Wang Yu, Paciok Paul, Pielsticker Lukas, Spriewald Luciano Alexander, Glatthaar Lorena, Xu Aijie, He Zimo, Ding Min, Hetaba Walid, Gallego Jaime, Guo Yanglong, Smarsly Bernd M, Over Herbert
State Key Laboratory of Green Chemical Engineering and Industrial Catalysis, Research Institute of Industrial Catalysis, School of Chemistry and Molecular Engineering, East China University of Science and Technology Shanghai 200237 PR China
Institute of Physical Chemistry, Justus Liebig University Heinrich-Buff-Ring 17 D-35392 Giessen Germany
Chem Sci. 2025 Mar 28;16(18):7739-7750. doi: 10.1039/d5sc00778j. eCollection 2025 May 7.
The exsolution of ruthenium from a 3 at% ruthenium-substituted LaFeO (LFR3) perovskite oxide is meticulously designed to produce a high-performance ruthenium-supported catalyst with high atomic efficiency. A high-temperature redox pretreatment at 800 °C enriches the Ru concentration in the near-surface region of LFR3, while a subsequent mild reduction step with H at 500 °C leads to the Ru exsolution from the Ru-enriched near-surface region (LFR3_Redox_500R), resulting in a high density of small particles that are not passivated by LaO . The performance of this catalyst is evaluated through its application in two prototypical catalytic reactions: the combustion of propane (oxidation reaction) and the reduction of CO by hydrogenation (reduction reaction). For both reactions, the activity of the redox-pretreated sample LFR3_Redox_500R exhibits a significant increase compared to the activity of the untreated sample (LFR3_500R). In the catalytic hydrogenation of CO, the high selectivity profile undergoes a transition from CO for LFR3_500R to methane for LFR3_Redox_500R.
精心设计从3at%钌取代的LaFeO（LFR3）钙钛矿氧化物中析出钌，以制备具有高原子效率的高性能钌负载催化剂。在800°C进行高温氧化还原预处理可使LFR3近表面区域的Ru浓度富集，而随后在500°C用H2进行温和还原步骤会导致Ru从富Ru近表面区域析出（LFR3_Redox_500R），从而产生高密度的未被LaO钝化的小颗粒。通过将该催化剂应用于两个典型催化反应来评估其性能：丙烷燃烧（氧化反应）和氢气还原CO（还原反应）。对于这两个反应，与未处理样品（LFR3_500R）的活性相比，氧化还原预处理样品LFR3_Redox_500R的活性显著提高。在CO催化加氢反应中，高选择性分布从LFR3_500R的CO转变为LFR3_Redox_500R的甲烷。
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