Photoelectrocatalysis on sulfur-doped carbon nitride hybrid materials Pablo Jiménez Calvo 1 , Maria Jerigova 1 , Yevheniia Markushyna 1 , Ivo F. Texeira 1,2 , Bolortuya Badamdorj 1 , Mark Isaacs 3,4 , Daniel Cruz 5 , Iver Lauerman 6 , Miguel Ángel Muñoz-Márquez 7 , Nadezda V. Tarakina 1 , Nieves Lopez Salas 1 , Aleksandr Savateev 1 1 Department of Materials Science,University of Erlangen-Nuremberg, Germany, 2 Department of Chemistry, Federal University of São Carlos, Brazil, 3 HarwellXPS, Research Complex at Harwell, UK, 4 Department of Chemistry, University College London, UK, 5 Department of Inorganic Chemistry, Fritz-Haber-Institut der Max-Planck-Gesellschaft, Germany, 6 Helmholtz-Zentrum Berlin für Materialien und Energie, Department, Germany, 7 Chemistry Division, School of Science and Technology, University of Camerino, Italy High-performing materials will dictate the pace of reinventing industrial chemical processes to achieve carbon neutrality [1] . Visible-light photoelectrocatalysts from abundant resources will play a key role in exploiting solar irradiation [2] . Anionic doping via pre-organization of precursors and further co-polymerization creates tuneable, extrinsic semiconductors. Triazole derivative-purpald, an unexplored precursor with sulfur (S) container, combined in different initial ratios with melamine during one solid-state polycondensation with two thermal steps yields hybrid S-doped carbon nitrides (C 3 N 4 ). The series of S-doped/C 3 N 4 -based materials showed enhanced optical, electronic, structural, textural, and morphological properties and exhibited higher performance in organic benzylamine photooxidation, oxygen evolution, and similar energy storage (capacitor brief investigation) [3] . 50M-50P exhibited the highest photooxidation conversion yield (84±3%) of benzylamine to imine at 535 nm – green light for 48h, due to a discrete shoulder reaching ~700 nm, an unusual high sulfur content, preservation of crystal size, new intraband energy states, deep structural defects by layer distortion, low porosity, and 10-16 nm pores. An in-depth analysis of S doping was investigated coupling x-ray photoelectron spectroscopy, transmission electron microscope, and elemental analysis, providing insights on bonds, distribution, and surface/bulk content. This work contributes to the development of disordered photocatalysts with long-visible-light for solar energy conversion and storage. References 1. Mark Isaacs, Julio Garcia-Navarro, Wee-Jun Ong, Pablo Jiménez-Calvo, Global Challenges, 2022 , 7, 2200165 2. Pablo Jiménez-Calvo, Valérie Caps, Valérie Keller, Renewable and Sustainable Energy Reviews , 2021 , 149, 111095 3. Maria Jerigova, Yevheniia Markushyna, Ivo F. Texeira, Bolortuya Badamdorj, Mark Isaacs, Daniel Cruz, Iver Lauerman, Miguel Ángel Muñoz-Márquez, Nadezda V. Tarakina, Nieves Lopez Salas, Aleksandr Savateev, Pablo Jimenéz-Calvo, ChemRxiv Cambridge Open Engage, 2022
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