1:15 PM - 1:30 PM

[2D10] New low-temperature methanol synthesis from syngas containing CO₂ via self-catalysis of methanol and Cu/ZnO catalysts

○Fei Chen¹, Guohui Yang¹, Noritatsu Tsubaki¹ (1. University of Toyama)

Binary Cu/ZnO catalysts were prepared by solid-state method and tested for vapor-phase low-temperature methanol synthesis from CO₂-containing syngas. The physicochemical properties were studied by XRD, XPS, XAES, XRF, H₂-TPR, SEM, TEM, N₂ physisorption, N₂O chemisorption, TG-DTA, FT-IR, CO₂-TPD and NH₃-TPD techniques. The H₂C₂O₄/(Cu+Zn) molar ratio had an obvious effect on the physicochemical properties and thus influenced the catalytic activity. The space time yield (STY) of methanol exhibited a linear relationship with the Cu⁰ surface area, and also increased linearly by enhancing the number of strongly acidic sites or moderately basic sites. The effects of reaction temperature, flow rate of accompanying methanol promoter and catalyst stability were also investigated in detail. A suitable H₂C₂O₄ amount was favorable for improving the catalytic activity. And maximum turnover frequency (TOF) and STY values were obtained over C_4-Red catalyst. The present work provided new insights in designing highly efficient Cu/ZnO catalysts for methanol synthesis.

1:30 PM - 1:45 PM

[2D11] Directly conversion of syngas to aromatics over Fe-based ZSM-5 catalysts

○Baizhang Zhang¹, Guohui Yang¹, Noritatsu Tsubaki¹ (1. Department of Applied Chemistry, School of Engineering, University of Toyama)

Synthesis gas derived from coal, natural gas and biomass can be selectively converted into various fuels and chemicals such as aromatics via the Fischer–Tropsch synthesis (FTS) reaction in which iron- and cobalt-based catalysts are most widely used.
The iron-based FTS catalyst prepared by co-precipitation was combined with ZSM-5 zeolite to reach high selectivity of aromatics.The effect of the Si/Al ratio and post-treatment conditions on the ZSM-5 zeolites were investigated. Specific morphologic ZSM-5 zeolites synthesized by hydrothermal reaction were also examined.

1:45 PM - 2:00 PM

[2D12] Low-temperature oxidative coupling of methane over Ce-containing MFI-supported Pd catalysts

○Mizuho Yabushita¹, Motohiro Yoshida², Ryota Osuga², Fumiya Muto², Shoji Iguchi³, Shuhei Yasuda⁴, Atsushi Neya², Mami Horie², Sachiko Maki^5,2, Kiyoshi Kanie^2,5, Ichiro Yamanaka^3,6, Toshiyuki Yokoi⁴, Atsushi Muramatsu^2,5,6 (1. School of Engineering, Tohoku University, 2. Institute of Multidisciplinary Research for Advanced Materials, Tohoku University, 3. School of Materials and Chemical Technology, Tokyo Institute of Technology, 4. Institute for Innovative Research, Tokyo Institute of Technology, 5. International Center for Synchrotron Radiation Innovation Smart, Tohoku University, 6. JST-CREST)

メタンを基幹化合物へと直接かつ温和な条件で変換可能な触媒反応系の確立が求められている。我々は、メカノケミカル法によってCe含有MFI型ゼオライトを調製し、これにPdを担持することで、400度以下でも酸化的カップリング反応が進行してC2化合物が生成することを見出した。高分解能STEMおよびXAFS測定の結果から、従来の担持法では形成できない高分散かつ微小なCe種が形成しており、これが重要な役割を果たしていることが示唆された。

2:00 PM - 2:15 PM

[2D13] Low-temperature oxidative coupling of methane over metal-supported Ce-containing zeolite catalyst

○Ryota Osuga¹, Motohiro Yoshida¹, Atsushi Neya¹, Shuhei Yasuda², Kakeru Ninomiya¹, Mizuho Yabushita¹, Sachiko Maki¹, Maiko Nishibori¹, Kiyoshi Kanie¹, Toshiyuki Yokoi², Atsushi Muramatsu^1,3 (1. Tohoku University, 2. Tokyo Institute of Technology, 3. JST-CREST)

メタンを基幹化学品へと転換する触媒開発は、古くから盛んに行われているが、そのほとんどは、700 °C以上の高温を必要とするため、環境調和型のプロセスとは言い難い。我々は、メカノケミカル法と呼ばれる独自のゼオライト合成手法により調製したCe含有ゼオライト担持金属触媒を用いることで、比較的温和な条件下（400 °C以下）でのメタン酸化カップリング反応の実現を目指した。本発表では、2種類の金属種を担持した触媒の反応活性について報告する。

2:15 PM - 2:30 PM

[2D14] Oxidative coupling of methane over La-Ca-Al-O perovskite catalysts in an electric field

○Shuhei Ogo^1,2, Yuna Takeno², Harunobu Tedzuka², Tadaharu Ueda¹, Yasushi Sekine² (1. Kochi University, 2. Waseda University)

La-Ca-Al-O系ペロブスカイト触媒を用いた低温電場中でのメタン酸化カップリングにおける酸化剤（O₂，H₂O）の影響について検討した。いずれの酸化剤を用いた時にも，電場中では触媒表面に形成された電子不足な表面酸素種の消費と再生を繰り返す酸化還元型の機構で反応が進行した。また酸化剤の種類や濃度が表面酸素種の埋め戻し速度に影響し，触媒活性は表面酸素種の埋め戻し速度に支配されることを見出した。

Session information

[2D10-14] C1 chemistry(1)

[2D10] New low-temperature methanol synthesis from syngas containing CO₂ via self-catalysis of methanol and Cu/ZnO catalysts

[2D11] Directly conversion of syngas to aromatics over Fe-based ZSM-5 catalysts

[2D12] Low-temperature oxidative coupling of methane over Ce-containing MFI-supported Pd catalysts

[2D13] Low-temperature oxidative coupling of methane over metal-supported Ce-containing zeolite catalyst

[2D14] Oxidative coupling of methane over La-Ca-Al-O perovskite catalysts in an electric field

Authentication

Session information

[2D10-14] C1 chemistry(1)

[2D10] New low-temperature methanol synthesis from syngas containing CO2 via self-catalysis of methanol and Cu/ZnO catalysts

[2D11] Directly conversion of syngas to aromatics over Fe-based ZSM-5 catalysts

[2D12] Low-temperature oxidative coupling of methane over Ce-containing MFI-supported Pd catalysts

[2D13] Low-temperature oxidative coupling of methane over metal-supported Ce-containing zeolite catalyst

[2D14] Oxidative coupling of methane over La-Ca-Al-O perovskite catalysts in an electric field

Authentication

[2D10] New low-temperature methanol synthesis from syngas containing CO₂ via self-catalysis of methanol and Cu/ZnO catalysts