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

IF 2.9 Q2 PUBLIC, ENVIRONMENTAL & OCCUPATIONAL HEALTH ACS Chemical Health & Safety 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
ACS Chemical Health & Safety
ACS Chemical Health & Safety PUBLIC, ENVIRONMENTAL & OCCUPATIONAL HEALTH-
CiteScore
3.10
自引率
20.00%
发文量
63
期刊介绍: The Journal of Chemical Health and Safety focuses on news, information, and ideas relating to issues and advances in chemical health and safety. The Journal of Chemical Health and Safety covers up-to-the minute, in-depth views of safety issues ranging from OSHA and EPA regulations to the safe handling of hazardous waste, from the latest innovations in effective chemical hygiene practices to the courts'' most recent rulings on safety-related lawsuits. The Journal of Chemical Health and Safety presents real-world information that health, safety and environmental professionals and others responsible for the safety of their workplaces can put to use right away, identifying potential and developing safety concerns before they do real harm.
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