文献类型：期刊文献

英文题名：Pd-N-C shelled Pd nanoparticle catalysts for high-performance hydrogen peroxide electrosynthesis

作者：Dong, Jiao[1,2];Su, Zixiang[3,4];Jia, Yanyan[5];Xing, Runjia[1,2];She, Sixuan[6];Guan, Daqin[7];Dai, Sheng[5];Wang, Jinling[1,2];Chai, Manqing[1,2];Hou, Zhenshan[1,2];Wang, Zhi-Qiang[1,2];Wei, Hehe[1,2];Hu, P.[1,2,8];Gong, Xue-Qing[3]

机构：[1]East China Univ Sci & Technol, Ctr Computat Chem, Sch Chem & Mol Engn, State Key Lab Green Chem Engn & Ind Catalysis, 130 Meilong Rd, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Res Inst Ind Catalysis, Sch Chem & Mol Engn, 130 Meilong Rd, Shanghai 200237, Peoples R China;[3]Shanghai Jiao Tong Univ, Sch Chem & Chem Engn, State Key Lab Synergist Chem Bio Synth, 800 Dongchuan Rd, Shanghai 200240, Peoples R China;[4]First Rare Mat Co Ltd, Natl Engn & Technol Res Ctr Scattered Met, Baijia Ind Pk 27-9B, Qingyuan 511517, Guangdong, Peoples R China;[5]East China Univ Sci & Technol, Key Lab Adv Mat & Feringa Nobel Prize Scientist Jo, Sch Chem & Mol Engn, 130 Meilong Rd, Shanghai 200237, Peoples R China;[6]Hong Kong Polytech Univ, Dept Appl Phys, Kowloon, Hong Kong, Peoples R China;[7]Curtin Univ, WA Sch Mines Minerals Energy & Chem Engn WASM MECE, Perth, WA 6102, Australia;[8]Shanghai Tech Univ, Sch Phys Sci & Technol, 393 Middle Huaxia Rd, Shanghai 201210, Peoples R China

年份：2026

外文期刊名：CHEMICAL SCIENCE

收录：;EI(收录号：20261620503571);WOS:【SCI-EXPANDED(收录号:WOS:001738423600001)】；

基金：This work was supported by the National Key R&D Program of China (2024YFA1509901, 2023YFA1508500, and 2021YFA1500700) and the National Nature Science Foundation of China (22572049 and 22203030).

语种：英文

外文关键词：Catalyst selectivity - Electrocatalysis - Electrolytic reduction - Hydrogen production - Nanocatalysts - Nanoparticles - Nitrogen - Nitrogen compounds - Orbital calculations - Palladium - Palladium compounds - Synthesis (chemical)

摘要：Metal-nitrogen-carbon (M-N-C) catalysts have attracted widespread attention due to their potential in promoting the electrochemical oxygen reduction reaction (ORR) for the selective production of hydrogen peroxide (H2O2). However, the effects of their diverse structures and complex compositions on the catalytic performance remain poorly understood. Herein, systematic theoretical calculations reveal that the Pd-N-C based single-atom catalyst featuring a 1 : 1 ratio of pyridinic and pyrrolic nitrogen adopts a centrosymmetric PdN4 structure (PdSAN2-2C), and the Pd dz2 orbital can strongly interact with the O 2p orbital of the adsorbed OOH intermediate, thereby strengthening its adsorption and facilitating subsequent conversion to H2O2. Guided by the theoretical insights, the PdSAN2-2C catalyst and a novel Pd@PdSAN2-2C core-shell catalyst with Pd nanoparticles encapsulated by an ultrathin PdSAN2-2C shell are synthesized, and the latter exhibits a remarkable H2O2 selectivity of 97% and a high yield of 35.88 mol gcat-1 h-1 at an industrially relevant current density of 200 mA cm-2, along with superior operational stability. This combined theoretical and experimental study provides useful guidance for the rational design of high-efficiency M-N-C catalysts for selective electrocatalysis.