Carbon–based metal organic framework composite adsorbent for the removal of contaminants of emerging concern from water

dc.contributor.advisor Hernández Maldonado, Arturo J. Muñoz Senmache, Juan Carlos College of Engineering en_US
dc.contributor.committee Méndez Román, Rafael
dc.contributor.committee Suleiman Rosado, David
dc.contributor.committee Curet Arana, María C.
dc.contributor.department Department of Chemical Engineering en_US
dc.contributor.representative Colón, Silvestre 2021-12-13T16:00:35Z 2021-12-13T16:00:35Z 2021-11-03
dc.description.abstract For more than two decades, the presence of contaminants of emerging concern (CECs) in sources of water has attracted attention from the scientific community due to their inherent capability to produce biological undesirable effect in living organisms and the overall impact to the environment, even at very low doses. Effective remediation of CECs also remains a challenge, even with current improvements in capacity of water treatment (WT) operations to mitigate pathways associated to the exposition to humans, animals, and edible plants. Therefore, there are significant opportunities in diverse WT areas to enable CEC remediation technologies that would allow for the attainment of higher clean water standards and also to prevent further potential environmental impact. This work offers a promising alternative to remove very low concentrations of CECs from water using composites adsorbents (CMOFs) based on the confined space synthesis of metal organic frameworks (MOFs) inside of activated carbon (AC) pores. This arrangement could offer a synergistic effect produced by the superior hydrophobicity from AC, which is providing not just hydrophobic interactions, but also an effective barrier to diminish water competition for the adsorption active sites given by the MOFs. The resulting CMOFs composite materials were tested in the removal of a specific target of CECs from water in both single- and multi-component matrix. These CECs were chosen not only by their occurrence in the environment, but also exhibit a considerable range of molecular structure and physio-chemical properties, and these include carbamazepine (CBZ), caffeine (CFN), naproxen (NPX), clofibric acid (CA), and metabolites such as salicylic acid (SA), 10,11-epoxycarbamazepine (Ep-CBZ), paraxanthine (PXN), and o-desmethylnaproxen (o-DMN). The latter three result from partial decomposition of primary molecules CBZ, CFN, and NPX, respectively. In addition, this work also evaluated the effect of the chemical environment constitution (i.e., organic linker and metal node) of the MOF over the affinity toward CECs. The obtained results showed that the overall adsorption capacity for the tested materials increases as follow: MIL-100Fe < MIL-100Cr < MIL-101Cr < CMOF-101Cr < AC-treated with acids < CMOF-100Fe < AC < CMOF-100Cr. These results have proven that getting simultaneous hydrophobicity and available active adsorption sites has a tremendous impact in the adsorption capacity of CECs specially in those molecules who remain without ionic charge during the process (i.e., CBZ and Ep-CBZ). Finally, this work has also demonstrated a suitable regeneration via thermal treatment to ensure multi cycle adsorption processes without affecting the overall uptake capacity en_US
dc.description.graduationSemester Spring en_US
dc.description.graduationYear 2022 en_US
dc.description.note This dissertation contains portions that were published by the author in the ACS Applied Nano Materials journal from ACS Publications, Environmental Pollutants and Bioavailability journal from Taylor and Francis Online, and Elsevier inc.; Abstracts in dissertation are both in English en_US
dc.description.sponsorship National Science Foundation (NSF), Center for the Sustainable Water, Energy and Food Nexus (SusWEF) under grant No. OIA –Research Infrastructure Improvement – 1632824; NSSAL Research en_US
dc.language.iso en en_US
dc.rights.holder (c) 2021 Juan Carlos Muñoz Senmache en_US
dc.subject Metal Organic Frameworks en_US
dc.subject Confined Space Synthesis en_US
dc.subject Contaminants of Emerging Concern en_US
dc.subject Adsorption en_US
dc.subject Water Treatment en_US
dc.subject.lcsh Emerging contaminants in water en_US
dc.subject.lcsh Hazardous waste site remediation en_US
dc.subject.lcsh Metal-organic frameworks en_US
dc.subject.lcsh Carbon--Absorption and adsorption en_US
dc.subject.lcsh Water--Purification--Adsorption en_US
dc.subject.lcsh Soil water repellency en_US
dc.title Carbon–based metal organic framework composite adsorbent for the removal of contaminants of emerging concern from water en_US
dc.type Dissertation en_US
dspace.entity.type Publication Chemical Engineering en_US Ph.D. en_US
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