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含氧基团和 P 掺杂多孔碳氮纳米片提高光催化活性。

Oxygen-containing groups and P doped porous carbon nitride nanosheets towards enhanced photocatalytic activity.

机构信息

College of Environment & Resource Sciences, Zhejiang University, Hangzhou, 310058, PR China.

College of Environment & Resource Sciences, Zhejiang University, Hangzhou, 310058, PR China.

出版信息

Chemosphere. 2022 Jan;287(Pt 4):132399. doi: 10.1016/j.chemosphere.2021.132399. Epub 2021 Sep 28.

DOI:10.1016/j.chemosphere.2021.132399
PMID:34597630
Abstract

Metal-free polymer graphite carbon nitride (CN) is a promising photocatalyst that has garnered significant research attention. However, unmodified CN possesses several shortcomings such as low specific surface area, poor dispersibility in water, and rapid photogenerated electron-hole recombination, which have severely impacted its mass adoption. Here, this study proposed a two-step heat treatment method to incorporate P dopant and the containing-oxygen groups successively into CN. The final product, denoted as PO-CN, possessed a porous ultrathin nanosheet-like morphology. The introduction of P dopant altered the intrinsic electronic structure of CN. Meanwhile, the presence of oxygen-containing groups improved the dispersibility of PO-CN in water. Also, it led to the formation of a porous ultrathin structure that could provide more active sites. Through the synergistic effects of these two methods, PO-CN demonstrated superior photocatalytic performance compared to the unmodified counterpart. Based on the collective results obtained experimentally and theoretically, PO-CN possessed a porous ultrathin structure, low resistance, and low carrier recombination. The results show an optimal hydrogen evolution rate of PO-CN (997.7 mol h g), which was 11.2 times and 3.22 times that of the CN (88.89 mol h g) and PCN (310.3 mol h g). Moreover, PO-CN was then used in the degradation of Rhodamine B, and a degradation kinetic constant (k) of 0.15009 was calculated, which was 18.42 times and 8.22 times higher as compared to those of CN (0.00815) and PCN (0.01826). Hence, this work provides a new strategy for the alteration of the morphology and electronic structure of CN.

摘要

无金属聚合物石墨相氮化碳(CN)是一种很有前途的光催化剂,引起了广泛的研究关注。然而,未经修饰的 CN 存在比表面积低、在水中分散性差以及光生电子-空穴复合速率快等缺点,这严重限制了其大规模应用。在此,本研究提出了一种两步热处理方法,将 P 掺杂剂和含氧基团依次引入到 CN 中。最终产物记为 PO-CN,具有多孔超薄纳米片状形貌。P 掺杂剂的引入改变了 CN 的本征电子结构。同时,含氧基团的存在提高了 PO-CN 在水中的分散性。此外,它形成了多孔超薄结构,可以提供更多的活性位点。通过这两种方法的协同作用,PO-CN 表现出比未修饰的 CN 更好的光催化性能。基于实验和理论上获得的综合结果,PO-CN 具有多孔超薄结构、低电阻和低载流子复合率。结果表明,PO-CN 的最佳析氢速率为 997.7 μmol h-1 g-1,是 CN(88.89 μmol h-1 g-1)和 PCN(310.3 μmol h-1 g-1)的 11.2 倍和 3.22 倍。此外,PO-CN 还用于罗丹明 B 的降解,计算得到的降解动力学常数(k)为 0.15009,分别是 CN(0.00815)和 PCN(0.01826)的 18.42 倍和 8.22 倍。因此,这项工作为改变 CN 的形貌和电子结构提供了一种新策略。

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