Liu Rongtao Hu Lunhui Guan 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2021年第12期521-527,I0012,共8页
Nitrogen-doped carbon-based materials are promising non-platinum group metal electrocatalysts for the oxygen reduction reaction(ORR).Understanding their ORR active sites is vital for the rational design and developmen... Nitrogen-doped carbon-based materials are promising non-platinum group metal electrocatalysts for the oxygen reduction reaction(ORR).Understanding their ORR active sites is vital for the rational design and development of nitrogen-doped carbon-based electrocatalysts with enhanced catalytic efficiency and selectivity.However,the conclusive analysis of the ORR mechanism of nitrogen-doped carbon-based electrocatalysts remains a grand challenge because the catalysts have a complex inhomogeneous structure.Here,we elucidate this problem using nitrogen-doped carbon nanotubes framework catalysts with fixed defect concentrations prepared by pre-thermal treatment at a low temperature.The generation of defects under high-temperature treatment was effectively suppressed to enable a simple model for ORR mechanism study.A correlation between ORR pathways and the different nitrogen species in the nitrogen-doped carbon catalysts was revealed through a combination of structural and electrochemical properties investigations.Besides,our results also demonstrate the importance of defects for ORR.We believe that the results will provide instructive guidance for designing and developing novel carbon nanomaterials for ORR. 展开更多
关键词 ELECTROCATALYSTS Oxygen reduction reaction DEFECTS nitrogen-doped carbon nanotube
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Metallurgical pyrolysis toward Co@Nitrogen-doped carbon composite for lithium storage 被引量:1
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作者 Yanyan Liu Kang Sun +4 位作者 Jianchun Jiang Wenshu Zhou Yuan Shang Chenxia Du Baojun Li b 《Green Energy & Environment》 SCIE CSCD 2021年第1期91-101,共11页
Elemental state matter-heteroatom-doped carbon composites are of great importance for the development of anode in lithium ion batteries(LIBs).In this article,metal–organic frameworks(MOFs)are adopted as precursor to ... Elemental state matter-heteroatom-doped carbon composites are of great importance for the development of anode in lithium ion batteries(LIBs).In this article,metal–organic frameworks(MOFs)are adopted as precursor to prepare Co composites via metallurgical pyrolysis under controllable conditions.The obtained nitrogen-doped porous carbon-Co nanocomposite possesses core–shell structure(Co@C–N).Co@C–N exhibits the best Li storage performances as anode active matter.After the 200th cycles at current density of 0.2 A g^(-1),a reversible capacity of 870 mAh g^(-1)is retained.A reversible capacity of 275 mAh g^(-1)still maintains with 5 A g^(-1).Co@C–N presents a high reversible capacity with excellent cycle stability.Considering the corresponding experimental and theoretical results,the Co0-based N-doped porous carbon composite is proposed to work as LIBs anode matter.These results provide a new design idea for electrode matters of metallic ion battery,and demonstrate that MOFs pyrolysis is an effective method for the construction of elemental state anode materials. 展开更多
关键词 Co nanoparticles(NPs) Core–shell structure Lithium ion battery anode Metal–organic framework(MOF) nitrogen-doped carbon
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Metal Oxide/Nitrogen-Doped Carbon Catalysts Enables Highly Effi cient CO_(2) Electroreduction 被引量:1
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作者 Han Shi Yingying Cheng Peng Kang 《Transactions of Tianjin University》 EI CAS 2021年第3期269-277,共9页
The metal oxide/nitrogen-doped carbon(NC)compounds zirconium oxide/NC(ZrO_(2)/NC)and cerium oxide/NC(CeO_(2)/NC)were synthesized via the pyrolysis of polyaniline on the metal oxide surface.The characterization of the ... The metal oxide/nitrogen-doped carbon(NC)compounds zirconium oxide/NC(ZrO_(2)/NC)and cerium oxide/NC(CeO_(2)/NC)were synthesized via the pyrolysis of polyaniline on the metal oxide surface.The characterization of the ZrO_(2)/NC and CeO_(2)/NC catalysts showed more active CO_(2) reduction reaction activity than that of NC catalyst without metal oxide.Gas chromatography analysis revealed that CO and H_(2)were the primary products,and no liquid-phase products were detected via proton nuclear magnetic resonance spectroscopy or high-performance liquid chromatography.The maximum Faraday effi ciency of ZrO_(2)/NC reached 90%at−0.73 V(vs.RHE),with the current density of CO at 5.5 mA/cm^(2);this Faraday effi ciency value was higher than that of NC(41%),with the current density of CO at 3.1 mA/cm^(2).The interaction between the metal oxide and carbon allowed the effi cient formation of defect sites,especially imine-type nitrogen,strengthening the adsorption of the key reaction intermediate CO_(2)^(•−) and thus promoting the CO_(2) reduction reaction. 展开更多
关键词 Metal oxide nitrogen-doped carbon Interface eff ect CO_(2)reduction reaction
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Stabilising Cobalt Sulphide Nanocapsules with Nitrogen-Doped Carbon for High-Performance Sodium-Ion Storage 被引量:1
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作者 Yilan Wu Rohit RGaddam +4 位作者 Chao Zhang Hao Lu Chao Wang Dmitri Golberg Xiu Song Zhao 《Nano-Micro Letters》 SCIE EI CAS CSCD 2020年第4期29-40,共12页
Conversion-type anode materials with a high charge storage capability generally su er from large volume expansion, poor electron conductivity, and sluggish metal ion transport kinetics. The electrode material describe... Conversion-type anode materials with a high charge storage capability generally su er from large volume expansion, poor electron conductivity, and sluggish metal ion transport kinetics. The electrode material described in this paper, namely cobalt sulphide nanoparticles encapsulated in carbon cages(Co9S8@NC), can circumvent these problems. This electrode material exhibited a reversible sodium-ion storage capacity of 705 mAh g^-1 at 100 mA g^-1 with an extraordinary rate capability and good cycling stability. Mechanistic study using the in situ transmission electron microscope technique revealed that the volumetric expansion of the Co9S8 nanoparticles is bu ered by the carbon cages, enabling a stable electrode–electrolyte interface. In addition, the carbon shell with high-content doped nitrogen significantly enhances the electron conductivity of the Co9S8@NC electrode material and provides doping-induced active sites to accommodate sodium ions. By integrating the Co9S8@NC as negative electrode with a cellulose-derived porous hard carbon/graphene oxide composite as positive electrode and 1 M NaPF6 in diglyme as the electrolyte, the sodium-ion capacitor full cell can achieve energy densities of 101.4 and 45.8 Wh kg^-1 at power densities of 200 and 10,000 W kg^-1, respectively. 展开更多
关键词 Cobalt sulphide nitrogen-doped carbon Core–shell structure Sodium-ion capacitors
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Synthesis of alumina-nitrogen-doped carbon support for CoMo catalysts in hydrodesulfurization process 被引量:2
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作者 Zhentao Chen Yaxin Liu +7 位作者 Jian Chen Yang Zhao Tao Jiang Fangyu Zhao Jiahuan Yu Haoxuan Yang Fan Yang Chunming Xu 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2022年第1期392-402,共11页
More stringent environmental legislation imposes severe requirements to reduce the sulfur content in diesel to ultra-low levels with high efficient catalysts.In this paper,a series of CoMo/NDC@alumina catalysts were s... More stringent environmental legislation imposes severe requirements to reduce the sulfur content in diesel to ultra-low levels with high efficient catalysts.In this paper,a series of CoMo/NDC@alumina catalysts were synthesized by combination of the chemical vapor deposition of nitrogen-doped carbon(NDC)using 1,10-phenanthroline and co-impregnation of Mo and Co active components.The optimal catalyst with additive of 25%1,10-phenanthroline was screened by a series of property characterization and the hydrodesulfrization(HDS)active test.The amount of“CoMoS”active phase of the optimal CoMo/C3 catalyst increased 5.3%as compared with the CoMo/c-Al_(2)O_(3).The introduction of NDC improved the sulfidation degree of Mo by 21.8%as compared to the CoMo/c-Al_(2)O_(3) catalyst,which was beneficial to form more active sites.The HDS conversion of the NDC supported catalysts are higher than CoMo/c-Al_(2)O_(3) whether for the dibenzothiophene(DBT)or 4,6-dimethyl dibenzothiophene(4,6-DMDBT).Further hydroprocessing evaluation with Dagang diesel revealed that the CoMo/C3 catalyst possessed higher HDS property and the removal rate of DBTs in the diesel increased by 4%–11%as compared to the CoMo/c-Al_(2)O_(3) catalyst. 展开更多
关键词 nitrogen-doped carbonmaterials Catalyst hydrodesulfurization(HDS) Diesel Dibenzothiophene(DBT)
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Hollow cobalt oxide nanoparticles embedded in nitrogen-doped carbon nanosheets as an efficient bifunctional catalyst for Zn–air battery 被引量:5
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作者 Yuhui Tian Li Xu +6 位作者 Jian Bao Junchao Qian Huaneng Su Huaming Li Haidong Gu Cheng Yan Henan Li 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2019年第6期59-66,共8页
Rational design of low-cost, highly electrocatalytic activity, and stable bifunctional electrocatalysts for oxygen reduction reaction(ORR) and oxygen evolution reaction(OER) has been a great significant for metal–air... Rational design of low-cost, highly electrocatalytic activity, and stable bifunctional electrocatalysts for oxygen reduction reaction(ORR) and oxygen evolution reaction(OER) has been a great significant for metal–air batteries. Herein, an efficient bifunctional electrocatalyst based on hollow cobalt oxide nanoparticles embedded in nitrogen-doped carbon nanosheets(Co/N-Pg) is fabricated for Zn–air batteries. A lowcost biomass peach gum, consisting of carbon, oxygen, and hydrogen without other heteroatoms, was used as carbon source to form carbon matrix hosting hollow cobalt oxide nanoparticles. Meanwhile, the melamine was applied as nitrogen source and template precursor, which can convert to carbon-based template graphitic carbon nitride by polycondensation process. Owing to the unique structure and synergistic effect between hollow cobalt oxide nanoparticles and Co-N-C species, the proposal Co/N-Pg catalyst displays not only prominent bifunctional electrocatalytic activities for ORR and OER, but also excellent durability. Remarkably, the assembled Zn–air battery with Co/N-Pg air electrode exhibited a low discharge-charge voltage gap(0.81 V at 50 mA cm^-2) and high peak power density(119 mW cm^-2) with long-term cycling stability. This work presents an effective approach for engineering transition metal oxides and nitrogen modified carbon nanosheets to boost the performance of bifunctional electrocatalysts for Zn–air battery. 展开更多
关键词 Zn-air batteries OXYGEN reduction REACTION OXYGEN evolution REACTION nitrogen-doped carbon NANOSHEETS Cobalt oxides
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