Ryu Seung-Hee, Kim Seungeun, Lee Hyunjoo, Choi Joon-Hwan, Jeong Hojin
Nano Materials Research Division, Korea Institute of Materials Science (KIMS), Changwon, Gyeongnam, Republic of Korea.
Department of Materials Science and Engineering, Pukyong National University, Busan, Republic of Korea.
Nat Commun. 2024 Sep 27;15(1):8348. doi: 10.1038/s41467-024-52698-4.
Optimizing metal catalyst structures to achieve desired states is vital for efficient surface reactions, yet remains challenging due to the lack of well-defined precursor materials and weak metal-support interaction. Palladium-based catalysts, when not properly tailored for complete methane oxidation exhibit insufficient performance. Herein, we fabricate Pd oxide nano-clusters supported on SSZ-13 using atomic ions with strong metal-support interaction (SMSI). Steam treatment of Pd/SSZ-13 transforms Pd particles into ions and induces SMSI. Subsequently, CO reduction and O oxidation yield mildly sintered Pd oxide nano-clusters firmly anchored on extra-framework Al sites of SSZ-13, facilitating superior activity. The robustness from SMSI prevents irreversible deactivation, and water-resistance by complete dehydration suppresses reversible degradation in wet conditions. This catalyst exhibits high performance in bench-scale reactions using monolith catalysts, ensuring applicability for industrial methane abatement. The results demonstrate that sequential treatment to Pd/SSZ-13 offers a promising approach for tailoring metal structures to enable high-performance methane oxidation.
优化金属催化剂结构以实现所需状态对于高效的表面反应至关重要,但由于缺乏明确的前驱体材料和较弱的金属-载体相互作用,这仍然具有挑战性。钯基催化剂在未针对完全甲烷氧化进行适当定制时表现出不足的性能。在此,我们使用具有强金属-载体相互作用(SMSI)的原子离子制备了负载在SSZ-13上的氧化钯纳米团簇。对Pd/SSZ-13进行蒸汽处理可将Pd颗粒转化为离子并诱导SMSI。随后,CO还原和O氧化产生了牢固锚定在SSZ-13骨架外Al位点上的轻度烧结的氧化钯纳米团簇,促进了优异的活性。SMSI带来的稳定性可防止不可逆失活,完全脱水产生的耐水性可抑制潮湿条件下的可逆降解。这种催化剂在使用整体催化剂的实验室规模反应中表现出高性能,确保了其在工业甲烷减排中的适用性。结果表明,对Pd/SSZ-13进行顺序处理为定制金属结构以实现高性能甲烷氧化提供了一种有前景的方法。