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Highly Efficient Ambient Temperature CO_2 Photomethanation Catalyzed by Nanostructured RuO_2 on Silicon Photonic Crystal Support

机译:硅光子晶体载体上纳米结构RuO_2催化高效室温CO_2光甲烷化

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摘要

Sunlight-driven catalytic hydrogenation of CO2 is an important reaction that generates useful chemicals and fuels and if operated at industrial scales can decrease greenhouse gas CO2 emissions into the atmosphere. In this work, the photomethanation of CO2 over highly dispersed nanostructured RuO2 catalysts on 3D silicon photonic crystal supports, achieving impressive conversion rates as high as 4.4 mmol g(cat)(-1) h(-1) at ambient temperatures under high-intensity solar simulated irradiation, is reported. This performance is an order of magnitude greater than photomethanation rates achieved over control samples made of nanostructured RuO2 on silicon wafers. The high absorption and unique light-harvesting properties of the silicon photonic crystal across the entire solar spectral wavelength range coupled with its large surface area are proposed to be responsible for the high methanation rates of the RuO2 photocatalyst. A density functional theory study on the reaction of CO2 with H-2 revealed that H-2 splits on the surface of the RuO2 to form hydroxyl groups that participate in the overall photomethanation process.
机译:阳光驱动的CO2催化加氢反应是重要的反应,可产生有用的化学物质和燃料,如果以工业规模运行,可以减少温室气体向大气中的排放。在这项工作中,CO2在3D硅光子晶体载体上的高度分散的纳米结构RuO2催化剂上的光甲烷化作用,在环境温度和高强度下实现了令人印象深刻的高达4.4 mmol g(cat)(-1)h(-1)的转化率。有太阳模拟辐射的报道。该性能比在硅晶片上由纳米结构的RuO2制成的控制样品所获得的光甲烷化速率高一个数量级。硅光子晶体在整个太阳光谱波长范围内的高吸收和独特的集光性能以及较大的表面积被认为是RuO2光催化剂甲烷化率高的原因。对CO2与H-2反应的密度泛函理论研究表明,H-2在RuO2表面分裂,形成羟基,参与整个光甲烷化过程。

著录项

  • 来源
    《Advanced energy materials》 |2018年第9期|1702277.1-1702277.10|共10页
  • 作者单位

    Univ Toronto, Dept Mat Sci & Engn, 184 Coll St, Toronto, ON M5S 3E4, Canada;

    Univ Toronto, Dept Mat Sci & Engn, 184 Coll St, Toronto, ON M5S 3E4, Canada;

    York Univ, Lassonde Sch Engn, Dept Mech Engn, Toronto, ON M3J 1P3, Canada;

    Amer Univ Beirut, Fac Arts & Sci, Dept Chem, POB 11-0236, Beirut, Lebanon;

    Univ Toronto, Dept Chem, Mat Chem & Nanochem Res Grp, Solar Fuels Cluster, 80 St George St, Toronto, ON M5S 3H6, Canada;

    Univ Toronto, Dept Mat Sci & Engn, 184 Coll St, Toronto, ON M5S 3E4, Canada;

    Univ Toronto, Dept Mat Sci & Engn, 184 Coll St, Toronto, ON M5S 3E4, Canada;

    Univ Toronto, Dept Chem Engn & Appl Chem, 200 Coll St, Toronto, ON M5S 3E5, Canada;

    Univ Toronto, Dept Chem, Mat Chem & Nanochem Res Grp, Solar Fuels Cluster, 80 St George St, Toronto, ON M5S 3H6, Canada;

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  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

    photochemical; photomethanation; photonic crystals; photothermal; solar fuels;

    机译:光化学;光甲烷化;光子晶体;光热;太阳能;

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