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Adsorption of oligo-DNA on Magnesium Aluminum Layered Double Hydroxide Nanoparticle Surfaces: Mechanistic Implication to Gene Delivery Kori A. Andrea, Li Wang, Andrew J. Carrier, Melanie Campbell, Margaret Buhariwalla, MacKenzi Mutch, Stephanie L. MacQuarrie, Craig Bennett, Martin Mkandawire, Ken D. Oakes, Mingsheng Lu, and Xu Zhang Langmuir, Just Accepted Manuscript • DOI: 10.1021/acs.langmuir.6b04172 • Publication Date (Web): 04 Apr 2017 Downloaded from http://pubs.acs.org on April 5, 2017
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Langmuir
Adsorption of oligo-DNA on Magnesium Aluminum Layered Double Hydroxide Nanoparticle Surfaces: Mechanistic Implication to Gene Delivery Kori A. Andrea,a Li Wang,b* Andrew J. Carrier,c Melanie Campbell,a Margaret Buhariwalla,d MacKenzi Mutch,a Stephanie L. MacQuarrie,c Craig Bennett,d Martin Mkandawire,a Ken Oakes,a Mingsheng Lu,e* and Xu Zhanga* a
Verschuren Center for Sustainability in Energy and the Environment, Cape Breton University, 1250 Grand Lake Rd, Sydney, Nova Scotia, B1P 6L2, Canada. b
College of Food Science and Biotechnology, Zhejiang Gongshang University, Hangzhou, Zhejiang 310018, People’s Republic of China.
c
Department of Chemistry, Cape Breton University, 1250 Grand Lake Rd, Sydney, Nova Scotia, B1P 6L2, Canada. d
Department of Physics, Acadia University, Wolfville, Nova Scotia, B4P 2R6, Canada.
e
College of Marine Life and Fisheries, Huaihai Institute of Technology, Lianyungang, Jiang Su, 222005, People’s Republic of China.
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Magnesium aluminum layered double hydroxide nanoparticles (LDH NPs) are promising drug delivery vehicles for gene therapy, particularly for siRNA interference; however, the interactions between oligo-DNA and LDH surfaces have not been adequately elucidated. Through a mechanistic study, oligo-DNA appears to initially rapidly bind strongly to the LDH outer surfaces through interactions with their phosphate backbones via ligand exchange with OH- on Mg2+ centers and electrostatic forces with Al3+. These initial interactions might precede diffusion into interlayer spaces and this knowledge can be used to design better gene therapy delivery systems.
Introduction Layered double hydroxide nanoparticles (LDH NPs) are 2D nanocrystals with cationic layers and sandwiched counterions.1–7 These nanoparticles are interesting gene and drug delivery materials because they have high loading capacity and cellular uptake, are biocompatible, and release their payload in a pH-dependent mechanism, e.g., at tumor sites. 8–10 Magnesium aluminum LDH NPs are widely studied for gene delivery including plasmid DNA, small interfering RNA (siRNA), and oligo-DNA siRNA mimics.11,12 Magnesium aluminum LDHs have the empirical formula [Mg1-x Alx (OH)2 ]x+[Xn-]x/n ·yH2 O, where 0
