Selective electrocatalytic transformation of highly toxic phenols in wastewater to para-benzoquinone at ambient conditions

IF 12.4 1区环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL

Water Research Pub Date : 2024-01-04 DOI:10.1016/j.watres.2024.121106

Fuqiang Liu , Hongyu Dong , Shifa Zhong , Xuechen Wu , Tong Wang , Xuelu Wang , Yanbiao Liu , Mingshan Zhu , Irene M.C. Lo , Sihui Zhan , Xiaohong Guan

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Abstract

The selective transformation of organics from wastewater to value-added chemicals is considered an upcycling process beneficial for carbon neutrality. Herein, we present an innovative electrocatalytic oxidation (ECO) system aimed at achieving the selective conversion of phenols in wastewater to para-benzoquinone (p-BQ), a valuable chemical widely utilized in the manufacturing and chemical industries. Notably, 96.4% of phenol abatement and 78.9% of p-BQ yield are synchronously obtained over a preferred carbon cloth-supported ruthenium nanoparticles (Ru/C) anode. Such unprecedented results stem from the weak Ru–O bond between the Ru active sites and generated p-BQ, which facilitates the desorption of p-BQ from the anode surface. This property not only prevents the excessive oxidation of the generated p-BQ but also reinstates the Ru active sites essential for the rapid ECO of phenol. Furthermore, this ECO system operates at ambient conditions and obviates the need for potent chemical oxidants, establishing a sustainable avenue for p-BQ production. Importantly, the system efficacy can be adaptable in actual phenol-containing coking wastewater, highlighting its potential practical application prospect. As a proof of concept, we construct an electrified Ru/C membrane for ECO of phenol, attaining phenol removal of 95.8% coupled with p-BQ selectivity of 73.1%, which demonstrates the feasibility of the ECO system in a scalable flow-through operation mode. This work provides a promising ECO strategy for realizing both phenols removal and valuable organics recovery from phenolic wastewater.

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在环境条件下将废水中的剧毒酚选择性地电催化转化为对苯醌

选择性地将废水中的有机物转化为高附加值化学品被认为是有利于实现碳中和的升级再循环过程。在此，我们提出了一种创新的电催化氧化（ECO）系统，旨在实现将废水中的苯酚选择性地转化为对苯醌（p-BQ），对苯醌是一种在制造业和化学工业中广泛使用的有价值的化学品。值得注意的是，在优选碳布支撑的钌纳米粒子（Ru/C）阳极上，同步获得了 96.4% 的苯酚减量和 78.9% 的对苯醌产量。这种前所未有的结果源于 Ru 活性位点与生成的对-BQ 之间的弱 Ru-O 键，这有利于对-BQ 从阳极表面解吸。这一特性不仅能防止生成的 p-BQ 过度氧化，还能恢复对苯酚快速 ECO 必不可少的 Ru 活性位点。此外，这种 ECO 系统可在环境条件下运行，无需使用强效化学氧化剂，从而为对-BQ 的生产开辟了一条可持续发展的途径。重要的是，该系统的功效可适用于实际的含酚焦化废水，突显了其潜在的实际应用前景。作为概念验证，我们构建了用于苯酚 ECO 的电气化 Ru/C 膜，苯酚去除率达到 95.8%，p-BQ 选择性达到 73.1%，这证明了 ECO 系统在可扩展的直流操作模式下的可行性。这项工作为实现酚类废水中酚的去除和有价值有机物的回收提供了一种前景广阔的 ECO 策略。

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来源期刊

Water Research 环境科学-工程：环境

CiteScore

20.80

自引率

9.40%

发文量

1307

审稿时长

38 days

期刊介绍： Water Research, along with its open access companion journal Water Research X, serves as a platform for publishing original research papers covering various aspects of the science and technology related to the anthropogenic water cycle, water quality, and its management worldwide. The audience targeted by the journal comprises biologists, chemical engineers, chemists, civil engineers, environmental engineers, limnologists, and microbiologists. The scope of the journal include: •Treatment processes for water and wastewaters (municipal, agricultural, industrial, and on-site treatment), including resource recovery and residuals management; •Urban hydrology including sewer systems, stormwater management, and green infrastructure; •Drinking water treatment and distribution; •Potable and non-potable water reuse; •Sanitation, public health, and risk assessment; •Anaerobic digestion, solid and hazardous waste management, including source characterization and the effects and control of leachates and gaseous emissions; •Contaminants (chemical, microbial, anthropogenic particles such as nanoparticles or microplastics) and related water quality sensing, monitoring, fate, and assessment; •Anthropogenic impacts on inland, tidal, coastal and urban waters, focusing on surface and ground waters, and point and non-point sources of pollution; •Environmental restoration, linked to surface water, groundwater and groundwater remediation; •Analysis of the interfaces between sediments and water, and between water and atmosphere, focusing specifically on anthropogenic impacts; •Mathematical modelling, systems analysis, machine learning, and beneficial use of big data related to the anthropogenic water cycle; •Socio-economic, policy, and regulations studies.