Unraveling the Dual-Capture Strategy in Surface-Grafted −NH2 on N-Defected g-C3N5 for Enhanced Photocatalytic Hydrogen Production

IF 3.8 3区 工程技术 Q2 ENGINEERING, CHEMICAL
Hongyin Liu, Jun Hu, Chenghui Hu, Syed Aamir Hussain and Feipeng Jiao*, 
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Abstract

N-rich carbon nitride (g-C3N5) became a promising photocatalyst due to its narrower band gap, larger π-conjugate network, and better visible light responsive hydrogen precipitation activity compared with g-C3N4. However, the inherent shortcomings still limited the development of g-C3N5. To reasonably address this issue, N defects and surface amino groups were successfully introduced into pristine g-C3N5 through facile one-step calcination. Systematical characterizations and theoretical calculation confirmed that the synergy of N defects and the surface-grafted amino group achieved a dual-capture strategy, endowing g-C3N5 with higher hydrophilicity and faster photogenerated carrier separation and transfer efficiency. With the modification of urea, the as-prepared samples exhibited a larger specific surface area to further provide more active sites during photocatalysis. The experimental results proved that the photocatalytic hydrogen evolution (PHE) performance of the novel material was significantly enhanced, with the optimal results reaching 5000.6 μmol·h–1·g–1, which was 24.5 and 4.5 times higher than that of the pristine g-C3N5 and the comparison sample, respectively. The stability and reusability of the N-defected g-C3N5 with surface-grafted amino groups were verified by the recycling tests without an obvious decrease after continuous 30 h visible light irradiation. This work provided perspective insight for designing and fabricating the surface functionalized g-C3N5 photocatalysts.

Abstract Image

揭示 N-缺陷 g-C3N5 表面接枝 -NH2 的双捕获策略,提高光催化制氢能力
与 g-C3N4 相比,富氮氮化碳(g-C3N5)具有更窄的带隙、更大的π-共轭网络和更好的可见光响应析氢活性,因此成为一种前景广阔的光催化剂。然而,其固有的缺陷仍然限制了 g-C3N5 的发展。为了合理地解决这一问题,我们通过简单的一步煅烧法成功地在原始 g-C3N5 中引入了 N 缺陷和表面氨基。系统表征和理论计算证实,N 缺陷和表面接枝氨基的协同作用实现了双重捕获策略,使 g-C3N5 具有更高的亲水性和更快的光生载流子分离和转移效率。在脲的修饰下,制备的样品具有更大的比表面积,从而在光催化过程中提供了更多的活性位点。实验结果证明,新型材料的光催化氢气进化(PHE)性能显著提高,最佳结果达到 5000.6 μmol-h-1-g-1,分别是原始 g-C3N5 和对比样品的 24.5 倍和 4.5 倍。通过回收试验验证了表面接枝氨基的 N 缺陷 g-C3N5 的稳定性和可再利用性,在连续 30 小时可见光照射后,其稳定性和可再利用性没有明显下降。这项工作为设计和制造表面功能化 g-C3N5 光催化剂提供了新的视角。
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来源期刊
Industrial & Engineering Chemistry Research
Industrial & Engineering Chemistry Research 工程技术-工程:化工
CiteScore
7.40
自引率
7.10%
发文量
1467
审稿时长
2.8 months
期刊介绍: ndustrial & Engineering Chemistry, with variations in title and format, has been published since 1909 by the American Chemical Society. Industrial & Engineering Chemistry Research is a weekly publication that reports industrial and academic research in the broad fields of applied chemistry and chemical engineering with special focus on fundamentals, processes, and products.
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