歷年計畫優良成果:發展催化劑能在常溫常壓下有效能地轉換甲烷至甲醇

15 4 月

104-105年度「國立臺灣大學與中央研究院創新性合作計畫」

發展催化劑能在常溫常壓下有效能地轉換甲烷至甲醇

 

計劃成員:

中央研究院化學研究所:陳長謙院士與俞聖法副研究員

台灣大學化學系:牟中原院士與劉之誠博士

 

研究成果摘要

 

模擬自然界所存在的微粒體甲烷單加氧酶,研發當今第一個,能在常溫常壓下,活化高惰性烷烴化合物的銅分子催化試劑,能有效能地將甲烷液化成為甲醇,天然氣轉化成為醇基綠能分子;目前將此催化平台應用於國內苗栗區域天然氣田的轉換測試,亦有初步成果。將有機會運用於大氣中低濃度小分子烷烴化合物等減碳應用。成果陸續發表於國際上一流的高影響力工程與科學期刊,包含Energy Environ. Sci. 2016、Chem. Rev. 2017、Angew. Chem. Int. Ed. 2018以及ACS Sustain. Chem. Eng. 2018等。美國發明專利,亦已於今年通過,並撰寫專書章節與高影響力之回顧性期刊文稿,報導研發歷程。

 

發表著作

 

  1. Thiyagarajan, N.; Janmanchi, D.; Tsai, Y.-F.; Wanna, W. H.; Ramu, R.; Chan, S. I.*; Zen, J.-M.*; Yu, S. S.-F.* “A Carbon Electrode Functionalized by a Tricopper Cluster Complex: Overcoming Overpotential and Production of Hydrogen Peroxide in the Oxygen Reduction Reaction,” Angew. Chem. Int. Ed. 2018, 57, 3612.
  2. Liu, C.-C.; Janmanchi, D., Wen, D.-R.; Oung, J.-N.; Mou, C.-Y.; Yu, S. S.-F.; Chan S. I.* “Catalytic Oxidation of Light Alkanes Mediated at Room Temperature by a Tricopper Cluster Complex Immobilized in Mesoporous Silica Nanoparticles,” ACS Sustain. Chem. Eng. 2018, 6, 5431.
  1. Yeh, C.-H.; Yu, S. S.-F.; Chan, S. I.; Jiang, J.-C.* “Quantum Chemical Studies of Methane Oxidation to Methanol on a Biomimetic Tricopper Complex: Mechanistic Insights,” ChemistrySelect 2018, 3, 5113.
    1. Wang, V. C.-C.; Maji, S.; Chen, P. P.-Y.; Lee, H. K.; Yu, S. S.-F.; Chan S. I.* “ Alkane Oxidation: Methane Monooxygenases, Related Enzymes, and Their Biomimetics” Chem. Rev. 2017, 117, 8574.
    2. Liu, C.-C.; Mou, C.-Y.; Yu, S. S.-F.; Chan, S. I.* “Heterogeneous Formulation of the Tricopper Complex for Efficient Catalytic Conversion of Methane into Methanol at Ambient Temperature and pressure,” Energy Environ. Sci. 2016, 9, 1361.
    3. Liu, C.-C.; Ramu, R.; Chan, S. I.*; Mou, C.-Y.*; Yu S. S.-F.* “Chemistry in Confined Space: A Strategy for Selective Oxidation of Hydrocarbons with High Catalytic Efficiencies and Conversion Yields under Ambient Conditions,” Sci. Technol. 2016, 6, 7623.

 

 

美國專利

Chan S. I.; Yu, S. S.-F.; Nagababu P.; Maji, S.; Chen, P. P.-Y.; Mou, C.-Y.; Liu, C. C. “Molecular Catalyst Capable of Catalyzing Oxidation of Hydrocarbons and Method for Oxidizing Hydrocarbons,” US Patent # 10,005,746; application no. 14/504,681, 2018/06, Academia Sinica Docket Number: 03A-1020729

 

專書章節

Chih-Cheng Liu, Yi-Fang Tsai, Wondemagegn H. Wanna, Ravirala Ramu, Damodar Janmanchi, Sunney I. Chan, Steve S.-F. Yu* “Selective Oxidation of Alkanes by Metallo-monooxygenase and Their Nano-biomimetics,” in ”Alkane Functionalization”, edited by Armando J. L. Pombeiro and Maria de Fatima Costa Guedes da Silva, Publisher: John Wiley & Sons, West Sussex, UK (2019), chapter 15.

Sunney I. Chan and Seung Jae Lee “ The Biochemistry of Methane Monooxygenase” in “ Methanotrophs:  Microbiology Fundamental and Biotechnological Applications Microbiology Monographs (Series Ed.: Alexander Steinbüchel))”, edited by Eun Yeol Lee, Publisher: Springer Nature, Switzerland, AG, in press.