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Chemisorption Mechanism of DNA on Mg/Fe Layered Double Hydroxide Nanoparticles: Insights into Engineering Effective SiRNA Delivery Systems Mingsheng Lu, Zhi Shan, Kori Andrea, Bruce MacDonald, Stefanie Beale , Dennis Everett Curry, Li Wang, Shujun Wang, Ken D. Oakes, Craig Bennett, Wen Hui Wu, and Xu Zhang Langmuir, Just Accepted Manuscript • DOI: 10.1021/acs.langmuir.5b04643 • Publication Date (Web): 26 Feb 2016 Downloaded from http://pubs.acs.org on March 4, 2016
Just Accepted “Just Accepted” manuscripts have been peer-reviewed and accepted for publication. They are posted online prior to technical editing, formatting for publication and author proofing. The American Chemical Society provides “Just Accepted” as a free service to the research community to expedite the dissemination of scientific material as soon as possible after acceptance. “Just Accepted” manuscripts appear in full in PDF format accompanied by an HTML abstract. “Just Accepted” manuscripts have been fully peer reviewed, but should not be considered the official version of record. They are accessible to all readers and citable by the Digital Object Identifier (DOI®). “Just Accepted” is an optional service offered to authors. Therefore, the “Just Accepted” Web site may not include all articles that will be published in the journal. After a manuscript is technically edited and formatted, it will be removed from the “Just Accepted” Web site and published as an ASAP article. Note that technical editing may introduce minor changes to the manuscript text and/or graphics which could affect content, and all legal disclaimers and ethical guidelines that apply to the journal pertain. ACS cannot be held responsible for errors or consequences arising from the use of information contained in these “Just Accepted” manuscripts.
Langmuir is published by the American Chemical Society. 1155 Sixteenth Street N.W., Washington, DC 20036 Published by American Chemical Society. Copyright © American Chemical Society. However, no copyright claim is made to original U.S. Government works, or works produced by employees of any Commonwealth realm Crown government in the course of their duties.
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Langmuir
Chemisorption Mechanism of DNA on Mg/Fe Layered Double Hydroxide Nanoparticles: Insights into Engineering Effective SiRNA Delivery Systems Mingsheng Lua, Zhi Shanb, Kori Andreab, Bruce MacDonaldb, Stefanie Beale c, Dennis E. Curryb,d , Li Wange, Shujun Wangf, Ken D. Oakesb,g, Craig Bennettc, Wenhui Wua*, and Xu Zhangb* a
College of Food Science & Technology, Shanghai Ocean University, Shanghai, 201306, China.
b
Verschuren Centre for Sustainability in Energy & the Environment, Cape Breton University, 1250 Grand Lake Rd, Sydney, Nova Scotia, B1P 6L2, Canada. c
Department of Physics, Acadia University, Wolfville, Nova Scotia, B4P 2R6, Canada.
d
Department of Biology, University of Waterloo, ON, N2L3G1, Canada
e
College of Food Science and Biotechnology, Zhejiang Gongshang University, Hangzhou, 310018, China
f
Jiangsu Marine Resources Development Research Institute, Lianyungang, 222001, China.
g
Department of Biology, Cape Breton University, 1250 Grand Lake Rd, Sydney, Nova Scotia, B1P 6L2, Canada.
________________________________________
ABSTRACT: Layered double hydroxide nanoparticles (LDH NPs) have attracted interest as an effective gene delivery vehicle in biomedicine. Recent advances in clinic trials have demonstrated the efficacy of Mg/Fe LDHs for hyperphosphatemia treatment, but their feasibility for gene delivery has not been systematically evaluated. As a starting point, we aimed to study the interaction between oligo-DNAs and Mg/Fe LDH nanoparticles. Our investigation revealed the chemisorption mechanism of DNA on Mg/Fe LDH surfaces, wherein the phosphate backbone of the DNA polymer coordinates with the metal cations of the LDH lattice via ligandexchange process. This mechanistic insight may facilitate future gene delivery applications using Mg/Fe LDH NPs.
ACS Paragon Plus Environment
Langmuir
1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60
INTRODUCTION Layered double hydroxides (LDHs), a group of anionic inorganic nanocrystals consisting of cationic brucite-like layers and interlayer counter anions, have demonstrated their utility as novel drug- and gene-delivery vehicles due to their excellent biocompatibility, high loading capacity, efficient cellular uptake, and pH-based controlled release1-21. The most studied LDH vehicle for delivery of genes such as plasmid DNAs and oligo-DNA mimics of siRNA is magnesium aluminum hydroxide (Mg/Al LDH)3-4,17,21-29, which can be described by the formula of [Mg (Ⅱ)1-x Al (Ⅲ)x (OH)2]x+(An-)x/n·yH20, where Mg (Ⅱ) and Al (Ⅲ) form the cationic layers and Anserve as interlayer guest anions, and where 0
Article
Chemisorption Mechanism of DNA on Mg/Fe Layered Double Hydroxide Nanoparticles: Insights into Engineering Effective SiRNA Delivery Systems Mingsheng Lu, Zhi Shan, Kori Andrea, Bruce MacDonald, Stefanie Beale , Dennis Everett Curry, Li Wang, Shujun Wang, Ken D. Oakes, Craig Bennett, Wen Hui Wu, and Xu Zhang Langmuir, Just Accepted Manuscript • DOI: 10.1021/acs.langmuir.5b04643 • Publication Date (Web): 26 Feb 2016 Downloaded from http://pubs.acs.org on March 4, 2016
Just Accepted “Just Accepted” manuscripts have been peer-reviewed and accepted for publication. They are posted online prior to technical editing, formatting for publication and author proofing. The American Chemical Society provides “Just Accepted” as a free service to the research community to expedite the dissemination of scientific material as soon as possible after acceptance. “Just Accepted” manuscripts appear in full in PDF format accompanied by an HTML abstract. “Just Accepted” manuscripts have been fully peer reviewed, but should not be considered the official version of record. They are accessible to all readers and citable by the Digital Object Identifier (DOI®). “Just Accepted” is an optional service offered to authors. Therefore, the “Just Accepted” Web site may not include all articles that will be published in the journal. After a manuscript is technically edited and formatted, it will be removed from the “Just Accepted” Web site and published as an ASAP article. Note that technical editing may introduce minor changes to the manuscript text and/or graphics which could affect content, and all legal disclaimers and ethical guidelines that apply to the journal pertain. ACS cannot be held responsible for errors or consequences arising from the use of information contained in these “Just Accepted” manuscripts.
Langmuir is published by the American Chemical Society. 1155 Sixteenth Street N.W., Washington, DC 20036 Published by American Chemical Society. Copyright © American Chemical Society. However, no copyright claim is made to original U.S. Government works, or works produced by employees of any Commonwealth realm Crown government in the course of their duties.
Page 1 of 25
1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60
Langmuir
Chemisorption Mechanism of DNA on Mg/Fe Layered Double Hydroxide Nanoparticles: Insights into Engineering Effective SiRNA Delivery Systems Mingsheng Lua, Zhi Shanb, Kori Andreab, Bruce MacDonaldb, Stefanie Beale c, Dennis E. Curryb,d , Li Wange, Shujun Wangf, Ken D. Oakesb,g, Craig Bennettc, Wenhui Wua*, and Xu Zhangb* a
College of Food Science & Technology, Shanghai Ocean University, Shanghai, 201306, China.
b
Verschuren Centre for Sustainability in Energy & the Environment, Cape Breton University, 1250 Grand Lake Rd, Sydney, Nova Scotia, B1P 6L2, Canada. c
Department of Physics, Acadia University, Wolfville, Nova Scotia, B4P 2R6, Canada.
d
Department of Biology, University of Waterloo, ON, N2L3G1, Canada
e
College of Food Science and Biotechnology, Zhejiang Gongshang University, Hangzhou, 310018, China
f
Jiangsu Marine Resources Development Research Institute, Lianyungang, 222001, China.
g
Department of Biology, Cape Breton University, 1250 Grand Lake Rd, Sydney, Nova Scotia, B1P 6L2, Canada.
________________________________________
ABSTRACT: Layered double hydroxide nanoparticles (LDH NPs) have attracted interest as an effective gene delivery vehicle in biomedicine. Recent advances in clinic trials have demonstrated the efficacy of Mg/Fe LDHs for hyperphosphatemia treatment, but their feasibility for gene delivery has not been systematically evaluated. As a starting point, we aimed to study the interaction between oligo-DNAs and Mg/Fe LDH nanoparticles. Our investigation revealed the chemisorption mechanism of DNA on Mg/Fe LDH surfaces, wherein the phosphate backbone of the DNA polymer coordinates with the metal cations of the LDH lattice via ligandexchange process. This mechanistic insight may facilitate future gene delivery applications using Mg/Fe LDH NPs.
ACS Paragon Plus Environment
Langmuir
1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 25 26 27 28 29 30 31 32 33 34 35 36 37 38 39 40 41 42 43 44 45 46 47 48 49 50 51 52 53 54 55 56 57 58 59 60
INTRODUCTION Layered double hydroxides (LDHs), a group of anionic inorganic nanocrystals consisting of cationic brucite-like layers and interlayer counter anions, have demonstrated their utility as novel drug- and gene-delivery vehicles due to their excellent biocompatibility, high loading capacity, efficient cellular uptake, and pH-based controlled release1-21. The most studied LDH vehicle for delivery of genes such as plasmid DNAs and oligo-DNA mimics of siRNA is magnesium aluminum hydroxide (Mg/Al LDH)3-4,17,21-29, which can be described by the formula of [Mg (Ⅱ)1-x Al (Ⅲ)x (OH)2]x+(An-)x/n·yH20, where Mg (Ⅱ) and Al (Ⅲ) form the cationic layers and Anserve as interlayer guest anions, and where 0
