Theses and Dissertations

Issuing Body

Mississippi State University

Advisor

Mlsna, Todd E.

Committee Member

Mlsna, Todd E.

Committee Member

Wipf, David O.

Committee Member

Emerson, Joseph P.

Committee Member

Mlsna, Debra Ann; Pittman, Charles U. Jr.

Date of Degree

4-30-2021

Original embargo terms

Complete embargo for 2 years

Document Type

Dissertation - Open Access

Major

Chemistry

Degree Name

Doctor of Philosophy

College

College of Arts and Sciences

Department

Department of Chemistry

Abstract

Heavy metals, oxyanions (NO3-, PO4-), pharmaceuticals, and dyes in aquatic environments are inevitable economic and health concerns. Ingestion of these contaminants, even in trace amounts, causes long and short-term serious threats to human health. Conventional pollutant mitigation strategies can be costly or ineffective. Due to high efficiency, simplicity, low price, adsorbent reuse, and pollutant (e.g., phosphates) recovery, adsorption has been widely used for wastewater purification. Many efficient, environmentally compatible, and cost-effective sorbents have been successfully applied in environmental remediation. Chapter I is about characterization of graphene-coated pinewood biochar hybrids and evaluation of their copper removal performances. Here, we synthesized three types of pinewood biochar-graphene composites consisting of three different graphene precursors and compared their aqueous Cu2+ removal performances against raw pinewood biochar. To the best of our knowledge, no previous work has characterized the copper decontamination by graphene-biochar hybrids. Chapter II is about thermally- and chemically-treated lignite adsorbents for phosphate remediation. We engineered a cost efficient lignite system with co-precipitated Ca2+/Mg2+ followed by pyrolysis at 600 ⁰C to remediate aqueous phosphates. Micro-sized surface deposited oxide/hydroxide/carbonate particles promoted phosphate uptake of Ca2+/Mg2+-modified-lignite by 31 and 72 times, compared to thermally treated lignite (w/o a chemical treatment) and the raw lignite, respectively. The exhausted adsorbent can act as a slow-release fertilizer, which is comparable with commercial phosphate fertilizers. Chapter III is about synthesis of activated lignite [A-L], Ca2+-modified lignite [Ca-L], and Fe3O4 nanoparticle-loaded activated lignite (Fe3O4-A-L) for phosphate remediation. Even though A-L has a very high surface area (2854 m2/g), it did not achieve much phosphate sorption. Ca-L phosphate uptake was highest due to the high concentrations of surface deposited CaCO3, CaO, and Ca(OH)2. A pH-independent (from pH 5 to 9) phosphate removal was reported by highly basic Ca-L. However, the Ca2+ leaching was highest at pH 5. Precipitation of Ca2+ phosphates/hydrophosphates is the major phosphate removal mechanism of Ca-L. Fe3O4 and Fe2O3 sites of Fe3O4-A-L enhanced phosphate adsorption capacity, 8-fold versus A-L (67.6 mg/g vs 8.0 mg/g at 25 ºC). Fe3O4-A-L remediated phosphates via inner-sphere surface complexation and precipitation.

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