Browsing by Author "Lin, Jian"
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Item A scientific machine learning framework to understand flash graphene synthesis(Royal Society of Chemistry, 2023) Sattari, Kianoosh; Eddy, Lucas; Beckham, Jacob L.; Wyss, Kevin M.; Byfield, Richard; Qian, Long; Tour, James M.; Lin, Jian; NanoCarbon Center; Welch Institute for Advanced MaterialsFlash Joule heating (FJH) is a far-from-equilibrium (FFE) processing method for converting low-value carbon-based materials to flash graphene (FG). Despite its promises in scalability and performance, attempts to explore the reaction mechanism have been limited due to the complexities involved in the FFE process. Data-driven machine learning (ML) models effectively account for the complexities, but the model training requires a considerable amount of experimental data. To tackle this challenge, we constructed a scientific ML (SML) framework trained by using both direct processing variables and indirect, physics-informed variables to predict the FG yield. The indirect variables include current-derived features (final current, maximum current, and charge density) predicted from the proxy ML models and reaction temperatures simulated from multi-physics modeling. With the combined indirect features, the final ML model achieves an average R2 score of 0.81 ± 0.05 and an average RMSE of 12.1% ± 2.0% in predicting the FG yield, which is significantly higher than the model trained without them (R2 of 0.73 ± 0.05 and an RMSE of 14.3% ± 2.0%). Feature importance analysis validates the key roles of these indirect features in determining the reaction outcome. These results illustrate the promise of this SML to elucidate FFE material synthesis outcomes, thus paving a new avenue to processing other datasets from the materials systems involving the same or different FFE processes.Item Addressable SiOX memory array with incorporated diodes(2016-07-05) Tour, James M.; Yao, Jun; Lin, Jian; Wang, Gunuk; Palem, Krishna; Rice University; Nanyang Technological University; United States Patent and Trademark OfficeVarious embodiments of the resistive memory cells and arrays discussed herein comprise: (1) a first electrode; (2) a second electrode; (3) resistive memory material; and (4) a diode. The resistive memory material is selected from the group consisting of SiOx, SiOxH, SiOxNy, SiOxNyH, SiOxCz, SiOxCzH, and combinations thereof, wherein each of x, y and z are equal to or greater than 1 and equal to or less than 2. The diode may be any suitable diode, such as n-p diodes, p-n diodes, and Schottky diodes.Item Graphene-carbon nanotube hybrid materials and use as electrodes(2016-09-27) Tour, James M.; Zhu, Yu; Li, Lei; Yan, Zheng; Lin, Jian; Rice University; United States Patent and Trademark OfficeProvided are methods of making graphene-carbon nanotube hybrid materials. Such methods generally include: (1) associating a graphene film with a substrate; (2) applying a catalyst and a carbon source to the graphene film; and (3) growing carbon nanotubes on the graphene film. The grown carbon nanotubes become covalently linked to the graphene film through carbon-carbon bonds that are located at one or more junctions between the carbon nanotubes and the graphene film. In addition, the grown carbon nanotubes are in ohmic contact with the graphene film through the carbon-carbon bonds at the one or more junctions. The one or more junctions may include seven-membered carbon rings. Also provided are the formed graphene-carbon nanotube hybrid materials.Item Hydrogen Diffusion and Stabilization in Single-Crystal VO2 Micro/Nanobeams by Direct Atomic Hydrogenation(American Chemical Society, 2014) Lin, Jian; Ji, Heng; Swift, Michael W.; Hardy, Will J.; Peng, Zhiwei; Fan, Xiujun; Nevidomskyy, Andriy H.; Tour, James M.; Natelson, Douglas; Smalley Institute for Nanoscale Science and TechnologyWe report measurements of the diffusion of atomic hydrogen in single crystalline VO2 micro/nanobeams by direct exposure to atomic hydrogen, without catalyst. The atomic hydrogen is generated by a hot filament, and the doping process takes place at moderate temperature (373 K). Undoped VO2 has a metal-to-insulator phase transition at ∼340 K between a high-temperature, rutile, metallic phase and a low-temperature, monoclinic, insulating phase with a resistance exhibiting a semiconductor-like temperature dependence. Atomic hydrogenation results in stabilization of the metallic phase of VO2 micro/nanobeams down to 2 K, the lowest point we could reach in our measurement setup. Optical characterization shows that hydrogen atoms prefer to diffuse along the c axis of rutile (a axis of monoclinic) VO2, along the oxygen “channels”. Based on observing the movement of the hydrogen diffusion front in single crystalline VO2 beams, we estimate the diffusion constant for hydrogen along the c axis of the rutile phase to be 6.7 × 10–10 cm2/s at approximately 373 K, exceeding the value in isostructural TiO2 by ∼38×. Moreover, we find that the diffusion constant along the c axis of the rutile phase exceeds that along the equivalent a axis of the monoclinic phase by at least 3 orders of magnitude. This remarkable change in kinetics must originate from the distortion of the “channels” when the unit cell doubles along this direction upon cooling into the monoclinic structure. Ab initio calculation results are in good agreement with the experimental trends in the relative kinetics of the two phases. This raises the possibility of a switchable membrane for hydrogen transport.Item Laser induced graphene materials and their use in electronic devices(2022-09-06) Tour, James M; Lin, Jian; Peng, Zhiwei; Kittrell, Wilbur Carter; Rice University; William Marsh Rice University; United States Patent and Trademark OfficeIn some embodiments, the present disclosure pertains to methods of producing a graphene material by exposing a polymer to a laser source. In some embodiments, the exposing results in formation of a graphene from the polymer. In some embodiments, the methods of the present disclosure also include a step of separating the formed graphene from the polymer to form an isolated graphene. In some embodiments, the methods of the present disclosure also include a step of incorporating the graphene material or the isolated graphene into an electronic device, such as an energy storage device. In some embodiments, the graphene is utilized as at least one of an electrode, current collector or additive in the electronic device. Additional embodiments of the present disclosure pertain to the graphene materials, isolated graphenes, and electronic devices that are formed by the methods of the present disclosure.Item Laser induced graphene materials and their use in electronic devices(2019-12-10) Tour, James M.; Lin, Jian; Peng, Zhiwei; Kittrell, Carter; Rice University; United States Patent and Trademark OfficeIn some embodiments, the present disclosure pertains to methods of producing a graphene material by exposing a polymer to a laser source. In some embodiments, the exposing results in formation of a graphene from the polymer. In some embodiments, the methods of the present disclosure also include a step of separating the formed graphene from the polymer to form an isolated graphene. In some embodiments, the methods of the present disclosure also include a step of incorporating the graphene material or the isolated graphene into an electronic device, such as an energy storage device. In some embodiments, the graphene is utilized as at least one of an electrode, current collector or additive in the electronic device. Additional embodiments of the present disclosure pertain to the graphene materials, isolated graphenes, and electronic devices that are formed by the methods of the present disclosure.Item Laser-induced porous graphene films from commercial polymers(Nature Publishing Group, 2014) Lin, Jian; Peng, Zhiwei; Liu, Yuanyue; Ruiz-Zepeda, Francisco; Ye, Ruquan; Samuel, Errol L.G.; Yacaman, Miguel Jose; Yakobson, Boris I.; Tour, James M.; Smalley Institute for Nanoscale Science and TechnologyThe cost effective synthesis and patterning of carbon nanomaterials is a challenge in electronic and energy storage devices. Here we report a one-step, scalable approach for producing and patterning porous graphene films with three-dimensional networks from commercial polymer films using a CO2 infrared laser. The sp3-carbon atoms are photothermally converted to sp2-carbon atoms by pulsed laser irradiation. The resulting laser-induced graphene (LIG) exhibits high electrical conductivity. The LIG can be readily patterned to interdigitated electrodes for in-plane microsupercapacitors with specific capacitances of >4 mF cm-2 and power densities of ~9 mW cm-2. Theoretical calculations partially suggest that enhanced capacitance may result from LIG's unusual ultra-polycrystalline lattice of pentagon-heptagon structures. Combined with the advantage of one-step processing of LIG in air from commercial polymer sheets, which would allow the employment of a roll-to-roll manufacturing process, this technique provides a rapid route to polymer-written electronic and energy storage devices.Item Methods of producing graphene quantum dots from coal and coke(2018-03-20) Tour, James M.; Ye, Ruquan; Xiang, Changsheng; Lin, Jian; Peng, Zhiwei; Ceriotti, Gabriel; Rice University; United States Patent and Trademark OfficeIn some embodiments, the present disclosure pertains to methods of making graphene quantum dots from a carbon source (e.g., coal, coke, and combinations thereof) by exposing the carbon source to an oxidant. In some embodiments, the methods of the present disclosure further comprise a step of separating the formed graphene quantum dots from the oxidant. In some embodiments, the methods of the present disclosure further comprise a step of reducing the formed graphene quantum dots. In some embodiments, the methods of the present disclosure further comprise a step of enhancing a quantum yield of the graphene quantum dots. In further embodiments, the methods of the present disclosure also include a step of controlling the diameter of the formed graphene quantum dots by selecting the carbon source. In some embodiments, the formed graphene quantum dots comprise oxygen addends or amorphous carbon addends on their edges.Item Programmed multimaterial assembly by synergized 3D printing and freeform laser induction(Springer Nature, 2024) Zheng, Bujingda; Xie, Yunchao; Xu, Shichen; Meng, Andrew C.; Wang, Shaoyun; Wu, Yuchao; Yang, Shuhong; Wan, Caixia; Huang, Guoliang; Tour, James M.; Lin, Jian; Smalley-Curl InstituteIn nature, structural and functional materials often form programmed three-dimensional (3D) assembly to perform daily functions, inspiring researchers to engineer multifunctional 3D structures. Despite much progress, a general method to fabricate and assemble a broad range of materials into functional 3D objects remains limited. Herein, to bridge the gap, we demonstrate a freeform multimaterial assembly process (FMAP) by integrating 3D printing (fused filament fabrication (FFF), direct ink writing (DIW)) with freeform laser induction (FLI). 3D printing performs the 3D structural material assembly, while FLI fabricates the functional materials in predesigned 3D space by synergistic, programmed control. This paper showcases the versatility of FMAP in spatially fabricating various types of functional materials (metals, semiconductors) within 3D structures for applications in crossbar circuits for LED display, a strain sensor for multifunctional springs and haptic manipulators, a UV sensor, a 3D electromagnet as a magnetic encoder, capacitive sensors for human machine interface, and an integrated microfluidic reactor with a built-in Joule heater for nanomaterial synthesis. This success underscores the potential of FMAP to redefine 3D printing and FLI for programmed multimaterial assembly.Item Rebar Graphene(American Chemical Society, 2014) Yan, Zheng; Peng, Zhiwei; Casillas, Gilberto; Lin, Jian; Xiang, Changsheng; Zhou, Haiqing; Yang, Yang; Ruan, Gedeng; Raji, Abdul-Rahman O.; Samuel, Errol L.G.; Hauge, Robert H.; Yacaman, Miguel Jose; Tour, James M.; Richard E. Smalley Institute for Nanoscale Science and TechnologyAs the cylindrical sp2-bonded carbon allotrope, carbon nanotubes (CNTs) have been widely used to reinforce bulk materials such as polymers, ceramics, and metals. However, both the concept demonstration and the fundamental understanding on how 1D CNTs reinforce atomically thin 2D layered materials, such as graphene, are still absent. Here, we demonstrate the successful synthesis of CNT-toughened graphene by simply annealing functionalized CNTs on Cu foils without needing to introduce extraneous carbon sources. The CNTs act as reinforcing bar (rebar), toughening the graphene through both π–π stacking domains and covalent bonding where the CNTs partially unzip and form a seamless 2D conjoined hybrid as revealed by aberration-corrected scanning transmission electron microscopy analysis. This is termed rebar graphene. Rebar graphene can be free-standing on water and transferred onto target substrates without needing a polymer-coating due to the rebar effects of the CNTs. The utility of rebar graphene sheets as flexible all-carbon transparent electrodes is demonstrated. The in-plane marriage of 1D nanotubes and 2D layered materials might herald an electrical and mechanical union that extends beyond carbon chemistry.Item Rebar Graphene from Functionalized Boron Nitride Nanotubes(American Chemical Society, 2015) Li, Yilun; Peng, Zhiwei; Larios, Eduardo; Wang, Gunuk; Lin, Jian; Yan, Zheng; Ruiz-Zepeda, Francisco; José-Yacamán, Miguel; Tour, James M.; Richard E. Smalley Institute for Nanoscale Science and TechnologyThe synthesis of rebar graphene on Cu substrates is described using functionalized boron nitride nanotubes (BNNTs) that were annealed or subjected to chemical vapor deposition (CVD) growth of graphene. Characterization shows that the BNNTs partially unzip and form a reinforcing bar (rebar) network within the graphene layer that enhances the mechanical strength through covalent bonds. The rebar graphene is transferrable to other substrates without polymer assistance. The optical transmittance and conductivity of the hybrid rebar graphene film was tested, and a field effect transistor was fabricated to explore its electrical properties. This method of synthesizing 2D hybrid graphene/BN structures should enable the hybridization of various 1D nanotube and 2D layered structures with enhanced mechanical properties.