Kang Leilei, Liu Xiao Yan, Wang Aiqin, Li Lin, Ren Yujing, Li Xiaoyu, Pan Xiaoli, Li Yuanyuan, Zong Xu, Liu Hua, Frenkel Anatoly I, Zhang Tao
CAS Key Laboratory of Science and Technology on Applied Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023, China.
University of Chinese Academy of Sciences, Beijing, 100049, China.
Angew Chem Int Ed Engl. 2020 Jul 27;59(31):12909-12916. doi: 10.1002/anie.202001701. Epub 2020 May 29.
Photo-thermo catalysis, which integrates photocatalysis on semiconductors with thermocatalysis on supported nonplasmonic metals, has emerged as an attractive approach to improve catalytic performance. However, an understanding of the mechanisms in operation is missing from both the thermo- and photocatalytic perspectives. Deep insights into photo-thermo catalysis are achieved via the catalytic oxidation of propane (C H ) over a Pt/TiO -WO catalyst that severely suffers from oxygen poisoning at high O /C H ratios. After introducing UV/Vis light, the reaction temperature required to achieve 70 % conversion of C H lowers to a record-breaking 90 °C from 324 °C and the apparent activation energy drops from 130 kJ mol to 11 kJ mol . Furthermore, the reaction order of O is -1.4 in dark but reverses to 0.1 under light, thereby suppressing oxygen poisoning of the Pt catalyst. An underlying mechanism is proposed based on direct evidence of the in-situ-captured reaction intermediates.
光热催化将半导体上的光催化与负载型非等离子体金属上的热催化相结合,已成为提高催化性能的一种有吸引力的方法。然而,从热催化和光催化的角度来看,对其运行机制仍缺乏了解。通过在Pt/TiO₂-WO₃催化剂上对丙烷(C₃H₈)进行催化氧化,深入了解了光热催化,该催化剂在高O₂/C₃H₈比下严重受氧中毒影响。引入紫外/可见光后,实现C₃H₈ 70%转化率所需的反应温度从324℃降至破纪录的90℃,表观活化能从130 kJ·mol⁻¹降至11 kJ·mol⁻¹。此外,O₂的反应级数在黑暗中为-1.4,但在光照下变为0.1,从而抑制了Pt催化剂的氧中毒。基于原位捕获反应中间体的直接证据,提出了一种潜在机制。