Atomically Dispersed Janus Nickel Sites on Red Phosphorus for Photocatalytic Overall Water Splitting

Single‐atom nickel catalysts hold great promise for photocatalytic water splitting due to their plentiful active sites and cost‐effectiveness. Herein, we adopt a reactive‐group guided strategy to prepare atomically dispersed nickel catalysts on red phosphorus. The hydrothermal treatment of red phosp...

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Bibliographic Details
Published in:Angewandte Chemie International Edition 2022-07, Vol.61 (29), p.e202204711-n/a
Main Authors: Wang, Menglong, Xu, Shuai, Zhou, Zhaohui, Dong, Chung‐Li, Guo, Xu, Chen, Jeng‐Lung, Huang, Yu‐Cheng, Shen, Shaohua, Chen, Yubin, Guo, Liejin, Burda, Clemens
Format: Article
Language:English
Subjects:
Active sites
Catalysts
Hydrogen evolution
Hydrothermal treatment
Irradiation
Light irradiation
Nanoparticles
Nickel
Oxidation
Phosphorus
Photocatalysis
Quantum efficiency
Radiation
Red Phosphorus
Single-Atom Catalysts
Water Splitting
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Summary:Single‐atom nickel catalysts hold great promise for photocatalytic water splitting due to their plentiful active sites and cost‐effectiveness. Herein, we adopt a reactive‐group guided strategy to prepare atomically dispersed nickel catalysts on red phosphorus. The hydrothermal treatment of red phosphorus leads to the formation of P−H and P−OH groups, which behave as the reactive functionalities to generate the dual structure of single‐atom P−Ni and P−O−Ni catalytic sites. The produced single‐atom sites provide two different functions: P−Ni for water reduction and P−O−Ni for water oxidation. Benefitting from this specific Janus structure, Ni‐red phosphorus shows an elevated hydrogen evolution rate compared to Ni nanoparticle‐modified red phosphorus under visible‐light irradiation. The hydrogen evolution rate was additionally enhanced with increased reaction temperature, reaching 91.51 μmol h−1 at 70 °C, corresponding to an apparent quantum efficiency of 8.9 % at 420 nm excitation wavelength. A reactive‐group guided approach is taken to synthesize atomically dispersed Ni catalysts on red phosphorus. The advanced system consists of Janus single‐atom Ni sites: P−Ni for water reduction and P−O−Ni for water oxidation, leading to the efficient separation of electron‐hole pairs and overall improved photocatalytic water splitting activity.
ISSN:1433-7851
1521-3773
1521-3773
DOI:10.1002/anie.202204711