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MOF-derived Cu embedded into N-doped mesoporous carbon as a robust support of PdAu nanocatalysts for ethanol electrooxidation

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Rare Metals 2024年第3期43卷 1083-1094页

作者： Yu-Fu Huang Peng Wu Jun-Ping Tang Jian Yang Jing Li Shuai Chen Xue-Ling Zhao ChengChen Bin-Wei Zhang Yan-Yun Ma Wei-Heng Shi Dong-Hai Lin Shi-Gang Sun School of Energy and Materials Shanghai Engineering Research Center of Advanced Thermal Functional MaterialsShanghai Key Laboratory of Engineering Materials Application and EvaluationShanghai Polytechnic UniversityShanghai201209China State Key Laboratory of Physical Chemistry of Solid Surfaces Department of ChemistryCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamen361005China School of Chemistry and Chemical Engineering Chongqing UniversityChongqing401331China Center of Advanced Energy Technology and Electrochemistry Institute of Advanced Interdisciplinary StudiesChongqing UniversityChongqing400044China Institute of Functional Nano&Soft Materials(FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials&DevicesSoochow UniversitySuzhou215123China Department of Materials Science and Engineering Drexel UniversityPhiladelphiaPA19104USA

Metal-organic frameworks(MOFs)h ave attracted widespread attention due to their large surface area and porous structure.Rationally designing the nanostructures of MOFs to promote their application in ethanol electrooxidation is still a challenge.Here,a novel Cu-NCNs(Cu-nitrogen-doped carbon nanotubes)support was synthesized by pyrolysis of melamine(MEL)and Cu-ZIF-8 together,and then,Pd-Au nanoalloys were loaded by sodium borohydride reduction method to prepare PdAu@Cu-NCNs catalysts.The generating mesoporous carbon with high specific surface area and favorable electron and mass transport can be used as a potential excellent carrier for PdAu nanoparticles.In addition,the balance of catalyst composition and surface structure was tuned by controlling the content of Pd and Au.Thus,the best-performed Pd_(2)Au_(2)@Cu-NCN-1000-2(where 1000 means the carrier calcination temperature,and 2 means the calcination constant temperature time)catalyst exhibits better long-term stability and electrochemical activity for ethanol oxidation in alkaline media(4.80 A·mg^(-1)),which is 5.05 times higher than that of commercial Pd/C(0.95 A·mg^(-1)).Therefore,this work is beneficial to further promoting the application of MOFs in direct ethanol fuel cells(DEFCs)and can be used as inspiration for the design of more efficient catalyst support structures.

关键词： Metal-organic frameworks(MOFs) N-doped mesoporous carbon PdAu Ethanol electrooxidation

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Sintering and mechanical properties of carbon bulks from ordered mesoporous carbon and nano diamond

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Journal of Advanced Ceramics 2022年第11期11卷 1815-1823页

作者： Bowen MIAO Junzhuo WANG Jianlin LI Shijia GU Lianjun WANG Wan JIANG State Key Laboratory for Modification of Chemical Fibers and Polymer Materials College of Materials Science and EngineeringDonghua UniversityShanghai 201620China State Key Laboratory of Marine Resource Utilization in South China Sea School of Materials Science and EngineeringHainan UniversityHaikou 570228China

Powder metallurgy is important in material preparation.Due to the inertness of carbon materials,however,sintering powdered carbon into physically coherent bulks has been a great challenge even at a high temperature(2000).Improving the sintering activity of carbon powders is℃the key to the success of the consolidation of the carbon powders.Here ordered mesoporous carbon(OMC)is used as the starting material to produce highly homogeneous novel carbon bulks.During sintering at 1800,the huge specific surface area of the OMC greatly promotes the migration of℃carbon atoms and thus the sintering of the OMC by surface diffusion mechanism.When nanodiamond(ND)is added,the volume expansion associated with the phase transformation of diamond to graphite facilitates the densification of the powder compacts.The strong connection between the OMC and the graphite onions derived from the ND bestows the as-prepared carbon bulks with excellent mechanical properties.The current research pioneers a novel way to prepare high-strength carbon materials at relatively low temperatures.

关键词： mesoporous carbon nanodiamond(ND) carbon material high strength

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Controllable assembly of nitrogen-doped mesoporous carbon with different pore structures onto CNTs for excellent lithium storage

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Nano Research 2023年第3期16卷 3879-3887页

作者： Haitao Li Xiao Fang Fengting Lv Wei Yu Hui Cheng Haijiao Zhang Institute of Nanochemistry and Nanobiology School of Environmental and Chemical EngineeringShanghai UniversityShanghai 200444China School of Environmental and Materials Engineering College of EngineeringShanghai Polytechnic UniversityShanghai 201209China Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education) Nankai UniversityTianjin 300071China

mesoporous carbon nanomaterials have shown a great application potential in energy storage and conversion fields due to their outstanding conductivity,tunable pore structure,and good chemical stability.Nevertheless,how to accurately control the pore structure,especially directly assembling the mesoporous carbon onto different substrates remains a big challenge.Herein,we have successfully assembled two kinds of highly nitrogen-doped mesoporous carbon onto carbon nanotubes(NMC/CNTs)based on a facile cooperative assembly process assisted by triblock PEO_(20)PPO_(70)PEO_(20)(P123)and PEO_(106)PPO_(70)PEO_(106)(F127)copolymers.The experimental results indicate that the P_(123)/F_(127)mass ratio has a profound effect on the pore structure,leading to the formation of NMC/CNTs composites with spherical pore structure(S-NMC/CNTs)and cylindrical pore structure(CNMC/CNTs).In virtue of fast electron/ion transfer kinetics,the as-prepared S-NMC/CNTs anode demonstrates an excellent electrochemical performance for lithium-ion batteries,and it delivers a high reversible capacity of 588.1 mAh∙g^(−1)at the current of 0.1 A∙g^(−1)after 100 cycles,along with a superior cycling stability.Specifically noted,the controlled assembly route developed in our work can also be applied to other support materials with different structures and compositions.

关键词： mesoporous carbon carbon nanotubes controllable assembly formation mechanism lithium-ion batteries

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Size and structure tuning of FePt nanoparticles on hollow mesoporous carbon spheres as efficient catalysts for oxygen reduction reaction

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Rare Metals 2023年第6期42卷 1865-1876页

作者： Cheng Yang Han-Bin Wang Pei Liang Bin-Feng Wu Lei Zhao Ping-Shu Leng Lin Lv Hou-Zhao Wan Hao Wang School of Microelectronics Hubei UniversityWuhan430062China Hubei Yangtze Memory Laboratories Wuhan430205China College of Optical and Electronic Technology China Jiliang UniversityHangzhou310018China

Finding and designing cathode oxygen reduction reaction(ORR) catalysts with high activity and stability in acidic electrolyte is essential for the large-scale application of fuel cells and metal-air batteries.Pt-based alloys have emerged as potential electrocatalysts for the oxygen reduction reaction.Herein,we adapted a simple pyrolytic reduction method to grow FePt nanoalloys on hollow mesoporous carbon supports.Benefiting from the ultra-high specific surface of the hollow mesoporous carbon,the in situ formed FePt NPs were homogenously deposited on the carbon supports with size smaller than5 nm.The optimized FePt-HMCS showed a remarkably increased mass activity(MA) of 0.582 A·mg^(-1)_(Pt) at 0.75 V in ORR,being 6.3 times higher than that of commercial Pt/C(0.093 A·mg^(-1)_(Pt)).Meanwhile,the FePt NPs showed negligible decay in mass activity with 21 mV of negative shift in the half-wave potential after 5000 electrochemical cycles,which is more stable than that of commercial Pt/C(6.6% decay in MA with 30 mV of negative shift).The study demonstrated a simple strategy for controlling the alloy size with enhanced metal-support interactions to boost their promising application in fuel cells.

关键词： Oxygen reduction Electrocatalysts mesoporous carbon FePt alloy

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Rational design of ultrafine FeSe_(2) nanocrystals emb e dde d within hollow mesoporous carbon bowls for potassium-ion batteries with long-term cycling stability and high volumetric capacity

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Journal of Materials Science & Technology 2023年第12期143卷 129-139页

作者： Yu Jin Jang Hong Geun Oh Seung-Keun Park Department of Advanced Materials Engineering Chung-Ang University4726Seodong-daeroDaedeok-myeonAnseong-siGyeonggi-do 17546Republic of Korea

Hollow structures are commonly used to alleviate the mechanical stress on electrode materials and to provide more active sites in potassium-ion batteries(KIBs).Nevertheless,the excessive internal voids within these structures significantly reduce the packing density of particles,resulting in a relatively low volumetric energy density of the fabricated electrodes,which is undesirable for practical use.We designed a hollow mesoporous carbon bowl embedded with ultrafine bis(selanylidene)iron(FeSe 2)nanocrystals(FeSe 2@HMCB)via a controllable impregnation method and subsequent selenization pro-cess for high-performance KIBs.The as-obtained FeSe 2@HMCB can inherit the advantages of conventional hollow carbon-based composites,such as alleviation of volume variation in active materials,abundant ion storage sites,and high electrical conductivity.Simultaneously,the bowl structure has a higher pack-ing density than the conventional hollow structure,resulting in a significant increase in the volumet-ric energy density of the fabricated electrodes.Because of these advantages,the FeSe 2@HMCB exhibits a high,stable reversible capacity of 326 mA h g^(-1) even after 1000 cycles at 0.5 A g^(-1),and excellent rate capacities(182 mA h g^(-1) at 3.0 A g^(-1)).Compared with the hollow structured counterpart,the vol-umetric capacity(mA h cm−3)of FeSe 2@HMCB increased by 60%.Furthermore,a full cell consisting of FeSe 2@HMCB//Prussian blue(PB)exhibits excellent electrochemical performance(99 mA h g^(-1) after 100 cycles at 0.1 A g^(-1)).

关键词： Potassium-ion batteries Iron selenide Bowl-like structure mesoporous carbon Anode material

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Semi-closed synthesis of nitrogen and oxygen Co-doped mesoporous carbon for selective aqueous oxidation

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Green Energy & Environment 2022年第1期7卷 43-52页

作者： Chen Xing Daihui Yang Yan Zhang Tian Sun Junfei Duan Hussein A.Younus Shiguo Zhang College of Materials Science and Engineering Hunan Province Key Laboratory for Advanced Carbon Materials and Applied TechnologyHunan UniversityChangsha410082China School of Materials Science and Engineering Changsha University of Science and TechnologyChangsha410004China Chemistry Department Faculty of ScienceFayoum UniversityFayoum63514Egypt

Heteroatom-doped meso/micro-porous carbon materials are conventionally produced by harsh carbonization under an inert atmosphere involving specific precursors,hard/soft templates,and heteroatom-containing agents.Herein,we report a facile synthesis of N and O co-doped meso/micro-porous carbon(NOMC)by template-free carbonization of a small-molecule precursor in a semi-closed system.The semi-closed carbonizaiton process yields hydrophilic NOMCs with large surface area in a high yield.The porous structure as well as the elemental composition of NOMCs can be modulated by changing the holding time at a particular temperature.NOMCs as metal-free heterogeneous catalysts can selectively oxidize benzyl alcohol and its derivatives into aldehydes/ketones with>85%conversion in aqueous solution,which is much higher than that of the control sample obtained in tube furnace(21%conversion),mainly due to their high N content,high percentage of pyridinic N,and large surface area.The presence of O-containing moieties also helps to improve the hydrophilicity and dispersion ability of catalysts and thus facilitates the mass transfer process during aqueous oxidation.The NOMC catalysts also dispayed excellent activity for a wide range of substrates with a selectivity of>99%.

关键词： Semi-closed carbonization Nitrogen and oxygen doping mesoporous carbon Metal-free catalyst Selective aqueous oxidation

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Two-dimensional CoNi@mesoporous carbon composite with heterogeneous structure toward broadband microwave absorber

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Nano Research 2022年第9期15卷 7769-7777页

作者： Yun Qiu Haibo Yang Fanfan Hu Ying Lin Shaanxi Key Laboratory of Green Preparation and Functionalization for Inorganic Materials School of Materials Science and EngineeringShaanxi University of Science and TechnologyXi’an 710021China Jiangsu Product Quality Testing&Inspection Institute Nanjing 210007China

Constructing composites with heterogeneous structure and dual loss mechanism shows great potential in designing microwave absorbers.In this work,two-dimensional cobalt and nickel alloys@mesoporous carbon(CoNi@MC)composites were constructed via using CoNi layered double hydroxide@mesoporous polydopamine(CoNi LDH@MPDA)as sacrifice template.During the pyrolysis process,the MPDA is transformed into mesoporous carbon coated the surface of CoNi LDH that is further reduced to CoNi alloys.The mesoporous structure is conducive to the multi-reflection of electromagnetic waves and facilitates optimizing impedance matching.Heterogeneous interfaces between CoNi alloys and mesoporous carbon induce interface polarization.Multiple attenuation mechanism promotes the electromagnetic waves conversion.The maximum reflection loss of CoNi@MC composite is−70.86 dB and the widest effective absorption bandwidth is 7.74 GHz covering almost the entire Ku band.This strategy will be a guidance for designing electromagnetic absorbers.

关键词： CoNi alloys mesoporous carbon microwave absorption broad efficient frequency

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Organic salt-derived phosphorus-doped mesoporous carbon for high performance supercapacitors

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中国化学快报:英文版 2023年第8期34卷 421-424页

作者： Huan Liu Longfeng Hu Razium A.Soomro Bin Xu College of Materials Science and Engineering Xi’an University of Science and TechnologyXi’an 710054China State Key Laboratory of Organic-Inorganic Composites Beijing Key Laboratory of Electrochemical Process and Technology for MaterialsBeijing University of Chemical TechnologyBeijing 100029China

Phosphorus-doped mesoporous carbons(PMCs)were prepared using a self-doping and self-templating approach via direct pyrolysis of sodium phytate(C_(6)H_(17)NaO_(24)P_(6)).The one-pot method allows simultaneous carbonization and P doping,eliminating the need for pre-synthesis or post-activation treatment.The C_(6)H_(17)NaO_(24)P_(6)is the source of both carbon and phosphorus,and the nano-Na_(4)P_(2)O_(7)particles produced during pyrolysis act as hard templates for the honeycomb mesoporous structure with high specific surface area(884–827m^(2)/g),large mesopore volume ratio(67%–75%)and rich phosphorus content(0.53–2.34 at%).As electrodes of supercapacitors in 6 mol/L KOH,the PMCs showed outstanding performance with a high capacitance of 202 F/g and excellent rate performance of 148 F/g at 30 A/g.In addition,the PMCs-based symmetrical supercapacitors can operate in an expanded working voltage of 0–1.6 V in 3mol/L H_(2)SO_(4)aqueous electrolytes with high-density energy of 11.8 Wh/kg.

关键词： Supercapacitors mesoporous carbon Phosphorus doping Expanded voltage window Heteroatoms doping

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g-C_(3)N_(4) templated mesoporous carbon with abundant heteroatoms as high-rate anode material for dual-carbon sodium ion hybrid capacitors

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Journal of Materiomics 2022年第6期8卷 1149-1157页

作者： Chong Wang Qingtao Yu Ning Zhao Bohan Li Wanci Shen Feiyu Kang Zheng-Hong Huang Ruitao Lv State Key Laboratory of New Ceramics and Fine Processing School of Materials Science and EngineeringTsinghua UniversityBeijing100084China Key Laboratory of Advanced Materials(MOE) School of Materials Science and EngineeringTsinghua UniversityBeijing100084China Engineering Laboratory for Functionalized carbon Materials Shenzhen Key Laboratory for Graphene-based MaterialsGraduate School at ShenzhenTsinghua UniversityShenzhen518055China School of Materials Science and Engineering University of Science and Technology BeijingBeijing100083China

Sodium ion hybrid capacitors(SIHCs)are regarded as advanced power supply systems.Nevertheless,the kinetics imbalance of cathode and anode suppresses the further performance improvement of SIHCs.The carbonaceous anode materials are promising and many strategies have been utilized to increase the capacity of sloping region or accelerate the reaction rate of plateau region.However,it is still challenging to simultaneously realize high mesopore/micropore volume ratio,large interlayer distance(>0.37 nm),and abundant and favorable heteroatoms-doping by a simple method.Herein,we report N,P,O ternarydoped mesoporous carbon(PNPOC-T,T=700,800 or 900)with large interlayer distance(~0.4 nm)as anode materials.The PNPOC-T were prepared by a simple in-situ polymerization of aniline and phytic acid on the exfoliated graphitic nitrogen carbide(g-C3N4)and subsequent carbonization.The obtained PNPOC-800 exhibits an excellent rate performance(101.5 mA·h·g^(-1) at 20 A·g^(-1)),which can be attributed to the high surface-controlled capacitive behavior ratio and rapid ion diffusion.The optimum SIHCs display a high energy density of 105.48 W·h·kg^(-1) and a high power density of 13.59 kW$kg1.Furthermore,the capacitance retention rate of SIHCs can reach 87.43%after 9000 cycles at 1 A·g^(-1).

关键词： Sodium ion hybrid capacitors N/P/O ternary doping mesoporous carbon Pseudocapacitive Rate performance

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Confined space synthesis of Ni(OH)_(2)-impregnated three-dimensional ordered mesoporous carbon as a high-performance supercapacitor electrode

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carbon Resources Conversion 2022年第2期5卷 101-110页

作者： Huiyong Chen Xin Yang Wencheng Yang Siyu Zhang Xingrui Wang Baoyu Liu Chengyi Dai Jianbo Zhang Xiaoxun Ma School of Chemical Engineering Northwest UniversityXi’anShaanxi 710069China International Science&Technology Cooperation Base for Clean Utilization of Hydrocarbon Resources Chemical Engineering Research Center of the Ministry of Education for Advanced Use Technology of Shanbei EnergyCollaborative Innovation Center for Development of Energy and Chemical Industry in Northern ShaanxiNorthwest UniversityXi’anShaanxi 710069China School of Cultural Heritage Northwest UniversityXi’anShaanxi 710069China School of Chemical Engineering and Light Industry Guangdong University of TechnologyGuangzhouGuangdong 510006China

Regulable loading of Ni(OH)_(2) crystals by using three dimensionally ordered mesoporous carbon(3DOMC)as a support is achieved through a confined growth strategy accompanied by steam-assisted crystallization.Dual forms of high-crystalline nanosheet-like Ni(OH)_(2) severally distribute within mesopores or over the outer surface of 3DOMC particles depending on the loading amount(3%^(−1)5%)of Ni(OH)_(2).Benefitted from the highly hybrid combination and efficient electrolyte diffusion,the obtained Ni(OH)_(2)/carbon nanocomposites exhibit an excellent electrochemical performance,and the optimal sample of 6%_Ni(OH)_(2)/3DOMC with confined extrasmall Ni(OH)_(2) nanosheets as dominant shows the highest specific capacitance of 552.5F.g^(−1) at 1.0A⋅g^(−1),which is 330%higher than the contrast sample by using actived carbon as the support.Furthermore,the assembled hybrid supercapacitor by using 6%_Ni(OH)_(2)/3DOMC and 3DOMC as positive and negative electrodes displays an energy density of 11.7 Wh.kg^(−1) at 288.1 W.kg^(−1) and a superior charge/discharge stability.It is expected that the flexible component,well-defined structure,and superior electrochemical performance could promote a great application potential of Ni(OH)_(2)/3DOMC nanocomposites as supercapacitor electrodes and in other energy storage devices.

关键词： Composite electrodes mesoporous carbon Ni(OH)_(2) Confined space synthesis Supercapacitors

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