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用于控制整体质子化 g-CN/氧化石墨烯气凝胶光催化去除一氧化氮过程中二次污染的表面修饰。

Surface modification to control the secondary pollution of photocatalytic nitric oxide removal over monolithic protonated g-CN/graphene oxide aerogel.

机构信息

State Key Laboratory of Oil and Gas Reservoir Geology and Exploitation, Southwest Petroleum University, Chengdu 610500, China; The Center of New Energy Materials and Technology, School of New Energy and Materials, Southwest Petroleum University, Chengdu 610500, China.

The Center of New Energy Materials and Technology, School of New Energy and Materials, Southwest Petroleum University, Chengdu 610500, China.

出版信息

J Hazard Mater. 2020 Oct 5;397:122822. doi: 10.1016/j.jhazmat.2020.122822. Epub 2020 May 12.

Abstract

Recently, photocatalytic NO treatment has attracted great attention on account of the use of environmental-friendly and tremendous energy source. However, the difficult recovery of most reported powdery photocatalysts and the high generation rate of toxic NO byproduct limit its application. Here, we designed a novel monolithic protonated g-CN/graphene oxide aerogel through a direct frozen-drying method. A remarkable surface electric charge change of negative g-CN to positive protonated g-CN can be observed after the protonating treatment, which connects with negative graphene oxide nanosheets through the formation of strong electrostatic self-assembly to accelerate the photogenerated charge carriers transfer. Graphene oxide aerogel acts as a monolithic substrate, which provides abundant porous structure, enhanced visible-light absorption, and electrons transport pathway to improve photocatalytic activity. Importantly, the introduction of H atoms on the N atoms of p-CN promotes the activation of oxygen atoms, thus improving the oxidization of NO to nitrate. As a result, protonated g-CN/graphene oxide aerogel reveals an excellent NO removal ratio (46.1%) and low NO generation (2.4%), demonstrating its excellent promising for air pollution purification. Our current work affords novel innovative insight for the construction of monolithic photocatalysts to control the secondary pollution for environmental remediation.

摘要

最近,由于使用了环保且能源丰富的光催化 NO 处理技术引起了人们的极大关注。然而,大多数报道的粉末状光催化剂的回收困难和有毒 NO 副产物的高生成率限制了其应用。在这里,我们通过直接冷冻干燥法设计了一种新型的整体质子化 g-CN/氧化石墨烯气凝胶。质子化处理后,可以观察到负 g-CN 的表面电荷从负到正的显著变化,这与通过形成强静电自组装连接的负石墨烯氧化物纳米片一起,加速光生载流子的转移。氧化石墨烯气凝胶作为整体基底,提供了丰富的多孔结构、增强的可见光吸收和电子传输途径,从而提高了光催化活性。重要的是,p-CN 上 N 原子的 H 原子的引入促进了氧原子的活化,从而提高了 NO 向硝酸盐的氧化。结果表明,质子化 g-CN/氧化石墨烯气凝胶具有优异的 NO 去除率(46.1%)和低的 NO 生成率(2.4%),展示了其在空气污染净化方面的应用前景。我们的研究为构建用于环境修复的整体光催化剂提供了新的创新思路,以控制二次污染。

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