Journal
ACS ES&T WATER
Volume 2, Issue 1, Pages 174-183Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsestwater.1c00331
Keywords
Fenton-like reaction; dual-reaction centers; cation-pi structure; pollutant utilization
Categories
Funding
- National Natural Science Foundation of China [52122009, 52070046, 51808140, 51838005]
- Introduced Innovative R&D Team Project under the Pearl River Talent Recruitment Program of Guangdong Province [2019ZT08L387]
- National College Students' Innovation and Entrepreneurship Training Program, China [202111078021, 202111078019, 202011078019]
- Special Funds for the Cultivation of Guangdong College Students' Scientific and Technological Innovation- Climbing Program Special Funds [pdjh2021b0395]
- Guangdong Province Universities and Colleges Pearl River Scholar Funded Scheme
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An innovative strategy utilizing organic pollutants and dissolved oxygen in wastewater has been developed to degrade refractory organic pollutants effectively and rapidly. The newly developed catalyst showed excellent stability and wide adaptability.
Excessive consumption of resources and energy is inevitable in a classical Fenton reaction due to the demand for electron donors or electron acceptors (H2O2) and the existence of reaction rate-limiting steps. In this work, we propose an innovative strategy to solve this key scientific problem by utilizing the organic pollutants and the dissolved oxygen (DO) naturally present in the wastewater through a newly developed carbonized metal-organic framework-coated zero-valent Cu catalyst (ZVC@CMOF). It has been found that the formation of a C-O-Cu bond bridge on the catalyst induces electron polarization distribution to form a non-equilibrium surface with electron-rich or electron-poor microareas based on a series of characterization techniques. This typical non-equilibrium surface feature leads to excellent performance for pollutant conversion and a new interfacial reaction mechanism. Various types of refractory organic pollutants can be rapidly degraded in a few minutes in the ZVC@CMOF Fenton-like systems, accompanied by good stability and a wide pH adaptation range. The interfacial reaction processes are revealed by experimental analysis and theoretical calculations, in which pollutants and DO act as electron donors and electron acceptors in the electron-poor and electron-rich microareas, respectively, which greatly reduce the consumption of H2O2 and improve the reaction efficiency and catalytic performance for pollutant removal.
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