Browsing by Author "Tiwary, Chandra Sekhar"
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Item Ambient solid-state mechano-chemical reactions between functionalized carbon nanotubes(Nature Publishing Group, 2015) Kabbani, Mohamad A.; Tiwary, Chandra Sekhar; Autreto, Pedro A.S.; Brunetto, Gustavo; Som, Anirban; Krishnadas, K.R.; Ozden, Sehmus; Hackenberg, Ken P.; Gong, Yongi; Galvao, Douglas S.; Vajtai, Robert; Kabbani, Ahmad T.; Pradeep, Thalappil; Ajayan, Pulickel M.Carbon nanotubes can be chemically modified by attaching various functionalities to their surfaces, although harsh chemical treatments can lead to their break-up into graphene nanostructures. On the other hand, direct coupling between functionalities bound on individual nanotubes could lead to, as yet unexplored, spontaneous chemical reactions. Here we report an ambient mechano-chemical reaction between two varieties of nanotubes, carrying predominantly carboxyl and hydroxyl functionalities, respectively, facilitated by simple mechanical grinding of the reactants. The purely solid-state reaction between the chemically differentiated nanotube species produces condensation products and unzipping of nanotubes due to local energy release, as confirmed by spectroscopic measurements, thermal analysis and molecular dynamic simulations.Item Cryo-mediated exfoliation and fracturing of layered materials into 2D quantum dots(AAAS, 2017) Wang, Yan; Liu, Yang; Zhang, Jianfang; Wu, Jingjie; Xu, Hui; Wen, Xiewen; Zhang, Xiang; Tiwary, Chandra Sekhar; Yang, Wei; Vajtai, Robert; Zhang, Yong; Chopra, Nitin; Odeh, Ihab Nizar; Wu, Yucheng; Ajayan, Pulickel M.Atomically thin quantum dots from layered materials promise new science and applications, but their scalable synthesis and separation have been challenging. We demonstrate a universal approach for the preparation of quantum dots from a series of materials, such as graphite, MoS2, WS2, h-BN, TiS2, NbS2, Bi2Se3, MoTe2, Sb2Te3, etc., using a cryo-mediated liquid-phase exfoliation and fracturing process. The method relies on liquid nitrogen pretreatment of bulk layered materials before exfoliation and breakdown into atomically thin two-dimensional quantum dots of few-nanometer lateral dimensions, exhibiting size-confined optical properties. This process is efficient for a variety of common solvents with a wide range of surface tension parameters and eliminates the use of surfactants, resulting in pristine quantum dots without surfactant covering or chemical modification.Item Damage-tolerant 3D-printed ceramics via conformal coating(AAAS, 2021) Sajadi, Seyed Mohammad; Vásárhelyi, Lívia; Mousavi, Reza; Rahmati, Amir Hossein; Kónya, Zoltán; Kukovecz, Ákos; Arif, Taib; Filleter, Tobin; Vajtai, Robert; Boul, Peter; Pang, Zhenqian; Li, Teng; Tiwary, Chandra Sekhar; Rahman, Muhammad M.; Ajayan, Pulickel M.Ceramic materials, despite their high strength and modulus, are limited in many structural applications due to inherent brittleness and low toughness. Nevertheless, ceramic-based structures, in nature, overcome this limitation using bottom-up complex hierarchical assembly of hard ceramic and soft polymer, where ceramics are packaged with tiny fraction of polymers in an internalized fashion. Here, we propose a far simpler approach of entirely externalizing the soft phase via conformal polymer coating over architected ceramic structures, leading to damage tolerance. Architected structures are printed using silica-filled preceramic polymer, pyrolyzed to stabilize the ceramic scaffolds, and then dip-coated conformally with a thin, flexible epoxy polymer. The polymer-coated architected structures show multifold improvement in compressive strength and toughness while resisting catastrophic failure through a considerable delay of the damage propagation. This surface modification approach allows a simple strategy to build complex ceramic parts that are far more damage-tolerant than their traditional counterparts. Conformal polymer coating leads to damage-tolerant architected ceramic structures with high strength and toughness. Conformal polymer coating leads to damage-tolerant architected ceramic structures with high strength and toughness.Item Development of a schwarzite-based moving bed 3D printed water treatment system for nanoplastic remediation(Royal Society of Chemistry, 2021) Gupta, Bramha; Ambekar, Rushikesh S.; Tromer, Raphael M.; Ghosal, Partha Sarathi; Sinha, Rupal; Majumder, Abhradeep; Kumbhakar, Partha; Ajayan, P. M.; Galvao, Douglas S.; Gupta, Ashok Kumar; Tiwary, Chandra Sekhar; Smalley-Curl InstituteThe impact of micro and nanoplastic debris on our aquatic ecosystem is among the most prominent environmental challenges we face today. In addition, nanoplastics create significant concern for environmentalists because of their toxicity and difficulty in separation and removal. Here we report the development of a 3D printed moving bed water filter (M-3DPWF), which can perform as an efficient nanoplastic scavenger. The enhanced separation of the nanoplastics happens due to the creation of a charged filter material that traps the more surface charged nanoparticles selectively. Synthetic contaminated water from polycarbonate waste has been tested with the filter, and enhanced nanoplastic removal has been achieved. The proposed filtration mechanism of surface-charge based water cleaning is further validated using density function theory (semi-empirical) based simulation. The filter has also shown good structural and mechanical stability in both static and dynamic water conditions. The field suitability of the novel treatment system has also been confirmed using water from various sources, such as sea, river, and pond. Our results suggest that the newly developed water filter can be used for the removal of floating nanoparticles in water as a robust advanced treatment system.Item Direct ink printing of multi-material composite structures(2024-01-02) Sajadi, Seyed Mohammad; Boul, Peter; Tiwary, Chandra Sekhar; Rahman, Muhammad M.; Ajayan, Pulickel M.; Thaemltiz, Carl; William Marsh Rice University; Saudi Arabian Oil Company; United States Patent and Trademark OfficeMethods for fabricating a multi-material composite structure are described. Methods for fabricating a multi-material composite structure include forming a first colloidal ink solution with a first material matrix, water, and a rheology modifying agent; forming a second colloidal ink solution with a second material matrix, water, and a rheology modifying agent; printing a first layer on a substrate using a first printing nozzle carrying the first colloidal ink solution; printing a second layer on top of the first layer using a second printing nozzle carrying the second colloidal ink solution; forming a 3D structure by printing a plurality of layers including the first layer and the second layer printed in an alternating pattern; and sintering the 3D structure to form the multi-material composite structure.Item Fluorinated h-BN as a magnetic semiconductor(American Association for the Advancement of Science, 2017) Radhakrishnan, Sruthi; Das, Deya; Samanta, Atanu; de los Reyes, Carlos A.; Deng, Liangzi; Alemany, Lawrence B.; Weldeghiorghis, Thomas K.; Khabashesku, Valery N.; Kochat, Vidya; Jin, Zehua; Sudeep, Parambath M.; Martí, Angel A.; Chu, Ching-Wu; Roy, Ajit; Tiwary, Chandra Sekhar; Singh, Abhishek K.; Ajayan, Pulickel M.We report the fluorination of electrically insulating hexagonal boron nitride (h-BN) and the subsequent modification of its electronic band structure to a wide bandgap semiconductor via introduction of defect levels. The electrophilic nature of fluorine causes changes in the charge distribution around neighboring nitrogen atoms in h-BN, leading to room temperature weak ferromagnetism. The observations are further supported by theoretical calculations considering various possible configurations of fluorinated h-BN structure and their energy states. This unconventional magnetic semiconductor material could spur studies of stable two-dimensional magnetic semiconductors. Although the high thermal and chemical stability of h-BN have found a variety of uses, this chemical functionalization approach expands its functionality to electronic and magnetic devices.Item High hardness in the biocompatible intermetallic compound β-Ti3Au(AAAS, 2016) Svanidze, Eteri; Besara, Tiglet; Ozaydin, M. Fevsi; Tiwary, Chandra Sekhar; Wang, Jiakui K.; Radhakrishnan, Sruthi; Mani, Sendurai; Xin, Yan; Han, Ke; Liang, Hong; Siegrist, Theo; Ajayan, Pulickel M.; Morosan, E.The search for new hard materials is often challenging, but strongly motivated by the vast application potential such materials hold. Ti3Au exhibits high hardness values (about four times those of pure Ti and most steel alloys), reduced coefficient of friction and wear rates, and biocompatibility, all of which are optimal traits for orthopedic, dental, and prosthetic applications. In addition, the ability of this compound to adhere to ceramic parts can reduce both the weight and the cost of medical components. The fourfold increase in the hardness of Ti3Au compared to other Ti–Au alloys and compounds can be attributed to the elevated valence electron density, the reduced bond length, and the pseudogap formation. Understanding the origin of hardness in this intermetallic compound provides an avenue toward designing superior biocompatible, hard materials.Item High-K dielectric sulfur-selenium alloys(AAAS, 2019) Susarla, Sandhya; Tsafack, Thierry; Owuor, Peter Samora; Puthirath, Anand B.; Hachtel, Jordan A.; Babu, Ganguli; Apte, Amey; Jawdat, BenMaan I.; Hilario, Martin S.; Lerma, Albert; Calderon, Hector A.; Hernandez, Francisco C. Robles; Tam, David W.; Li, Tong; Lupini, Andrew R.; Idrobo, Juan Carlos; Lou, Jun; Wei, Bingqing; Dai, Pengcheng; Tiwary, Chandra Sekhar; Ajayan, Pulickel M.Upcoming advancements in flexible technology require mechanically compliant dielectric materials. Current dielectrics have either high dielectric constant, K (e.g., metal oxides) or good flexibility (e.g., polymers). Here, we achieve a golden mean of these properties and obtain a lightweight, viscoelastic, high-K dielectric material by combining two nonpolar, brittle constituents, namely, sulfur (S) and selenium (Se). This S-Se alloy retains polymer-like mechanical flexibility along with a dielectric strength (40 kV/mm) and a high dielectric constant (K = 74 at 1 MHz) similar to those of established metal oxides. Our theoretical model suggests that the principal reason is the strong dipole moment generated due to the unique structural orientation between S and Se atoms. The S-Se alloys can bridge the chasm between mechanically soft and high-K dielectric materials toward several flexible device applications.Item Metal-Free Dual Modal Contrast Agents Based on Fluorographene Quantum Dots(Wiley, 2016) Radhakrishnan, Sruthi; Samanta, Atanu; Sudeep, Parambath M.; Maldonado, Kiersten L.; Mani, Sendurai A.; Acharya, Ghanashyam; Tiwary, Chandra Sekhar; Singh, Abhishek K.; Ajayan, Pulickel M.Fluorographene quantum dots prepared from fluorinated graphene oxide (FGO) show a linear dependence of the magnetization on the applied field. This is further supported by DFT calculations taking into account a few possible systems of functionalized graphene quantum dots. The inherent magnetism, high concentration of fluorine and cyto-compatibility of these quantum dots promise potential application as a dual modal agent for proton and 19F based Magnetic Resonance Imaging which is investigated here. A metal free dual modal contrast agent would bring about a great change in the efficiency and resolution of this widely used imaging tool.Item Super-elasticity of three-dimensionally cross-linked graphene materials all the way to deep cryogenic temperatures(AAAS, 2019) Zhao, Kai; Zhang, Tengfei; Chang, Huicong; Yang, Yang; Xiao, Peishuang; Zhang, Hongtao; Li, Chenxi; Tiwary, Chandra Sekhar; Ajayan, Pulickel M.; Chen, YongshengUntil now, materials with high elasticity at deep cryogenic temperatures have not been observed. Previous reports indicated that graphene and carbon nanotube–based porous materials can exhibit reversible mechano-elastic behavior from liquid nitrogen temperature up to nearly a thousand degrees Celsius. Here, we report wide temperature–invariant large-strain super-elastic behavior in three-dimensionally cross-linked graphene materials that persists even to a liquid helium temperature of 4 K, a property not previously observed for any other material. To understand the mechanical properties of these graphene materials, we show by in situ experiments and modeling results that these remarkable properties are the synergetic results of the unique architecture and intrinsic elastic/flexibility properties of individual graphene sheets and the covalent junctions between the sheets that persist even at harsh temperatures. These results suggest possible applications for such materials at extremely low temperature environments such as those in outer space.Item Synthesis and 3D Interconnected Nanostructured h-BN-Based Biocomposites by Low-Temperature Plasma Sintering: Bone Regeneration Applications(American Chemical Society, 2018) Gautam, Chandkiram; Chakravarty, Dibyendu; Gautam, Amarendra; Tiwary, Chandra Sekhar; Woellner, Cristiano Francisco; Mishra, Vijay Kumar; Ahmad, Naseer; Ozden, Sehmus; Jose, Sujin; Biradar, Santoshkumar; Vajtai, Robert; Trivedi, Ritu; Galvao, Douglas S.; Ajayan, Pulickel M.Recent advances and demands in biomedical applications drive a large amount of research to synthesize easily scalable low-density, high-strength, and wear-resistant biomaterials. The chemical inertness with low density combined with high strength makes h-BN one of the promising materials for such application. In this work, three-dimensional hexagonal boron nitride (h-BN) interconnected with boron trioxide (B2O3) was prepared by easily scalable and energy efficient spark plasma sintering (SPS) process. The composite structure shows significant densification (1.6–1.9 g/cm3) and high surface area (0.97–14.5 m2/g) at an extremely low SPS temperature of 250 °C. A high compressive strength of 291 MPa with a reasonably good wear resistance was obtained for the composite structure. The formation of strong covalent bonds between h-BN and B2O3 was formulated and established by molecular dynamics simulation. The composite showed significant effect on cell viability/proliferation. It shows a high mineralized nodule formation over the control, which suggests its use as a possible osteogenic agent in bone formation.Item Ultrafast non-radiative dynamics of atomically thin MoSe2(Springer Nature, 2017) Lin, Ming-Fu; Kochat, Vidya; Krishnamoorthy, Aravind; Bassman, Lindsay; Weninger, Clemens; Zheng, Qiang; Zhang, Xiang; Apte, Amey; Tiwary, Chandra Sekhar; Shen, Xiaozhe; Li, Renkai; Kalia, Rajiv; Ajayan, Pulickel; Nakano, Aiichiro; Vashishta, Priya; Shimojo, Fuyuki; Wang, Xijie; Fritz, David M.; Bergmann, UwePhoto-induced non-radiative energy dissipation is a potential pathway to induce structural-phase transitions in two-dimensional materials. For advancing this field, a quantitative understanding of real-time atomic motion and lattice temperature is required. However, this understanding has been incomplete due to a lack of suitable experimental techniques. Here, we use ultrafast electron diffraction to directly probe the subpicosecond conversion of photoenergy to lattice vibrations in a model bilayered semiconductor, molybdenum diselenide. We find that when creating a high charge carrier density, the energy is efficiently transferred to the lattice within one picosecond. First-principles nonadiabatic quantum molecular dynamics simulations reproduce the observed ultrafast increase in lattice temperature and the corresponding conversion of photoenergy to lattice vibrations. Nonadiabatic quantum simulations further suggest that a softening of vibrational modes in the excited state is involved in efficient and rapid energy transfer between the electronic system and the lattice.