Cooperating oxidative half-reaction deactivate electrocatalyst for nitrate reduction in real wastewater

IF 11.4 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL
Chunxia Zhang, Zhuanzhuan Li, Kemeng Zhang, Yunpu Zhai, Changsen Zhang, Panpan Liu
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Abstract

Electrocatalytic nitrate reduction to ammonia (eNO3RA) paves a promising way toward nitrate mitigation and ammonia recovery from real wastewater. While the complex constituents in real wastewater raise concerns about the stability of catalysts. Here, the comprehensive investigation of the stability of easy-to-prepare CuxO nanowires for eNO3RA is performed in real wastewater. Irreversible catalyst deactivation is observed in short-term operation for eNO3RA and ammonia selectivity decreases from 82.02 to 28.37 % due to the ineffective hydrogenation of intermediates. Conversely, the performance decrease for long-term eNO3RA in confined electrolytes can be recovered with oven drying of the catalyst. The irreversible deactivation of the catalyst proceeds with the aggregation of nanowires as the oxidation of Cu+ to Cu2+. Chloride ion is recognized as the main contributor due to the cooperating oxidative half-reaction at the anode. These findings emphasize the need for careful consideration of the catalysts’ stability in the design of electrochemical systems for eNO3RA.

Abstract Image

协同氧化半反应失活电催化剂在实际废水中还原硝酸盐
电催化硝酸还原制氨(eNO3RA)为从实际废水中减少硝酸盐和回收氨铺平了有希望的道路。而实际废水中复杂的成分引起了人们对催化剂稳定性的关注。本文在实际废水中对易于制备的CuxO纳米线的稳定性进行了全面的研究。在短期操作中,en3ra催化剂发生不可逆失活,由于中间产物加氢无效,氨选择性从82.02下降到28.37%。相反,en3ra在受限电解质中长期的性能下降可以通过烘箱干燥催化剂来恢复。随着Cu+氧化成Cu2+,纳米线聚集,催化剂发生不可逆失活。由于氯离子在阳极的协同氧化半反应,氯离子被认为是主要的贡献者。这些发现强调了在设计en3ra电化学系统时需要仔细考虑催化剂的稳定性。
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来源期刊
Water Research
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.
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