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- Plastic waste-derived carbon nanotubes: Influence of growth catalyst and catalytic activity in CWPOPublication . Roman, Fernanda; Silva, Adriano S.; Tuesta, Jose L. Diaz de; Baldo, Arthur P.; Lopes, Jessica P.M.; Gonçalves, Giane; Pereira, Ana I.; Praça, Paulo; Silva, Adrián M.T.; Faria, Joaquim L.; Bañobre-López, Manuel; Gomes, HelderLow-density polyethylene (LDPE) was used in this work to grow carbon nanotubes (CNTs) by chemical vapor deposition (CVD) over catalysts based on Ni, Fe and Al, synthesized either by co-precipitation (C) or wet impregnation (I) methods, with CNT yields in the range of 16–33 %. The morphology of the CNTs was directly influenced by the route used for the CVD catalyst synthesis, with co-precipitation-derived CVD catalysts resulting in CNT samples with curly walls. CNTs were purified with H2SO4 (10–50 wt.%) to remove attached metal particles. All synthesized materials (CVD-catalysts, as-synthesized CNTs, and purified CNTs) were tested as catalysts in the catalytic wet peroxide oxidation (CWPO) of paracetamol (PCM), chosen as a model pharmaceutical compound. Removals of 100 % of PCM in 8 h and 71 % of total organic carbon (TOC) in 24 h were achieved, with an H2O2 consumption efficiency of 76 % in 24 h for purified CNT (CNT@NiFeAl-C-P). The same CVD-catalyst (NiFeAl-C) was used to grow CNTs using real LDPE waste, and it was tested under the same reaction conditions, resulting in a PCM and TOC abatement of 90 % and 65 %, respectively. The synthesis of CNTs using LDP waste was a good alternative, given the environmental benefits associated with its reintroduction into the economic cycle as a material with higher value than initially (upcycling).
- Carbon-Coated Magnetic Catalysts for Enhanced Degradation of Nitrophenols: Stability and Efficiency in Catalytic Wet Peroxide OxidationPublication . Baldo, Arthur P.; Bezerra, Ana Júlia B.; Silva, Adriano S.; Silva, Ana P. F.; Roman, Fernanda; Çaha, Ihsan; Bañobre-López, Manuel; Deepak, Francis Leonard; Gomes, HelderNitrophenols are persistent organic pollutants that pose serious environmental and health risks due to their toxic and lipophilic nature. Their persistence arises from strong aromatic stability and resistance to biodegradation, while their lipophilicity facilitates bioaccumulation, exacerbating ecological and human health concerns. To address this challenge, this study focuses on the synthesis and characterization of two different types of hybrid multi-core magnetic catalysts: (i) cobalt ferrite (Co-Fe2O4), which exhibits ferrimagnetic properties, and (ii) magnetite (Fe3O4), which demonstrates close superparamagnetic behavior and is coated with a novel and less hazardous phloroglucinol–glyoxal-derived resin. This approach aims to enhance catalytic efficiency while reducing the environmental impact, offering a sustainable solution for the degradation of nitrophenols in aqueous matrices. Transmission electron microscopy (TEM) images revealed the formation of a multi-core shell structure, with carbon layer sizes of 6.6 ± 0.7 nm for cobalt ferrite and 4.2 ± 0.2 nm for magnetite. The catalysts were designed to enhance the stability and performance in catalytic wet peroxide oxidation (CWPO) processes using sol–gel and solution combustion synthesis methods, respectively. In experiments of single-component degradation, the carbon-coated cobalt ferrite (CoFe@C) catalyst achieved 90% removal of 2-nitrophenol (2-NP) and 96% of 4-nitrophenol (4-NP), while carbon-coated magnetite (Fe3O4@C) demonstrated similar efficiency, with 86% removal of 2-NP and 94% of 4-NP. In the multi-component system, CoFe@C exhibited the highest catalytic activity, reaching 96% removal of 2-NP, 99% of 4-NP, and 91% decomposition of H2O2. No leaching of iron was detected in the coated catalysts, whereas the uncoated materials exhibited similar and significant leaching (CoFe: 5.66 mg/L, Fe3O4: 12 mg/L) in the single- and multi-component system. This study underscores the potential of hybrid magnetic catalysts for sustainable environmental remediation, demonstrating a dual-function mechanism that enhances catalytic activity and structural stability.
- Polyolefin and Polystyrene‐Derived Carbon Nanotubes: Catalysts for Oxidative Desulfurization Under a Biphasic SystemPublication . Roman, Fernanda; Batista, Maria C.; Silva, Adriano S.; Bezerra, Ana Júlia Briganti; Tuesta, Jose L. de Diaz de; Mambrini, Raquel V.; Silva, Adrián M. T.; Faria, Joaquim L.; Gomes, HelderThe conversion of plastic solid waste into carbon nanotubes (CNTs) via chemical vapor deposition (CVD) and the effectiveness of these CNTs as catalysts for oxidative desulfurization (ODS) of a simulated fuel were investigated. The primary focus is on the use of CNTs synthesized from various polymer sources, including polyolefins and polystyrene (PS), to remove sulfur compounds using hydrogen peroxide (H 2 O2 ) as an oxidant. The surface modification of CNTs by using acids (H2 SO4 or HNO3 ), the influence of the carbon feedstock (polyolefins vs PS), the use of co-catalysts, and the effect of the extractant phase were all evaluated on the oxidative removal of dibenzothiophene from a simulated fuel. Results revealed that CNTs derived from polyolefins displayed higher desulfurization efficiency (up to 77% in 8 h), with nitric acid-treated CNTs showing the best performance under oil-water biphasic systems. Replacing water with acetonitrile and adding a co-catalyst (formic acid) resulted in a desulfurization of 91% in 2 h of reaction. Under certain conditions, C─S bond cleav-age was observed. This research contributes to the valorization of plastic solid waste and the reduction of atmospheric pollution, promoting circular economy practices and environmental sustainability.
- Simultaneous removal of o-and p-nitrophenol from contaminated water by wet peroxide oxidation using carbon-coated magnetic ferrite as catalystPublication . Dias, Arnaldo; Silva, Adriano S.; Silva, Ana P. F.; Roman, Fernanda; Díaz de Tuesta, Jose Luis; Oliveira, Jéssica; Ferrari, Ana M.; Lenzi, Giane G.; Gomes, Helder; Oliveira, JessícaGroundwater is the most common source of drinking water worldwide and is currently facing contamination problems with the discharge of pollutants into aquatic systems through different means, namely through municipal, industrial and agricultural activities. Contaminants, such as herbicides, pharmaceuticals, phenolic compounds and personal care products are not removed by conventional treatments from wastewater treatment plants, leading to their accumulation in the environment. In this regard, o-nitrophenol (o-NP) and p-nitrophenol (p-NP), commonly used as raw materials in chemical and pharmaceutical engineering, represent a severe risk to humans and aquatic life, leading to the necessity to properly treat wastewaters containing these contaminants before discharge into the aquatic environment. Catalytic wet peroxide oxidation (CWPO) showed promising results for removing nitrophenols from wastewater in previous works. In this technology, H2O2 is used as an oxidant, and its interaction with a suitable catalyst leads to the formation of hydroxyl radicals under determined conditions already established in literature (pH and temperature have a strong influence) [1]. Typical catalysts employed have a transition metal in its structure. Carbon-based catalysts also have activity in this technology, mostly ascribed to the electronic properties of the carbonaceous surface. Furthermore, carbon-coated metal oxide materials (hybrid) have also demonstrated potential applications in CWPO. Those structures combine carbon and metal activities with the advantage of protecting the metal core from leaching, increasing the efficiency and stability of the catalysts.
- Assisted hydrothermal carbonization of agroindustrial byproducts as effective step in the production of activated carbon catalysts for wet peroxide oxidation of micro-pollutantsPublication . Díaz de Tuesta, Jose Luis; Saviotti, Marcus Chamahum; Roman, Fernanda; Pantuzza, Gabriel F.; Sartori, Hiram J.F.; Shinibekova, Assem A.; Kalmakhanova, Marzhan; Massalimova, Bakytgul Kabykenovna; Pietrobelli, Juliana Martins Teixeira; Lenzi, Giane G.; Gomes, HelderThis work deals with the valorisation of bagasse of sugarcane – BC, bagasse of malt – BM and seed of chia – SC, through its transformation into pyrochars, hydrochars and activated carbons (ACs) by pyrolysis, hydrothermal carbonization (HTC) and sequential HTC and pyrolysis, respectively. The HTC process was carried out in the presence of H2O, FeCl3 and H2SO4 solutions. The materials resulting by HTC in the presence of FeCl3 revealed the highest burn-off, but the contents of carbon released into the liquid phase, measured as total organic carbon, and to the gaseous phase, determined by carbon balance, depend strongly on the carbon precursor. In this sense, BC generates more volatile organic compounds (up to 34% of the initial carbon content), followed by BM (< 15%) and SC (< 5%) in their HTC and pyrolysis (70%). The pyrochars, hydrochars and ACs prepared from BC also show the highest specific surface areas (SBET < 447 m2⋅g-1) when compared to the specific surface areas of the materials prepared from BM and SC. The carbon-based materials prepared with FeCl3 show the highest catalytic activity, but iron leaching into solution is observed. On the other hand, the materials prepared with H2SO4 show high activity, enabling its application in successive cycles and the complete degradation of caffeine in concentrations ranging from 1 to 100 mg⋅L-1, after 5–60 min of reaction.
- Plastic waste-derived carbon nanotubes: Influence of growth catalyst and catalytic activity in CWPOPublication . Roman, Fernanda; Silva, Adriano S.; Díaz de Tuesta, Jose Luis; Baldo, Arthur Pietrobon; Lopes, Jéssica Paula Marim; Gonçalves, Giane; Pereira, Ana I.; Praça, Paulo; Silva, Adrián; Faria, Joaquim; Bañobre-López, Manuel; Gomes, HelderLow-density polyethylene (LDPE) was used in this work to grow carbon nanotubes (CNTs) by chemical vapor deposition (CVD) over catalysts based on Ni, Fe and Al, synthesized either by co-precipitation (C) or wet impregnation (I) methods, with CNT yields in the range of 16–33 %. The morphology of the CNTs was directly influenced by the route used for the CVD catalyst synthesis, with co-precipitation-derived CVD catalysts resulting in CNT samples with curly walls. CNTs were purified with H2SO4 (10–50 wt.%) to remove attached metal particles. All synthesized materials (CVD-catalysts, as-synthesized CNTs, and purified CNTs) were tested as catalysts in the catalytic wet peroxide oxidation (CWPO) of paracetamol (PCM), chosen as a model pharmaceutical compound. Removals of 100 % of PCM in 8 h and 71 % of total organic carbon (TOC) in 24 h were achieved, with an H2O2 consumption efficiency of 76 % in 24 h for purified CNT (CNT@NiFeAl-C-P). The same CVD-catalyst (NiFeAl-C) was used to grow CNTs using real LDPE waste, and it was tested under the same reaction conditions, resulting in a PCM and TOC abatement of 90 % and 65 %, respectively. The synthesis of CNTs using LDPE waste was a good alternative, given the environmental benefits associated with its reintroduction into the economic cycle as a material with higher value than initially (upcycling).
- Degradation of paracetamol by wet peroxide oxidation using carbon nanotubes synthesized from plastic solid wastePublication . Sanches, Lucas Fenato; Silva, Adriano S.; Roman, Fernanda; Díaz de Tuesta, Jose Luis; Silva, Fernando Alves; Pereira, Ana I.; Silva, Adrián; Gomes, HelderWithin increased production and economic/social dependence of plastic utilization, an environmental problem has also emerged. In this scenario, plastic solid waste (PSW) recycling/management/recovery has become a problem of public concern, with a global generation estimated at 150 million tonnes per year. Materials produced from PSW can be classified as primary (performance/characteristics equivalent to virgin plastic), secondary (performance’s requirement lower than the original application), tertiary (PSW used as feedstock for the generation of chemicals and fuels), and quaternary (energy recovery via incineration) recycled materials [1]. For instance, pyrolysis of PSW has been extensively used for the thermochemical conversion of useless PSW into oil, gas, and carbon materials, thus classified as terciary recycled material.
- Selective oxidation of 4-nitrophenol with H2O2 in a biphasic system by janus-like carbon nanotubesPublication . Sanches, Flávia Kim; Roman, Fernanda; Silva, Adriano S.; Díaz de Tuesta, Jose Luis; Silva, Adrián; Faria, Joaquim; Machado, Bruno; Serp, Philippe; Marin, Pricila; Gomes, HelderThe use of petroleum-based products has increased drastically with the increase in population, resulting in the deposition of oily products in aquatic systems. It is estimated that for each ton of petroleum that undergoes refinement processes, between 0.5 and 1 ton of oily wastewaters are generated, bearing an oil concentration that may reach 40 g L-1 [1,2]. Hazardous pollutants dissolved both in oily and aqueous phases may also be found in those oily wastewaters [3], hindering their treatment through conventional processes. Furthermore, the oil phase is, in some cases, an added-value product, and its degradation results in economic losses. Thus, the development of processes that allow the removal of hazardous contaminants from oily and aqueous phases, providing an opportunity for recovering both phases, should be advantageous [3]. This work deals with the selective removal of a hazardous compound (4-nitrophenol, 4-NP) from a simulated oily wastewater (2,2,4-trimethylpentane:water = 10:90 v/v) by an oxidative process considering H2O2 as oxidant and amphiphilic Janus-like carbon nanotubes as catalysts. Amphiphilic catalysts were selected since they should present advantages in this process due to their ability to interact with both aqueous and oily compounds and phases [4]
- Selective denitrification of simulated oily wastewater by oxidation using Janus-structured carbon nanotubesPublication . Roman, Fernanda; Díaz de Tuesta, Jose Luis; Sanches, Flávia Kim; Silva, Adriano S.; Marin, Pricila; Machado, Bruno F.; Serp, Philippe; Pedrosa, Marta; Silva, Adrián; Faria, Joaquim; Gomes, HelderThe intense industrial development has resulted in several consequences for human and environmental health, including the increased discharge of oily products in water bodies. Oily products are widely used in industry, often bearing an associated high cost. Finding alternatives to treat oily wastewater aiming at recovering oily and water phases is an approach allowing recovery of products of economic interest. In this work, Janus-like carbon nanotubes (CNTs) were synthesized by varying the feed time of acetonitrile and ethylene, respectively, as nitrogen/ carbon and carbon precursors in a chemical vapor deposition (CVD) approach. The CVD approach allowed the synthesis of completely undoped, completely doped and partially doped CNTs with a Janus structure. The CNTs were then tested as catalysts for the selective oxidation of 4-nitrophenol (4-NP) contained in a simulated oily wastewater (2,2,4-trimethylpentane/water (O/W) = 1:9, volume basis) by catalytic wet peroxide oxidation (CWPO). The CWPO experiments were conducted for 24 h, 80 ◦C, 2.5 g L-1 of catalyst, and the stoichiometric concentration of H2O2 (3.6 g L-1) for the degradation of 4-NP (1 g L-1). The same conditions were kept for experiments conducted under a biphasic system. The catalysts bearing a Janus-like structure were demonstrated to be more effective in CWPO experiments in aqueous-only and biphasic systems for the abatement of 4-NP.
- Hybrid multi-core shell magnetic nanoparticles for wet peroxide oxidation of paracetamol: application in synthetic and real matricesPublication . Silva, Adriano S.; Roman, Fernanda; Dias, Arnaldo; Díaz de Tuesta, Jose Luis; Narcizo, Alexandre; Silva, Ana P. F.; Çaha, Ihsan; Deepak, Francis Leonard; Bañobre-López, Manuel; Ferrari, Ana M.; Gomes, HelderClean water availability is becoming a matter of global concern in the last decades. The responsible entities for wastewater treatment do not have the proper facilities to deal with a wide range of pollutants. Special attention should be given to emerging contaminants, whose presence in water bodies may cause adverse effects on the aquatic ecosystem and human health. Most studies in the literature do not consider the development of their solution in real matrices, which can hinder the applicability of the explored alternative in the real scenario. Therefore, in this work, we demonstrate the applicability of hybrid magnetic nanoparticles for removing paracetamol (PCM) from simulated and real matrices by catalytic wet peroxide oxidation (CWPO). To achieve carbon coating, the nanoparticles were prepared via the traditional route (resorcinol/formaldehyde, CoFe@CRF). A new methodology was also considered for synthesizing thin-layered carbon-coated magnetic nanoparticles (phloroglucinol/ glyoxalic acid, CoFe@CPG). TEM images revealed a multi-core shell structure formation, with an average carbon layer size of 7.8 ± 0.5 and 3.2 ± 0.3 nm for resorcinol/formaldehyde and phloroglucinol/ glyoxalic acid methodology, respectively. Screening the materials’ activity for PCM oxidation by CWPO revealed that the nanoparticle prepared by phloroglucinol/glyoxalic acid methodology has higher performance for the degradation of PCM, achieving 63.5% mineralization after 24 h of reaction, with similar results for more complex matrices. Iron leaching measured at the end of all reactions has proven that the carbon layer protects the core against leaching.