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Interfacial peroxydisulfate activation over graphene nanoplatelet-integrated polymeric iron phthalocyanine for petroleum hydrocarbon degradation in crude-oil-contaminated water
Department of Petroleum Chemistry, American University of Nigeria, Yola, Nigeria.
Department of Petroleum Chemistry, American University of Nigeria, Yola, Nigeria.
Department of Petroleum Chemistry, American University of Nigeria, Yola, Nigeria.
School of Science & Engineering, University of Dundee, Dundee, United Kingdom.
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2026 (English)In: Chemical Engineering Journal Advances, E-ISSN 2666-8211, Vol. 27, article id 101403Article in journal (Refereed) Published
Abstract [en]

Petroleum hydrocarbon-contaminated water remains difficult to remediate because crude-oil-derived pollutants are chemically diverse, hydrophobic, and persistent. Herein, a graphene nanoplatelet-integrated polymeric iron phthalocyanine framework (GNP-PFePc) was developed as an interfacial peroxydisulfate (PDS) activator for the removal and oxidative attenuation of total petroleum hydrocarbons (TPH) in crude-oil-contaminated water. The contaminated-water matrix contained an initial GC–MS-detectable TPH concentration of 11.47 g L⁻¹ dominated by C11-C29 linear and branched aliphatic hydrocarbons. GNP-PFePc integrates polymeric Fe-N-C domain containing Fe-N4-type coordination environments with a conductive and hydrophobic graphene nanoplatelet scaffold, thereby enhancing active-site accessibility, hydrocarbon enrichment and localized PDS activation at the catalyst-water interfaces. Under optimized conditions, GNP-PFePc/PDS achieved 89.7 % TPH removal within 30 min and 94.9 % within 150 min. The apparent pseudo-first-order rate constant calculated over the 150 min reaction interval was 0.0198 min⁻¹, corresponding to 17.2-fold and 5.7-fold enhancements relative to PDS alone and GNP-PFePc alone, respectively. Control and kinetic analyses showed that the coupled system outperformed adsorption or direct PDS oxidation alone, supporting an adsorption-assisted interfacial oxidation pathway. Compound-resolved analysis further showed that parent-hydrocarbon removal and oxidative attenuation were structure-dependent, with different responses across linear, branched, long chain and halogenated hydrocarbon fractions. Radical-scavenging and surface-probe experiments indicated that SO₄•⁻ and •OH participated in the oxidation process, with a substantial contribution from surface- reactive species generated at the GNP-PFePc/PDS interface. Overall, the results demonstrate that GNP-PFePc provides an effective Fe-N-C-type catalytic interface for localized PDS activation and surface-associated reactive oxidative- removal of petroleum hydrocarbons in crude-oil-contaminated water.

Place, publisher, year, edition, pages
Elsevier, 2026. Vol. 27, article id 101403
Keywords [en]
Advanced oxidation processes, Fe-Nₓ-C based catalytic sites, Peroxydisulfate activation, Petroleum hydrocarbon remediation, Polymeric iron phthalocyanine, Surface-bound reactive species
National Category
Organic Chemistry
Identifiers
URN: urn:nbn:se:umu:diva-257941DOI: 10.1016/j.ceja.2026.101403ISI: 001850792600001Scopus ID: 2-s2.0-105046979499OAI: oai:DiVA.org:umu-257941DiVA, id: diva2:2096978
Available from: 2026-08-31 Created: 2026-08-31 Last updated: 2026-08-31Bibliographically approved

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Manavalan, GopinathanTesfalidet, SolomonAdeniyi, Omotayo

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