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A General Synthesis Method for Covalent Organic Framework and Inorganic 2D Materials Hybrids

Precision Chemistry 2024年第8期2卷 398-405页

作者： Yifan Zhu Yunrui Yan Yuren Feng Yifeng Liu Chen-Yang Lin Qing Ai Tianshu Zhai Bongki Shin Rui Xu Hongchen Shen Qiyi Fang Xiang Zhang Dayanni Bhagwandin Yimo Han Hanyu Zhu Nicholas R.Glavin pulickel M ajayan Qilin Li Jun Lou Department of Materials Science and Nanoengineering Rice UniversityHoustonTexas 77005United States Department of Civil and Environmental Engineering Rice UniversityHoustonTexas 77005United States NSF Nanosystems Engineering Research Center Nanotechnology-Enabled Water Treatment Rice UniversityHoustonTexas 77005United States UES Inc.BeavercreekOhio 45432United States Materials and Manufacturing Directorate Air Force Research LaboratoryWright-Patterson AFBOhio 45433United States Department of Chemistry Rice UniversityHoustonTexas 77005United States

Two-dimensional(2D)inorganic/organic hybrids provide a versatile platform for diverse applications,including electronic,catalysis,and energy storage *** recent surge in 2D covalent organic frameworks(COFs)has introduced an organic counterpart for the development of advanced 2D organic/inorganic hybrids with improved electronic coupling,charge separation,and carrier ***,existing synthesis methods have primarily focused on few-layered film structures,which limits scalability for practical ***,we present a general synthesis approach for a range of COF/inorganic 2D material hybrids,utilizing 2D inorganic materials as both catalysts and inorganic building *** leveraging the intrinsic Lewis acid sites on the inorganic 2D materials such as hexagonal boron nitride(hBN)and transition metal dichalcogenides,COFs with diverse functional groups and topologies can grow on the surface of inorganic 2D *** controlled 2D morphology and excellent solution dispersibility of the resulting hybrids allow for easy processing into films through vacuum *** proof of concept,hBN/COF films were employed as filters for Rhodamine 6G removal under flow-through conditions,achieving a removal rate exceeding 93%.The present work provides a simple and versatile synthesis method for the scalable fabrication of COF/inorganic 2D hybrids,offering exciting opportunities for practical applications such as water treatment and energy storage.

关键词： Covalent organic frameworks Transition-metal dichalcogenides Lewis acid catalysts Hexagonal boron nitride Hybrid Materials

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Characterization of tin（Ⅱ） sulfide defects/vacancies and correlation with their photocurrent

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Nano Research 2017年第1期10卷 218-228页

作者： Mingyang Liu Luqing Wang Linan Zhou Sidong Lei Jarin Joyner Yingchao Yang Robert Vajtai pulickel ajayan Boris I. Yakobson Pol Spanos Department of Materials Science and Nanoengineering Rice University Houston Texas 77005 USA Department of Chemistry Rice University Houston Texas 77005 USA

The presence of defects/vacancies in nanomaterials influences the electronic structure of materials, and thus, it is necessary to study the correlation between the optoelectronic properties of a nanomaterial and its defects/vacancies. Herein, we report a facile solvothermal route to synthesize three-dimensional （3D） SnS nanostructures formed by {131} faceted nanosheet assembly. The 3D SnS nanostructures were calcined at temperatures of 350, 400, and 450 ~C and used as counter electrodes, before their photocurrent properties were investigated. First principle computation revealed the photocurrent properties depend on the defect/vacancy concentration within the samples. It is very interesting that characterization with positron annihilation spectrometry confirmed that the density of defects/vacancies increased with the calcination temperature, and a maximum photocurrent was realized after treatment at 400 ℃. Further, the defect/vacancy density decreased when the calcination temperature reached 450℃ as the higher calcination temperature enlarged the mesopores and densified the pore walls, which led to a lower photocurrent value at 450℃ than at 400℃.

关键词： SnS microspheres mesoporous nanosheetassembly defects/vacancies positron annihilationspectrometry photocurrent.

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Thermodynamics of order and randomness in dopant distributions inferred from atomically resolved imaging

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npj Computational Materials 2021年第1期7卷 397-405页

作者： Lukas Vlcek Shize Yang Yongji Gong pulickel ajayan Wu Zhou Matthew FChisholm Maxim Ziatdinov Rama K.Vasudevan Sergei V.Kalinin Materials Science and Technology Division Oak Ridge National LaboratoryOak RidgeTNUSA Joint Institute for Computational Sciences University of TennesseeKnoxvilleOak RidgeTNUSA Center for Functional Nanomaterials Brookhaven National LaboratoryBrookhavenNYUSA School of Materials Science and Engineering Beihang UniversityBeijingChina Department of Materials Science and NanoEngineering Rice UniversityHoustonTXUSA Center for Nanophase Materials Sciences Oak Ridge National LaboratoryOak RidgeTNUSA

Exploration of structure-property relationships as a function of dopant concentration is commonly based on mean field theories for solid ***,such theories that work well for semiconductors tend to fail in materials with strong correlations,either in electronic behavior or chemical *** these cases,the details of atomic arrangements are generally not explored and *** knowledge of the generative physics and chemistry of the material can obviate this problem,since defect configuration libraries as stochastic representation of atomic level structures can be generated,or parameters of mesoscopic thermodynamic models can be *** obtain such information for improved predictions,we use data from atomically resolved microscopic images that visualize complex structural correlations within the system and translate them into statistical mechanical models of structure *** the significant uncertainties about the microscopic aspects of the material’s processing history along with the limited number of available images,we combine model optimization techniques with the principles of statistical hypothesis *** demonstrate the approach on data from a series of atomically-resolved scanning transmission electron microscopy images of Mo_(x)Re_(1-x)S_(2) at varying ratios of Mo/Re stoichiometries,for which we propose an effective interaction model that is then used to generate atomic configurations and make testable predictions at a range of concentrations and formation temperatures.

关键词： atomic resolved dopant

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Temperature dependent Raman and photoluminescence of vertical WS2/MoS2 monolayer heterostructures

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Science Bulletin 2017年第1期62卷 16-21页

作者： Zhijian Hu Yanjun Bao Ziwei Li Yongji Gong Rui Feng Yingdong Xiao Xiaochun Wu Zhaohui Zhang Xing Zhu pulickel M. ajayan Zheyu Fang State Key Laboratory for Mesoscopic Physics School of PhysicsPeking UniversityCollaborative Innovation Center of Quantum MatterBeijing 100871China Key Laboratory of Nanoscale Measurement and Standardization National Center for Nanoscience and Technology Beijing 100190China Department of Materials Science and NanoEngineering Rice UniversityHouston7X 77005USA

Heterostructures from two-dimensional transition-metal dichalcogenides MX2 have emerged as a hot topic in recent years due to their various fascinating properties. Here, we investigated the temperature dependent Raman and photoluminescence （PL） spectra in vertical stacked WS2/MoS2 monolayer heterostructures. Our result shows that both E^g and Alg modes of WS2 and MoS2 vary linearly with tem- perature increasing from 300 to 642 K. The PL measurement also reveals strong temperature dependencies of the PL intensity and peak position. The activation energy of the thermal quenching of the PL emission has been found to be equal to 69.6 meV. The temperature dependence of the peak energy well follows the band- gap shrinkage of bulk semiconductor.

关键词： Temperature-dependent Raman spectra Photoluminescence Transition metal dichalcogenides Heterostructures

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Correlation between types of defects/vacancies of Bi2S3 nanostructures and their transient photocurrent

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Nano Research 2017年第7期10卷 2405-2414页

作者： Mingyang Liu Luqing Wang Pei Dong Liangliang Dong Xifan Wang Jarin Joyner Xiangjian Wan Boris I. Yakobson Robert Vajtai pulickel ajayan PolSpanos Department of Materials Science and Nanoengineeriing Rice University Houston TX 77005 USA Department of Chemistry Rice University Houston TX 77005 USA College of Chemistry Nankai University Tianjin 300071 China

Crystalline nanostructures possess defects/vacancies that affect their physical and chemical properties. In this regard, the electronic structure of materials can be effectively regulated through defect engineering; therefore, the correlation between defects/vacancies and the properties of a material has attracted extensive attention. Here, we report the synthesis of Bi2S3 microspheres by nanorod assemblies with exposed {211} facets, and the investigation of the types and concentrations of defects/vacancies by means of positron annihilation spectrometry. Our studies revealed that an increase in the calcined temperature, from 350 to 400 ℃, led the predominant defect/vacancy densities to change from isolated bismuth vacancies （VBi） to septuple Bi3＋-sulfur vacancy associates （VBiBiBiSSSS）. Furthermore, the concentration of septuple BiB＋-sulfur vacancy associates increased as the calcined temperature was increased from 400 to 450 ℃. The characterized transient photocurrent spectrum demonstrates that the photocurrent values closely correlate with the types and concentrations of the predominant defects/vacancies. Our theoretical computation, through first principles, showed that VBiBiBiSSSS strongly absorbs I2（sol）, easily desorbs I-（sol）, and enhances the electrocatalytic activity of the nanostructures.

关键词： Bi2S3 microspheres nanorod assembly defects/vacancies positron annihilationspectrometry transient photocurrent

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Synthesis of large-scale atomic-layer SnS2 through chemical vapor deposition

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Nano Research 2017年第7期10卷 2386-2394页

作者： Gonglan Ye Yongji Gong Sidong Lei Yongmin He Bo Li Xiang Zhang Zehua Jin Liangliang Dong Jun Lou Robert Vajtai Wu Zhou pulickel M. ajayan Department of Materials Science & NanoEngineering Rice University Houston Texas 77005 USA Department of Chemistry Rice University Houston Texas 77005 USA Department of Applied Physics Rice University Houston Texas 77005 USA Materials Science & Technology Division Oak Ridge National Lab Oak Ridge TN 37831 USA School of Materials Science and Engineering Beihang University Beijing 100191 China

Two-dimensional layers of metal dichalcogenides have attracted much attention because of their ultrathin thickness and potential applications in electronics and optoelectronics. Monolayer SnS2, with a band gap of -2.6 eV, has an octahedral lattice made of two atomic layers of sulfur and one atomic layer of tin. Till date, there have been limited reports on the growth of large-scale and high quality SnS2 atomic layers and the investigation of their properties as a semiconductor. Here, we report the chemical vapor deposition （CVD） growth of atomic-layer SnS2 with a large crystal size and uniformity. In addition, the number of layers can be changed from a monolayer to few layers and to bulk by changing the growth time. Scanning transmission electron microscopy was used to analyze the atomic structure and demonstrate the 2H stacking poly-type of different layers. The resultant SnS2 crystals is used as a photodetector with external quantum efficiency as high as 150%, suggesting promise for optoelectronic applications.

关键词： metal dichalcogenides tin disulfide two-dimensional materials chemical vapor deposition photodetector

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Controlled Nanocutting of Graphene

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Nano Research 2008年第2期1卷 116-122页

作者： Lijie Ci Zhiping Xu Lili Wang Wei Gao Feng Ding Kevin F.Kelly Boris I.Yakobson pulickel M.ajayan Department of Mechanical Engineering&Materials Science Rice UniversityHouston TX 77005USA Department of Electrical and Computer Engineering Rice UniversityHouston TX 77005USA

Rapid progress in graphene-based applications is calling for new processing techniques for creating graphene components with different shapes,sizes,and edge *** we report a controlled cutting process for graphene sheets,using nickel nanoparticles as a knife that cuts with nanoscale *** cutting proceeds via catalytic hydrogenation of the graphene lattice,and can generate graphene pieces with specifi c zigzag or armchair *** size of the nanoparticle dictates the edge structure that is produced during the *** cutting occurs along straight lines and along symmetry lines,defined by angles of 60ºor 120º,and is defl ected at free edges or defects,allowing practical control of graphene nano-engineering.

关键词： Graphene nano-engineering electronics catalytic hydrogenation

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High thermal conductivity of suspended few-layer hexagonal boron nitride sheets

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Nano Research 2014年第8期7卷 1232-1240页

作者： Haiqing Zhou Jixin Zhu Zheng Liu Zheng Yan Xiujun Fan Jian Lin Gunuk Wang Qingyu Yan Ting Yu pulickel M. ajayan James M. Tour Department of Chemistry Rice University 6100 Main Street Houston Texas 77005 USA Division of Physics and Applied Physics School of Physical and Mathematical Sciences Nanyang Technological University 537371 Singapore Department of Materials Science and NanoEngineering Rice University 6100 Main Street Houston Texas 77005 USA School of Materials Science and Engineering Nanyang Technological University Nanyang Avenue 639798 Singapore College of Electronic Information and Control Engineering Beijing University of Technology Beijing I00124 China The Smalley Institute for Nanoscale Science and Technology Rice University 6100 Main Street Houston Texas 77005 USA

The thermal conduction of suspended few-layer hexagonal boron nitride （h-BN） sheets was experimentally investigated using a noncontact micro-Raman spectroscopy method. The first-order temperature coefficients for monolayer （1L）, bilayer （2L） and nine-layer （9L） h-BN sheets were measured to be -（3.41 ± 0.12）× 10-2, -（3.15 ± 0.14） × 10-2 and -（3.78 ±0.16）× 10-2 cm-1.K-1, respectively. The room-temperature thermal conductivity of few-layer h-BN sheets was found to be in the range from 227 to 280 W.m-1-K-1, which is comparable to that of bulk h-BN, indicating their potential use as important components to solve heat dissipation problems in thermal management configurations.

关键词： two-dimensional hexagonal boron nitride(h-BN) thermal conductivity Raman spectroscopy

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One-pot synthesis of nickel-cobalt hydroxyfluorides nanowires with ultrahigh energy density for an asymmetric supercapacitor

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Science Bulletin 2018年第5期63卷 322-330页

作者： Jian-Fang Zhang Yan Wang Xia Shu Cui-Ping Yu Ming-Feng Xiao Jie-Wu Cui Yong-Qiang Qin Hong-Mei Zheng Yong Zhang Dong Chen pulickel M. ajayan Yu-Cheng Wu School of Materials Science and Engineering Hefei University of Technology Hefei 230009 China Department of Material Science and Nanoengineering Rice University Houston TX 77005 USA School of Instrument Science and Opto-electronics Ensineering Hefei University of Technology Hefei 230009 China Key Laboratory of Advanced Functional Materials and Devices of Anhui Province Hefei 230009 China

A novel and unique nickel-cobalt hydroxyfluorides(NiCo-HF)nanowires material is fabricated by one-pot solvothermal synthesis method for asymmetric *** synthesis mechanism and factors that influence the formation of the Ni Co-HF nanowires have been further *** as-prepared NiCo-HF electrode exhibits a high specific capacitance of 3,372.6 F g^(à1),and the capacitance retention of 94.3%can be achieved at a high current density of 20 A g^(à1)after 10,000 *** outstanding electrochemical performance of the electrode can be attributed to the synergistic effect of the nanowires morphology and complicated redox process of active ***,an asymmetric supercapacitor assembled with Ni Co-HF nanowires as positive electrode and activated carbon as the negative electrode shows an ultrahigh energy density of 83.6 Wh kg^(à1)at a power density of 379.4 W kg^(à1)and an excellent cycling stability with 86.3%capacitance retention after 10,000 cycles,indicating that this novel material has great promise for potential application in energy storage device.

关键词： Nickel-cobalt hydroxyfluorides Solvothermal synthesis Asymmetric supercapacitor Energy density

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Pseudobrookite based heterostructures for efficient electrocatalytic hydrogen evolution

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Materials Reports(Energy) 2021年第2期1卷 90-98页

作者： Niranjala Fernando Jayashree Swaminathan Francisco Carlos Robles Hernandez Gayan Priyadarshana Chanaka Sandaruwan Wenli Yang Veranja Karunaratne Zixing Wang Gehan AJAmaratunga Nilwala Kottegoda Ashokkumar Meiyazhagan pulickel M.ajayan Department of Design and Engineering Faculty of Science and TechnologyBournemouth UniversityDorsetBH125BBUK Department of Materials Science&NanoEngineering Rice UniversityTexas77005USA Department of Mechanical Engineering Technology University of HoustonHoustonTX77204USA Materials Science&Engineering Cullen College of EngineeringUniversity of HoustonHoustonTX77204USA Department of Materials and Mechanical Technology Faculty of TechnologyUniversity of Sri JayewardenepuraPitipanaHomagamaSri Lanka Sri Lanka Institute of Nanotechnology PitipanaHomagamaSri Lanka Department of Engineering University of CambridgeCambridgeCB21TNUK Department of Chemistry Center for Advanced Materials ResearchUniversity of Sri JayewardenepuraGangodawilaNugegodaSri Lanka

Synthesis of ultrathin heterostructures has received much attention in the recent past due to their unique physical and chemical *** this work,we report the synthesis of Fe_(2)TiO_(5)–TiO_(2)heterostructures using a simple hydrothermal technique employing natural ilmenite as the *** arranged nanostructures with interconnected nano-petals of thickness around 50 nm are *** electrocatalytic properties of the synthesized Fe_(2)TiO_(5)–TiO_(2)heterostructures are enhanced following the cathodization *** observed enhancement in the synthesized materials’electrocatalytic property can be attributed to the defect-rich Fe_(2-x)TiO_(5-x)-TiO_(2-x)*** current approach and technique discussed in this work offer a simple method to synthesize a nanostructured heterostructure material and create defects for enhancing electrocatalytic activity.

关键词： Heterostructures Cathodization Green catalyst 2D materials Hydrogen evolution Electrocatalysis Pseudobrookite

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