Electrosynthesis of an Improbable Directly Bonded Phosphorene-Fullerene Heterodimensional Hybrid toward Boosted Photocatalytic Hydrogen Evolution.

Autor: Zhang H; Key Laboratory of Precision and Intelligent Chemistry, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), School of Chemistry and Materials Science, University of Science and Technology of China, Hefei, 230026, China., Li Y; Key Laboratory of Precision and Intelligent Chemistry, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), School of Chemistry and Materials Science, University of Science and Technology of China, Hefei, 230026, China., Liu S; Hefei National Research Center for Physical Sciences at the Microscale, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), School of Chemistry and Materials Science, University of Science and Technology of China, Hefei, 230026, China., Xu Z; Hefei National Research Center for Physical Sciences at the Microscale, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), School of Chemistry and Materials Science, University of Science and Technology of China, Hefei, 230026, China.; Key Laboratory of Functional Molecular Solids, Ministry of Education, Anhui Laboratory of Molecule-Based Materials, School of Chemistry and Materials Science, Anhui Normal University, Wuhu, 241002, China., Liu Z; Hefei National Research Center for Physical Sciences at the Microscale, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), School of Chemistry and Materials Science, University of Science and Technology of China, Hefei, 230026, China., Gao C; Hefei National Research Center for Physical Sciences at the Microscale, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), School of Chemistry and Materials Science, University of Science and Technology of China, Hefei, 230026, China., Zhang G; Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, 230026, China., Fu Q; Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China, Hefei, 230026, China., Du P; Key Laboratory of Precision and Intelligent Chemistry, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), School of Chemistry and Materials Science, University of Science and Technology of China, Hefei, 230026, China., Jiang J; Key Laboratory of Precision and Intelligent Chemistry, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), School of Chemistry and Materials Science, University of Science and Technology of China, Hefei, 230026, China., Zhu J; National Synchrotron Radiation Laboratory, Department of Chemical Physics, University of Science and Technology of China, Hefei, 230026, China., Xiong Y; Hefei National Research Center for Physical Sciences at the Microscale, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), School of Chemistry and Materials Science, University of Science and Technology of China, Hefei, 230026, China., Wang GW; Hefei National Research Center for Physical Sciences at the Microscale, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), School of Chemistry and Materials Science, University of Science and Technology of China, Hefei, 230026, China.; Key Laboratory of Functional Molecular Solids, Ministry of Education, Anhui Laboratory of Molecule-Based Materials, School of Chemistry and Materials Science, Anhui Normal University, Wuhu, 241002, China., Yang S; Key Laboratory of Precision and Intelligent Chemistry, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM), School of Chemistry and Materials Science, University of Science and Technology of China, Hefei, 230026, China.
Jazyk: angličtina
Zdroj: Angewandte Chemie (International ed. in English) [Angew Chem Int Ed Engl] 2024 Sep 16; Vol. 63 (38), pp. e202407551. Date of Electronic Publication: 2024 Aug 14.
DOI: 10.1002/anie.202407551
Abstrakt: Phosphorene and fullerene are representative two-dimensional (2D) and zero-dimensional (0D) nanomaterials respectively, constructing their heterodimensional hybrid not only complements their physiochemical properties but also extends their applications via synergistic interactions. This is however challenging because of their diversities in dimension and chemical reactivity, and theoretical studies predicted that it is improbable to directly bond C 60 onto the surface of phosphorene due to their strong repulsion. Here, we develop a facile electrosynthesis method to synthesize the first phosphorene-fullerene hybrid featuring fullerene surface bonding via P-C bonds. Few-layer black phosphorus nanosheets (BPNSs) obtained from electrochemical exfoliation react with C 60 2- dianion prepared by electroreduction of C 60 , fulfilling formation of the "improbable" phosphorene-fullerene hybrid (BPNS-s-C 60 ). Theoretical results reveal that the energy barrier for formation of [BPNS-s-C 60 ] 2- intermediate is significantly decreased by 1.88 eV, followed by an oxidization reaction to generate neutral BPNS-s-C 60 hybrid. Surface bonding of C 60 molecules not only improves significantly the ambient stability of BPNSs, but also boosts dramatically the visible light and near-infrared (NIR) photocatalytic hydrogen evolution rates, reaching 1466 and 1039 μmol h -1  g -1 respectively, which are both the highest values among all reported BP-based metal-free photocatalysts.
(© 2024 Wiley-VCH GmbH.)
Databáze: MEDLINE
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