Insight into methane conversion Dr. Cao yang Supervised by Pro. Mo 2016.09.23

Contents Methane conversion route Catalysts for methane conversion Technique for study the catalysts Product detection Summary for methane conversion Perspective

Methane Conversion Route

Methane Conversion Route

Catalysts for Methane Conversion Fe@SiO2 catalytic system FeC2Si3Ox catalytic site Xiaoguang Guo et. al., Science, 2014, 344, 616-619.

Catalysts for Methane Conversion Li-MgO catalytic system Robert Schlçgl et. al., Angew. Chem. Int. Ed., 2014, 53, 1 – 6.

Catalysts for Methane Conversion CuOx/FeOxMolecular sieve system Edward I. Solomon et. al., PNAS, 2009, 106, 18908-18913. Edward I. Solomon et. al., Nature, 2016, 536, 317-321.

Catalysts for Methane Conversion MO+· catalytic site (Dr. Helmut Schwarz) Nicolas Dietl, Angew. Chem. Int. Ed., 2012, 51, 5544 – 5555. Jilai Li et. al., Angew. Chem. Int. Ed. 2015, 54, 12298 –12302.

Catalysts for Methane Conversion Tl3+-TFA system Roy A. Periana et. al., Science, 2014, 343, 1232-1236.

Catalysts for Methane Conversion Periana system Roy A. Periana et. al., Science, 1998, 280, 560-564. Roy A. Periana et. al., J. Am. Chem. Soc., 2013, 135, 14644−14658.

Catalysts for Methane Conversion Ag catalysis in sc CO2 Pedro J. Pérez et. al.,Science, 2011, 332, 835−838.

Catalysts for Methane Conversion Ag catalysis in sc CO2 Pedro J. Pérez et. al.,Science, 2011, 332, 835−838.

Catalysts for Methane Conversion Sanford system Melanie S. Sanford et. al., Science, 2016, 351, 1421-1424.

Characterization Techniques In-situ FT-IR 原位红外技术 In-situ ESR 原位顺磁技术 In-situ NMR 原位核磁技术 In-situ UV-Vis 原位紫外-可见光谱技术 Raul F. Lubo et. al., Chem. Soc. Rev., 2010, 39, 4783-4793. Francisco Zaera, Chem. Soc. Rev., 2014, 43, 7624-7663. Teresa Blasco, Chem. Soc. Rev., 2010, 39, 4685-4702. Edward I. Solomon et. al., Nature, 2016, 536, 317-321.

Characterization Techniques 各种原位测试表征技术通过对产品在仪器上进行测试，发现其催化反应前后和催化反应过程中样品中元素的价态、催化活性位点的变化，进而对催化机理进行理解。 这些测试方法是理解反应过程的必要手段。在研究过程中需要对这些手段灵活运用。 EXAFS X-射线光电子能谱技术 In-situ FT-IR 原位红外技术 In-situ ESR 原位顺磁技术 In-situ NMR 原位核磁技术 In-situ UV-Vis 原位紫外-可见光谱技术

Characterization Techniques VUV-SPI-MBMS system 单光子电离质谱技术 (ultraviolet soft photoionization molecular-beam mass spectrometry) Xiaoguang Guo et. al., Science, 2014, 344, 616-619.

Characterization Techniques Xiaoguang Guo et. al., Science, 2014, 344, 616-619.

Characterization Techniques Xiaoguang Guo et. al., Science, 2014, 344, 616-619.

Product Detection 产 物 组 成 分 析 质 谱 分 析 核 磁 分 析 气 相 色 谱 分 析

Summary Methane is the most stable reactant (even more stable than solvent) The product may be more reactive than methane The methane reaction can be studied in solution phase with strong oxidants.

Plan to do Design in-situ experiment to study the methane reaction. Design suitable catalytic system to activate methane.