Alendronate-Anionic Clay Nanohybrid for Enhanced Osteogenic Proliferation and Differentiation

PIAO HUIYAN,김명훈,Meiling Cui,최고은,최진호 대한의학회 2019 Journal of Korean medical science Vol.34 No.5

Background: Alendronate (AL), a drug for inhibiting osteoclast-mediated bone- resorption, was intercalated into an inorganic drug delivery nanovehicle, layered double hydroxide (LDH), to form a new nanohybrid, AL-LDH, with 1:1 heterostructure along the crystallographic C-axis. Based on the intercalation reaction strategy, the present AL-LDH drug delivery system (DDS) was realized with an enhanced drug efficacy of AL, which was confirmed by the improved proliferation and osteogenic differentiation of osteoblast-like cells (MG63). Methods: The AL-LDH nanohybrid was synthesized by conventional ion-exchange reaction and characterized by powder X-ray diffraction (PXRD), high-resolution transmission electron microscopy (HR-TEM), and Fourier transform infrared (FT-IR) spectroscopy. Additionally, in vitro efficacy tests, such as cell proliferation and alkaline phosphatase (ALP) activity, were analyzed. Results: The AL was successfully intercalated into LDH via ion-exchange reaction, and thus prepared AL-LDH DDS was X-ray single phasic and chemically well defined. The accumulated AL content in MG63 cells treated with the AL-LDH DDS nanoparticles was determined to be 10.6-fold higher than that within those treated with the intact AL after incubation for 1 hour, suggesting that intercellular permeation of AL was facilitated thanks to the hybridization with drug delivery vehicle, LDH. Furthermore, both in vitro proliferation level and ALP activity of MG63 treated with the present hybrid drug, AL-LDH, were found to be much more enhanced than those treated with the intact AL. This is surely due to the fact that LDH could deliver AL drug very efficiently, although LDH itself does not show any effect on proliferation and osteogenic differentiation of MG63 cells. Conclusion: The present AL-LDH could be considered as a promising DDS for improving efficacy of AL.

Atomic and electronic structures of graphene-decorated graphitic carbon nitride (<i>g</i>-C₃N₄) as a metal-free photocatalyst under visible-light

Jeong, Taehwan,Piao, Huiyan,Park, Sangwoo,Yang, Jae-Hun,Choi, Goeun,Wu, Qinke,Kang, Hyunmin,Woo, Hwi Je,Jung, Seong Jun,Kim, Hanchul,Shin, Bong Gyu,Kim, Youngkuk,Hwang, Euy Heon,Choy, Jin-Ho,Song, You Elsevier 2019 Applied catalysis. B, Environmental Vol.256 No.-

<P><B>Abstract</B></P> <P>Industrial demands for sustainable and renewable energy resources have inspired studies on photonic and electronic properties of graphitic-carbon nitride (<I>g</I>-C<SUB>3</SUB>N<SUB>4</SUB>) as a promising photocatalyst without precious metal. The absorption and the yield by metal-free pristine <I>g</I>-C<SUB>3</SUB>N<SUB>4</SUB> are, however, still limited with hydrogen/oxygen evolution reaction (HER/OER) mostly around ultraviolet-light. Here, we propose the graphene-decorated <I>g</I>-C<SUB>3</SUB>N<SUB>4</SUB> as a metal-free photocatalyst under visible-light, based on our atomic-scale measurements and calculations. The <I>g</I>-C<SUB>3</SUB>N<SUB>4</SUB> nanosheets on highly-oriented pyrolytic graphite (HOPG) exhibit band-gaps appropriate for visible-light absorption and work-functions tuned for band alignments to supply electrons and holes for HER/OER. Scanning probe microscopy (SPM) measurements for local density of states (LDOS) in atomic scale and work-functions in nanometer scale with ab initio calculations confirmed the various electronic transitions for each nitrogen and carbon atom in different atomic registries. The graphene-decorated <I>g</I>-C<SUB>3</SUB>N<SUB>4</SUB>, therefore, could provide a breakthrough enabling the efficient water-splitting reactions under visible-light without precious metal.</P> <P><B>Highlights</B></P> <P> <UL> <LI> The potocatalytic mechanism of graphene/<I>g</I>-C<SUB>3</SUB>N<SUB>4</SUB> was unveiled by STM measurements and DFT calculations at the atomic scale. </LI> <LI> This heterostructure has a direct and indirect band-gaps of 2.51 and 1.64 eV, representing the best fit to a visible light. </LI> <LI> Band alignments appropriate for HER and OER could be confirmed by thickness-dependent CPD measurements by KPFM and STS. </LI> </UL> </P> <P><B>Graphical abstract</B></P> <P>Summary of the research: Graphene-decorated graphitic carbon nitride (<I>g</I>-C<SUB>3</SUB>N<SUB>4</SUB>) can be a metal-free photocatalyst for hydrogen and oxygen evolution reaction (HER/OER) under visible light. Epitaxially-stacked graphene can induce an appropriate bandgap and work-function on <I>g</I>-C<SUB>3</SUB>N<SUB>4</SUB>. The role of carbon and different nitrogen atoms for bandgap and work-function modulations could be described by scanning tunneling microscopy/spectroscopy (STM/STS) measurements in atomic scale along with DFT calculations.</P> <P>[DISPLAY OMISSION]</P>

Anionic clay as the drug delivery vehicle: tumor targeting function of layered double hydroxide-methotrexate nanohybrid in C33A orthotopic cervical cancer model

Choi, Goeun,Piao, Huiyan,Alothman, Zeid A,Vinu, Ajayan,Yun, Chae-Ok,Choy, Jin-Ho DOVE MEDICAL PRESS 2016 INTERNATIONAL JOURNAL OF NANOMEDICINE Vol.11 No.-

<P>Methotrexate (MTX), an anticancer agent, was successfully intercalated into the anionic clay, layered double hydroxides to form a new nanohybrid drug. The coprecipitation and subsequent hydrothermal method were used to prepare chemically, structurally, and morphologically well-defined two-dimensional drug-clay nanohybrid. The resulting two-dimensional drug-clay nanohybrid showed excellent colloidal stability not only in deionized water but also in an electrolyte solution of Dulbecco’s Modified Eagle’s Medium with 10% fetal bovine serum, in which the average particle size in colloid and the polydispersity index were determined to be around 100 and 0.250 nm, respectively. The targeting property of the nanohybrid drug was confirmed by evaluating the tumor-to-blood and tumor-to-liver ratios of the MTX with anionic clay carrier, and these ratios were compared to those of free MTX in the C33A orthotopic cervical cancer model. The biodistribution studies indicated that the mice treated with the former showed 3.5-fold higher tumor-to-liver ratio and fivefold higher tumor-to-blood ratio of MTX than those treated with the latter at 30 minutes postinjection.</P>

Enabling Nanohybrid Drug Discovery through the Soft Chemistry Telescope

Choi, Goeun,Piao, Huiyan,Kim, Myung Hun,Choy, Jin-Ho American Chemical Society 2016 INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH - Vol.55 No.43

<P>An attempt is made to describe an emerging convergence science: 'nanomedicine'. In particular, inorganic compounds such as anionic clays, layered double hydroxides (LDHs), at nanoscale, are underlined, with regard to how they could interact with bioactive and/or drug molecules to form novel intercalative hybrid drug systems with biocompatibility, imaging and targeting functions eventually for gene and/or drug delivery. In this regard, LDHs are focused as an important inorganic biomaterial for drug and gene delivery carriers with very high additive value in the near future, especially in biomedical industries including pharmaceutical, cosmeceutical, and nutraceutical ones, compared to any other industrial applications. In this review, the drug delivery systems based on clay nanoparticles are described in terms of nanotoxicity, intercellular uptake mechanism, and intracellular trafficking pathways in vitro, and finally passive and active targeting functions in vivo. In addition, several studies highlighting recent advances in chemotherapy and gene therapy with nano LDHs are also discussed, from the viewpoint of state-of-the-art convergence technology based on nanomedicine.</P>

Synbiotic of Pediococcus acidilactici and Inulin Ameliorates Dextran Sulfate Sodium-Induced Acute Ulcerative Colitis in Mice

( Mingzhu Wang ),( Longzhou Zhang ),( Huiyan Piao ),( Yuanming Jin ),( Chengdu Cui ),( Xin Jin ),( Lianhua Cui ),( Chunri Yan ) 한국미생물생명공학회 2024 Journal of microbiology and biotechnology Vol.34 No.3

Colitis is a major gastrointestinal disease that threatens human health. In this study, a synbiotic composed of inulin and Pediococcus acidilactici (P. acidilactici) was investigated for its ability to alleviate dextran sulfate sodium (DSS)-induced colitis. The results revealed that the synbiotic, composed of inulin and P. acidilactici, attenuated the body weight loss and disease activity index (DAI) score in mice with DSS-mediated colitis. Determination of biochemical indicators found that the synbiotic increased anti-oxidation and alleviated inflammation in mice. Additionally, histopathological examination revealed that colonic goblet cell loss and severe mucosal damage in the model group were significantly reversed by the combination of inulin and P. acidilactici. Moreover, synbiotic treatment significantly reduced the levels of IL-1β, TNF-α, and IL-6 in the serum of mice. Thus, a synbiotic composed of inulin and P. acidilactici has preventive and therapeutic effects on DSS-induced colitis in mice.

Implantable multireservoir device with stimulus-responsive membrane for on-demand and pulsatile delivery of growth hormone

Lee, Seung Ho,Piao, Huiyan,Cho, Yong Chan,Kim, Se-Na,Choi, Goeun,Kim, Cho Rim,Ji, Han Bi,Park, Chun Gwon,Lee, Cheol,Shin, Chong In,Koh, Won-Gun,Choy, Young Bin,Choy, Jin-Ho National Academy of Sciences 2019 Proceedings of the National Academy of Sciences Vol.116 No.24

<P><B>Significance</B></P><P>We propose an implantable multireservoir device equipped with stimulus-responsive membrane to allow for on-demand and pulsatile drug delivery. The stimulus-responsive membrane is made of a thermosensitive polymer, POSS(MEO<SUB>2</SUB>MA-co-OEGMA), and photothermal nanoparticles of reduced graphene oxide. Each of the drug reservoirs is filled with the same amount of human growth hormone and capped with the stimulus-responsive membrane. Therefore, when implanted in living animals, the device herein can deliver drug reproducibly by rupturing a stimulus-responsive membrane only at the times of near-infrared irradiation applied from the outside body without showing complications.</P><P>Implantable devices for on-demand and pulsatile drug delivery have attracted considerable attention; however, many devices in clinical use are embedded with the electronic units and battery inside, hence making them large and heavy for implantation. Therefore, we propose an implantable device with multiple drug reservoirs capped with a stimulus-responsive membrane (SRM) for on-demand and pulsatile drug delivery. The SRM is made of thermosensitive POSS(MEO<SUB>2</SUB>MA-co-OEGMA) and photothermal nanoparticles of reduced graphene oxide (rGO), and each of the drug reservoirs is filled with the same amount of human growth hormone (hGH). Therefore, with noninvasive near-infrared (NIR) irradiation from the outside skin, the rGO nanoparticles generate heat to rupture the SRM in the implanted device, which can open a single selected drug reservoir to release hGH. Therefore, the device herein is shown to release hGH reproducibly only at the times of NIR irradiation without drug leakage during no irradiation. When implanted in rats with growth hormone deficiency and irradiated with an NIR light from the outside skin, the device exhibits profiles of hGH and IGF1 plasma concentrations, as well as body weight change, similar to those in animals treated with conventional s.c. hGH injections.</P>

Toward an effective control of the H₂ to CO ratio in the electroreduction of CO₂ over Titanate Nanosheets incorporating Au Nanoparticles

( Filipe Marques Mota ),( Dang Nguyen ),이지은,( Huiyan Piao ),( Jin-ho Choy ),황윤정,김동하 한국공업화학회 2018 한국공업화학회 연구논문 초록집 Vol.2018 No.0

The electroreduction of CO₂ has emerged as a rational answer to uprising CO₂ emissions and a strategy to incorporate renewable electricity into the global energy supply. In particular, CO₂RR to CO has been highlighted in the industrial conversion of syngas (H₂ and CO) to fuels through subsequent technologies. Here we report for the first time a strategy to tune the H₂ to CO ratio by facile composition control of the components of a rationally designed binary nanostructure. By adjusting the loading of Au nanoparticles immobilized on ultra-thin titanate nanosheets in a 0 to 93 wt.% range, the CO Faradaic efficiency balanced by exclusive H₂ formation could be effectively varied in a 3 to 80% range. A variation of the electronic properties of these nanostructures, corroborated by XPS characterization, was proposed to dictate the stabilization of formed reaction intermediates and subsequent product selectivity.

Tuning the H₂ to CO Ratio in the Electroreduction of CO₂ via Electronic Reconstruction of Gold Nanoparticles on Layered Titanate Nanosheets

( Filipe Marques Mota ),( Dang Nguyen ),이지은,( Huiyan Piao ),최진호,황윤정,김동하 한국공업화학회 2018 한국공업화학회 연구논문 초록집 Vol.2018 No.1

Molecular Orientation of Intercalants Stabilized in the Interlayer Space of Layered Ceramics: 1-D Electron Density Simulation

Yang, Jae-Hun,Pei, Yi-Rong,Piao, Huiyan,Vinu, Ajayan,Choy, Jin-Ho The Korean Ceramic Society 2016 한국세라믹학회지 Vol.53 No.4

In this review, an attempt is made to calculate one-dimensional (1-D) electron density profiles from experimentally determined (00l) XRD intensities and possible structural models as well in an effort to understand the collective intracrystalline structures of intercalant molecules of two-dimensional (2-D) nanohybrids with heterostructures. 2-D ceramics, including layered metal oxides and clays, have received much attention due to their potential applicability as catalysts, electrodes, stabilizing agents, and drug delivery systems. 2-D nanohybrids based on such layered ceramics with various heterostructures have been realized through intercalation reactions. In general, the physico-chemical properties of such 2-D nanohybrids are strongly correlated with their heterostructures, but it is not easy to solve the crystal structures due to their low crystallinity and high anisotropic nature. However, the powder X-ray diffraction (XRD) analysis method is thought to be the most powerful means of understanding the interlayer structures of intercalant molecules. If a proper number of well-developed (00l) XRD peaks are available for such 2-D nanohybrids, the 1-D electron density along the crystallographic c-axis can be calculated via a Fourier transform analysis to obtain structural information about the orientations and arrangements of guest species in the interlayer space.

Superior role of MXene nanosheet as hybridization matrix over graphene in enhancing interfacial electronic coupling and functionalities of metal oxide

Jin, Xiaoyan,Shin, Seung-Jae,Kim, Najin,Kang, Bohyun,Piao, Huiyan,Choy, Jin-Ho,Kim, Hyungjun,Hwang, Seong-Ju Elsevier 2018 Nano energy Vol.53 No.-

<P><B>Abstract</B></P> <P>A superior efficiency of MXene (Ti<SUB>3</SUB>C<SUB>2</SUB>) nanosheet as a hybridization matrix over graphene is evidenced by comparative investigation on uniformly-stacked MnO<SUB>2</SUB>–Ti<SUB>3</SUB>C<SUB>2</SUB> and MnO<SUB>2</SUB>–reduced graphene oxide (rGO) nanohybrids. Density functional theory calculation and spectroscopic analyses demonstrate a stronger interfacial electronic coupling and greater charge transfer of polar MnO<SUB>2</SUB> with hydrophilic Ti<SUB>3</SUB>C<SUB>2</SUB> nanosheet than with hydrophobic rGO one, which maximizes the hybridization effect with the conductive nanosheet. Also, hybridization with Ti<SUB>3</SUB>C<SUB>2</SUB> nanosheet is more effective in enhancing the ion diffusivity and porosity of MnO<SUB>2</SUB> than that with strongly self-stacking rGO, which is attributable to weaker self-stacking tendency of Ti<SUB>3</SUB>C<SUB>2</SUB>. Due to these hybridization effects, the MnO<SUB>2</SUB>–Ti<SUB>3</SUB>C<SUB>2</SUB> nanohybrid delivers larger specific capacitance with improved rate performance than does the MnO<SUB>2</SUB>–rGO nanohybrid, underscoring higher efficiency of MXene hybridization in improving electrode performance. This study clearly demonstrates that exfoliated MXene nanosheet can act as a superior hybridization matrix over rGO to explore strongly-coupled nanohybrids with improved energy-related functionality.</P> <P><B>Highlights</B></P> <P> <UL> <LI> MXene nanosheet shows superior efficiency as a hybridization matrix over graphene. </LI> <LI> Efficient electrode materials are synthesized by hybridization with MXene nanosheet. </LI> <LI> There is a stronger interfacial electronic coupling of MnO<SUB>2</SUB> with MXene than with rGO. </LI> <LI> Hybridization with less self-stacking MXene nanosheet remarkably increases porosity. </LI> </UL> </P> <P><B>Graphical abstract</B></P> <P>[DISPLAY OMISSION]</P>