Potential Difference Driving Electron Transfer via Defective Carbon Nanotubes toward Selective Oxidation of Organic Micropollutants
Top Cited Papers
- 10 June 2020
- journal article
- research article
- Published by American Chemical Society (ACS) in Environmental Science & Technology
- Vol. 54 (13), 8464-8472
- https://doi.org/10.1021/acs.est.0c02645
Abstract
Nanocarbon-based persulfate oxidation emerges as a promising technology for the elimination of organic micropollutants (OMPs). However, the nature of the active site and its working mechanism remain elusive, impeding developments of high-performance oxidative technology for water treatment practice. Here, we report that defect-rich carbon nanotubes (CNTs) exhibit a superior activity in the activation of peroxymonosulfate (PMS) for OMP oxidation. Quantitative structure–activity relationship studies combined with theoretical calculations unveil that the double-vacancy defect on CNTs may be the intrinsic active site, which works as a conductive bridge to facilitate the potential difference-dominated electron transfer from the highest occupied molecular orbital of OMPs to the lowest unoccupied molecular orbital of PMS. Based on this unique mechanism, the established [email protected] oxidative system achieves outstanding selectivity and realizes the target-oriented elimination of specific OMPs in a complicated aquatic environment. This work sheds new light on the mechanism of carbocatalysis for selective oxidation and develops an innovative technology toward remediation of practical wastewater.Keywords
Funding Information
- Inner Mongolia Autonomous Region (2019ZD001)
- Ministry of Science and Technology of the People's Republic of China (2018YFC0406400, 2019YFC1907900)
- National Natural Science Foundation of China (51678285, 51908270)
- Natural Science Foundation of Jiangxi Province (20192BAB213016)
- Jiangxi Province (20181BCB18002, 20192AEI91001)
- Key Research and Development Program of Inner Mongolia Autonomous Region (2019ZD001)
This publication has 45 references indexed in Scilit:
- Persulfate-Based Advanced Oxidation: Critical Assessment of Opportunities and RoadblocksEnvironmental Science & Technology, 2020
- Activation of Peroxydisulfate on Carbon Nanotubes: Electron-Transfer MechanismEnvironmental Science & Technology, 2019
- Peroxydisulfate activation by positively polarized carbocatalyst for enhanced removal of aqueous organic pollutantsWater Research, 2019
- Emerging opportunities for nanotechnology to enhance water securityNature Nanotechnology, 2018
- High-silica zeolites for adsorption of organic micro-pollutants in water treatment: A reviewWater Research, 2018
- The role of nanotechnology in tackling global water challengesNature Sustainability, 2018
- Advanced Materials, Technologies, and Complex Systems Analyses: Emerging Opportunities to Enhance Urban Water SecurityEnvironmental Science & Technology, 2017
- Rapid removal of organic micropollutants from water by a porous β-cyclodextrin polymerNature, 2015
- Global threats to human water security and river biodiversityNature, 2010
- The Challenge of Micropollutants in Aquatic SystemsScience, 2006