Construction and elucidation of zerovalent iron@terephthalic acid/iron oxide catalyst to activate peroxymonosulfate for accelerating and long-lasting NOx removal

Hafiz Muhammad Adeel Sharif, Muhammad Asif, Yuwei Wang, Kifayatullah Khan, Yang Cai, Xu Xiao, Changping Li

Research output: Contribution to journalArticlepeer-review

9 Scopus citations

Abstract

Recently peroxymonosulfate (PMS)-based advanced oxidation techniques (AOTs) have been widely used nowadays for pollutant removal. However, Fenton/Fenton-like reactions using Fe-based catalysts are highly promising for the NOx treatment due to their improved catalytic efficiency, low cost, and offering effectual reactive oxygen species (ROS). However, the long-term reusability without generating (Fe) sludge and its inactivation due to the non-spontaneous conversion of Fe(II)/Fe(III) are problematic. Hence, a variety of catalysts had been employed to activate Fe(II) and for efficient ROS generation. In this work, we designed a single metal-based stable and heterogeneous Fenton-like technology (SMHFT) with Fe3O4 (base material) functionalized using 2-amino terephthalic acid (ATA) to increase stability and surface area. The Fe3O4@ATA composite was finally decorated using solid zero-valent-iron (Fe0) (i.e., MTAFe0), where terminal Fe0 offers an active surface for ultrafast PMS activation and efficient ROS generation. The ROS containing SO4-•, HO•, and 1O2 entities are entirely used for NO oxidation with better mass transfer without using an electron (e-) mediator and restored Fe-efficiency. The electron paramagnetic resonance (EPR) and various scavengers verified the ROS participating in NO oxidation significantly, as well as in-situ regeneration of the catalyst. The synthesized MTAFe0 showed ∼ 94 % efficiency, and the density functional theory (DFT) elucidated PMS adsorption and its ultrafast activation by ROS generation. Finally, the reusability of MTAFe0 was investigated, and it showed over 90% efficiency after 10-continuous cycles. Hence, the developed SMHFT system has great potential for fast NO removal with long-term utilization, which is promising and could be implemented sustainability for air pollution treatment.
Original languageEnglish (US)
Pages (from-to)142782
JournalChemical Engineering Journal
Volume465
DOIs
StatePublished - Apr 11 2023

Bibliographical note

KAUST Repository Item: Exported on 2023-05-09
Acknowledgements: This study was supported by the National Natural Science Foundation of China (Grant No. 22050410268 and 52070042). Special thnaks to Ayaz Mahmood for his constructive and healthy suggestions for DFT work.

ASJC Scopus subject areas

  • Environmental Chemistry
  • General Chemical Engineering
  • General Chemistry
  • Industrial and Manufacturing Engineering

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