Published June 4, 2019 | Version Published + Supplemental Material
Journal Article Open

Multiphase Porous Electrochemical Catalysts Derived from Iron-Based Metal–Organic Framework Compounds

  • 1. ROR icon Zhejiang University
  • 2. ROR icon California Institute of Technology

Abstract

Herbicide use has attracted attention recently due to potential damage to human health and lethality to the honey bees and other pollinators. Fenton reagent treatment processes can be applied for the degradation of herbicidal contaminants from water. However, the need to carry out the normal Fenton reactions under acidic conditions often hinders their practical application for pollution control. Herein, we report on the synthesis and application of multiphasic porous electro-Fenton catalysts prepared from calcinated metal–organic framework compounds, CMOF@PCM, and their application for the mineralization of herbicides in aqueous solution at circum-neutral pH. CMOF nanoparticles (NPs) are anchored on porous carbon monolithic (PCM) substrates, which allow for binder-free application. H_2O_2 is electrochemically generated on the PCM substrate which serves as a cathode, while ·OH is generated by the CMOF NPs at low applied potentials (−0.14 V). Results show that the structure and reactivity of the CMOF@PCM electro-Fenton catalysts are dependent on the specific MOF precursor used during synthesis. For example, CMIL-88-NH_2, which is prepared from MIL-88(Fe)–NH_2, is a porous core–shell structured NP comprised of a cementite (Fe_3C) intermediate layer that is sandwiched between a graphitic shell and a magnetite (Fe_3O_4) core. The electro-Fenton production of hydroxyl radical on the CMOF@PCM composite material is shown to effectively degrade an array of herbicides.

Additional Information

© 2019 American Chemical Society. ACS AuthorChoice - This is an open access article published under a Creative Commons Attribution (CC-BY) License, which permits unrestricted use, distribution and reproduction in any medium, provided the author and source are cited. Received: February 22, 2019; Revised: May 8, 2019; Accepted: May 10, 2019; Published: May 10, 2019. This work was supported by the Bill and Melinda Gates Foundation (Grant OPP1149755), National Natural Science Foundations of China (Grant No. 21777137), International Cooperation Grant of China (Grant No. 21320102007), and the Caltech Rosenburg Innovation Initiative. Author Contributions: K.L. and M.Y. contributed equally to the work. The authors declare no competing financial interest.

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Published - acs.est.9b01143.pdf

Supplemental Material - es9b01143_si_001.pdf

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Additional details

Additional titles

Alternative title
Multi-Phase Porous Electrochemical Catalysts Derived from Iron-Based Metal-Organic Framework Compounds

Identifiers

PMCID
PMC6551571
Eprint ID
95393
Resolver ID
CaltechAUTHORS:20190510-105529564

Funding

Bill and Melinda Gates Foundation
OPP1149755
National Natural Science Foundation of China
21777137
National Natural Science Foundation of China
21320102007
Rothenberg Innovation Initiative (RI2)

Dates

Created
2019-05-10
Created from EPrint's datestamp field
Updated
2021-11-16
Created from EPrint's last_modified field