He Zhang, Dr. Yanbo Li, Shengkun Liu, Zhiwei Xu, Zehua Liu, Dr. Chao Gao, Dr. Guozhen Zhang, Dr. Qiang Fu, Prof. Pingwu Du, Prof. Jun Jiang, Prof. Junfa Zhu, Prof. Yujie Xiong, Prof. Guan-Wu Wang, Prof. Shangfeng Yang
{"title":"电合成一种不可能直接键合的磷烯-富勒烯异维混合体,以促进光催化氢气转化。","authors":"He Zhang, Dr. Yanbo Li, Shengkun Liu, Zhiwei Xu, Zehua Liu, Dr. Chao Gao, Dr. Guozhen Zhang, Dr. Qiang Fu, Prof. Pingwu Du, Prof. Jun Jiang, Prof. Junfa Zhu, Prof. Yujie Xiong, Prof. Guan-Wu Wang, Prof. Shangfeng Yang","doi":"10.1002/anie.202407551","DOIUrl":null,"url":null,"abstract":"<p>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<sub>60</sub> 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<sub>60</sub><sup>2−</sup> dianion prepared by electroreduction of C<sub>60</sub>, fulfilling formation of the <i>“improbable</i>” phosphorene-fullerene hybrid (BPNS-s-C<sub>60</sub>). Theoretical results reveal that the energy barrier for formation of [BPNS-s-C<sub>60</sub>]<sup>2−</sup> intermediate is significantly decreased by 1.88 eV, followed by an oxidization reaction to generate neutral BPNS-s-C<sub>60</sub> hybrid. Surface bonding of C<sub>60</sub> 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<sup>−1</sup> g<sup>−1</sup> respectively, which are both the highest values among all reported BP-based metal-free photocatalysts.</p>","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":null,"pages":null},"PeriodicalIF":16.1000,"publicationDate":"2024-06-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Electrosynthesis of an Improbable Directly Bonded Phosphorene-Fullerene Heterodimensional Hybrid toward Boosted Photocatalytic Hydrogen Evolution\",\"authors\":\"He Zhang, Dr. Yanbo Li, Shengkun Liu, Zhiwei Xu, Zehua Liu, Dr. Chao Gao, Dr. Guozhen Zhang, Dr. Qiang Fu, Prof. Pingwu Du, Prof. Jun Jiang, Prof. Junfa Zhu, Prof. Yujie Xiong, Prof. Guan-Wu Wang, Prof. Shangfeng Yang\",\"doi\":\"10.1002/anie.202407551\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p>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<sub>60</sub> 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<sub>60</sub><sup>2−</sup> dianion prepared by electroreduction of C<sub>60</sub>, fulfilling formation of the <i>“improbable</i>” phosphorene-fullerene hybrid (BPNS-s-C<sub>60</sub>). Theoretical results reveal that the energy barrier for formation of [BPNS-s-C<sub>60</sub>]<sup>2−</sup> intermediate is significantly decreased by 1.88 eV, followed by an oxidization reaction to generate neutral BPNS-s-C<sub>60</sub> hybrid. 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Electrosynthesis of an Improbable Directly Bonded Phosphorene-Fullerene Heterodimensional Hybrid toward Boosted Photocatalytic Hydrogen Evolution
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 C60 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 C602− dianion prepared by electroreduction of C60, fulfilling formation of the “improbable” phosphorene-fullerene hybrid (BPNS-s-C60). Theoretical results reveal that the energy barrier for formation of [BPNS-s-C60]2− intermediate is significantly decreased by 1.88 eV, followed by an oxidization reaction to generate neutral BPNS-s-C60 hybrid. Surface bonding of C60 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.
期刊介绍:
Angewandte Chemie, a journal of the German Chemical Society (GDCh), maintains a leading position among scholarly journals in general chemistry with an impressive Impact Factor of 16.6 (2022 Journal Citation Reports, Clarivate, 2023). Published weekly in a reader-friendly format, it features new articles almost every day. Established in 1887, Angewandte Chemie is a prominent chemistry journal, offering a dynamic blend of Review-type articles, Highlights, Communications, and Research Articles on a weekly basis, making it unique in the field.