Fortunato, Guilherme V. Gunnarson, Alexander Hosseini, Hannaneh You, Xiangyu Bhuyan, Pallabi Choi, Ji Sik Jeon, Hyo Sang Zhao, Xingshen Lourenco, Julio C. Lim, Sumin Wang, Huize Buzanich, Ana Guilherme Radtke, Martin Paciok, Paul Lanza, Marcos R. V. Schuth, Ferdi Ledendecker, Marc 2025-09-30T07:03:18Z 2025-09-30T07:03:18Z 2025-09-30 2026-03 1616-301X https://pubs.kist.re.kr/handle/201004/153289 Single-atom catalysts (SACs) offer significant potential for the sustainable electrosynthesis of hydrogen peroxide (H2O2) via the two-electron oxygen reduction reaction (2e- ORR). However, their practical deployment is hindered by challenges related to limited operational stability and intricate synthetic procedures. Here, a family of cationic Pd single-atom complexes anchored on nitrogen-, sulfur-, and dual N,S-doped hollow carbon spheres (HCS) is reported, prepared via mild vapor-phase doping combined with wet impregnation of Pd(acac)2. Systematic tuning of the heteroatom environment enables precise control over the Pd electronic state and local coordination, enhancing selectivity and long-term stability under acidic, peroxide-rich conditions. Operando ICP-MS and advanced spectroscopy reveal that sulfur-doping induces favorable charge redistribution, reinforcing Pd-support interactions and suppressing demetallation, while nitrogen doping enhances ORR activity. Notably, dual N,S-co-doping achieves a synergistic balance between catalytic performance and stability. This strategy offers a rational design framework for robust ligand-containing SACs, advancing sustainable electrocatalytic technologies well beyond H2O2 synthesis. English John Wiley & Sons Ltd. Stabilizing Cationic Palladium Single-Atom Sites on Heteroatom-Doped Carbon for Selective Hydrogen Peroxide Electrosynthesis Article 10.1002/adfm.202516600 1 Advanced Functional Materials, v.36, no.21 Advanced Functional Materials 36 21 Y scie scopus 2-s2.0-105016632847 Chemistry, Multidisciplinary Chemistry, Physical Nanoscience & Nanotechnology Materials Science, Multidisciplinary Physics, Applied Physics, Condensed Matter Chemistry Science & Technology - Other Topics Materials Science Physics Article; Early Access OXYGEN REDUCTION NITROGEN CATALYSTS ELECTROCATALYSTS MECHANISMS COMPLEXES OXIDATION CATHODE hetero-atom doping hydrogen peroxide electrosynthesis oxygen reduction reaction single-atom catalysts catalyst stability demetallation