文献类型：期刊文献

英文题名：Defect-engineered nonstoichiometric perovskite hosting high-activity PdO sites for enhanced hydrocarbon oxidation

作者：Yu, Jihang[1];Wang, Zhi-Qiang[1];Jiang, Yongjun[2,3];Yan, Jiaorong[1];Guo, Yanglong[1];Guo, Yun[1];Wang, Li[1];Wang, Aiyong[1];Dai, Sheng[2,3];Gao, Feng[4];Zhan, Wangcheng[1,3]

机构：[1]East China Univ Sci & Technol, Sch Chem & Mol Engn, State Key Lab Green Chem Engn & Ind Catalysis, 130 Meilong Rd, Shanghai, Peoples R China;[2]East China Univ Sci & Technol, Inst Fine Chem, Key Lab Adv Mat & Feringa Nobel Prize Scientist Jo, Sch Chem & Mol Engn, Shanghai, Peoples R China;[3]East China Univ Sci & Technol, Frontiers Sci Ctr Materiobiol & Dynam Chem, Shanghai, Peoples R China;[4]Tianjin Univ, State Key Lab Engines, Tianjin, Peoples R China

年份：2026

卷号：17

期号：1

外文期刊名：NATURE COMMUNICATIONS

收录：;WOS:【SCI-EXPANDED(收录号:WOS:001777091000004)】；

基金：W.Z. acknowledges financial support from the National Natural Science Foundation of China (22076047). J.Y. thanks the support by Science and Technology Commission of Shanghai Municipality (25ZR1401090). S.D. thanks the support by the National Natural Science Foundation of China (22376062), Science and Technology Commission of Shanghai Municipality (22ZR1415700) and Shanghai Rising-star Program (20QA1402400). Y.G. thanks the support by the Fundamental Research Funds for the Central Universities. Z.W thanks the support by the National Key Research and Development Program (2023YFA1508500, 2024YFA1509901, 2021YFA1500700), the National Natural Science Foundation of China (22572049, 22203030).

语种：英文

摘要：Supported noble metal catalysts are central to industrial, environmental, and energy applications, yet precisely constructing active sites with optimized geometry remains a formidable challenge beyond conventional particle size control. Here, we introduce a perovskite-based surface defect engineering strategy that enables atomic-level regulation of noble metal active sites. By tailoring La stoichiometry in LaAlO3, we engineer three distinct surface morphologies (planar, stepped, and crater-like) that serve as templates for anchoring and replicating supported PdO nanoparticles. Among these, the step-rich PdO configuration on La0.9AlO3-delta exhibits the highest methane oxidation activity, with a linear correlation between Pd step-site density and catalytic performance. The enhancement arises from low-coordination Pd atoms at step sites, which form stable Pd-C(CH3) covalent bonds and facilitate C-H bond activation, the rate-determining step in methane oxidation. This work establishes a generalizable approach to precisely tailor noble metal active sites through perovskite surface engineering, providing a robust framework for the rational design of efficient and durable oxidation catalysts.