Jiaqi Chen, Yuan Yao, Yu Yan, Xiaoxiao Li, Yang Liu
{"title":"Self-Recycled Electron Donor Resists Disfavored Oxidation Reconstruction of Cu(I)-based Electrocatalyst for Nitrate Removal by Charge Compensation","authors":"Jiaqi Chen, Yuan Yao, Yu Yan, Xiaoxiao Li, Yang Liu","doi":"10.1016/j.watres.2024.122959","DOIUrl":null,"url":null,"abstract":"The overuse of nitrate has led to the accumulation in natural water, being a globe issue in environment and human health. Electrochemical NO<sub>3</sub><sup>−</sup> reduction reaction (eNO<sub>3</sub>RR) to ammonia occurs under ambient condition with low energy consumption and the yield of value-added product, being promising for NO<sub>3</sub><sup>−</sup> removal. Cu<sup>(I)</sup>-based eNO<sub>3</sub>RR catalysts suffer from unavoidable oxidation reconstruction to Cu<sup>(II)</sup>, reducing the performance of NO<sub>3</sub><sup>−</sup> removal. In this work, we demonstrate charge compensation strategy to resist oxidation reconstruction of Cu<sup>(I)</sup>-based eNO<sub>3</sub>RR catalysts by introducing self-recycled electron donor. Taking Ti<sup>(III)</sup>-modified Cu<sub>2</sub>O/Cu as the proof-of-concept model, electron donor Ti<sup>(III)</sup> can donate electron to Cu<sup>(II)</sup> to regenerate Cu<sup>(I)</sup>, meanwhile the expended Ti<sup>(III)</sup> can be recycled from the generated Ti<sup>(IV)</sup> via intervalence charge transfer (IVCT). Benefiting from those, Ti-Cu<sub>2</sub>O/Cu-10 exhibits significantly improved activity and durability for NO<sub>3</sub><sup>−</sup> removal compared to Cu<sub>2</sub>O/Cu. The percentage of NO<sub>3</sub><sup>−</sup> removal keeps at ∼95.0% with the initial concentration of 60 mg•L<sup>−1</sup> NO<sub>3</sub><sup>−</sup>-N at -0.9 V <em>vs.</em> RHE in 15 consecutive cycling tests (corresponding to 30 hours). This work presents a feasible strategy to resist oxidation reconstruction of Cu<sup>(I)</sup>-based eNO<sub>3</sub>RR catalysts, making NO<sub>3</sub><sup>−</sup> removal more effective, more durable, and more sustainable.","PeriodicalId":443,"journal":{"name":"Water Research","volume":"28 1","pages":""},"PeriodicalIF":11.4000,"publicationDate":"2024-12-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Water Research","FirstCategoryId":"93","ListUrlMain":"https://doi.org/10.1016/j.watres.2024.122959","RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, ENVIRONMENTAL","Score":null,"Total":0}
引用次数: 0
Abstract
The overuse of nitrate has led to the accumulation in natural water, being a globe issue in environment and human health. Electrochemical NO3− reduction reaction (eNO3RR) to ammonia occurs under ambient condition with low energy consumption and the yield of value-added product, being promising for NO3− removal. Cu(I)-based eNO3RR catalysts suffer from unavoidable oxidation reconstruction to Cu(II), reducing the performance of NO3− removal. In this work, we demonstrate charge compensation strategy to resist oxidation reconstruction of Cu(I)-based eNO3RR catalysts by introducing self-recycled electron donor. Taking Ti(III)-modified Cu2O/Cu as the proof-of-concept model, electron donor Ti(III) can donate electron to Cu(II) to regenerate Cu(I), meanwhile the expended Ti(III) can be recycled from the generated Ti(IV) via intervalence charge transfer (IVCT). Benefiting from those, Ti-Cu2O/Cu-10 exhibits significantly improved activity and durability for NO3− removal compared to Cu2O/Cu. The percentage of NO3− removal keeps at ∼95.0% with the initial concentration of 60 mg•L−1 NO3−-N at -0.9 V vs. RHE in 15 consecutive cycling tests (corresponding to 30 hours). This work presents a feasible strategy to resist oxidation reconstruction of Cu(I)-based eNO3RR catalysts, making NO3− removal more effective, more durable, and more sustainable.
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.