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Highly Efficient Ambient Temperature CO2 Photomethanation Catalyzed by Nanostructured RuO2 on Silicon Photonic Crystal Support
Advanced Energy Materials ( IF 24.4 ) Pub Date : 2018-01-11 , DOI: 10.1002/aenm.201702277
Abdinoor A. Jelle 1 , Kulbir K. Ghuman 1 , Paul G. O'Brien 2 , Mohamad Hmadeh 3 , Amit Sandhel 4 , Doug D. Perovic 1 , Chandra Veer Singh 1 , Charles A. Mims 5 , Geoffrey A. Ozin 4
Affiliation  

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 gcat−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 H2 revealed that H2 splits on the surface of the RuO2 to form hydroxyl groups that participate in the overall photomethanation process.

中文翻译:

硅光子晶体载体上纳米结构RuO2催化高效室温CO2光甲烷化

阳光驱动的CO 2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CO 2排放。在这项工作中,CO 2在3D硅光子晶体载体上的高度分散的纳米结构RuO 2催化剂上的光甲烷化作用,在高强度太阳模拟辐射下,在环境温度下实现了令人印象深刻的转化率,高达4.4 mmol g cat -1 h -1,被报道。该性能比通过纳米结构化的RuO 2制成的对照样品的光甲烷化速率高一个数量级。在硅片上。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RuO 2光催化剂甲烷化率高的原因。关于CO 2与H 2的反应的密度泛函理论研究表明,H 2在RuO 2的表面分裂,形成参与整个光甲烷化过程的羟基。
更新日期:2018-01-11
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