Yan Xiaoliang, Sun Wei, Fan Liming, Duchesne Paul N, Wang Wu, Kübel Christian, Wang Di, Kumar Sai Govind Hari, Li Young Feng, Tavasoli Alexandra, Wood Thomas E, Hung Darius L H, Wan Lili, Wang Lu, Song Rui, Guo Jiuli, Gourevich Ilya, Ali Feysal M, Lu Jingjun, Li Ruifeng, Hatton Benjamin D, Ozin Geoffrey A
College of Chemistry and Chemical Engineering, Taiyuan University of Technology, Taiyuan, Shanxi, 030024, P. R. China.
Materials Chemistry and Nanochemistry Research Group, Solar Fuels Cluster, Department of Chemistry, University of Toronto, 80 St. George Street, Toronto, ON, M5S 3H6, Canada.
Nat Commun. 2019 Jun 13;10(1):2608. doi: 10.1038/s41467-019-10464-x.
Two-dimensional (2D) materials are of considerable interest for catalyzing the heterogeneous conversion of CO to synthetic fuels. In this regard, 2D siloxene nanosheets, have escaped thorough exploration, despite being composed of earth-abundant elements. Herein we demonstrate the remarkable catalytic activity, selectivity, and stability of a nickel@siloxene nanocomposite; it is found that this promising catalytic performance is highly sensitive to the location of the nickel component, being on either the interior or the exterior of adjacent siloxene nanosheets. Control over the location of nickel is achieved by employing the terminal groups of siloxene and varying the solvent used during its nucleation and growth, which ultimately determines the distinct reaction intermediates and pathways for the catalytic CO methanation. Significantly, a CO methanation rate of 100 mmol g h is achieved with over 90% selectivity when nickel resides specifically between the sheets of siloxene.
二维（2D）材料在催化CO非均相转化为合成燃料方面具有相当大的吸引力。在这方面，尽管二维硅氧烯纳米片由储量丰富的元素组成，但尚未得到充分探索。在此，我们展示了镍@硅氧烯纳米复合材料卓越的催化活性、选择性和稳定性；发现这种有前景的催化性能对镍组分在相邻硅氧烯纳米片内部或外部的位置高度敏感。通过利用硅氧烯的端基并改变其成核和生长过程中使用的溶剂来控制镍的位置，这最终决定了催化CO甲烷化的不同反应中间体和途径。值得注意的是，当镍特别位于硅氧烯片层之间时，可实现100 mmol g⁻¹ h⁻¹的CO甲烷化速率，选择性超过90%。
