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Spatial construction of ultrasmall Pt-decorated 3d spinel oxidemodified N-doped graphene nanoarchitectures as high-efficiency methanol oxidation electrocatalysts

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Rare Metals 2024年第1期43卷 186-197页

作者： Qi Zhang Min-Min Yan Wen-Fa du Chen-Yu Yin Jian Zhang Lu Yang Yun-Qing Kang Hai-Yan He Hua-Jie Huang College of Mechanics and Materials Hohai UniversityNanjing 210098China New Energy Technology Engineering Lab of Jiangsu Province College of ScienceNanjing University of Posts&Telecommunications(NUPT)Nanjing 210023China International Center for Materials Nanoarchitectonics(WPIMANA) National Institute for Materials ScienceTsukuba 305-0044IbarakiJapan

direct methanol fuel cell technology recently becomes the focus of both academic and engineering circles,which stimulates the exploitation and utilization of advanced electrode catalysts with high activity and long lifespan.Herein,we demonstrate a robust bottom-up approach to the spatial construction of three-dimensional(3d) spinel manganese-cobalt oxide-modified N-doped graphene nanoarchitectures decorated with ultrasmall Pt nanoparticles(Pt/MnCo_(2)O_(4)-NG) via a controllable selfassembly process.The incorporation of MnCo_(2)O_(4)nanocrystals provides abundant hydroxyl sources to promote the oxidative removal of CO-like byproducts on Pt sites,while the existence of 3d porous N-doped graphene networks facilitates the transportation of both ions and electrons in the hybrid system,thus giving rise to remarkable synergetic coupling effects during the methanol oxidation process.Consequently,the optimized Pt/MnCo_(2)O_(4)-NG nano architecture expres ses exceptional electrocatalytic properties with a large electrochemically active surface area of 99.5 m^(2)·g^(-1),a high mass activity of1508.3 mA·mg^(-1),strong toxicity resistance and reliable long-term durability,which have obvious competitive advantages over those of conventional Pt/carbon black,Pt/carbon nano tube,Pt/graphene,and Pt/N-doped graphene catalysts with the same Pt usage.

关键词： Platinum MnCo_(2)O_(4) 3d graphene Electrocatalysts Methanol oxidation

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MOF-Like 3d graphene-Based Catalytic Membrane Fabricated by One-Step Laser Scribing for Robust Water Purification and Green Energy Production

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Nano-Micro Letters 2022年第11期14卷 48-61页

作者： Xinyu Huang Liheng Li Shuaifei Zhao Lei Tong Zheng Li Zhuiri Peng Runfeng Lin Li Zhou Chang Peng Kan-Hao Xue Lijuan Chen Gary J.Cheng Zhu Xiong Lei Ye School of Optical and Electronic Information and Wuhan National Laboratory for Optoelectronics Huazhong University of Science and TechnologyWuhan 430074People’s Republic of China Hubei Yangtze Memory Laboratories Wuhan 430205People’s Republic of China Institute for Frontier Materials Deakin UniversityGeelongVIC 3216Australia Key Laboratory of New Processing Technology for Nonferrous Metal and Materials(Ministry of Education) Guangxi Key Laboratory of Optical and Electronic Materials and DevicesCollege of Materials Science and EngineeringGuilin University of TechnologyGuilin 541004People’s Republic of China College of Chemistry and Materials Science Hunan Agricultural UniversityHunan 410128People’s Republic of China School of Material Science and Engineering Hunan University of Science and TechnologyXiangtanHunan ProvincePeople’s Republic of China School of Industrial Engineering and Birck Nanotechnology Centre Purdue UniversityWest LafayetteIN 47907USA Institute of Environmental Research at Greater Bay Key Laboratory for Water Quality and Conservation of the Pearl River DeltaMinistry of EducationGuangzhou UniversityGuangzhou 510006GuangdongPeople’s Republic of China

Increasing both clean water and green energy demands for survival and development are the grand challenges of our age.Here,we successfully fabricate a novel multifunctional 3d graphene-based catalytic membrane(3d-GCM)with active metal nanoparticles(AMNs)loading for simultaneously obtaining the water purification and clean energy generation,via a“green”one-step laser scribing technology.The as-prepared 3d-GCM shows high porosity and uniform distribution with AMNs,which exhibits high permeated fluxes(over 100 L m^(−2) h^(−1))and versatile super-adsorption capacities for the removal of tricky organic pollutants from wastewater under ultra-low pressure-driving(0.1 bar).After adsorption saturating,the AMNs in 3d-GCM actuates the advanced oxidization process to self-clean the fouled membrane via the catalysis,and restores the adsorption capacity well for the next time membrane separation.Most importantly,the 3d-GCM with the welding of laser scribing overcomes the lateral shear force damaging during the long-term separation.Moreover,the 3d-GCM could emit plentiful of hot electrons from AMNs under light irradiation,realizing the membrane catalytic hydrolysis reactions for hydrogen energy generation.This“green”precision manufacturing with laser scribing technology provides a feasible technology to fabricate high-efficient and robust 3d-GCM microreactor in the tricky wastewater purification and sustainable clean energy production as well.

关键词： 3d graphene Laser scribing Catalytic membrane Water purification Hydrogen production

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Caterpillar-like 3d graphene nanoscrolls@CNTs hybrids decorated with Co-doped MoSe_(2)nanosheets for electrocatalytic hydrogen evolution

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Journal of Materials Science & Technology 2023年第5期136卷 43-53页

作者： Hao Luo Hongfei Gao Xudong Zhang Fan Yang Chen Liu Kewei Xu dagang Guo State Key Laboratory for Mechanical Behavior of Materials School of Materials Science and EngineeringXi’an Jiaotong UniversityXi’an 710049China Center for High Performance Computing Network Information CenterXi’an Jiaotong UniversityXi’an 710049China

Hydrogen is a clean and flexible energy carrier that has the promising to satisfy urgent demands of the energy crisis and environmental protection.Electrochemical hydrogen evolution reaction(HER),a critical half-reaction in water splitting,is one of the greenest and most common methods to obtain high-purity hydrogen.designing preeminent activity and stability electrocatalysts for hydrogen precipitation reac-tion(HER)to reduce energy consumption is of great essential.3d carbon-based materials have attracted widespread concern as the potential scaffolds of highly active and durable electrocatalysts for HER.To boost the HER activity and prolong the lifespan of electrocatalysts,multifarious 3d carbon architectures make an appearance to be engineered for accelerating electronic/mass transfer and maximizing the expo-sure of active sites.Herein,we designed and fabricated high-performance electrocatalysts based on a spe-cial caterpillar-like 3d graphene nanoscrolls@CNTs(GNS@CNTs)scaffold decorated with Co-doped MoSe_(2)nanosheets for HER.In the caterpillar-like hierarchical structure,CNTs were seamlessly co-bonded and dilated the interlayer and outer spacing of GNS through CVd growth technology,and nickel nanoparticles were covered by the CNTs tips.Taking advantage of the plentiful hierarchical pore,larger specific surface area,and higher chemical stability of the caterpillar-like structure,the catalysts exhibited enhanced elec-trocatalytic properties than some existing data reported.density functional theory calculations showed that the encapsulated nickel nanoparticle could tune the electronic structure of the outer anchored Co-doped MoSe_(2)and optimize itsG of H∗adsorption by electron traversing effect and doping effect.These indicate that caterpillar-like GNS@CNT is an ideal scaffold f or anchoring actives substance and is suit-able for high-efficient HER.This study provides new insights for designing hierarchical carbon composite nanostructures for catalysts,sensors,energy materials,and other applications.

关键词： Electron traversing effect 3d graphene graphene nanoscrolls CNT MoSe_(2),Hydrogen evolution reaction

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Porous monoliths of 3d graphene for electric double-layer supercapacitors

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Carbon Energy 2021年第2期3卷 193-224页

作者： Jinjue Zeng Chenyang Xu Tian Gao Xiangfen Jiang Xue‐Bin Wang National Laboratory of Solid State Microstructures(NLSSM) Jiangsu Key Laboratory of Artificial Functional MaterialsCollaborative Innovation Center of Advanced MicrostructuresCollege of Engineering and Applied SciencesNanjing UniversityNanjingChina WPI Center for Materials Nanoarchitectonics National Institute for Materials Science(NIMS)TsukubaJapan

For delivering the nanoscaled extraordinary characteristics in macroscopical bulk,it is essential to integrate two-dimensional nanosheets into threedimensional(3d)porous monoliths,alternatively called as 3d architectures,3d networks,or aerogels.The intersupported structure of porous monolithic 3d graphene(3dG)can prevent aggregation or restacking of graphene individuals,and the interconnected sp^(2) network of 3dG not only can provide the highway for the transport of electron/phonon but also can present continual cavities/channels for mass transfer.This review summarizes the synthesis methodology of 3dG porous monoliths and highlights the application for electric double-layer capacitors.Present challenges and future prospects about the manufacture and application of 3dG are also discussed.

关键词： 3d graphene electric double-layer capacitor graphene aerogel porous monolith supercapacitor

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Scaling laws governing the elastic properties of 3d graphenes

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Science China Technological Sciences 2024年第6期67卷 1748-1756页

作者： LI Ming LU Guo YU Haodong LI MengLei ZHENG FaWei Centre for Quantum Physics Key Laboratory of Advanced Optoelectronic Quantum Architecture and Measurement(MOE)School of PhysicsBeijing Institute of Technology Beijing Key Lab of Nanophotonics & Ultrafine Optoelectronic Systems School of PhysicsBeijing Institute of Technology Laboratory of Computational Physics Institute of Applied Physics and Computational Mathematics department of Physics Capital Normal University

In this study, we comprehensively investigated the scaling law for elastic properties of three-dimensional honeycomb-like graphenes（3d graphenes） using hybrid neural network potential-based molecular dynamics simulations and theoretical analyses. The elastic constants were obtained as functions of honeycomb hole size, denoted by the graphene wall length L. All five independent elastic constants in the large-L limit are proportional to L-1. The associated coefficients are combinations of elastic constants of two-dimensional graphene. High-order terms including L-2and L-3emerge for finite L values. They have three origins, the distorted areas close to the joint lines of 3d graphenes, the variation in solid angles between graphene plates, and the bending distortion of graphene plates. Significantly, the chirality becomes essential with decreasing L because the joint line structures are different between the armchair and zigzag-type 3d graphenes. Our findings provide insights into the elastic properties of graphene-based superstructures and can be used for further studies on graphene-based materials.

关键词： scaling law neural network elastic properties 3d graphene

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direct electron transfer of hemoglobin at 3d graphene–nitrogen doped carbon nanotubes network modified electrode and electrocatalysis toward nitromethane

Direct electron transfer of hemoglobin at 3D graphene–nitro...

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河南省化学会2018年学术年会

作者： Yanju Wu Fei Wang Lijie Wang Kui Lu School of Material and Chemistry Engineering Henan University of Engineering College of Chemistry and Molecular Engineering Zhengzhou University School of Chemical Engineering and Food Science Zhengzhou Institute of Technology

In this work,pulsed potentiostatic reduction method was presented to directly construct a three dimensional graphene-nitrogen doped carbon nanotubes(3dG-NCNTs)network on the surface of a glassy carbon electrode(GCE).Scanning electron microscopy(SEM),Raman spectra and electrochemical experiments revealed the characteristics of the 3dG-NCNTs network.Further,such 3dG-NCNTs network was employed to immobilize a model molecule,hemoglobin(Hb),for the construction of an electrochemical nitromethane(CHNO)biosensor.The electrochemical properties of the biosensor were studied in detail,including the direct electron transfer of Hb and the electrochemical determination of CHNO.due to the 3dG-NCNTs network,electrochemical biosensor demonstrated fast electron transfer rate(7.12 s)and excellent catalytic activity towards CHNO.Under optimal conditions,the proposed biosensor exhibited a wide linear response in the range of 5.0×10～3.5×10 mol L,with a low detection limit of 1.5×10 mol L.In addition,the biosensor had high reproducibility,stability and selectivity,which provided the possibility for the monitoring of CHNO in real samples.

关键词： direct electron transfer 3d graphene graphene-nitrogen doped carbon nanotubes hemoglobin

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Pulse-electropolymerization of polyaniline in 3d graphene hydrogel for high-performance supercapacitor

Pulse-electropolymerization of polyaniline in 3D graphene hy...

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河南省化学会2016年学术年会

作者： Shuya Gao Pei dong Jian Liu Li Zhang Shaokui Cao School of Materials Science and Engineering Zhengzhou University

Three dimensional(3d) graphene monoliths with a porous network have received increasing attention for the electrochemical energy storage, mainly due to their high specific surface areas, ordered macroporous structures, strong mechanical strengths and fast mass and electron transport kinetics.These structural characteristics also enable 3d graphene a promising platform to incorporate with electroactive materials to further improve its capacitive performance as a supercapacitor electrode material. On the other hand, polyaniline(PANI) can be considered as a promising pesudocapacitive material which has an instrinsic nanofiber structure, the unique mechanism of proton doping, rich redox states and low cost. Therefore, we attempted to evenly deposit PANI on the framework of 3d graphene by pulse-electropolymerization technique, aimed to increase the energy density of the free-standing composite-based supercapacitor without deteriorating its power density. Through changing the potential-pulse cycle numbers, the GH/PANI composites with different PANI nanofiber content were prepared. The resulting GH/PANI composites were then characterized by SEM, FTIR and Raman analysis. The elelctrochemical properties of the samples were studied in three-electrode system using cyclic voltammograms(CV), galvanostatic charge-discharge and electrochemical impedance spectroscopy(EIS) techniques. The results showed that the capacitive performance of GH/PANI is significantly improved due to the reinforcing effects coming from PANI. The best specific capacitance of 734 F/g can be achieved at the charge and discharge rate of 1.7A/g for the optimized GH/PANI sample with 300 pulse cycles. This composite sample also exhibited excellent rate capability up to 100A/g with a capacitance retention of 72%, and good cycling stability with 83% capacitance retention after 1000 cycles.

关键词： Supercapacitor 3d graphene Polyaniline nanofiber Pulse-electropolymerization

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direct fabrication of 3d graphene–multi walled carbon nanotubes network and its application for sensitive electrochemical determination of hyperin

Direct fabrication of 3D graphene–multi walled carbon nanot...

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河南省化学会2018年学术年会

作者： Lijie Wang Wenke Jia Yaxin ding Fei Wang Lu Kui School of Material and Chemistry Engineering Henan University of Engineering College of Chemistry and Molecular Engineering Zhengzhou University School of Chemical Engineering and Food Science Zhengzhou Institute of Technology

In this work, a novel electrochemical sensor was proposed for hyperin determination. Pulse potential method(PPM) was presented to fabricate directly three dimensional graphene-multiwalled nanotubes(3 dG-MWCNTs) network on the surface of glassy carbon electrode(GCE) in graphite oxide-multi walled carbon nanotubes(GO-MWCNTs) dispersion. 3 dG-MWCNTs and GO-MWCNTs were characterized and morphology by scanning electron microscopy(SEM), Raman spectra and electrochemical experiments. The 3 dG-MWCNTs was successfully applied in hyperin determination with satisfactory results. Systematic electrochemical tests confirmed the 3 dG-MWCNTs network modified electrode can effectively increase response to the oxidation of hyperin. Under the optimized conditions, the modified electrode showed a linear voltammetric response to hyperin at concentrations ranging from 5.0×10-9 ～ 1.5×10-6 mol L-1 with a low detection limit of 1.0 × 10-9 mol L-1. Moreover, the proposed method showed good performance in stability, sensitivity, selectivity and reproducibility for the determination of hyperin.

关键词： 3d graphene voltammetric sensor ulse potentiostatic method hyperin

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Three-dimensional fuzzy graphene ultra-microelectrodes for subcellular electrical recordings

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Nano Research 2020年第5期13卷 1444-1452页

作者： Sahil K.Rastogi Jacqueline Bliley Laura Matino Raghav Garg Francesca Santoro Adam W.Feinberg Tzahi Cohen-Karni department of Biomedical Engineering Carnegie Mellon UniversityPittsburghPA15213USA Center for Advanced Biomaterials for Healthcare Istituto Italiano di TecnologiaNaples80125Italy department of Chemical Materials and Industrial Production EngineeringUniversity of Naples Federico IINaples80125Italy department of Materials Science and Engineering Carnegie Mellon UniversityPittsburghPA15213USA

Microelectrode arrays(MEAs)have enabled investigation of cellular networks at sub-millisecond temporal resolution.However,current MEAs are limited by the large electrode footprint since reducing the electrode’s geometric area to sub-cellular dimensions leads to a significant increase in impedance thus affecting its recording capabilities.We report a breakthrough ultra-microelectrodes platform by leveraging the outstanding surface-to-volume ratio of nanowire-templated out-of-plane synthesized three-dimensional fuzzy graphene(NT-3dFG).The enormous surface area of NT-3dFG leads to 140-fold reduction in electrode impedance compared to bare Au microelectrodes,thus enabling scaling down the geometric size by 625-fold to ca.2µm×2µm.The out-of-plane morphology of NT-3dFG leads to a tight seal with the cell membrane thus enabling recording of electrical signals with high signal-to-noise ratio(SNR)of>6.This work highlights the possibility to push the limits of the conventional MEA technology to enable electrophysiological investigation at sub-cellular level without the need of any surface coatings.This presented approach would greatly impact our basic understanding of signal transduction within a single cell as well as complex cellular assemblies.

关键词： microelectrode array ultra-microelectrodes electrical recordings biocompatible hybrid-nanomaterial 3d graphene cardiomyocytes

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Fabrication of three-dimensional graphene anode for augmenting performance in microbial fuel cells

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Carbon Resources Conversion 2019年第2期2卷 134-140页

作者： Alka Pareek J.Shanthi Sravan S.Venkata Mohan Bioengineering and Environmental Science Lab CEEFFCSIR-Indian Institute of Chemical Technology(CSIR-IICT)Hyderabad 500007India Academy of Scientific and Innovative Research(AcSIR) India

In the present work,we have reported the synthesis of 3d graphene structures by simple chemical reduction method for application in microbial fuel cell(MFC)as an anode.The synthesis procedure includes synthesis of graphene oxide by modified Hummers method followed by simultaneous reduction of graphene oxide and the formation of hydrogels.The 3d graphene structures are characterized using X-ray diffraction and Raman spectroscopy techniques.Electrochemical characterization is carried out to study the capacitive properties and impedance studies of electrodes in conductive electrolyte.3d graphene electrodes show remarkably high capacitive current,charge storage and lower charge transfer resistance as estimated through cyclic voltammetry and Nyquist plots.In order to evaluate the performance of 3d graphene electrodes in MFC,power density and polarization curves are recorded in three configurations by varying terminal electron acceptors(TEA)viz.,dissolved oxygen(MFC-dO),potassium ferricyanide and MFC without TEA(MFC-NdO).3d graphene electrodes exhibits maximum power density of 0.49 mW/m^(2) in potassium ferricyanide followed by MFC-dO(0.36 mW/m^(2))and MFC-NdO(0.34 mW/m^(2)).Present work highlights the viability of chemically synthesized 3d graphene electrodes as an efficient anode material in MFC.

关键词： Microbial fuel cell 3d graphene Wastewater treatment Chemical reduction graphene electrodes

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