R-3 Repository :: Browsing by Author "Peng, Zhiwei"

Browsing by Author "Peng, Zhiwei"

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Atomic cobalt on nitrogen-doped graphene for hydrogen generation
(Nature Publishing Group, 2015) Fei, Huilong; Dong, Juncai; Arellano-Jiménez, M. Josefina; Ye, Gonglan; Kim, Nam Dong; Samuel, Errol L.G.; Peng, Zhiwei; Zhu, Zhuan; Qin, Fan; Bao, Jiming; Yacaman, Miguel Jose; Ajayan, Pulickel M.; Chen, Dongliang; Tour, James M.
Reduction of water to hydrogen through electrocatalysis holds great promise for clean energy, but its large-scale application relies on the development of inexpensive and efficient catalysts to replace precious platinum catalysts. Here we report an electrocatalyst for hydrogen generation based on very small amounts of cobalt dispersed as individual atoms on nitrogen-doped graphene. This catalyst is robust and highly active in aqueous media with very low overpotentials (30 mV). A variety of analytical techniques and electrochemical measurements suggest that the catalytically active sites are associated with the metal centres coordinated to nitrogen. This unusual atomic constitution of supported metals is suggestive of a new approach to preparing extremely efficient single-atom catalysts.
Atomic H-Induced Mo2C Hybrid as an Active and Stable Bifunctional Electrocatalyst
(American Chemical Society, 2017) Fan, Xiujun; Liu, Yuanyue; Peng, Zhiwei; Zhang, Zhenhua; Zhou, Haiqing; Zhang, Xianming; Yakobson, Boris I.; Goddard, William A. III; Guo, Xia; Hauge, Robert H.; Tour, James M.; NanoCarbon Center
Mo2C nanocrystals (NCs) anchored on vertically aligned graphene nanoribbons (VA-GNR) as hybrid nanoelectrocatalysts (Mo2C–GNR) are synthesized through the direct carbonization of metallic Mo with atomic H treatment. The growth mechanism of Mo2C NCs with atomic H treatment is discussed. The Mo2C–GNR hybrid exhibits highly active and durable electrocatalytic performance for the hydrogen-evolution reaction (HER) and oxygen-reduction reaction (ORR). For HER, in an acidic solution the Mo2C–GNR has an onset potential of 39 mV and a Tafel slope of 65 mV dec–1, and in a basic solution Mo2C–GNR has an onset potential of 53 mV, and Tafel slope of 54 mV dec–1. It is stable in both acidic and basic media. Mo2C–GNR is a high-activity ORR catalyst with a high peak current density of 2.01 mA cm–2, an onset potential of 0.93 V that is more positive vs reversible hydrogen electrode (RHE), a high electron transfer number n (∼3.90), and long-term stability.
Cobalt Nanoparticles Embedded in Nitrogen-Doped Carbon for the Hydrogen Evolution Reaction
(American Chemical Society, 2015) Fei, Huilong; Yang, Yang; Peng, Zhiwei; Ruan, Gedeng; Zhong, Qifeng; Li, Lei; Samuel, Errol L.G.; Tour, James M.; Smalley Institute for Nanoscale Science and Technology
There is great interest in renewable and sustainable energy research to develop low-cost, highly efficient, and stable electrocatalysts as alternatives to replace Pt-based catalysts for the hydrogen evolution reaction (HER). Though nanoparticles encapsulated in carbon shells have been widely used to improve the electrode performances in energy storage devices (e.g., lithium ion batteries), they have attracted less attention in energy-related electrocatalysis. Here we report the synthesis of nitrogen-enriched core–shell structured cobalt–carbon nanoparticles dispersed on graphene sheets and we investigate their HER performances in both acidic and basic media. These catalysts exhibit excellent durability and HER activities with onset overpotentials as low as ∼70 mV in both acidic (0.5 M H2SO4) and alkaline (0.1 M NaOH) electrolytes, and the overpotentials needed to deliver 10 mA cm–2 are determined to be 265 mV in acid and 337 mV in base, further demonstrating their potential to replace Pt-based catalysts. Control experiments reveal that the active sites for HER might come from the synergistic effects between the cobalt nanoparticles and nitrogen-doped carbon.
Growth of graphene films from non-gaseous carbon sources
(2015-08-04) Tour, James; Sun, Zhengzong; Yan, Zheng; Ruan, Gedeng; Peng, Zhiwei; Rice University; United States Patent and Trademark Office
In various embodiments, the present disclosure provides methods of forming graphene films by: (1) depositing a non-gaseous carbon source onto a catalyst surface; (2) exposing the non-gaseous carbon source to at least one gas with a flow rate; and (3) initiating the conversion of the non-gaseous carbon source to the graphene film, where the thickness of the graphene film is controllable by the gas flow rate. Additional embodiments of the present disclosure pertain to graphene films made in accordance with the methods of the present disclosure.
High Performance Electrocatalytic Reaction of Hydrogen and Oxygen on Ruthenium Nanoclusters
(American Chemical Society, 2017) Ye, Ruquan; Liu, Yuanyue; Peng, Zhiwei; Wang, Tuo; Jalilov, Almaz S.; Yakobson, Boris I.; Wei, Su-Huai; Tour, James M.; Smalley Institute for Nanoscale Science and Technology
The development of catalytic materials for the hydrogen oxidation, hydrogen evolution, oxygen reduction or oxygen evolution reactions with high reaction rates and low overpotentials are key goals for the development of renewable energy. We report here Ru(0) nanoclusters supported on nitrogen-doped graphene as high-performance multifunctional catalysts for the hydrogen evolution reaction (HER) and oxygen reduction reaction (ORR), showing activities similar to that of commercial Pt/C in alkaline solution. For HER performance in alkaline media, sample Ru/NG-750 reaches 10 mA cm–2 at an overpotential of 8 mV with a Tafel slope of 30 mV dec–1. The high HER performance in alkaline solution is advantageous because most catalysts for ORR and oxygen evolution reaction (OER) also prefer alkaline solution environment whereas degrade in acidic electrolytes. For ORR performance, Ru/NG effectively catalyzes the conversion of O2 into OH– via a 4e process at a current density comparable to that of Pt/C. The unusual catalytic activities of Ru(0) nanoclusters reported here are important discoveries for the advancement of renewable energy conversion reactions.
High-Performance Hydrogen Evolution from MoS2(1–x)P x Solid Solution
(Wiley, 2016) Ye, Ruquan; Vicente, Paz Del Angel; Liu, Yuanyue; Arellano-Jimenez, Josefina; Peng, Zhiwei; Wang, Tuo; Li, Yilun; Yakobson, Boris I.; Wei, Su-Huai; Yacaman, Miguel Jose; Tour, James M.; Smalley Institute for Nanoscale Science and Technology
A MoS2(1-x)Px solid solution (x = 0 to 1) is formed by thermally annealing mixtures of MoS2 and red phosphorus. The effective and stable electrocatalyst for hydrogen evolution in acidic solution holds promise for replacing scarce and expensive platinum that is used in present catalyst systems. The high performance originates from the increased surface area and roughness of the solid solution.
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 Technology
We 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.
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 Office
In 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.
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 Office
In 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.
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 Technology
The 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.
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 Office
In 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.
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 Technology
As 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.
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 Technology
The 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.
Rebar hybrid materials and methods of making the same
(2018-02-20) Tour, James M.; Yan, Zheng; Peng, Zhiwei; Hauge, Robert H.; Li, Yilun; Rice University; United States Patent and Trademark Office
In some embodiments, the present disclosure pertains to methods of forming a reinforcing material by: (1) depositing a first material onto a catalyst surface; and (2) forming a second material on the catalyst surface, where the second material is derived from and associated with the first material. In some embodiments, the first material includes, without limitation, carbon nanotubes, graphene nanoribbons, boron nitride nanotubes, chalcogenide nanotubes, carbon onions, and combinations thereof. In some embodiments, the formed second material includes, without limitation, graphene, hexagonal boron nitride, chalcogenides, and combinations thereof. In additional embodiments, the methods of the present disclosure also include a step of separating the formed reinforcing material from the catalyst surface, and transferring the separated reinforcing material onto a substrate without the use of polymers. Additional embodiments of the present disclosure pertain to reinforcing materials formed by the aforementioned methods.
Synthesis and Application of Graphene Based Nanomaterials
(2015-04-08) Peng, Zhiwei; Tour, James M.; Engel, Paul S; Ringe, Emilie
Graphene, a two-dimensional sp2-bonded carbon material, has recently attracted major attention due to its excellent electrical, optical and mechanical properties. Depending on different applications, graphene and its derived hybrid nanomaterials can be synthesized by either bottom-up chemical vapor deposition (CVD) methods for electronics, or various top-down chemical reaction methods for energy generation and storage devices. My thesis begins with the investigation of CVD synthesis of graphene thin films in Chapter 1, including the direct growth of bilayer graphene on insulating substrates and synthesis of “rebar graphene”: a hybrid structure with graphene and carbon or boron nitride nanotubes. Chapter 2 discusses the synthesis of nanoribbon-shaped materials and their applications, including splitting of vertically aligned multi-walled carbon nanotube carpets for supercapacitors, synthesis of dispersable ferromagnetic graphene nanoribbon stacks with enhanced electrical percolation properties in magnetic field, graphene nanoribbon/SnO2 nanocomposite for lithium ion batteries, and enhanced electrocatalysis for hydrogen evolution reactions from WS2 nanoribbons. Next, Chapter 3 discusses graphene coated iron oxide nanomaterials and their use in energy storage applications. Finally, Chapter 4 introduces the development, characterization, and fabrication of laser induced graphene and its application as supercapacitors.
Three-Dimensional Nanoporous Fe2O3/Fe3C-Graphene Heterogeneous Thin Films for Lithium-Ion Batteries
(American Chemical Society, 2014) Yang, Yang; Fan, Xiujun; Casillas, Gilberto; Peng, Zhiwei; Ruan, Gedeng; Wang, Gunuk; Yacaman, Miguel Jose; Tour, James M.; Smalley Institute for Nanoscale Science and Technology
Three-dimensional self-organized nanoporous thin films integrated into a heterogeneous Fe2O3/Fe3C-graphene structure were fabricated using chemical vapor deposition. Few-layer graphene coated on the nanoporous thin film was used as a conductive passivation layer, and Fe3C was introduced to improve capacity retention and stability of the nanoporous layer. A possible interfacial lithium storage effect was anticipated to provide additional charge storage in the electrode. These nanoporous layers, when used as an anode in lithium-ion batteries, deliver greatly enhanced cyclability and rate capacity compared with pristine Fe2O3: a specific capacity of 356 μAh cm–2 μm–1 (3560 mAh cm–3 or ∼1118 mAh g–1) obtained at a discharge current density of 50 μA cm–2 (∼0.17 C) with 88% retention after 100 cycles and 165 μAh cm–2 μm–1(1650 mAh cm–3 or ∼518 mAh g–1) obtained at a discharge current density of 1000 μA cm–2(∼6.6 C) for 1000 cycles were achieved. Meanwhile an energy density of 294 μWh cm–2 μm–1(2.94 Wh cm–3 or ∼924 Wh kg–1) and power density of 584 μW cm–2 μm–1 (5.84 W cm–3 or ∼1834 W kg–1) were also obtained, which may make these thin film anodes promising as a power supply for micro- or even nanosized portable electronic devices.

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