Yao Yuan, Li Ben, Gao Xiaowen, Yang Yuying, Yu Jianbo, Lei Jianan, Li Qi, Meng Xiangchao, Chen Langxing, Xu Dongsheng
Beijng National Laboratory for Molecular Sciences, State Key Laboratory for Structural Chemistry of Unstable Species, College of Chemistry and Molecular Engineering, Peking University, Beijing, 100871, China.
College of Chemistry and Chemical Engineering, Ocean University of China, Qingdao, Shandong, 266100, China.
Adv Mater. 2023 Sep;35(39):e2303654. doi: 10.1002/adma.202303654. Epub 2023 Jul 27.
As an energy-saving and green method, solar-driven dry reforming of methane (DRM) is expected to introduce new activation processes and prevent sintering and coking of the catalysts. However, it still lacks an efficient way to coordinate the regulation of activation of reactants and lattice oxygen migration. In this study, Rh/LaNiO is designed as a highly efficient photothermal catalyst for solar-driven DRM, which performs production rates of 452.3 mmol h g for H and 527.6 mmol h g for CO under a light intensity of 1.5 W cm , with an excellent stability. Moreover, a remarkable light-to-chemical energy efficiency (LTCEE) of 10.72% is achieved under a light intensity of 3.5 W cm . The characterizations of surface electronic and chemical properties and theoretical analysis demonstrate that strong adsorption for CH and CO , light-induced metal-to-metal charge transfer (MMCT) process and high oxygen mobility together bring Rh/LaNiO excellent performance for solar-driven DRM.
作为一种节能且绿色的方法，太阳能驱动的甲烷干重整（DRM）有望引入新的活化过程，并防止催化剂烧结和结焦。然而，它仍然缺乏一种有效的方式来协调反应物活化和晶格氧迁移的调控。在本研究中，Rh/LaNiO被设计为用于太阳能驱动DRM的高效光热催化剂，在1.5 W/cm²的光强下，其H₂的产率为452.3 mmol h⁻¹ g⁻¹，CO的产率为527.6 mmol h⁻¹ g⁻¹，具有出色的稳定性。此外，在3.5 W/cm²的光强下，实现了10.72%的显著光化学能效率（LTCEE）。表面电子和化学性质的表征以及理论分析表明，对CH₄和CO₂的强吸附、光致金属-金属电荷转移（MMCT）过程和高氧迁移率共同赋予了Rh/LaNiO在太阳能驱动DRM方面的优异性能。
