Directed holey and ordered g-C3N4.5 nanosheets by a hard template nanocasting approach for sustainable visible-light hydrogen evolution with prominent quantum efficiency

文献情報

出版日 2020-06-15

DOI 10.1039/D0TA02734K

インパクトファクター 12.732

著者

Bindu Antil, Sasanka Deka

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要旨

It is desirable yet challenging to synthesize a highly ordered holey carbon nitride material with excess nitrogen atoms for a sustainable solar H2 evolution. Herein, we report the development of directed highly ordered nitrogen-rich honeycomb-like mesoporous carbon nitride nanosheets by using a novel synthetic approach for this purpose. The unique formation route, surface structure and charge carrier dynamics of the two dimensional holey nanosheets are comprehensively monitored and confirmed by SAXS, HRTEM, AFM, BET, XPS and TRPL analyses. Non-stoichiometric high nitrogen content mesoporous nanosheets with the final stoichiometry of g-C3N4.5 acquiring a high specific surface area (382 m2 g−1), remarkable pore size (7.2 nm) and sheet thickness ∼5–6 nm are realized in this first report. This elegant material possesses unique low band-gap energy (2.42 eV). Remarkably, the as-synthesized g-C3N4.5 NSs exhibit a record high photocatalytic H2 evolution rate of 8180 μmol g−1 h−1 under the present light irradiation (420 ≤ λ ≤ 510 nm) condition. The apparent quantum efficiency is found to be as high as 27.14% at 420 nm and retains its photocatalytic activity for longer consecutive catalytic cycles. Bigger pore size and pore volume, and thin walls leading to shortening of the path length of exciton pairs, efficient charge separation and the prolonged average life time of the charge carriers, and lone electron pairs associated with the excess nitrogen content are found to be the reasons behind the excellent visible light driven water splitting reaction.

掲載誌

Journal of Materials Chemistry A

CiteScore: 19.5

自己引用率: 4.7%

年間論文数: 2211

Journal of Materials Chemistry A, B & C cover high quality studies across all fields of materials chemistry. The journals focus on those theoretical or experimental studies that report new understanding, applications, properties and synthesis of materials. The journals have a strong history of publishing quality reports of interest to interdisciplinary communities and providing an efficient and rigorous service through peer review and publication. The journals are led by an international team of Editors-in-Chief and Associate Editors who are all active researchers in their fields. Journal of Materials Chemistry A, B & C are separated by the intended application of the material studied. Broadly, applications in energy and sustainability are of interest to Journal of Materials Chemistry A, applications in biology and medicine are of interest to Journal of Materials Chemistry B, and applications in optical, magnetic and electronic devices are of interest to Journal of Materials Chemistry C. More than one Journal of Materials Chemistry journal may be suitable for certain fields and researchers are encouraged to submit their paper to the journal that they feel best fits for their particular article. Example topic areas within the scope of Journal of Materials Chemistry A are listed below. This list is neither exhaustive nor exclusive. Artificial photosynthesis Batteries Carbon dioxide conversion Catalysis Fuel cells Gas capture/separation/storage Green/sustainable materials Hydrogen generation Hydrogen storage Photocatalysis Photovoltaics Self-cleaning materials Self-healing materials Sensors Supercapacitors Thermoelectrics Water splitting Water treatment

Directed holey and ordered g-C3N4.5 nanosheets by a hard template nanocasting approach for sustainable visible-light hydrogen evolution with prominent quantum efficiency

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