Engineered nanomaterials are capable of solving challenges in industries important to society such as energy, agriculture, and health care. Antimicrobial silver nanoparticles (AgNPs) are the most widely used nanoparticles by number of commercial products in commerce today. However, the increased introduction of AgNPs in industrial applications may lead to discharge of persistent nanoparticles in the environment and undesired impacts on living organisms. This dissertation will present a new class of antimicrobial environmentallybenign nanoparticles (EbNPs) designed with green chemistry principles, which can serve as highly efficient microbicide substitutes of the AgNPs. The EbNP core is made of biodegradable lignin, and is infused with an optimal amount of silver ions.
We report on the fabrication of environmentally benign nanoparticles (EbNPs) using two types of lignin precursors with simple, inexpensive, and non-toxic processes, (i) by employing a solvent exchange precipitation method at room temperature and (ii) by applying an environmentally friendly water-based acid precipitation method. The synthesis of Organosolv (High Purity Lignin) nanoparticles via antisolvent flash precipitation method in water resulted in particles in the size range of 45 to 250 nm in diameter. We investigate the synthesis parameters of Kraft (Indulin AT) lignin nanoparticles by flash precipitation induced by pH drop in ethylene glycol. Furthermore, we evaluate the ionic strength and pH stability of both lignin nanoparticle suspensions and highlight differences in the systems. After silver ion infusion of Indulin AT nanoparticles followed by surface modification, we show that the EbNPs exhibit higher antimicrobial activity towards Gram-negative human pathogens Escherichia coli and Pseudomonas aeruginosa and Gram-positive human pathogens Staphylococcus epidermidis in direct comparison with silver nanoparticles and silver nitrate solution, and that the particles are effective against quaternary ammonium resistant Ralstonia bacteria. The enhanced antimicrobial action is due to highly-biocidal silver ions released from the EbNP matrix at the cell. High-throughput bioactivity screening using mammalian cell and zebrafish embryo assays performed in collaboration with the U.S. Environmental Protection Agency did not reveal increased safety concerns of the EbNPs, when compared to equivalent amount of AgNPs or AgNO3 solution.
The silver ion functionalized EbNPs exhibit broad spectrum microbicide action and are capable of neutralizing common gram-negative human pathogens as well as quaternary amineresistant bacteria, while using ten times less silver when compared with conventional AgNPs and AgNO3 aqueous solution. We envisage that the overall environmental impact of silver ion functionalized EbNPs is likely to be significantly smaller when compared to AgNPs. As more general impact, the approach of engineering environmentally-benign lignin-core nanoparticles with matching functionality to persistent nanoparticles illustrates how green chemistry principles including atom economy, use of renewable feedstocks, and design for degradation can be applied to design more sustainable nanomaterials with increased functionality and decreased environmental footprint.
|Advisor:||Velev, Orlin D., Spontak, Richard J.|
|School:||North Carolina State University|
|School Location:||United States -- North Carolina|
|Source:||DAI-B 78/08(E), Dissertation Abstracts International|
|Subjects:||Chemical engineering, Nanotechnology|
|Keywords:||Antimicrobials, Colloids, Lignin nanoparticles, Silver nanoparticles|
Copyright in each Dissertation and Thesis is retained by the author. All Rights Reserved
The supplemental file or files you are about to download were provided to ProQuest by the author as part of a
dissertation or thesis. The supplemental files are provided "AS IS" without warranty. ProQuest is not responsible for the
content, format or impact on the supplemental file(s) on our system. in some cases, the file type may be unknown or
may be a .exe file. We recommend caution as you open such files.
Copyright of the original materials contained in the supplemental file is retained by the author and your access to the
supplemental files is subject to the ProQuest Terms and Conditions of use.
Depending on the size of the file(s) you are downloading, the system may take some time to download them. Please be