Publications by authors named "Shiguo Sun"

114 Publications

In-vitro and in-vivo monitoring of gold(III) ions from intermediate metabolite of sodium aurothiomalate through water-soluble ruthenium (II) complex-based luminescent probe.

Bioorg Chem 2021 Feb 19;110:104749. Epub 2021 Feb 19.

Key Laboratory of Xinjiang Phytomedicine Resources of Ministry of Education, School of Pharmacy, Shihezi University, Shihezi 832002, China. Electronic address:

Real-time monitoring of drug metabolism in vivo is of great significance to drug development and toxicology research. The purpose of this study is to establish a rapid and visual in vivo detection method for the detection of an intermediate metabolite of the gold (I) drug. Gold (I) drugs such as sodium aurothiomalate (AuTM) have anti-inflammatory effects in the treatment of rheumatoid arthritis. Gold(III) ions (Au) are the intermediate metabolite of gold medicine, and they are also the leading factor of side effects in the treatment of patients. However, the rapid reduction of Au to Au by thiol proteins in organisms limits the in-depth study of metabolism of gold drugs in vivo. Here we describe a luminescence Au probe (RA) based on ruthenium (II) complex for detecting Au in vitro and in vivo. RA with large Stokes shift, good water solubility and biocompatibility was successfully applied to detect Au in living cells and vivo by luminescence imaging, and to trap the fluctuation of Au level produced by gold (I) medicine. More importantly, the luminescent probe was used to the detection of the intermediate metabolites of gold (I) drugs for the first time. Overall, this work offers a new detection tool/method for a deeper study of gold (I) drugs metabolite.
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http://dx.doi.org/10.1016/j.bioorg.2021.104749DOI Listing
February 2021

Assembly of multifunction dyes and heat shock protein 90 inhibitor coupled to bovine serum albumin in nanoparticles for multimodal photodynamic/photothermal/chemo-therapy.

J Colloid Interface Sci 2021 May 27;590:290-300. Epub 2021 Jan 27.

Shaanxi Key Laboratory of Natural Products & Chemical Biology, College of Chemistry & Pharmacy, Northwest A&F University, Yangling, Shaanxi 712100, PR China. Electronic address:

The proangiogenic protein, survivin, is a client protein for heat shock protein 90 (Hsp-90), whose overexpression is induced by photodynamic therapy (PDT), leading to the inhibition of capase-9 and the blockage of apoptosis. The overexpression of Hsp-90 in cancer cells can rapidly acquire thermoresistance during photothermal therapy (PTT), leading to insufficient apoptosis, increased cell viability, and tumor recurrence. A potential approach to block the PTT-induced overexpression of Hsp-90 and the overexpression of survivin is developed by using an Hsp-90 inhibitor and anticancer agent, namely, geldanamycin (GM). These inhibitors also develop a mild-temperature PTT strategy to reach synergistic PDT and PTT efficiency. Thus, Cy7-SQ is designed by a covalent disulfide linkage between a photothermal agent (i.e., canine dye 7 [Cy7]) and a photosensitizer (i.e., squaraine dye [SQ]) for the improved photostability and thermal stability of Cy7 and SQ. The cleavage of the Cy7-SQ linkage by glutathione in a tumor microenvironment increases the efficiency of synergistic PDT and PTT. In the current study, bovine serum albumin (BSA)/Cy7-SQ/GM nanoparticles are developed through the self-assembly of BSA, Cy7-SQ, and GM to accelerate the apoptosis of cancer cells via near-infrared (NIR) laser irradiation, thus realizing Hsp-90-regulated synergistic PDT/PTT combined with chemotherapy.
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http://dx.doi.org/10.1016/j.jcis.2021.01.052DOI Listing
May 2021

Nanoscale photosensitizer with tumor-selective turn-on fluorescence and activatable photodynamic therapy treatment for COX-2 overexpressed cancer cells.

J Mater Chem B 2021 03;9(8):2001-2009

Shaanxi Key Laboratory of Natural Products & Chemical Biology, College of Chemistry & Pharmacy, Northwest A&F University, Yangling, Shaanxi 712100, P. R. China.

Effective targeting and in situ imaging-guided treatment are particularly important for accurate clinical photodynamic therapy (PDT) of malignant tumors. Herein, we propose a single molecule, named IMC-DAH-SQ, which possesses dual-targeting components, including structure-inherent targeting (SIT) and cyclooxygenase-2 (COX-2) targeting units, and controllable turn-on near infrared (NIR) fluorescence. Due to its amphiphilicity, IMC-DAH-SQ assembles into a nanoprobe with low background fluorescence. After incubation with tumor cells, the SIT and COX-2 recognition characteristics of IMC-DAH-SQ endow it with preferential tumor-targeting activity. The strong binding with overexpressed COX-2 can collapse the nanoprobe to monomers after accumulation in tumor cells, leading to turn-on NIR fluorescence that is completely different from normal cells. Additionally, benefiting from the single molecular model tactic, the nanoprobe has the advantages of simple synthesis without ever considering the loading rate and separation between the photosensitizer and targeting unit. Other favorite features, including superior biocompatibility, weak dark toxicity, and mitochondria enrichment capability, are implemented. All these traits not only afford nanoprobe precision tumor cell targeting capability but also provide promising imaging-guided antitumor therapy. We believe that the single molecular protocol will establish a novel strategy for simultaneous diagnosis and anticancer medicine treatment utilizing versatile but small compounds.
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http://dx.doi.org/10.1039/d0tb02828bDOI Listing
March 2021

A novel MIP-ECL sensor based on RGO-CeONP/Ru(bpy)-chitosan for ultratrace determination of trimipramine.

J Mater Chem B 2021 01;9(2):471-478

College of Chemistry and Pharmaceutical Engineering, Hebei University of Science and Technology, Shijiazhuang 050018, China.

A novel molecularly imprinted polymer (MIP)-electrochemiluminescence (MIP-ECL) sensor based on CeO2NP-RGO/Ru(bpy)32+-MIP-chitosan was introduced for the ultrasensitive and ultraselective detection of trimipramine (TRI). TRI-MIP was synthesized via the precipitation polymerization process. A nanocomposite of reduced graphene oxide decorated with ceria (CeO2NP-RGO) was synthesized through a facile sonochemical process. CeO2NP-RGO was utilized for modifying the surface of an electrode which consequently led to an excellent electrical conductivity, enhanced electrochemical and ECL characteristics of Ru(bpy)32+. Electrochemical and ECL behaviors of the MIP-ECL sensor were evaluated. Accordingly, the ECL intensity was significantly enhanced via TRI molecule adsorption on the MIP composite film. The prepared MIP-ECL sensor demonstrated high sensitivity and selectivity as well as good reproducibility and stability for TRI determination under the applied optimal conditions. The assays response for TRI concentration was linear in the range of 0.2-100 pM with a 0.995 correlation coefficient. The limit of detection (LOD) was as small as 0.025 pM (S/N = 3). The recoveries between 91-107% for human serum (RSDs < 4.1%) and 94-104.6% for human urine (RSDs < 3.4%) approve that the MIP-ECL sensor can be used for precise detection of TRI in complex biological matrices. Ultimately, this sensor was utilized successfully for the analysis of TRI in human serum and urine samples without any special pretreatment.
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http://dx.doi.org/10.1039/d0tb01666gDOI Listing
January 2021

Targeted antimicrobial peptide delivery in vivo to tumor with near infrared photoactivated mesoporous silica nanoparticles.

Int J Pharm 2020 Oct 13;588:119767. Epub 2020 Aug 13.

School of Life Science, Liaoning Normal University, Dalian 116081, China; Liaoning Provincial Key Laboratory of Biotechnology and Drug Discovery, Liaoning Normal University, Dalian 116081, China. Electronic address:

Antimicrobial peptide PA-C1b (chensinin-1b conjugated with palmitic acid) showed potent anticancer activity with no obvious hemolytic activity, which made it a potential agent for treating cancers. However, after in vivo administration, peptides can be degraded by proteases because there is no effective protection. In this study, a tumor-targeting photoresponsive antimicrobial peptide delivery system was developed, and the peptide PA-C1b labeled with the dye sulfo-cyanine7 (Cy7) was loaded into mesoporous silica nanoparticles (MSNs). The final MSN@Cy7-PA-C1b nanoparticles were wrapped by graphene oxide (GO), and then folic acid was conjugated to the surface of the MSNs for targeting purposes. The final MSN@Cy7-PA-C1b@FA-GO nanoparticles were constructed to allow light-mediated peptide release and folate receptor-targeted cancer therapy. The Cy7 dye serves as a real-time indicator, and GO acts as a gatekeeper to prevent leakage of the loaded peptides in the absence of near-infrared light irradiation. Upon light irradiation, the GO wrapping detaches, and the photoresponsive peptide delivery system works well both in in vitro cell experiments and during in vivo administration in mouse tumor experiments. The construction of the MSN@Cy7-PA-C1b@FA-GO platform provides a novel approach to deliver antimicrobial peptides in vivo for the treatment of infections by pathogenic microorganisms and cancers.
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http://dx.doi.org/10.1016/j.ijpharm.2020.119767DOI Listing
October 2020

Product-boosted fluorescence signal: a new approach for designing small-molecule probes for detection of peroxynitrite.

Chem Commun (Camb) 2020 Jul 12;56(57):7925-7928. Epub 2020 Jun 12.

Shaanxi Key Laboratory of Natural Products & Chemical Biology, College of Chemistry & Pharmacy, Northwest A&F University, Yangling, Shaanxi 712100, P. R. China.

In situ self-assembled boronate ester comprising commercially available 2-formylphenylboronic acid and 2-(2',3'-bihydroxyphenyl)benzothiazole (BHBT) is explored for the detection of ONOO with product-boosted fluorescence. The self-assembly can detect ONOO in the endoplasmic reticulum of living cells.
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http://dx.doi.org/10.1039/d0cc02963gDOI Listing
July 2020

MnO-Based nanosystems for cancer therapy.

Chem Commun (Camb) 2020 Jul 4;56(52):7065-7079. Epub 2020 Jun 4.

Key Laboratory of Pharmaceutical Quality Control of Hebei Province, College of Pharmaceutical Science, Hebei University, Baoding 071002, China.

Cancer is one of the most dangerous diseases worldwide, the treatment of which is still a great problem. The increasing demand of clinical biomedicine and fast development of nanotechnology have quickly promoted the generation of diverse nanosystems for various cancer therapies. As one kind of redox active transition-metal dioxide nanomaterials, manganese dioxide (MnO) and its nanocomposites have emerged as a novel class of nanomaterials that show superior advantages and unprecedented performances in cancer therapy due to their large surface area, good absorption and degradation ability, strong fluorescence quenching ability, high oxidation and catalytic activity, etc. According to different morphologies of MnO, MnO can be divided into MnO nanosheets, MnO quantum dots (QDs), MnO nanocrystals, MnO nanowires, etc. In this review, the synthesis of MnO, especially MnO nanosheets, is first introduced, followed by an introduction of the classification of MnO nanomaterials. Then, recent cancer therapeutic applications of MnO and its nanocomposites are comprehensively overviewed, which are categorized into three parts: chemotherapy, phototherapy and synergistic therapy. In addition, treatment of other diseases based on MnO and its nanocomposites is also discussed. Finally, some crucial unresolved problems, probable challenges and future perspectives about the rational design and construction of MnO-based nanosystems for further biomedical applications are also discussed.
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http://dx.doi.org/10.1039/d0cc02782kDOI Listing
July 2020

Investigation of endogenous malondialdehyde through fluorescent probe MDA-6 during oxidative stress.

Anal Chim Acta 2020 Jun 13;1116:9-15. Epub 2020 Apr 13.

Key Laboratory of Xinjiang Phytomedicine Resources of Ministry of Education, School of Pharmacy, Shihezi University, Shihezi, 832002, China. Electronic address:

The malondialdehyde (MDA)-specific detection probe (MDA-6) was successfully synthesised through the photoinduced electron transfer (PET) mechanism which possesses many biological applications. In vivo biological applicability of this probe was proved in different cell lines, zebrafish and mice. In these models, the MDA was produced by oxygen stress injury and the relationship between MDA and probe were evaluated in vitro as well as in vivo under different stress conditions. After comparing evaluated results with commercial MDA kit, MDA-6 was concluded with high specificity, low limit of detection (0.03 μM), and can achieve micro-detection of MDA with low cytotoxicity, demonstrating MDA-6 enables safe and effective detection.
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http://dx.doi.org/10.1016/j.aca.2020.04.030DOI Listing
June 2020

Width-Consistent Mesoporous Silica Nanorods with a Precisely Controlled Aspect Ratio for Lysosome Dysfunctional Synergistic Chemotherapy/Photothermal Therapy/Starvation Therapy/Oxidative Therapy.

ACS Appl Mater Interfaces 2020 Jun 19;12(22):24611-24622. Epub 2020 May 19.

Shaanxi Key Laboratory of Natural Products & Chemical Biology, College of Chemistry & Pharmacy, Northwest A&F University, Xinong Road 22, Yangling, Shaanxi 712100, China.

Although differently shaped mesoporous silica is widely studied, the formation of width-consistent mesoporous silica nanorods (MSNRs) with a precisely controlled aspect ratio (AR: length/width) is challenging and has not been reported. Herein, width-consistent (100 nm) MSNRs with ARs of 2, 3, 4, 6, 8, and 10 were obtained by increasing the concentrations while maintaining the molar ratio of cetyltrimethylammonium bromide (CTAB) and tetraethyl orthosilicate (TEOS). The results demonstrated that the as-prepared MSNR with an AR of 6 (AR6) possesses high cellular-uptake efficiency and drug-loading capacity. Thus, AR6-based cancer-cell-targeting nanosystems were designed. These nanosystems encapsulated doxorubicin (DOX) into the porous channel of AR6, adsorbed glucose oxidase (GOx), and then formed a polydopamine (PDA) layer for Siramesine (Siram, a lysosome dysfunctional drug) adsorption and folic acid modification. In this design, the PDA shell could prevent the leakage of loading components and keep the activity of GOx during delivery while achieving an on-demand drug release in the targeted location and photothermal therapy under near-infrared irradiation. The increase in temperature was highly beneficial for elevating the catalytic efficiency of GOx, accelerating the consumption of intracellular glucose, and generating a relatively high level of cytotoxic HO, all of which enhanced starvation and oxidative therapies. Siram was employed to inhibit lysosomal metabolism and accompany GOx to reach a dual-enhanced starvation therapy effect. In addition, DOX entered the nucleus and altered DNA for chemotherapy. The results showed that the nanosystems have superior therapeutic efficacy against cancer cells and not much toxicity to normal cells. Therefore, this study provides a novel strategy for lysosome dysfunctional synergistic chemotherapy/photothermal therapy/starvation therapy/oxidative therapy based on MSNR.
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http://dx.doi.org/10.1021/acsami.0c06117DOI Listing
June 2020

Cyanide Boosting Copper Catalysis: A Mild Approach to Fluorescent Benzazole Derivatives from Nonemissive Schiff Bases in Biological Media.

Org Lett 2020 05 10;22(9):3361-3366. Epub 2020 Apr 10.

Shaanxi Key Laboratory of Natural Products & Chemical Biology, College of Chemistry & Pharmacy, Northwest A&F University, Yangling, Shaanxi 712100, P. R. China.

An application of nucleophilic cyclization and oxidation of nonemissive Schiff bases via cyanide boosting copper catalysis to synthesize fluorescent benzazole derivatives in high conversion yield is disclosed. This approach is highlighted by broad substrate scope, fast reaction time, and mild conditions and can efficiently proceed in living cells or root tissues. Furthermore, this methodology can be applied for selective detection of Cu and CN.
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http://dx.doi.org/10.1021/acs.orglett.0c00784DOI Listing
May 2020

A novel fluorescent probe based on naphthalimide for imaging nitroreductase (NTR) in bacteria and cells.

Bioorg Med Chem 2020 02 24;28(3):115280. Epub 2019 Dec 24.

Shaanxi Key Laboratory of Natural Products & Chemical Biology, College of Chemistry & Pharmacy, Northwest A&F University, Xinong Road 22, Yangling, Shaanxi 712100, PR China. Electronic address:

A nitroreductase (NTR) responsive fluorescent probe, Na-NO, comprising p-nitrobenzyl as the unique recognition group and 1,8-naphthalimide as fluorophore, was synthesized. Na-NO showed remarkable fluorescence "turn-on" signal in the presence of NTR under DMSO/HO (1:19, v/v) buffered with PBS (pH = 7) solution in the presence of NADH (300 µM). Furthermore, the probe has a low detection limit down to 3.4 ng/mL and it is very sensitive towards the NTR in Escherichia coli (E. coli), Staphylococcus aureus (S. aureus), normal and tumor cells such as HL-7702, HepG-2 and MCF-7.
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http://dx.doi.org/10.1016/j.bmc.2019.115280DOI Listing
February 2020

PAMAM-cRGD mediating efficient siRNA delivery to spermatogonial stem cells.

Stem Cell Res Ther 2019 12 18;10(1):399. Epub 2019 Dec 18.

Key Laboratory for Animal Genetics, Breeding and Reproduction of Shaanxi Province, Key Laboratory for Animal Biotechnology, Ministry of Agriculture of China, College of Animal Science and Technology, Northwest A&F University, Yangling, Shaanxi, China.

Background: Spermatogonial stem cells (SSCs) are the cornerstone of sperm production and thus perpetual male fertility. In clinics, transplantation of patient's own SSCs into testes is a promising technique to restore fertility when male germ cells have been depleted by gonadotoxic therapies. Auto-transplantation of genetically modified SSCs even has the potential to treat male infertility caused by genetic mutations. However, SSCs are refractory to transfection approaches. Poly(amidoamine) (PAMAM) dendrimers have the unique three-dimensional architecture, surface charge, and high density of surface groups that are suitable for ligand attachment, thereby facilitating target delivery. The goal of this study was to elucidate whether PAMAM dendrimers can efficiently deliver short interfering RNAs (siRNAs) to SSCs.

Methods And Results: We introduced cyclic arginine-glycine-aspartic acid (cRGD) peptides to the fifth generation of PAMAM dendrimers (G5) to generate PAMAM-cRGD dendrimers (G5-cRGD). The characterization of G5-cRGD was detected by Fourier transform infrared spectroscope (FTIR), transmission electron microscope (TEM), and the Cell Counting Kit-8 (CCK-8) assay. Confocal microscopy and flow cytometry were used to evaluate the delivery efficiency of siRNA by G5-cRGD to SSCs. The results showed that G5-cRGD encompassing siRNA could self-assemble into spherical structures with nanoscale size and possess high transfection efficiency, excellent endosomal escape ability, and low cytotoxicity, superior to a commercial transfection reagent Lipofectamine® 2000. Moreover, we demonstrated that G5-cRGD efficiently delivered siRNAs and triggered gene silencing.

Conclusions: This study thus provides a promising nanovector for siRNA delivery in SSCs, facilitating the future clinical application of SSC auto-transplantation with genetically modified cells with a hope to cure male infertility that is caused by genetic disorders.
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http://dx.doi.org/10.1186/s13287-019-1506-4DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC6921429PMC
December 2019

Recent development in biodegradable nanovehicle delivery system-assisted immunotherapy.

Biomater Sci 2019 Nov 31;7(11):4414-4443. Epub 2019 Jul 31.

Shaanxi Key Laboratory of Natural Products & Chemical Biology, College of Chemistry & Pharmacy, Northwest A&F University, Yangling, Shaanxi 712100, P. R. China.

Based on the stimulation of the patient's own innate and adaptive immunity, immunotherapy is used in tumor treatment, and in recent years, it has developed rapidly. To generate strong and long-lasting antitumor immune responses and to boost clinical efficiency, various nanovehicle delivery systems (NDSs) have been designed to achieve specific release and avoid premature leakage in the delivery process. However, most of them are nondegradable, and they are taken up by the liver and spleen. This process leads to the accumulation of these substances in the human body, raising long-term toxicity concerns and causing potential undesirable side effects. To solve this problem, biodegradable NDSs (BNDSs) have been developed. Once these substances reach their target, they can only be degraded under specific internal or external stimuli, such as enzymes, irradiation, temperature, redox potential, pH, or a combination of these stimuli. Therefore, they are quite significant for potential clinical applications. In this review article, we highlight the recent literature on the design and working mechanism of various BNDSs. According to their type and characteristics, BNDSs are categorized as follows: (1) polymers, (2) lipid based materials, (3) inorganic nanomaterials, (4) biomacromolecules, (5) hybrid materials and (6) other materials. The existing challenges and future prospects of these materials will also be discussed.
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http://dx.doi.org/10.1039/c9bm00961bDOI Listing
November 2019

GSH-responsive anti-mitotic cell penetrating peptide-linked podophyllotoxin conjugate for improving water solubility and targeted synergistic drug delivery.

Bioorg Med Chem Lett 2019 04 6;29(8):1019-1022. Epub 2019 Feb 6.

Key Laboratory of Xinjiang Phytomedicine Resource and Utilization, Ministry of Education, School of Pharmacy, Shihezi University, Shihezi 832002, China. Electronic address:

Podophyllotoxin (PPT) is a chemotherapeutic agent which has shown significant anti-cancer effects through inhibiting microtubule assembly. However, because of the poor water solubility and obvious side effects, PPT cannot be used in clinical cancer therapy. In order to solve these problems, a novel glutathione-responsive PPT conjugate has been synthesized in which PPT was linked to an anti-mitotic cell penetrating peptide (PRA) via a disulfide linkage. In particular, the as-prepared PPT-PRA conjugate can self-assemble into vesicle in water, furthermore, another anti-cancer drug (doxorubicin was chosen as an example) can be loaded in the vesicle for synergistic drug delivery. For better cancer cells targeting, the vesicle was then modified with folic acid (FA). The results indicated that the as-prepared FA modified drug-loaded vesicle not only could overcome the poor water solubility and side effects of PPT but also exhibited targeted toxicity and synergistic therapeutic effect.
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http://dx.doi.org/10.1016/j.bmcl.2019.02.005DOI Listing
April 2019

In Situ Formation of Homogeneous Tellurium Nanodots in Paclitaxel-Loaded MgAl Layered Double Hydroxide Gated Mesoporous Silica Nanoparticles for Synergistic Chemo/PDT/PTT Trimode Combinatorial Therapy.

Inorg Chem 2019 Mar 15;58(5):2987-2996. Epub 2019 Feb 15.

Shaanxi Key Laboratory of Natural Products & Chemical Biology, College of Chemistry & Pharmacy , Northwest A&F University , Yangling , Shaanxi 712100 , People's Republic of China.

A folic acid (FA) functional drug delivery system (MT@L-PTX@FA) based on in situ formation of tellurium nanodots (Te NDs) in paclitaxel (PTX)-loaded MgAl layered double hydroxide (LDHs) gated mesoporous silica nanoparticles (MSNs) has been designed and fabricated for targeted chemo/PDT/PTT trimode combinatorial therapy. X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM), high-resolution transmission electron microscopy (HRTEM), N adsorption-desorption, Fourier transform infrared (FT-IR) spectra, and UV-vis spectra were used to demonstrate the successful fabrication of MT@L-PTX@FA. In particular, the in situ generated Te NDs showed a homogeneous ultrasmall size. Reactive oxygen species (ROS) generation, photothermal effects, and photostability evaluations indicated that the in situ generated homogeneous Te NDs could serve as the phototherapeutic agent, converting the photon energy to ROS and heat under near-infrared (NIR) irradiation efficiently. The drug-release test revealed that MT@L-PTX@FA showed an apparent sustained release character in a pH-sensitive manner. In addition, cell imaging experiments demonstrated that MT@L-PTX@FA could selectively enter into cancer cells owing to the function of FA and release of PTX efficiently for chemotherapy for the reason that the low intracellular pH would dissolve MgAl LDHs to Mg and Al. Cytotoxicity tests also indicated that MT@L-PTX@FA exhibited enhanced therapeutic effect in cancer cells under NIR irradiation, benefiting from the synergy based on targeted chemo/PDT/PTT trimode combinatorial therapy. The preliminary results reported here will shed new light on the future design and applications of nanosystems for synergistic combinatorial therapy.
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http://dx.doi.org/10.1021/acs.inorgchem.8b02821DOI Listing
March 2019

A novel label free electrochemiluminescent aptasensor for the detection of lysozyme.

Mater Sci Eng C Mater Biol Appl 2019 Mar 13;96:146-152. Epub 2018 Nov 13.

Key Laboratory of Xinjiang Phytomedicine Resource and Utilization, Ministry of Education, School of Pharmacy, Shihezi University, Shihezi 832000, China. Electronic address:

In this paper we describe a novel ultrasensitive electrochemiluminescent (ECL) aptasensor based on the quenching effect of aptamer and lysozyme incubation on co-reactant ECL mechanism of nitrogen-doped graphene quantum dots and persulfate. Incorporation of gold nanoparticles let to enhancement of electron transfer process of co-reactant mechanism species. The electrochemical behavior of each step modification of aptasensor was investigated using electrochemical impedance spectroscopy and verified by ECL responses. The aptasensor showed high stability, sensitivity, reliable reproducibility, wide linear range (10 fM to 10 nM) with a low detection limit of 0.8 fM (at an S/N ratio of 3, n = 10) can be successively applied to the human serum samples analysis. Recoveries ranged between 91 and 104% (with RSDs of <3.1%).
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http://dx.doi.org/10.1016/j.msec.2018.11.016DOI Listing
March 2019

Media Dependent Switching of Selectivity and Continuous near Infrared Turn-on Fluorescence Response through Cascade Interactions from Noncovalent to Covalent Binding for Detection of Serum Albumin in Living Cells.

ACS Appl Mater Interfaces 2018 Dec 13;10(51):44336-44343. Epub 2018 Dec 13.

Shaanxi Key Laboratory of Natural Products & Chemical Biology, College of Chemistry & Pharmacy , Northwest A&F University , Yangling , Shaanxi 712100 , P.R. China.

Abnormal level of proteins is proved to be associated with diseases. Thus, protein sensing is helpful for clinical diagnosis and therapy. However, there is a great variety of protein species and relatively low concentration of each protein in complicated biological systems including other nonprotein biomolecules. Therefore, it remains challenging to develop an effective method for detecting protein with high selectivity and sensitivity. Herein, a new self-assembly method based on a robust dye SQSS of which two squaraine molecules were conjugated through disulfide bond was developed for highly selective and sensitive detection of serum albumin (SA) in aqueous solution and live cells. SQSS can self-assemble into "compact" aggregates, offering "inert" disulfide group and very low background fluorescence through the combination of aggregation quenching and homogeneous fluorescence resonance energy transfer (homoFRET) quenching. The response of SQSS to SA undergoes two cascade stages. At the first stage, SA drives the compact assemblies of SQSS to form loose ones with fast speed (30 s) through noncovalent interaction, resulting in the enhancement of fluorescence to some extent. In this loose assembly state, the disulfide bond in SQSS is reactive. At the second stage, the Cys34 in SA slowly induced further disassembly through covalent binding with reactive disulfide bond, resulting in fluorescence further increasing and SQSS labeling to SA that cannot be displaced by site binding ligands of SA. The self-assemblies of SQSS can selectively detect SA with continuous near-infrared (NIR) turn-on fluorescence response in 100% aqueous buffer solution. In addition, SQSS showed the potential application of imaging SA in living cells. On the other hand, the loose assembly state of SQSS was also achieved in aqueous solution with 20% CHCN. In this media, thiol-containing glutathione (GSH) caused the disassembly of SQSS with turn-on fluorescence response through interaction with disulfide bond. SQSS can selectively recognize GSH over other amino acids even in the presence of other sulfhydryl amino acids. As a proof-of-concept method, the molecular self-assembly through multisteps interactions would provide an ideal strategy for detection and live-cell imaging of biorelated molecules with high selectivity and signal-to-noise ratio.
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http://dx.doi.org/10.1021/acsami.8b19768DOI Listing
December 2018

Construction of a biodegradable, versatile nanocarrier for optional combination cancer therapy.

Acta Biomater 2019 01 7;83:359-371. Epub 2018 Nov 7.

Shaanxi Key Laboratory of Natural Products & Chemical Biology, College of Chemistry & Pharmacy, Northwest A&F University, Yangling, Shaanxi 712100, China. Electronic address:

A novel biodegradable versatile nanocarrier (FA-CM) was fabricated based on the self-assembly of delaminated CoAl-layered double hydroxides (LDHs) and manganese dioxide (MnO) for optional combination cancer therapy. Biodegradation, versatility, targeting, bioimaging, in vitro cytotoxicity and in vivo antitumor efficacy were evaluated. The results showed that FA-CM could not only be effectively degraded into Co, Al and Mn to overcome the long-term toxic side effects, but also successfully load any positive-charged, negative-charged, hydrophilic, and hydrophobic drug, meeting the critical requirement of versatile nanocarrier. Meanwhile, the presence of FA led to the higher uptake efficiency, cytotoxicity, and excellent fluorescence imaging of FA-CM toward cancerous cells. In particular, FA-CM exhibited glutathione and pH dual-response drug release, avoiding any premature leakage and side effects. The applicability of the FA-CM was determined by co-loading hydrophilic (doxorubicin (DOX)) and hydrophobic drug (paclitaxel (PTX)) for synergistic combination chemotherapy. In vitro cytotoxicity evaluation and a xenograft tumor model of hepatoma showed that this combination exhibited more efficient anticancer effects compared with either free drug alone or the corresponding cocktail solutions. Especially, the ratios of DOX and PTX loaded on FA-CM could be tuned as needed. A powerful approach is provided for the design and preparation of a biodegradable versatile nanocarrier with targeted ability and excellent biocompatibility, which can be potentially applied in clinical practice and medical imaging. STATEMENT OF SIGNIFICANCE: Drug delivery nanocarriers that can transport an effective dosage of drug molecules to targeted cells and tissues have been extensively designed to overcome the adverse side effects and low effectiveness of conventional chemotherapy. However, lack of biodegradability and versatility existing in majority of nanocarriers limit their further clinical applications. Thus, constructing a novel biodegradable versatile nanocarrier that can carry various types of drugs, is in urgent need and more suitable for commercial production and clinical use. In this study, we developed a novel biodegradable versatile nanocarrier (FA-CM) based on the self-assembly of delaminated CoAl-layered double hydroxides (LDHs) and manganese dioxide (MnO) for optional combination cancer therapy. This work provides a new strategy for constructing versatile biodegradable platform for targeted drug delivery, which would have broad applications in cancer theranostics.
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http://dx.doi.org/10.1016/j.actbio.2018.11.009DOI Listing
January 2019

Electrochemiluminescent aptasensor for thrombin using nitrogen-doped graphene quantum dots.

Mikrochim Acta 2018 08 24;185(9):430. Epub 2018 Aug 24.

Key Laboratory of Xinjiang Endemic Phytomedicine Resources, Ministry of Education, School of Pharmacy, Shihezi University, Shihezi, 832000, China.

An electrochemiluminescent (ECL) aptamer based method is described for the determination of thrombin. Three-dimensional nitrogen-doped graphene oxide (3D-NGO) was placed on a glassy carbon electrode (GCE) to provide an electrode surface that displays excellent electrical conductivity and acts as a strong emitter of ECL. The modified electrode was further coated with chitosan via electrodeposition. Finally, the amino-modified aptamer was immobilized on the modified GCE. The interaction between thrombin and aptamer results in a decrease in ECL. The assay has a linear response in the 1 fM to 1 nM thrombin concentration range and a 0.25 fM lower detection limit (at an S/N ratio of 3). The method was applied to the determination of thrombin in spiked human plasma samples, and recoveries ranged between 94 and 105% (with RSDs of <3.6%). The calibration plot was recorded at potential and wavelength of fluorescence emission (wavelength: 445 nm; potential: 0 to -2 V). Graphical abstract A bare glassy carbon electrode (GCE) does not display electrochemiluminescence (ECL). If, however, nitrogen-doped graphene quantum dots, chitosan, and three-dimensional nitrogen-doped graphene oxide (NGQD-chitosan/3D-NGO) are electrodeposited on the GCE, strong ECL can be observed. The ECL intensity decreased after aptamer and bovine serum albumin (BSA) were dropped onto the electrode (curve a). However, the ECL further decreases after addition of thrombin (TB; curve b).
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http://dx.doi.org/10.1007/s00604-018-2942-zDOI Listing
August 2018

One-step synthesis of Nickle Iron-layered double hydroxide/reduced graphene oxide/carbon nanofibres composite as electrode materials for asymmetric supercapacitor.

Sci Rep 2018 Jun 11;8(1):8908. Epub 2018 Jun 11.

Shaanxi Key Laboratory of Natural Products & Chemical Biology, College of Chemistry & Pharmacy, Northwest A&F University, Xinong Road 22, Yangling, Shaanxi, 712100, P.R. China.

A novel NiFe-LDH/RGO/CNFs composite was produced by using a facile one-step hydrothermal method as electrode for supercapacitor. Compared with NiFe-LDH/CNFs, NiFe-LDH/CNTs and NiFe-LDH/RGO, NiFe-LDH/RGO/CNFs demonstrated a high specific capacitance of 1330.2 F g at 1 A g and a super rate capability of 64.2% from 1 to 20 A g, indicating great potential for supercapacitor application. Additionally, an asymmetric supercapacitor using NiFe-LDH/RGO/CNFs composite as positive electrode material and activated carbon as negative electrode material was assembled. The asymmetric supercapacitor can work in the voltage range of 0-1.57 V. It displayed high energy density of 33.7 W h kg at power density of 785.8 W kg and excellent cycling stability with 97.1% of the initial capacitance after 2500 cycles at 8 A g. Two flexible AC//LDH-RGO-CNFs ASC devices connected in series were able to light up a red LED indicator after being fully charged. The results demonstrate that the AC//LDH-RGO-CNFs ASC has a promising potential in commercial application.
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http://dx.doi.org/10.1038/s41598-018-27171-0DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC5995954PMC
June 2018

Correction: A luminescent bimetallic iridium(iii) complex for ratiometric tracking intracellular viscosity.

Chem Commun (Camb) 2018 04;54(32):4061

State Key Laboratory of Fine Chemicals, School of Chemistry, Dalian University of Technology, No. 2 linggong Road, Ganjingzi, District, Dalian 116023, China.

Correction for 'A luminescent bimetallic iridium(iii) complex for ratiometric tracking intracellular viscosity' by Fengyu Liu et al., Chem. Commun., 2018, 54, 1371-1374.
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http://dx.doi.org/10.1039/c8cc90157kDOI Listing
April 2018

A Rhodamine B-based fluorescent probe for imaging Cu in maize roots.

Bioorg Med Chem 2018 05 23;26(8):1448-1452. Epub 2017 Sep 23.

Shaanxi Key Laboratory of Natural Products & Chemical Biology, College of Chemistry & Pharmacy, Northwest A&F University, Xinong Road 22, Yangling, Shaanxi 712100, PR China. Electronic address:

A new Rhodamine B-based fluorescent probe (RBO) is successfully designed and synthesized, which is a higher selective and sensitive chemosensor for Cu than other ions. Under physiological conditions (pH = 7.0), the non emission RBO displays a rapid fluorescence increase together with a color change after addition of Cu and the detection limit is down to 28nM, which can clearly illustrate the distribution of Cu with the help of laser scanning confocal microscope in plant tissues. Eventually, it confirmed that the Cu accumulates mostly in the vascular cylinder and very less in the epidermal cells of maize roots, which is important to understand how the plants take up, transport and store in the Cu.
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http://dx.doi.org/10.1016/j.bmc.2017.09.026DOI Listing
May 2018

A luminescent bimetallic iridium(iii) complex for ratiometric tracking intracellular viscosity.

Chem Commun (Camb) 2018 Feb;54(11):1371-1374

State Key Laboratory of Fine Chemicals, School of Chemistry, Dalian University of Technology, No. 2 linggong Road, Ganjingzi, District, Dalian 116023, China.

A luminescent bimetallic iridium probe C10 was developed through a long soft carbon chain linkage to achieve ratiometric detection of viscosity. C10 features high sensitivity and selectivity for viscosity. More importantly, C10 is living cell permeable and can be employed to distinguish cancer cells from normal cells and track viscosity changes during MCF-7 cell apoptosis.
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http://dx.doi.org/10.1039/c7cc09723aDOI Listing
February 2018

A water-soluble near-infrared fluorescent probe for specific Pd detection.

Bioorg Med Chem 2018 02 6;26(4):931-937. Epub 2017 Dec 6.

Shaanxi Key Laboratory of Natural Products & Chemical Biology, College of Chemistry & Pharmacy, Northwest A&F University, Yangling, Shaanxi 712100, China. Electronic address:

Palladium (Pd) is widely used in chemistry, biology, environmental science etc., and Pd is the most plenitudinous oxidation state of the Pd that can exist under physiological conditions or in living cells, which could have adverse effects on both our health and environment. Thus, it is of great significance to monitor the changes of Pd. Hence, a novel near-infrared fluorescent probe M-PD has been developed for selective detection of Pd based on naphthofluorescein in this work. The result demonstrated that M-PD exhibited favorable properties for sensing Pd such as excellent water solubility, high selectivity and sensitivity. And the limit of detection was estimated as 10.8 nM, much lower than the threshold in drugs (5-10 ppm) specified by European Directorate for the Quality Control of Medicines. More importantly, detection and recovery experiments of Pd in aspirin aqoeous solution and soil are satisfactory. In addition, M-PD has also been successfully used for near-infrared fluorescence imaging of Pd in living cells, indicating that the probe has better feasibility and application potential in the determination of Pd.
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http://dx.doi.org/10.1016/j.bmc.2017.12.003DOI Listing
February 2018

A water-soluble nucleolin aptamer-paclitaxel conjugate for tumor-specific targeting in ovarian cancer.

Nat Commun 2017 11 9;8(1):1390. Epub 2017 Nov 9.

Institute of Precision Medicine and Innovative Drug Discovery (PMID), School of Chinese Medicine, Hong Kong Baptist University, Hong Kong SAR, 999077, China.

Paclitaxel (PTX) is among the most commonly used first-line drugs for cancer chemotherapy. However, its poor water solubility and indiscriminate distribution in normal tissues remain clinical challenges. Here we design and synthesize a highly water-soluble nucleolin aptamer-paclitaxel conjugate (NucA-PTX) that selectively delivers PTX to the tumor site. By connecting a tumor-targeting nucleolin aptamer (NucA) to the active hydroxyl group at 2' position of PTX via a cathepsin B sensitive dipeptide bond, NucA-PTX remains stable and inactive in the circulation. NucA facilitates the uptake of the conjugated PTX specifically in tumor cells. Once inside cells, the dipeptide bond linker of NucA-PTX is cleaved by cathepsin B and then the conjugated PTX is released for action. The NucA modification assists the selective accumulation of the conjugated PTX in ovarian tumor tissue rather than normal tissues, and subsequently resulting in notably improved antitumor activity and reduced toxicity.
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http://dx.doi.org/10.1038/s41467-017-01565-6DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC5680242PMC
November 2017

Diverse gatekeepers for mesoporous silica nanoparticle based drug delivery systems.

Chem Soc Rev 2017 Oct;46(19):6024-6045

Shaanxi Key Laboratory of Natural Products & Chemical Biology, College of Chemistry & Pharmacy, Northwest A&F University, Yangling, Shaanxi 712100, P. R. China.

Conventional cancer chemotherapy is often associated with toxicity issues. Thus, new drug delivery systems (DDSs) are developed as alternatives owing to their potential to selectively target affected cells while sparing normal tissues. Among them, noninvasive and biocompatible mesoporous silica nanoparticle (MSN)-based targeted DDSs have developed rapidly. In particular, controlled gatekeepers capping the pore entrances of MSNs play prominent and crucial roles in achieving specific drug release and avoiding premature leakage in the delivery process before the target is reached, and perfect gatekeepers can only be removed under specific internal or external stimuli, such as pH, redox potential, temperature, biomolecules, light, magnetic field and ultrasound, or a combination of these stimuli, which is significant for precise therapeutic treatments and potential applications in human bodies. Thus, the main focus of this review is to highlight the most recent progress on the design of various controlled MSN gatekeepers to achieve 'zero premature release' drug delivery. The diverse gatekeepers are categorised into the following kinds according to their types and characteristics: (1) polymers; (2) inorganic nanomaterials; (3) host-guest assemblies; and (4) biomacromolecules. This review will offer a broad palette of opportunities for researchers with interests including nanomaterial fabrication and modification, targeted drug delivery and stimuli-responsive drug release.
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http://dx.doi.org/10.1039/c7cs00219jDOI Listing
October 2017

Recent trends in electrochemiluminescence aptasensors and their applications.

Chem Commun (Camb) 2017 Aug;53(65):9042-9054

State Key Laboratory of Fine Chemicals, Dalian University of Technology, No. 2 Linggong Road, Ganjingzi, District, Dalian 116023, China.

Aptamers are single stranded DNA or RNA ligands which can be selected for different targets from proteins to small organic dyes. In the past few years great progress has been accomplished in the development of aptamer based bioanalytical assays with different detection techniques. Among them, electrochemiluminescence (ECL) aptasensors are very promising because they have the advantages of both electrochemical and chemiluminescence biosensors, such as high sensitivity, low background, cost effectiveness, and ease of control. In this review, we summarize the recent efforts to construct novel and improved ECL aptasensors and their application.
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http://dx.doi.org/10.1039/c7cc04300gDOI Listing
August 2017

High performance asymmetric supercapacitor based on Cobalt Nickle Iron-layered double hydroxide/carbon nanofibres and activated carbon.

Sci Rep 2017 07 5;7(1):4707. Epub 2017 Jul 5.

Shaanxi Key Laboratory of Natural Products & Chemical Biology, School of Chemistry & Pharmacy, Northwest A&F University, Xinong Road 22, Yangling, Shaanxi, 712100, P.R. China.

A novel Cobalt Nickle Iron-layered double hydroxide/carbon nanofibres (CoNiFe-LDH/CNFs-0.5) composite was successfully fabricated through an easy in situ growth approach. The morphology and composition of the obtained materials were systematically investigated. When the two derived materials were used for supercapacitor electrodes, the CoNiFe-LDH/CNFs-0.5 composite displayed high specific surface area (114.2 m g), specific capacitance (1203 F g at 1 A g) and rate capability (77.1% from 1 A g to 10 A g), which were considerably higher than those of pure CoNiFe-LDH. Moreover, the specific capacitance of CoNiFe-LDH/CNFs-0.5 composite remained at 94.4% after 1000 cycles at 20 A g, suggesting excellent long-time cycle life. The asymmetric supercapacitor based on CoNiFe-LDH/CNFs-0.5 as a positive electrode and activated carbon as a negative electrode was manufactured and it exhibited a specific capacitance of 84.9 F g at 1 A g and a high energy density of 30.2 W h kg. More importantly, this device showed long-term cycling stability, with 82.7% capacity retention after 2000 cycles at 10 A g. Thus, this composite with outstanding electrochemical performance could be a promising electrode material for supercapacitors.
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http://dx.doi.org/10.1038/s41598-017-04807-1DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC5498571PMC
July 2017

Hierarchical self-assembly of squaraine and silica nanoparticle functionalized with cationic coordination sites for near infrared detection of ATP.

Sci Rep 2017 02 27;7:43491. Epub 2017 Feb 27.

Shaanxi Key Laboratory of Natural Products &Chemical Biology, College of Chemistry &Pharmacy, Northwest A&F University, Yangling, Shaanxi, 712100, P. R. China.

Optical activity of hierarchical supramolecular assemblies based on organic dyes would create multiple functional architectures. In this work, three kinds of silica nanoparticles with or without functional groups were synthesized. For the first time, silica nanoparticles can induce positively charged squaraine (SQ) to aggregate to form supramolecular assemblies. Adenosine-5'-triphosphate (ATP) as building blocks was absorbed on the surface of silica nanoparticles through metal-anion coordination and electrostatic interactions, in which the aggregates of SQ was transferred to monomer. The thickness being composed of ATP and SQ on the outside of nanoparticles is about 5 nm. These supramolecular assemblies showed selective turn-on fluorescence response to ATP in near infrared (NIR) region over other ions through metal-anion coordination and electrostatic interactions. These functional silica nanoparticles possessing many advantages provide proof-of-principle "seed crystals" for construction of supramolecular assemblies and platforms for sensing with facile performance.
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http://dx.doi.org/10.1038/srep43491DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC5327475PMC
February 2017

Electrochemical microfluidic chip based on molecular imprinting technique applied for therapeutic drug monitoring.

Biosens Bioelectron 2017 May 19;91:714-720. Epub 2017 Jan 19.

College of Science, Harbin Institute of Technology (Shenzhen), Shenzhen, China; Key Laboratory of Xinjiang Endemic Phytomedicine Resources, Ministry of Education, School of Pharmacy, Shihezi University, Shihezi, China. Electronic address:

In this work, a novel electrochemical detection platform was established by integrating molecularly imprinting technique with microfluidic chip and applied for trace measurement of three therapeutic drugs. The chip foundation is acrylic panel with designed grooves. In the detection cell of the chip, a Pt wire is used as the counter electrode and reference electrode, and a Au-Ag alloy microwire (NPAMW) with 3D nanoporous surface modified with electro-polymerized molecularly imprinted polymer (MIP) film as the working electrode. Detailed characterization of the chip and the working electrode was performed, and the properties were explored by cyclic voltammetry and electrochemical impedance spectroscopy. Two methods, respectively based on electrochemical catalysis and MIP/gate effect were employed for detecting warfarin sodium by using the prepared chip. The linearity of electrochemical catalysis method was in the range of 5×10-4×10M, which fails to meet clinical testing demand. By contrast, the linearity of gate effect was 2×10-4×10M with remarkably low detection limit of 8×10M (S/N=3), which is able to satisfy clinical assay. Then the system was applied for 24-h monitoring of drug concentration in plasma after administration of warfarin sodium in rabbit, and the corresponding pharmacokinetic parameters were obtained. In addition, the microfluidic chip was successfully adopted to analyze cyclophosphamide and carbamazepine, implying its good versatile ability. It is expected that this novel electrochemical microfluidic chip can act as a promising format for point-of-care testing via monitoring different analytes sensitively and conveniently.
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http://dx.doi.org/10.1016/j.bios.2017.01.037DOI Listing
May 2017