The utilization of solar energy in driving methane dry reforming (MDR) reaction through photo-thermal synergetic catalysis could simultaneously realize the reduction of carbon footprint and the fixation of solar energy, which is an environmentally and economically beneficial route. However, the currently developed catalysts still require further optimization in catalytic performance and stability. Here, we prepared RuNC, a Ru nanoclusters catalyst anchored on CeO2 with strong metal-support interaction (SMSI) effect via a facile preparation method. The formation rates of H2 and CO over RuNC catalyst were 1.41 and 2.16 mol·gcat−1·h−1 respectively under photo-thermal catalysis (PTC) at 500 °C, which is up to one order of magnitude higher than existing PTC-MDR catalysts. Moreover, the prepared catalyst did not show significant deactivation under 100 hour test. The in-depth structure-function relationship between catalytic activity/stability and Ru nanocluster sites/induced SMSI effect were determined by systematic structural characterization. The advantages of RuNC catalyst structure under PTC catalytic conditions were demonstrated by optical characterization. Besides, the excitation-migration path of photo-electron under PTC conditions was determined by ISI-XPS experiments. Finally, the mechanism of PTC-MDR reaction and the specific reaction steps enhanced by light irradiation were determined by operando experiments. This work provided theoretical basis and excellent catalyst for the industrial application of PTC-MDR route.

中文翻译：

---

强金属-载体相互作用诱导了 Ru-cluster-ceria 催化剂上光热催化甲烷干重整的优异性能


利用太阳能通过光热协同催化驱动甲烷干重整 （MDR） 反应，可以同时实现碳足迹的减少和太阳能的固定，这是一种环境和经济有益的途径。然而，目前开发的催化剂在催化性能和稳定性方面仍需进一步优化。在这里，我们通过简单的制备方法制备了 RuNC，这是一种锚定在 CeO2 上的 Ru 纳米团簇催化剂，具有很强的金属-支持相互作用 （SMSI） 效应。在 500 °C 的光热催化 （PTC） 下，RuNC 催化剂上 H2 和 CO 的生成速率分别为 1.41 和 2.16 mol·gcat−1·h−1，比现有的 PTC-MDR 催化剂高出一个数量级。此外，制备的催化剂在 100 小时测试下未显示出明显的失活。通过系统结构表征确定了催化活性/稳定性与 Ru 纳米团簇位点/诱导的 SMSI 效应之间的深入结构-功能关系。通过光学表征证明了 RuNC 催化剂结构在 PTC 催化条件下的优势。此外，通过 ISI-XPS 实验确定了 PTC 条件下光电子的激发-迁移路径。最后，通过原位实验确定了 PTC-MDR 反应的机理和光照射增强的具体反应步骤。这项工作为 PTC-MDR 路线的工业应用提供了理论基础和优良的催化剂。