Solar-driven CO₂ hydrogenation can provide a renewable source of fuels and reduce greenhouse gas emissions if operated at industrial scales. Herein we investigate the photomethanation (light-driven Sabatier reaction) rates over Ru films sputtered onto silica opal (Ru/SiO₂) and inverted silicon opal photonic crystal (Ru/i-Si-o) supports at ambient temperature under solar-simulated radiation as a function of incident light intensity. Photomethanation rates over both the Ru/SiO₂ and Ru/i-Si-o catalysts increase significantly with increasing light intensity, and rates as large as 2.8 mmol g⁻¹ h⁻¹ are achieved over the Ru/i-Si-o catalyst. Furthermore, the quantum efficiency of the photomethanation reaction is almost three times larger when measured over the Ru/i-Si-o catalyst as compared to the Ru/SiO₂ catalyst. The large photomethanation rates over the Ru/i-Si-o catalyst are attributed to its exceptional light-harvesting properties. Moreover, we perform DFT analysis to investigate the potential role of photo-induced charges on the Ru surface. The results from the simulation indicate that charged Ru surfaces can destabilize adsorbed CO₂ molecules and adsorb and dissociate H₂ such that it can readily react with CO₂, thereby accelerating the Sabatier reaction.

中文翻译：

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在环境温度下在硅光子晶体负载的钌上 增强了气态CO _2的光热还原†

如果以工业规模运行，太阳能驱动的CO ₂加氢可以提供可再生燃料，并减少温室气体排放。在本文中，我们研究了在环境温度下在太阳模拟辐射下溅射到硅石蛋白石（Ru / SiO ₂）和倒硅蛋白石光子晶体（Ru / i-Si-o）上的Ru膜上的光甲烷化（光驱动Sabatier反应）速率。作为入射光强度的函数。随着光强度的增加，Ru / SiO ₂和Ru / i-Si-o催化剂上的光甲烷化速率均显着增加，且速率高达2.8 mmol g ^-1 h ^-1通过Ru / i-Si-o催化剂可实现。此外，当在Ru / i-Si-o催化剂上测量时，与Ru / SiO ₂催化剂相比，光甲烷化反应的量子效率几乎大三倍。Ru / i-Si-o催化剂上较大的光甲烷化速率归因于其出色的光收集性能。此外，我们进行DFT分析以研究Ru表面上光诱导电荷的潜在作用。模拟的结果表明，带电的Ru表面可以使所吸附的CO ₂分子不稳定，并吸附和离解H ₂，从而使其易于与CO ₂反应，从而加速了Sabatier反应。