Stabilizing Cationic Palladium Single-Atom Sites on Heteroatom-Doped Carbon for Selective Hydrogen Peroxide Electrosynthesis

Fortunato GV, Gunnarson A, Hosseini H, You X, Bhuyan P, Choi JS, Jeon HS, Zhao X, Lourenço JC, Lim S, Wang H, Buzanich AG, Radtke M, Paciok P, Lanza MR, Schüth F, Ledendecker M (2025)

Publication Type: Journal article

Publication year: 2025

Journal

Advanced Functional Materials Wiley-VCH Verlag

DOI: 10.1002/adfm.202516600

Abstract

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.

Involved external institutions

Technische Universität München (TUM) DE Germany (DE) Max-Planck-Institut für Kohlenforschung (MPI KoFo) / Max Planck Institute for Coal Research DE Germany (DE) Korea Institute of Science and Technology (KIST) / 한국과학기술연구원 KR Korea, Republic of (KR) Bundesanstalt für Materialforschung und -prüfung (BAM) DE Germany (DE) Forschungszentrum Jülich / Research Centre Jülich (FZJ) DE Germany (DE) University of São Paulo / Universidade de São Paulo (USP) BR Brazil (BR)

How to cite

APA:

Fortunato, G.V., Gunnarson, A., Hosseini, H., You, X., Bhuyan, P., Choi, J.S.,... Ledendecker, M. (2025). Stabilizing Cationic Palladium Single-Atom Sites on Heteroatom-Doped Carbon for Selective Hydrogen Peroxide Electrosynthesis. Advanced Functional Materials. https://doi.org/10.1002/adfm.202516600

MLA:

Fortunato, Guilherme V., et al. "Stabilizing Cationic Palladium Single-Atom Sites on Heteroatom-Doped Carbon for Selective Hydrogen Peroxide Electrosynthesis." Advanced Functional Materials (2025).

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