Synergistic effect of ozonation and filtration with graphene-based membranes in the removal of flame retardants in multi-compound systems: Experimental and DFT study

Autor(es)

Neves, Tauany de Figueiredo ; Cristale, Joyce ; Camparotto, Natalia Gabriele ; Mastelaro, Valmor Roberto ; Dantas, Renato Falcao ; Prediger, Patricia

• Tipo de documento: Artigo Científico
• Fonte: JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING; v. 13, n. 1, p. 16-pg., 2024-12-07.

Resumo

Ozonation, although widely applied to treat water and effluents contaminated by organophosphate flame retardants (OPFRs), it can result in the generation of by-products that may be more toxic than the starting molecules. An alternative method for surmounting this challenge is the coupling of ozonation with filtration membranes. In this study, new polyacrylonitrile (PAN) membranes modified with graphene oxide (GO) functionalized with Safranin dye (SF) were synthesized, characterized and applied to remove organophosphate flame retardants (OPFRs) in multi-compound systems remaining after ozonation treatment. The PAN@fGO membrane, endowed with phenyl groups, phenazinium cations, electron-rich organic functions, with a rougher morphological profile and lower hydrophilicity, outperformed the PAN membrane in removing OPFRs. With a removal potential of 31.2, 42.7, 50.8, 59.5 and 62.6 % for tris(2-chloroisopropyl) phosphate (TCIPP), tris(2-chloroethyl) phosphate (TCEP), tri-n-butyl phosphate (TNBP), tris(2-butoxyethyl) phosphate (TBOEP), and triphenyl phosphate (TPHP), respectively. A synergistic effect was observed when the modified membrane was coupling with ozonation in multi-compound systems, reaching removal efficiencies of 43.7, 54.9, 59.6, 65.8 and 97.95 % for TCIPP, TCEP, TNBP, TBOEP and TPHP, respectively. Moreover, the combination of ozonation followed by PAN@fGO membrane filtration demonstrated efficacy in reducing the toxicity of the treated effluent to the vegetable Eruca sativa. The results, corroborated by calculations of molecular chemical descriptors based on DFT and characterizations of the membrane after the removal process, that the reaction with O3 in multi-compound systems was more effective in molecules with higher reactivity and the PAN@fGO interacts with the contaminants through hydrophobic, H-bonding, and it-it interactions. (AU)

• Processo FAPESP: 23/02041-8 - Preparação de membranas poliméricas a base de MOF contendo nióbio por rotofiação e sua aplicação na remoção de contaminantes em água
• Beneficiário: Natália Gabriele Camparotto
• Modalidade de apoio: Bolsas no Brasil - Doutorado
• Processo FAPESP: 22/14834-0 - Síntese de novos nanoadsorventes através de protocolos verdes e suas aplicações na remoção de poluentes em águas
• Beneficiário: Patricia Prediger
• Modalidade de apoio: Auxílio à Pesquisa - Regular
• Processo FAPESP: 19/25228-0 - Desenvolvimento de novas membranas baseadas em óxido de grafeno para a remoção de contaminantes em água
• Beneficiário: Tauany de Figueiredo Neves
• Modalidade de apoio: Bolsas no Brasil - Doutorado Direto
• Processo FAPESP: 22/00454-0 - Avaliação de tratamento terciário multibarreira para a remoção de microcontaminantes de ETEs de São Paulo
• Beneficiário: Renato Falcão Dantas
• Modalidade de apoio: Auxílio à Pesquisa - Regular
• Processo FAPESP: 13/07296-2 - CDMF - Centro de Desenvolvimento de Materiais Funcionais
• Beneficiário: Elson Longo da Silva
• Modalidade de apoio: Auxílio à Pesquisa - Centros de Pesquisa, Inovação e Difusão - CEPIDs