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Fully Exposed Pd Ensembles on Ultrathin Co3O4 Nanosheets: A Reductive–Oxidative Dual-Active Catalyst for the Detoxification of Chlorophenol
ACS ES&T Engineering Pub Date : 2024-03-15 , DOI: 10.1021/acsestengg.4c00003
Ziang Du 1 , Wei Ran 1, 2 , Huachao Zhao 1, 2 , Juan Ma 1, 2 , Jiefang Sun 3 , Beizi Liu 1 , Sijia Lin 1 , Rui Liu 1, 2, 4
Affiliation  

The complete detoxification of hazardous organic pollutants is crucial for water treatment. However, this often requires the cooperation of multiple treatment processes catalyzed by different catalysts, leading to a complex water treatment infrastructure design and high operational costs. To address this challenge, we developed fully exposed palladium (Pd) ensemble (Pdn)-loaded ultrathin Co3O4 nanosheets (NSs) (Pdn/Co3O4 NSs) as a reductive–oxidative dual-active catalyst for the efficient detoxification of halogenated organic pollutants. During the treatment of simulated water contaminated by 4-chlorophenol (4-CP), a representative persistent organic pollutant, Pdn reactive centers rapidly hydrodechlorinate 4-CP into low-toxicity phenol with activity ≥10 times that of benchmark catalysts. The synergy between the Pd ensembles and oxygen vacancies further promotes the rapid and selective hydrogenation of phenol into cyclohexanone on Co3O4 NSs. Subsequently, cyclohexanone is oxidized by peroxymonosulfate (PMS) under Co3O4 activation. A cell assay-based toxicity study confirmed that stimulated polluted environmental water is fully detoxified after treatment with the designed Pdn/Co3O4 NSs catalyst. This study provides new insights into the rational design of Pd catalysts for the catalytic removal of persistent organic pollutants, particularly halogenated aromatics, paving the way for facile, low-cost, and highly efficient water treatment processes.

中文翻译:

超薄 Co3O4 纳米片上完全暴露的 Pd 整体:用于氯苯酚解毒的还原氧化双活性催化剂

有害有机污染物的彻底解毒对于水处理至关重要。然而,这往往需要不同催化剂催化的多种处理工艺的配合,导致水处理基础设施设计复杂且运营成本高昂。为了应对这一挑战,我们开发了完全暴露的钯(Pd)整体(Pd n)负载的超薄Co 3 O 4纳米片(NSs)(Pd n /Co 3 O 4 NSs)作为还原-氧化双活性催化剂高效解毒卤代有机污染物。在处理典型持久性有机污染物4-氯苯酚(4-CP)污染的模拟水时,Pd n反应中心将4-CP快速加氢脱氯为低毒苯酚,其活性≥基准催化剂的10倍。Pd系综和氧空位之间的协同作用进一步促进了苯酚在Co 3 O 4 NSs上快速选择性加氢成环己酮。随后,环己酮在Co 3 O 4活化下被过一硫酸盐(PMS)氧化。基于细胞分析的毒性研究证实,受刺激的污染环境水在用设计的Pd n /Co 3 O 4 NSs催化剂处理后完全解毒。这项研究为钯催化剂的合理设计提供了新的见解,用于催化去除持久性有机污染物,特别是卤代芳烃,为简便、低成本和高效的水处理工艺铺平了道路。
更新日期:2024-03-16
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