Surface modification to control the secondary pollution of photocatalytic nitric oxide removal over monolithic protonated g-C3N4/graphene oxide aerogel

IF 11.3 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Journal of Hazardous Materials Pub Date : 2020-10-05 DOI:10.1016/j.jhazmat.2020.122822
Ruiyang Zhang , Aili Zhang , Ye Yang , Yuehan Cao , Fan Dong , Ying Zhou
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引用次数: 27

Abstract

Recently, photocatalytic NOx 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 NO2 byproduct limit its application. Here, we designed a novel monolithic protonated g-C3N4/graphene oxide aerogel through a direct frozen-drying method. A remarkable surface electric charge change of negative g-C3N4 to positive protonated g-C3N4 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-C3N4 promotes the activation of oxygen atoms, thus improving the oxidization of NO2 to nitrate. As a result, protonated g-C3N4/graphene oxide aerogel reveals an excellent NO removal ratio (46.1%) and low NO2 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.

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表面改性控制单片质子化g-C3N4/氧化石墨烯气凝胶光催化去除一氧化氮的二次污染
近年来,光催化处理NOx因其环境友好、能源巨大而备受关注。然而,大多数报道的粉状光催化剂的回收困难和有毒二氧化氮副产物的高生成率限制了其应用。在这里,我们设计了一种新的单片质子化g-C3N4/氧化石墨烯气凝胶,通过直接冷冻干燥的方法。质子化处理后,负g-C3N4表面电荷发生了显著的变化,并与负的氧化石墨烯纳米片形成强静电自组装,加速了光生载流子的转移。氧化石墨烯气凝胶作为单片衬底,提供了丰富的多孔结构、增强的可见光吸收和电子传递途径,提高了光催化活性。重要的是,在p-C3N4的N原子上引入H原子,促进了氧原子的活化,从而改善了NO2氧化成硝酸盐的过程。结果表明,质子化g-C3N4/氧化石墨烯气凝胶具有良好的NO去除率(46.1%)和低NO2生成量(2.4%),显示了其在空气污染净化方面的良好前景。本研究为单片光催化剂的构建提供了新的创新思路,以控制环境修复中的二次污染。
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来源期刊
Journal of Hazardous Materials
Journal of Hazardous Materials 工程技术-工程:环境
CiteScore
25.40
自引率
5.90%
发文量
3059
审稿时长
58 days
期刊介绍: The Journal of Hazardous Materials serves as a global platform for promoting cutting-edge research in the field of Environmental Science and Engineering. Our publication features a wide range of articles, including full-length research papers, review articles, and perspectives, with the aim of enhancing our understanding of the dangers and risks associated with various materials concerning public health and the environment. It is important to note that the term "environmental contaminants" refers specifically to substances that pose hazardous effects through contamination, while excluding those that do not have such impacts on the environment or human health. Moreover, we emphasize the distinction between wastes and hazardous materials in order to provide further clarity on the scope of the journal. We have a keen interest in exploring specific compounds and microbial agents that have adverse effects on the environment.
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