Supported Atomically-Precise Gold Nanoclusters for Enhanced Flow-through Electro-Fenton
- 9 April 2020
- journal article
- research article
- Published by American Chemical Society (ACS) in Environmental Science & Technology
- Vol. 54 (9), 5913-5921
- https://doi.org/10.1021/acs.est.0c00427
Abstract
Gold (Au) has been considered catalytically inert for decades, but recent reports have described the ability of Au nanoparticles to catalyze H2O2 decomposition in the Haber-Weiss cycle. Herein, the design and demonstration of a flow-through electro-Fenton system based on an electrochemical carbon nanotube (CNT) filter functionalized with atomically precise Au nanoclusters (AuNCs) is described. The functionality of the device was then tested for its ability to catalyze antibiotic tetracycline degradation. In the functional filters, the Au core of AuNCs served as a high-performance Fenton catalyst; while the AuNCs ligand shells enabled CNT dispersion in aqueous solution for easy processing. The hybrid filter enabled in situ H2O2 production and catalyzed the subsequent H2O2 decomposition to HO.. The catalytic function of AuNCs lies in their ability to undergo redox cycling of Au+/Au-0 under an electric field. The atomically precise AuNCs catalysts demonstrated superior catalytic activity to larger nanoparticles; while the flow-through design provided convection-enhanced mass transport, which yielded a superior performance compared to a conventional batch reactor. The adsorption behavior and decomposition pathway of H2O2 on the filter surfaces were simulated by density functional theory calculations. The research outcomes provided atomic-level mechanistic insights into the Au-mediated Fenton reaction.Keywords
Funding Information
- Natural Science Foundation of Shanghai (18ZR1401000)
- Ministry of Education of the People's Republic of China (2232019G-11)
- Ministry of Science and Technology of the People's Republic of China (2018YFF0215703)
- Science and Technology Commission of Shanghai Municipality (18PJ1400400)
This publication has 53 references indexed in Scilit:
- Au/carbon as Fenton-like catalysts for the oxidative degradation of bisphenol AApplied Catalysis B: Environmental, 2013
- Nitrogen Doping Effects on Carbon Nanotubes and the Origin of the Enhanced Electrocatalytic Activity of Supported Pt for Proton-Exchange Membrane Fuel CellsThe Journal of Physical Chemistry C, 2011
- Magnetic Fe2MO4 (M:Fe, Mn) activated carbons: Fabrication, characterization and heterogeneous Fenton oxidation of methyl orangeJournal of Hazardous Materials, 2011
- A strong support-effect on the catalytic activity of gold nanoparticles for hydrogen peroxide decompositionChemical Communications, 2011
- Gold on Diamond Nanoparticles as a Highly Efficient Fenton CatalystAngewandte Chemie, 2010
- Chromate-Induced Activation of Hydrogen Peroxide for Oxidative Degradation of Aqueous Organic PollutantsEnvironmental Science & Technology, 2010
- Electro-Fenton Process and Related Electrochemical Technologies Based on Fenton’s Reaction ChemistryChemical Reviews, 2009
- Catalytic activity of Au nanoparticlesNano Today, 2007
- Size- and support-dependency in the catalysis of goldCatalysis Today, 1997
- Why gold is the noblest of all the metalsNature, 1995