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Nanomaterials & Self-Organization

Let us think about the future clean energy systems. For large-scale electric power generation by solar cells, efficient use of high purity silicon is the key so that we are trying to improve the efficiency several-ten times by making single-crystalline thin films. Transparent electrodes are important for both solar cells (yielding electricity from light) and displays & lightings (generating lights from electricity), and we try to replace metal oxide semiconductors using rare-elements with carbon nanotubes or graphene. Nanotube-silicon hybrids are promising to realize Li ion batteries of larger capacities for (hybrid) electric vehicles. In this way, nanotechnology can bring innovations widely even if we use abundant carbon and silicon elements only, and contributes to sustainable technological society.

But nanomaterials can never be made in macro-scale if we artificially manipulate atoms/molecules one-by-one. Self-organization, i.e. spontaneous formation of materials from numerous atoms/molecules, is the key. We are trying to fundamentally understand the processes of chemical reactions of atoms/molecules, formation of nanostructures, and evolution of higher-order structures. Based on the fundamental understandings with flexible thinking and idea, we are proposing and developing novel processes for nanomaterials and their devices.

Synthesis of Carbon Nanotubes

Single-wall carbon nanotubes (SWCNTs) are a unique 1D nanomaterial quite thin ~nm and long ~mm. Extensive research made in physics/science fields clarified many unique properties and potential applications for them. On the other hand, as their price (more expensive than gold) shows, their fabrication process is still under development and their practical applications are very much limited. Chemistry & engineering should lead the innovations for their production and manufacturing. We have developed rapid growth process of millimeter-long SWCNTs and are trying to realize their practical production. Please click here for details. We are developing mass-production processes of CNTs by utilizing three-dimensional space of reactors, and direct fabrication of various devices by growing CNTs on substrates. (3D Synthesis) Soichiro HACHIYA (M2): Production of long single-wall CNTs by fluidized-bed. Shohei OKADA (M1): Flame synthesis of single-wall CNTs. Gaiya OGAWA (B4): Gas-phase continuous synthesis of CNTs by floating-supported catalyst. Katsuya NAMIKI (B4): Continuous production of single-wall CNTs and their fibers by floating catalyst CVD method. Yohei MAEDA (B4): Development of gas-phase continuous production process of carbon nanoparticle-nanotube hybrids. Risa MAEDA (B4): Wet preparation of catalysts on ceramic powders and fluidized-bed synthesis of long CNTs. Masahiro YOSHIDA (B4): Dry preparation of catalysts on ceramic powders and fluidized-bed synthesis of long CNTs. (2D Synthesis) Mami TAKABATAKE (M2): Pattern growth, hybridization, and conductive application of vertically aligned CNTs. Ryo YAMADA (M2): Packing carbon fiber into polymer sheet at high density and vertical alignment for thermal interface material application. Shunji KOBAYASHI (M1): Synthesis of CNTs on both faces of Cu, their structure control and thermal interface material application. Michiko EDO (B4): Combinatorial screening of binary metal catalyst for chirality controlled synthesis of CNTs. Sae KITAGAWA (B4): On metal synthesis, morphology control, and electron emitter application of CNTs. Toshihiro SATO (B4): Reactivity evaluation of various carbon feed gases for CNTs by cold-gas CVD method. Tatsuya TOMINAGA (B4): On-foil growth, structure control, and battery application of CNTs. Shota MIURA (B4): On Al synthesis, morphology control, and heat-transfer application of carbon nanotubes.

Rapid SWCNT growth Larger Movie. Continuous production by fluidized bed: Movie

Graphene and Thin Films

Battery Applications of CNTs

Rapid Vapor Deposition

Thin films of silicon and various metals are supporting the modern society widely. They are essential components in solar cells and rechargeable batteries, and such clean energy devices needs to be produced simply and rapidly at low cost to be widely used. Vacuum deposition is normally used in basic research to fabricate thin films slowly and carefully under ultrahigh vacuum, however, it realizes rapid low-cost production of thin films such as aluminum-coated plastic films for potato crisps packages. By heating the source material at temperature much higher than its melting point, rapid deposition at 10 um/min becomes possible. We are developing rapid vapor deposition processes of highly crystalline Si films for solar cells, porous Si films for lithium secondary batteries, and functionalized metal films for current collectors in secondary batteries and electrochemical capacitors. Shigeki AOI (M2): Rapid vapor deposition of Cu, hybridization with CNTs, and application to Li secondary battery anodes. Eri MURAMOTO (M2): Simple fabrication and performance improvement of CNT-coated Si solar cells. Makoto FUJITA (M1): Rapid vapor deposition and transfer processes of crystalline Si films for solar cells. Yoichiro HONDA (M1): Rapid vapor deposition of Al, hybridization with CNTs, and current collector application for battery/capacitors. Naoya ISHIJIMA (B4): Development of CNT-printed flexible Si solar cells Yuta HASHIZUME (B4): Rapid vapor deposition of self-supporting Si/metal/Si films and their application to lithium secondary battery anodes

1-min-epitaxy and lift-off of Si films for solar cells 1-min deposition of porous Si films for Li ion batteries

Previous Ph. D. Theses

• Ricardo QUINTERO RESTREPO, "Development of lightweight electrochemical capacitor electrodes based on a three dimensional carbon capturing capacitive particles," Univ. Tokyo (2015).
• Zhongming CHEN, "Development of production methods of submillimeter-long carbon nanotubes," Univ. Tokyo (2014).
• Kei HASEGAWA, "Millimeter-scale growth of single-walled carbon nanotubes on substrates," Univ. Tokyo (2011).
• Hisashi SUGIME, "Clarification of catalytic growth mechanism of single-walled carbon nanotubes and control of their synthesis," Univ. Tokyo (2010).
• Kazunori KAKEHI, "Growth of single- and multi-walled carbon nanotubes catalyzed by sputter-deposited metal nanoparticles," Univ. Tokyo (2008).

Previous Master Theses

• Ittetsu OHBA, "Suspending supported catalysts in the gas-phase and continuous production of carbon nanotubes," Waseda University (2016).
• Kosuke KAWABATA, "Gas-phase deposition of catalyst on fine ceramic powders and fluidized-bed production of carbon nanotubes," Waseda University (2016).
• Yuri KISHIDA, "Direct formation of graphene on SiO₂ substrates by dissolving carbon in Co films and etching Co by Cl₂," Waseda University (2016).
• Masaaki KURIYA, "Development of seamless gas-phase production process of acetylene black-carbon nanotube hybrids," Waseda University (2016).
• Yusuke SUGINO, "Formation of floating-supported catalysts in the gas-phase and continuous production of carbon nanotubes," Waseda University (2016).
• Noriyoshi NAKAMURA, "Catalyst particle formation by rapid heating and cooling of ferrocene and gas-phase continuous production of carbon nanotubes," Waseda University (2016).
• Misato NARUBAYASHI, "Development of electrochemical capacitor electrodes by hybridizing self-supporting films of carbon nanotubes with MnO₂ particles," Waseda University (2016).
• Kohtaro YAMAGUCHI, "Interface and seed control of solid-phase growth of graphene and gas-phase growth of carbon nanotubes," Waseda University (2016).
• Yuhei YAMASAKI, "Fabrication of large-grain crystalline Si thin films by rapid vapor deposition with in situ melt-crystallization," Waseda University (2016).
• Yu YOSHIHARA, "Fabrication and control of carbon nanotube structures via gas- and liquid-phase processes," Waseda University (2016).
• Asahi OHKAWA, "Development of practical CVD synthesis and transfer processes of graphene," Waseda University (2015).
• Hiroyuki SHIRAE, "Loss-free fabrication process of highly-conductive, flexible CNT films," Waseda University (2015).
• Nan FANG, "Rapid vapor deposition and electrochemical evaluation of porous Si films on flexible current collectors for Li secondary battery anodes," Waseda University (2015).
• Mai YAMAGUCHI, "Flame synthesis of single-wall carbon nanotube and control over the temperature field and reactions," Waseda University (2015).
• Masaki KOSAKA, "Direct fabrication of metal-free graphene on substrates and its structural control," Univ. Tokyo (2014).
• Yusuke KON, "Development of fluidized-bed process for synthesis of single-wall carbon nanotubes," Univ. Tokyo (2013).
• Kosuke HIROTA, "Fabrication of large-diameter crystalline silicon thin films for solar-cells by rapid vapor deposition method," Univ. Tokyo (2013).
• Tatsuya MASUDA, "Control of crystal growth of graphene via chemical vapor deposition using copper catalysts in face-to-face layout," Univ. Tokyo (2013).
• Jun OHSHIMA, "Flame synthesis of single-wall carbon nanotubes," Univ. Tokyo (2011).
• Yoshikuni SATO, "Gas-phase synthesis of single-wall carbon nanotubes and their structure control," Univ. Tokyo (2011).
• Nu-Ri NA, "Low temperature growth of vertically aligned dense carbon nanotube arrays on substrates," Univ. Tokyo (2011).
• Kotaro SEKIGUCHI, "Instant implementation of carbon nanotube field emitters by pulse-current heating CVD," Univ. Tokyo (2011).
• Soichiro TAKANO, "Direct fabrication of metal-free graphene films on substrates," Univ. Tokyo (2011).
• Kyu-Ha LEE, "Fabrication of dense FePt nanorod arrays by separation of sputtered polycrystalline films at their grain boundaries," Univ. Tokyo (2011).
• Heunku KANG, "Fabrication of graphene from amorphous carbon by metal-induced crystallization and crystal growth mechanism," Univ. Tokyo (2011).
• Suarpa KETPREECHASAWAT, "Self-organized networks of carbon nanotubes and their transparent conducting properties (2010).
• Sang Wook PARK, "Sustainable centimeter-scale growth of carbon nanotubes," Univ. Tokyo (2010).
• Yoko ISHITSUKA, "Gas-phase synthesis of single-walled carbon nanotubes by gas-suspended catalysts and their growth mechanism," Univ. Tokyo (2010).
• Yukie TSUJI, "Structural control of polycrystalline cobalt silicide thin films," Univ. Tokyo (2010).
• Keisuke NOMURA, "Development of catalysts for low temperature growth of carbon nanotubes," Univ. Tokyo (2010).
• Takashi SHIRAI, "Low temperature growth of carbon nanotubes and their dense growth by thin-film catalysts (2009).
• F. Kanyiri MUNGAI, "Rapid epitaxial growth and lift-off process for fabrication of single-crystalline silicon thin films for solar cells," Univ. Tokyo (2009).
• Shingo MOROKUMA, "Development of Si thin film anode for Li ion secondary battery," Univ. Tokyo (2009).
• Ryuhei ITO, "Separate control of the gas-phase and catalytic reactions in catalytic CVD synthesis of carbon nanotubes," Univ. Tokyo (2008).
• Satoshi TAKASHIMA, "Understanding of Cu deposition mechanism under chlorine atmosphere and development of via-filling process," Univ. Tokyo (2008).
• Kei HASEGAWA, "Rapid growth of single-walled carbon nanotubes on substrate by thermal CVD method," Univ. Tokyo (2008).
• Hiroshi OHSHIMA, "Synthesis and characterization of amorphous silica film showing phase transition from semiconductor to insulator," Univ. Tokyo (2007).
• Yuichi KUWAHARA, "Fabrication of crystalline silicon thin films for solar cells by epitaxial lift-off method (2007).
• Hisashi SUGIME, "Combinatorial screening of catalysts and basics and control of single-walled carbon nanotube growth," Univ. Tokyo (2007).
• Azusa MORISHITA, "Grain boundary control of sputtered, magnetic FePt nanocrystalline thin films," Univ. Tokyo (2007).

Previous Bachelor Theses

• Shohei OKADA, "Flame synthesis of carbon nanotubes with controlled gas-mixing," Waseda University (2016).
• Sohki KUZUHARA, "Development of electrode for oxygen reduction by hybridization of carbon nanotubes with zirconium oxide," Waseda University (2016).
• Shunji KOBAYASHI, "Fabrication and structure control of vertically aligned carbon nanotubes on Cu foils for thermal interface materials," Waseda University (2016).
• Yukuya NAGAI, "Synthesis of graphene from Sn-containing organic molecules and carbon monoxide," Waseda University (2016).
• Kohki HAMADA, "Purification of carbon nanotubes by dry-process and formation of hexagonal boron nitride on substrates," Waseda University (2016).
• Makoto FUJITA, "Fabrication of polycrystalline silicon films by vapor deposition of liquid and their separation from growth substrates," Waseda University (2016).
• Yoichiro HONDA, "Fabrication of aluminum-carbon nanotube hybrid foils by rapid vapor deposition and their application to electrodes in electric storage devices," Waseda University (2016).
• Taisuke MINAMIDE, "Fabrication of epitaxial Cu films by rapid vapor deposition and their use for controlled synthesis of graphene," Waseda University (2016).
• Kohei MIYADERA, "Trial of metal-foil-less capacitors based on carbon nanotube current collectors," Waseda University (2016).
• Go YAMAGATA, "Development of hybrid film of carbon nanotubes and lithium iron phosphate for lithium ion battery cathodes," Waseda University (2016).
• Ryo WATANABE, "Development of transfer process of graphene for graphene-silicon solar cells," Waseda University (2016).
• Shigeki AOI, "Rapid vapor deposition of Cu films for Li secondary batteries," Waseda University (2015).
• Sachie AKIBA, "Direct fabrication and structural control of few-layer graphene on substrates by etching-precipitation method," Waseda University (2015).
• Naiao XU, "Hybrid electrodes of graphene oxide with carbon nanotubes for electrochemical capacitors," Waseda University (2015).
• Takayuki KOWASE, "Gas-phase synthesis of silicon nanoparticles by evaporation method and fabrication of thick 3D anodes for Li secondary batteries," Waseda University (2015).
• Mami TAKABATAKE, "Resistivity reduction and mechanism of various carbon materials by Br2-doping," Waseda University (2015).
• Soichiro HACHIYA, "Synthesis of carbon nanotubes on powders by fluidized bed and their total collection by gas flow," Waseda University (2015).
• Keisuke HORI,"CNT-sponge-base cathodes capturing sulfur for Li-S batteries," Waseda University (2015).
• Eri MURAMOTO, "Structure requirements and optimization of solar cells based on crystalline Si coated with CNTs," Waseda University (2015).
• Yusuke MORIKAWA, "Direct fabrication of silicon particle films on current collectors for Li secondary batteries," Waseda University (2015).
• Ryo YAMADA, "Loss-free printing of flexible carbon nanotube films with controlled patterns," Waseda University (2015).
• Ittetsu OHBA, "Creation of aerosol supported catalyst from colloidal solution and gas-phase synthesis of carbon nanotubes," Waseda Univ. (2014).
• Kosuke KAWABATA, "Synthesis of submillimeter-long carbon nanotubes using catalysts by impregnation," Waseda Univ. (2014).
• Yuri KISHIDA, "Direct synthesis of graphene on dielectric substrates from Co-C mixture films by etching-precipitation method," Waseda Univ. (2014).
• Masaaki KURIYA, "Hybrid formation through carbon nanotube growth on acetylene black particles and reaction control in 1-second time scale ," Waseda Univ. (2014).
• Yusuke SUGINO, "Creation of aerosol supported catalyst from catalyst salt solution and gas-phase synthesis of carbon nanotube," Waseda Univ. (2014).
• Noriyoshi NAKAMURA, "Continuous production of carbon nanotubes using arc-discharge and gaseous carbon source," Waseda Univ. (2014).
• Misato NARUBAYASHI, "Fabrication of hybrid electrodes of self-supporting carbon nanotube films with MnO2 particles for electrochemical capacitors," Waseda Univ. (2014).
• Kohtaro YAMAGUCHI, "Fabrication and structure control of graphene thin films by gas-phase and solid-phase processes," Waseda Univ. (2014).
• Yuhei YAMASAKI, "Fabrication method of crystalline silicon thin films for flexible solar cells ," Waseda Univ. (2014).
• Yu YOSHIHARA, "Fabrication of Cu-C hybrid films by sputter-deposition and evaluation of their conductivity and current-carrying capacity," Waseda Univ. (2014).
• Asahi OHKAWA, "Transfer of graphene synthesized by CVD on catalysts and repeated use of the catalysts," Waseda Univ. (2013).
• Hiroyuki SHIRAE, "Facile fabrication of flexible wirings and transparent electrodes of carbon nanotubes," Waseda Univ. (2013).
• Nan FANG, "Rapid vapor deposition of silicon-based porous films for anodes of lithium ion batteries," Waseda Univ. (2013).
• Mai YAMAGUCHI, "Flame synthesis of single-wall carbon nanotubes," Waseda Univ. (2013).
• Kosuke HIROTA, "Fabrication of single-crystalline silicon thin films for solar cells by rapid vapor deposition and epitaxial lift-off methods," Univ. Tokyo (2011).
• Tatsuya MASUDA, "Fabrication and structural control of graphene by chemical vapor deposition using Cu thin film catalysts," Univ. Tokyo (2011).
• Yoshikuni SATO, "Gas-phase synthesis of single-walled carbon nanotube seeds," Univ. Tokyo (2010).
• Kotaro SEKIGUCHI, "Instant implementation of carbon nanotube field emitters by pulse-current heating (2009).
• Soichiro TAKANO, "Developing a selective filling method of micro-pores," Univ. Tokyo (2009).
• Yukie TSUJI, "Understanding and controlling crystal growth of cobalt silicide thin films for electronic devices (2008).
• Keisuke NOMURA, "Low temperature growth of carbon nanotubes by function-shared catalysts," Univ. Tokyo (2008).
• Shingo MOROKUMA, "Structural change of catalyst nanoparticles during carbon nanotube growth," Univ. Tokyo (2007).

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