Publications by authors named "Siyu Lu"

89 Publications

Decoration of Ru/RuO hybrid nanoparticles on MoO plane as bifunctional electrocatalyst for overall water splitting.

J Colloid Interface Sci 2021 Jul 10;604:508-516. Epub 2021 Jul 10.

Green Catalysis Center, College of Chemistry, Zhengzhou University, 100 Science Road, Zhengzhou 450001, PR China.

Hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) are the two branches of artificial overall water splitting (OWS), in which the reaction efficiency usually depends on different specific catalysts. Although effective bifunctional electrocatalyst for OWS (HER and OER) are highly desired, designing and constructing such suitable materials is full of challenges to overcome several difficulties, involving slow kinetics, differences in catalytic mechanisms, large overpotential values, and low round-trip efficiencies. In this work, we reported a new bifunctional electrocatalyst Ru/RuO-MoO catalyst (RRMC) via a redox solid phase reaction (RSPR) strategy to achieve the high electrocatalytic activity of OWS. Briefly, due to the restricted transport behavior of atoms in solid state precursor, the designed redox reaction occurred between the adjacent part of RuO and MoS, forming Ru/RuO hybrid NPs and MoO plane. Therefore, the newly formed Ru/RuO hybrid NPs and MoO plane were tightly combined and used as an electrocatalyst for OWS. Benefiting from the exposed active sites and optimized electronic structure, the RRMC sample annealed at 500 °C (RRMC-500) exhibited low overpotential for HER (18 mV) and for OER (260 mV) at 10 mA cm under alkaline conditions. Especially, a low cell voltage of 1.54 V was required at 10 mA cm under alkaline condition.
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http://dx.doi.org/10.1016/j.jcis.2021.07.038DOI Listing
July 2021

Synthesis of an AIEgen functionalized cucurbit[7]uril for subcellular bioimaging and synergistic photodynamic therapy and supramolecular chemotherapy.

Chem Sci 2021 Apr 21;12(22):7727-7734. Epub 2021 Apr 21.

State Key Laboratory of Quality Research in Chinese Medicine, Institute of Chinese Medical Sciences, University of Macau Taipa Macau 999078 China

Aggregation-induced emission (AIE) based fluorophores (AIEgens) have attracted increasing attention for biomedical applications due to their unique optical properties. Here we report an AIE photosensitizer functionalized CB[7], namely AIECB[7], which could spontaneously self-assemble into nanoaggregates in aqueous solutions. Interestingly, the carbonyl-lace of CB[7] may potentially act as a proton acceptor in an acidic environment to fine-tune the fluorescence and singlet oxygen generation of AIECB[7] nanoaggregates by regulating the inner stacking of AIEgens. Additionally, benefiting from the guest-binding properties of CB[7], oxaliplatin was included into AIECB[7] nanoaggregates for combined photodynamic therapy and supramolecular chemotherapy. To show the modular versatility of this supramolecular system, a hypoxia-activatable prodrug banoxantrone (AQ4N) was loaded into AIECB[7] nanoaggregates, which exhibited synergistic antitumor effects on a multicellular tumor spheroid model (MCTS). This work not only provides AIECB[7] for versatile theranostic applications, but also offers important new insights into the design and development of macrocycle-conjugated AIE materials for diverse biomedical applications.
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http://dx.doi.org/10.1039/d1sc01139aDOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8188462PMC
April 2021

Facile Synthesis of Water-Stable Multicolor Carbonized Polymer Dots from a Single Unconjugated Glucose for Engineering White Light-Emitting Diodes with a High Color Rendering Index.

ACS Appl Mater Interfaces 2021 Jun 18;13(25):30098-30105. Epub 2021 Jun 18.

Green Catalysis Center, and College of Chemistry, Zhengzhou University, Zhengzhou 450001, China.

Tunable emission carbonized polymer dots (CPDs) are highly desirable for the preparation of optoelectronic devices, especially white light-emitting diodes (WLEDs). In most available studies, polychromatic CPDs are synthesized using aromatic molecules as precursors. However, few studies report the successful synthesis of polychromatic CPDs using two or more unconjugated precursors. In this work, we prepare multicolor fluorescent CPDs from a single unconjugated precursor, glucose, via a hydrothermal reaction. By controlling the particle size and degree of graphitization of the synthesized CPDs, their emission wavelength can be tuned in the range 440-625 nm (i.e., almost the entire visible region). Furthermore, the CPDs can be used to construct LEDs of varying colors, including WLEDs (CIE coordinates: 0.34, 0.36) with the correlated color temperature and color rendering index of 4997 K and 92.69, respectively. In brief, the strategy proposed in this study successfully converts unconjugated glucose into high-performance LEDs with great application potential.
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http://dx.doi.org/10.1021/acsami.1c07444DOI Listing
June 2021

Aqueous Self-Assembly of Block Copolymers to Form Manganese Oxide-Based Polymeric Vesicles for Tumor Microenvironment-Activated Drug Delivery.

Nanomicro Lett 2020 Jun 11;12(1):124. Epub 2020 Jun 11.

Green Catalysis Center, College of Chemistry, and Laboratory Animal Center, Zhengzhou University, Zhengzhou, 450001, People's Republic of China.

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http://dx.doi.org/10.1007/s40820-020-00447-9DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7770723PMC
June 2020

Red-light-responsive coordination polymers nanorods: New strategy for ultrasensitive photothermal detection of targeted cancer cells.

Biosens Bioelectron 2021 Oct 8;190:113417. Epub 2021 Jun 8.

State Key Laboratory of Applied Organic Chemistry and Key Laboratory of Nonferrous Metal Chemistry and Resources Utilization of Gansu Province, Lanzhou University, Gansu Lanzhou, 730000, PR China. Electronic address:

The development of highly sensitive and simple detection methods for cancer cells is an important challenge to achieve early cancer diagnosis and effective treatment. In this paper, folic acid (FA)-conjugated platinum (IV) methylene blue (MB) coordination polymers nanorods (denoted as FA-PtCPs NRs) were developed by the photochemical method. The structure of the PtCPs NRs was investigated using the meta-dynamics and genetic algorithms (MTD-GC) method, and it was found that the coordination bond was formed between platinum (IV) and N atoms of MB. The field emission scanning electron microscope (FE-SEM) and transmission electron microscope (TEM) indicated that the morphology of PtCPs NRs was rod-like. The resulting FA-PtCPs NRs was used for the specific and ultra-sensitive temperature detection of cancer cells based on PtCPs NRs as a signal trigger unit and FA as a target recognition tool. After three-step reaction, oxidized 3,3',5,5'-tetramethylbenzidine (ox-TMB) with photothermal effect was obtained. Under 660 nm laser irradiation, such detection platform can convert the molecular recognition signal between FA and folate receptor (FR) of cancer cells into readable temperature value, which can be directly read by an ordinary thermometer, with a detection limit as low as 2 cells/mL. In addition, FA-PtCPs NRs could be used as fluorescent probes for in-situ bioimaging. Therefore, this photothermal sensing platform has a broad prospect in the field of point-of-care detection of cancer cells.
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http://dx.doi.org/10.1016/j.bios.2021.113417DOI Listing
October 2021

The evolution of the concept of stress and the framework of the stress system.

Cell Stress 2021 Apr 26;5(6):76-85. Epub 2021 Apr 26.

Center for Aging Biomedicine, Key Laboratory of Protein Chemistry and Developmental Biology of Fish of Ministry of Education, College of Life Sciences, Hunan Normal University, Changsha, Hunan 410081, China.

Stress is a central concept in biology and has now been widely used in psychological, physiological, social, and even environmental fields. However, the concept of stress was cross-utilized to refer to different elements of the stress system including stressful stimulus, stressor, stress response, and stress effect. Here, we summarized the evolution of the concept of stress and the framework of the stress system. We find although the concept of stress is developed from Selye's "general adaptation syndrome", it has now expanded and evolved significantly. Stress is now defined as a state of homeostasis being challenged, including both system stress and local stress. A specific stressor may potentially bring about specific local stress, while the intensity of stress beyond a threshold may commonly activate the hypothalamic-pituitary-adrenal axis and result in a systematic stress response. The framework of the stress system indicates that stress includes three types: sustress (inadequate stress), eustress (good stress), and distress (bad stress). Both sustress and distress might impair normal physiological functions and even lead to pathological conditions, while eustress might benefit health through hormesis-induced optimization of homeostasis. Therefore, an optimal stress level is essential for building biological shields to guarantee normal life processes.
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http://dx.doi.org/10.15698/cst2021.06.250DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8166217PMC
April 2021

Spatiotemporally controlled O and singlet oxygen self-sufficient nanophotosensitizers enable the high-yield synthesis of drugs and efficient hypoxic tumor therapy.

Chem Sci 2020 Jul 28;11(33):8817-8827. Epub 2020 Jul 28.

State Key Laboratory of Applied Organic Chemistry, Key Laboratory of Nonferrous Metal Chemistry and Resources Utilization of Gansu Province, Lanzhou University Lanzhou Gansu 730000 China

Carrying out the syntheses of drugs toxic to tumors based on the specific features of the tumor microenvironment is critical for ensuring specific antitumor efficacy. However, achieving high-yield synthetic toxic drugs from non-toxic agents and reducing their drug resistance in hypoxic tumors remain challenges. Herein we created a tumor-microenvironment-responsive porous Pt/Pt(iv) methylene blue coordination polymer nanoshuttle (Pt/PtMBCPNS) photosensitizer with spatiotemporally controlled O and singlet oxygen (O) self-sufficient for the high-yield synthesis of drugs and efficient hypoxic tumor therapy. After being endocytosed, the nanophotosensitizer as a cascade catalyst was observed to effectively catalyze the conversion of endogenous HO to O, and was hence found to play a dual role in the enhanced tumor therapy. PtMBCPNSs, upon being irradiated with red light, efficiently converted O into O. Subsequently, O oxidized non-toxic 1,5-dihydroxynaphthalene to form the anticancer agent juglone with a high yield. In addition, O was found to be able to improve the hypoxic microenvironment without light irradiation, thus enhancing the antitumor efficacy of the produced drugs and reducing drug resistance. As a result, by enhancing the synergistic effect of the treatment, this nanophotosensitizer significantly inhibited the growth of tumors and avoided damage to normal tissues/organs. Collectively, this work highlights a robust nanoplatform with the spatiotemporally controlled high-yield synthesis of drugs and generation of O to help overcome the current limitations of chemical-based therapies against hypoxic tumors.
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http://dx.doi.org/10.1039/d0sc02387fDOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8163376PMC
July 2020

Polyamine-Responsive Morphological Transformation of a Supramolecular Peptide for Specific Drug Accumulation and Retention in Cancer Cells.

Small 2021 Jun 10:e2101139. Epub 2021 Jun 10.

State Key Laboratory of Quality Research in Chinese Medicine Institute of Chinese Medical Sciences, University of Macau, Taipa, Macau SAR, 999078, China.

The precise accumulation and extended retention of nanomedicines in the tumor tissue has been highly desired for cancer therapy. Here a novel supramolecular-peptide derived nanodrug (SPN) that can be transformed to microfibers in response to intracellular polyamine in cancer cells for significantly enhanced tumor specific accumulation and retention is developed. The supramolecular-peptide is constructed via the non-covalent interactions between cucurbit[7]uril (CB[7]) and Phe on Phe-Phe-Val-Leu-Lys-camptothecin conjugates (FFVLK-CPT, PC). The resultant amphiphilic supramolecular complex subsequently self-assembles into nanoparticles with a hydrodynamic diameter of 164.2 ± 3.7 nm. Upon internalization into spermine-overexpressed cancer cells, the CB[7]-Phe host-guest pairs can be competitively dissociated by spermine and can release free PC, which immediately form β-sheet structures and subsequently reorganize into microfibers, leading to dramatically improved accumulation, retention, and sustained release of CPT in tumor cells for highly effective cancer therapy. Accordingly, this SPN exhibit rather low toxicity against non-cancerous cells due to the morphological stability and fast exocytosis of the nanodrugs in those cells without abundant spermine. This study reports the first supramolecular peptide capable of polyamine-responsive "nanoparticle-to-microfiber" transformation for specific tumor therapy with minimal side effects. This work also offers novel insights to the design and development of stimuli-responsive nanomaterials as precision medicine.
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http://dx.doi.org/10.1002/smll.202101139DOI Listing
June 2021

Self-Standing Film Assembled using SnS-Sn/Multiwalled Carbon Nanotubes Encapsulated Carbon Fibers: A Potential Large-Scale Production Material for Ultra-stable Sodium-Ion Battery Anodes.

ACS Appl Mater Interfaces 2021 Jun 9;13(24):28359-28368. Epub 2021 Jun 9.

Centre for Future Materials, University of Southern Queensland, Springfield Central, Queensland 4300, Australia.

High-energy sodium-ion batteries have a significant prospective application as a next-generation energy storage technology. However, this technology is severely hindered by the lack of large-scale production of battery materials. Herein, a self-standing film, assembled with SnS-Sn/multiwalled carbon nanotubes encapsulated in carbon fibers (SnS-Sn/[email protected]), is prepared using ball milling and electrospinning techniques and used as sodium-ion battery anodes. To compensate the poor internal conductivity of SnS-Sn nanoparticles, MCNTs are used to interweave SnS-Sn nanoparticles to improve the conductivity. Moreover, the designed three-dimensional carbon fiber conductive network can effectively shorten the diffusion path of electron/Na, accelerate the reaction kinetics, and provide abundant active sites for sodium absorption. Benefiting from these unique features, the self-standing film offers a high reversible capacity of 568 mA h g at 0.1 A g and excellent cycling stability at 1 A g with a reversible capacity of 359.3 mA h g after 1000 cycles. In the sodium-ion full cell device, the capacity is stable at 283.7 mA h g after 100 cycles at a current of 100 mA g. This work provides a new strategy for electrode design and facilitates the large-scale application of the sodium-ion battery.
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http://dx.doi.org/10.1021/acsami.1c07152DOI Listing
June 2021

Boron-nitrogen-doped carbon dots on multi-walled carbon nanotubes for efficient electrocatalysis of oxygen reduction reactions.

J Colloid Interface Sci 2021 Oct 18;600:865-871. Epub 2021 May 18.

Green Catalysis Center, College of Chemistry, Zhengzhou University, No. 100 Science Avenue, Zhengzhou City 450001, China. Electronic address:

Cost-effective production of metal-free catalysts for the oxygen-reduction reaction (ORR), to supersede Pt-based catalysts, is challenging. Here, a three-dimensional nanocatalyst was prepared by compounding multi-wall carbon nanotubes (MWCNTs) with easily modified and doped carbon dots (CDs) as sources of B and N. The catalyst has high conductivity and a large specific surface area similar to the MWCNTs, allowing exposure of many CDs with rich edge active sites and enhancing electron transfer. The catalyst exhibits excellent ORR performance, with 0.92 V of E vs reversible hydrogen electrode (RHE). The E value exhibits a reduction of 50 mV compared with that of Pt/C (0.85 V) with a limited current density of 5.95 mA cm. The enhanced catalytic performance is attributed to the synergy of pyridine N and BC. This work describes a simple and economical strategy for metal-free catalysts, and promotes the development of such catalysts for metal-air batteries and fuel cells.
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http://dx.doi.org/10.1016/j.jcis.2021.05.089DOI Listing
October 2021

New-phase retention in colloidal core/shell nanocrystals pressure-modulated phase engineering.

Chem Sci 2021 Apr 2;12(19):6580-6587. Epub 2021 Apr 2.

State Key Laboratory of Superhard Materials, College of Physics, Jilin University Changchun 130012 China

Core/shell nanocrystals (NCs) integrate collaborative functionalization that would trigger advanced properties, such as high energy conversion efficiency, nonblinking emission, and spin-orbit coupling. Such prospects are highly correlated with the crystal structure of individual constituents. However, it is challenging to achieve novel phases in core/shell NCs, generally non-existing in bulk counterparts. Here, we present a fast and clean high-pressure approach to fabricate heterostructured core/shell MnSe/MnS NCs with a new phase that does not occur in their bulk counterparts. We determine the new phase as an orthorhombic MnP structure (B31 phase), with close-packed zigzagged arrangements within unit cells. Encapsulation of the solid MnSe nanorod with an MnS shell allows us to identify two separate phase transitions with recognizable diffraction patterns under high pressure, where the heterointerface effect regulates the wurtzite → rocksalt → B31 phase transitions of the core. First-principles calculations indicate that the B31 phase is thermodynamically stable under high pressure and can survive under ambient conditions owing to the synergistic effect of subtle enthalpy differences and large surface energy in nanomaterials. The ability to retain the new phase may open up the opportunity for future manipulation of electronic and magnetic properties in heterostructured nanostructures.
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http://dx.doi.org/10.1039/d1sc00498kDOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8133026PMC
April 2021

Cell density-dependent regulation of microcystin synthetase genes (mcy) expression and microcystin-LR production in Microcystis aeruginosa that mimics quorum sensing.

Ecotoxicol Environ Saf 2021 Sep 18;220:112330. Epub 2021 May 18.

Xiang Ya School of Public Health, Central South University, Changsha, Hunan 410078, China; College of Chemistry and Chemical Engineering, Central South University, Changsha, Hunan 410083, China. Electronic address:

As the secondary metabolites of cyanobacterial harmful algal blooms (Cyano-HABs), microcystins (MCs) were generated under various environmental and cellular conditions. The understanding of the causes of MCs generation is of great interest in the field of water treatment and environmental science. In this work, we studied how Microcystis aeruginosa (FACHB-905) cell densities affect the MCs synthetase genes (mcy) expression, microcystin-LR (MC-LR) and quorum sensing molecules (Acyl-homoserine lactones (AHLs)) production. An electrochemical sensor was developed here for sensitive and quantitative detection of MC-LR that cultured at different cell densities. The results showed that mcy expression and MC-LR concentration started to increase when the cell density reached ca. 22 × 10 cells/mL, and was significantly increased with increasing cell densities. Moreover, the up-regulation of AHLs with increasing cell densities revealed that MC-LR is quorum sensing-mediated. Our results undoubtedly confirmed that MC-LR was produced in a cell density-dependent way that mimics quorum sensing, and the minimum cell density (ca. 22 × 10 cells/mL) that was required to produce MC-LR was provided and offered a reference standard for the prevention and control of MCs pollution in the actual water environment.
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http://dx.doi.org/10.1016/j.ecoenv.2021.112330DOI Listing
September 2021

Pressure-Triggered Blue Emission of Zero-Dimensional Organic Bismuth Bromide Perovskite.

Adv Sci (Weinh) 2021 May 15;8(9):2004853. Epub 2021 Feb 15.

Green Catalysis Center and College of Chemistry Zhengzhou University Zhengzhou 450001 P. R. China.

Understanding the structure-property relationships in Zero-dimensional (0D) organic-inorganic metal halide perovskites (s) is essential for their use in optoelectronic applications. Moreover, increasing the emission intensity, particularly for blue emission, is considerably a challenge. Here, intriguing pressure-induced emission () is successfully achieved from an initially nonluminous 0D [(CHNH)BiBr]Br·CHCN ( ) upon compression. The emission intensity increases significantly, even reaching high-efficiency blue luminescence, as the external pressure is increased to 4.9 GPa. Analyses of the high-pressure experiments and first-principle calculations indicate that the observed PIE can be attributed to the enhanced exciton binding energy associated with [BiBr] octahedron distortion under pressure. This study of sheds light on the relationship between the structure and optical properties of s. The results may improve potential applications of such materials in the fields of pressure sensing and trademark security.
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http://dx.doi.org/10.1002/advs.202004853DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8097370PMC
May 2021

Engineering white light-emitting diodes with high color rendering index from biomass carbonized polymer dots.

J Colloid Interface Sci 2021 Sep 9;598:274-282. Epub 2021 Apr 9.

Green Catalysis Center, and College of Chemistry, Zhengzhou University, Zhengzhou 450001, China. Electronic address:

Carbonized polymer dots (CPDs) have promise in the fields of sensing, bioimaging, and optoelectronic devices due to their excellent optical properties, favorable biocompatibility, and superior stability. Biomass CPDs present greater advantages in terms of their lack of toxicity, low cost, easy preparation, and feasibility in terms of luminescence-related applications. Here, two kinds of fluorescent CPDs were obtained through the simple hydrothermal method using biomass avocado peel (CPDs-P) and sarcocarp (CPDs-S) as carbon sources. Interestingly, these two biomass CPDs have excellent applications in ion detection and light-emitting diodes (LEDs). Analysis and results show that CPDs-P possess better sensitivity to Fe because they have more oxygen-containing functional groups. After mixing with epoxy resin, warm and cold white LEDs with CIE (Commission Internationale de L 'Eclairage) coordinates (0.38, 0.39) and (0.29, 0.34) were constructed successfully from extremely stable CPDs-P and CPDs-S. The high color rendering index of the prepared white LEDs are 90.47 and 84.54. This study shows that these biomass CPDs are promising materials in sensing and white LEDs illumination.
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http://dx.doi.org/10.1016/j.jcis.2021.04.022DOI Listing
September 2021

Rational Design of Multicolor-Emitting Chiral Carbonized Polymer Dots for Full-Color and White Circularly Polarized Luminescence.

Angew Chem Int Ed Engl 2021 Jun 10;60(25):14091-14099. Epub 2021 May 10.

Green Catalysis Center, and College of Chemistry, Zhengzhou University, Zhengzhou, 450000, China.

Light-emitting chiral carbonized polymer dots (Ch-CPDs) are attracting great interest because of their extraordinary photonic properties, but modulating their band-gap emission, especially at long wavelength, and maintaining their chiral structure to achieve multicolor, high-emission Ch-CPDs remains challenging. Reported here for the first time is the synthesis of red- and multicolor-emitting Ch-CPDs using the common precursors L-/D-tryptophan and o-phenylenediamine, and a solvothermal approach at one temperature. The quantum yield of the Ch-CPDs was between 31 % and 54 %. Supramolecular self-assembly provided multicolor-emitting Ch-CPDs showing novel circularly polarized luminescence, with the highest dissymmetric factor (g ) of 1×10 . Importantly, circularly polarized white-emitting CPDs were fabricated for the first time by tuning the mixing ratio of the three colored Ch-CPDs in a gel. This strategy affords exciting opportunities for designing functional chiroptical materials.
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http://dx.doi.org/10.1002/anie.202103336DOI Listing
June 2021

The role of Notch ligand Jagged1 in osteosarcoma proliferation, metastasis, and recurrence.

J Orthop Surg Res 2021 Mar 29;16(1):226. Epub 2021 Mar 29.

Department of Orthopedic Surgery, 920th Hospital of Joint Logistics Support Force, Daguan Road 212#, Kunming, 650032, China.

Background: Osteosarcoma is the most common primary bone cancer occurring in young adults and the 5-year survival rate of patients with metastatic osteosarcoma is less than 30% due to high metastatic recurrence and drug resistance. Notch is a highly conserved cell to cell signaling pathway in evolution, and Jagged1 is an important ligand of Notch. Although some studies have found that Notch receptors and ligands including Jagged1 were highly expressed in osteosarcoma tissues and osteosarcoma cells, the role of Jagged1 in osteosarcoma progression and metastasis are still not clear.

Methods: Tumor tissues were collected from 68 patients and immunohistochemical staining was employed to group these patients by expression of Jagged1. Real-time quantitative PCR and Western blotting were used to detect the expression of Jagged1. We used siRNA to knockdown the expression of Jagged1 in F5M2 cells. Colony formation assay and MTT were employed to detect and analyze the proliferation of F5M2 cells with or without knockdown of Jagged1. Transwell assay were used to detect the migration and invasion of F5M2 cells.

Results: In this study, we found that the high expression of Jagged1 is closely related to the metastasis and recurrence of osteosarcoma in 68 clinical specimens. The expression of Jagged1 in F5M2 cells with high metastasis was significantly higher than that in F4 cells with low metastasis. Knockdown of Jagged1 led to lower ability of proliferation, migration, and invasion in F5M2 cells.

Conclusion: The high expression of Jagged1 is closely related to the metastasis and recurrence of osteosarcoma. Knockdown of Jagged1 significantly reduced the proliferation, migration, and invasion of osteosarcoma cells. Our results suggested that knockdown of Jagged1 may be a potentially effective treatment for metastatic osteosarcoma.
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http://dx.doi.org/10.1186/s13018-021-02372-yDOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC8006358PMC
March 2021

Suppressing Water Dissociation via Control of Intrinsic Oxygen Defects for Awakening Solar H O-to-H O Generation.

Small 2021 Apr 9;17(13):e2100400. Epub 2021 Mar 9.

MIIT Key Laboratory of Advanced Display Material and Devices, College of Materials Science and Engineering, Nanjing University of Science and Technology, Nanjing, 210094, P. R. China.

BiVO theoretically has a thermodynamic activity trend toward highly selective water oxidative H O formation, but it is more inclined to generate O in practical. The influence of intrinsic oxygen vacancy (O ), especially, on surface reactivity, has never been considered as a possible activity loss mechanism in the synthetic BiVO . In this work, it is theoretically and experimentally demonstrated that the intrinsic surface O is responsible for lower H O evolution activity via promoting water dissociation to form intermediate. Through an annealing process under a V O rich atmosphere, the surface O can be eliminated that awakens the photoelectrochemical (PEC) water oxidative H O activity in a NaHCO electrolyte, which achieves an average of 58.4%, and increases by up to 4.28 times of the one annealed in air. This work offers a general understanding of catalytic activity loss and may be extended to other photo or electrocatalysts for catalytic selectivity regulation.
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http://dx.doi.org/10.1002/smll.202100400DOI Listing
April 2021

Efficient Combination of G-C N and CDs for Enhanced Photocatalytic Performance: A Review of Synthesis, Strategies, and Applications.

Small 2021 Mar 8:e2007523. Epub 2021 Mar 8.

Green Catalysis Center, College of Chemistry, Zhengzhou University, Zhengzhou, 450001, P. R. China.

Recently, heterogeneous photocatalysts have achieved much interest on account of their great potential applications in resolving many tough energy and environmental troubles around the world through an ecologically sustainable way. Heterogeneous nanocomposites composed of graphitic carbon nitride (g-C N ) and carbon dots (CDs) possess broad spectrum absorption, appropriate electronic band structures, rapid carrier mobility, abundant reserves, excellent chemical stability, and facile synthesis methods, which make them promising composite photocatalysts for suitable applications such as photocatalytic solar fuels production and contaminant decomposition. With the rapid development in photocatalysis by hybridization of g-C N and CDs, a systematic summary and prospection of performance improvement are urgent and meaningful. This review first focuses on various kinds of effectively synthetic methods of composites. Following, the strategies available for enhanced performance, including morphology optimization, spectral absorption improvement, ternary or quaternary composition hybrid, lateral or vertical heterostructures construction, heteroatom doping, and so forth, are fully discussed. Then, the applications mainly in efficient photocatalytic hydrogen generation, photocatalytic carbon dioxide reduction, and organic pollutants degradation are systematically demonstrated. Finally, the remaining issues and prospect of further development are proposed as some kind of guidance for powerful combination of g-C N and CDs with high efficiency to photocatalysis.
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http://dx.doi.org/10.1002/smll.202007523DOI Listing
March 2021

Recent advances in perovskite oxides as electrode materials for supercapacitors.

Chem Commun (Camb) 2021 Mar 17;57(19):2343-2355. Epub 2021 Feb 17.

School of Physics and Electrical Engineering, Chongqing Normal University, Chongqing 401331, China.

Owing to the high power density and ultralong cycle life, supercapacitors represent an alternative to electrochemical batteries in energy storage applications. However, the relatively low energy density is the main challenge for supercapacitors in the current drive to push the entire technology forward to meet the benchmark requirements for commercialization. To effectively solve this issue, it is crucial to develop electrode materials with excellent electrochemical performance since the electrode used is closely related to the specific capacitance and energy density of supercapacitors. With the unique structure, compositional flexibility, and inherent oxygen vacancy, perovskite oxides have attracted wide attention as promising electrode materials for supercapacitors. In this review, we summarize the recent advances in perovskite oxides as electrode materials for supercapacitors. Firstly, the structures and compositions of perovskite oxides are critically reviewed. Following this, the progress in various perovskite oxides, including single perovskite and derivative perovskite oxides, is depicted, focusing on their electrochemical performance. Furthermore, several optimization strategies (i.e., modulating the stoichiometry of the anion or cation, A-site doping, B-site doping, and constructing composites) to improve their electrochemical performance are also discussed. Finally, the significant challenges facing the advancement of perovskite oxide electrodes for supercapacitor applications and future outlook are proposed.
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http://dx.doi.org/10.1039/d0cc07970gDOI Listing
March 2021

Single Atom Ruthenium-Doped CoP/CDs Nanosheets via Splicing of Carbon-Dots for Robust Hydrogen Production.

Angew Chem Int Ed Engl 2021 Mar 24;60(13):7234-7244. Epub 2021 Feb 24.

Green Catalysis Center, and College of Chemistry, Zhengzhou University, Zhengzhou, 450000, China.

Ultrathin two-dimensional catalysts are attracting attention in the field of electrocatalytic hydrogen evolution. This work describe a composite material design in which CoP nanoparticles doped with Ru single-atom sites supported on carbon dots (CDs) single-layer nanosheets formed by splicing CDs (Ru CoP/CDs). Small CD fragments bore abundant functional groups, analogous to pieces of a jigsaw puzzle, and could provide a high density of binding sites to immobilize Ru CoP. The single-particle-thick nanosheets formed by splicing CDs acted as supports, which improved the conductivity of the electrocatalyst and the stability of the catalyst during operation. The Ru CoP/CDs formed from doping atomic Ru dispersed on CoP showed very high efficiency for the hydrogen evolution reaction (HER) over a wide pH range. The catalyst prepared under optimized conditions displayed outstanding stability and activity: the overpotential for the HER at a current density of 10 mA cm was as low as 51 and 49 mV under alkaline and acidic conditions, respectively. Density functional theory calculations showed that the substituted Ru single atoms lowered the proton-coupled electron transfer energy barrier and promoted H-H bond formation, thereby enhancing catalytic performance for the HER. The findings open a new avenue for developing carbon-based hybridization materials with integrated electrocatalytic performance for water splitting.
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http://dx.doi.org/10.1002/anie.202017102DOI Listing
March 2021

Rational Design of Multi-Color-Emissive Carbon Dots in a Single Reaction System by Hydrothermal.

Adv Sci (Weinh) 2020 Jan 23;8(1):2001453. Epub 2020 Nov 23.

Green Catalysis Center and College of Chemistry Zhengzhou University Zhengzhou 450000 China.

As an emerging building unit, carbon dots (CDs) have been igniting the revolutionaries in the fields of optoelectronics, biomedicine, and bioimaging. However, the difficulty of synthesizing CDs in aqueous solution with full-spectrum emission severely hinders further investigation of their emission mechanism and their extensive applications in white light emitting diodes (LEDs). Here, the full-color-emission CDs with a unique structure consisting of -hybridized carbon cores with small domains of partially -hybridized carbon atoms are reported. First-principle calculations are initially used to predict that the transformation from to hybridization redshifts the emission of CDs. Guided by the theoretical predictions, a simple, convenient, and controllable route to hydrothermally prepare CDs in a single reaction system is developed. The prepared CDs have full-spectrum emission with an unprecedented two-photon emission across the whole visible color range. These full-color-emission CDs can be further nurtured by slight modifications of the reaction conditions (e.g., temperature, pH) to generate the emission color from blue to red. Finally a flexible LEDs with full-color emission by using epoxy CDs films is developed, indicating that the strategy affords an industry translational potential over traditional fluorophores.
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http://dx.doi.org/10.1002/advs.202001453DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7788586PMC
January 2020

Recent advances in supramolecular antidotes.

Theranostics 2021 1;11(3):1513-1526. Epub 2021 Jan 1.

State Key Laboratory of Quality Research in Chinese Medicine, Institute of Chinese Medical Sciences, University of Macau, Taipa, Macau, China.

Poisons always have fascinated humankind. Initially considered as deleterious or hazardous substances, the modern era has witnessed the controlled utilization of dangerous poisons in medicine and cosmetics. Simultaneously, antidotes have become crucial as reversal agents to counteract the effects of a poison, and they are also used today to positively cancel the benefits of a poison after use. Currently, the majority of poisons are composed of small molecules. This review focuses on recent developments to reverse or prevent toxic effects of poisons by encapsulation in host molecules. Cyclodextrins, cucurbiturils, acyclic cucurbituril derivatives, calixarenes, and pillararenes, have been reported to largely impact the effects of toxic compounds, thus extending the current paradigm of small molecule antidotes by adding a new family of macrocyclic compounds to the current arsenal of antidotes. Along this line of research, endogenous "harmful" species are also sequestered by one or more of these supramolecular host molecules, expanding the potential of supramolecular antidotes to diverse therapeutic areas.
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http://dx.doi.org/10.7150/thno.53459DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7738896PMC
July 2021

CCTs as new biomarkers for the prognosis of head and neck squamous cancer.

Open Med (Wars) 2020 13;15(1):672-688. Epub 2020 Jul 13.

Department of Otolaryngology Head and Neck Surgery, Beijing Friendship Hospital, Capital Medical University, 95th Yong'an Road, Xicheng District, Beijing 100050, China.

The chaperonin-containing T-complex protein 1 (CCT) subunits participate in diverse diseases. However, little is known about their expression and prognostic values in human head and neck squamous cancer (HNSC). This article aims to evaluate the effects of CCT subunits regarding their prognostic values for HNSC. We mined the transcriptional and survival data of CCTs in HNSC patients from online databases. A protein-protein interaction network was constructed and a functional enrichment analysis of target genes was performed. We observed that the mRNA expression levels of CCT1/2/3/4/5/6/7/8 were higher in HNSC tissues than in normal tissues. Survival analysis revealed that the high mRNA transcriptional levels of CCT3/4/5/6/7/8 were associated with a low overall survival. The expression levels of CCT4/7 were correlated with advanced tumor stage. And the overexpression of CCT4 was associated with higher N stage of patients. Validation of CCTs' differential expression and prognostic values was achieved by the Human Protein Atlas and GEO datasets. Mechanistic exploration of CCT subunits by the functional enrichment analysis suggests that these genes may influence the HNSC prognosis by regulating PI3K-Akt and other pathways. This study implies that CCT3/4/6/7/8 are promising biomarkers for the prognosis of HNSC.
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http://dx.doi.org/10.1515/med-2020-0114DOI Listing
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7706129PMC
July 2020

Transformable Honeycomb-Like Nanoassemblies of Carbon Dots for Regulated Multisite Delivery and Enhanced Antitumor Chemoimmunotherapy.

Angew Chem Int Ed Engl 2021 03 16;60(12):6581-6592. Epub 2021 Feb 16.

Green Catalysis Center, College of Chemistry, Zhengzhou University, Zhengzhou, 450001, China.

Tumor fibrotic stroma forms complex barriers for therapeutic nanomedicine. Although nanoparticle vehicles are promising in overcoming biological barriers for drug delivery, fibrosis causes hypoxia, immunosuppression and limited immunocytes infiltration, and thus reduces antitumor efficacy of nanosystems. Herein, we report the development of cancer-associated fibroblasts (CAFs) responsive honeycomb-like nanoassemblies of carbon dots (CDs) to spatially program the delivery of multiple therapeutics for enhanced antitumor chemoimmunotherapy. Doxorubicin (DOX) and immunotherapeutic enhancer (Fe ions) are immobilized on the surface of CDs, whereas tumor microenvironment modifier (losartan, LOS) is encapsulated within the mesopores. The drugs-loaded nanoassemblies disassociate into individual CDs to release LOS to mitigate stroma and hypoxia in response to CAFs. The individual CDs carrying DOX and Fe ion efficiently penetrate deep into tumor to trigger intensified immune responses. Our in vitro and in vivo studies show that the nanoassemblies exhibit effective T cells infiltration, tumor growth inhibition and lung metastasis prevention, thereby providing a therapeutic platform for desmoplasia solid tumor.
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http://dx.doi.org/10.1002/anie.202014397DOI Listing
March 2021

Tumor Microenvironment-"AND" Near-Infrared Light-Activated Coordination Polymer Nanoprodrug for On-Demand CO-Sensitized Synergistic Cancer Therapy.

Adv Healthc Mater 2021 04 11;10(7):e2001728. Epub 2020 Dec 11.

State Key Laboratory of Applied Organic Chemistry, Key Laboratory of Nonferrous Metal Chemistry and Resources Utilization of Gansu Province, Lanzhou University, Gansu, Lanzhou, 730000, China.

Carbon monoxide (CO) as an emerging treatment holds great promise for inducing the apoptosis of cancer cells. Here coordination assembled strategy is first reported for synthesis of Cu(II)-flavone coordination polymer (NCu-FleCP) CO nanoprodrug that is stable in normal physiological conditions, and yet readily reduces to small size prodrug complex and releases CO on demand under glutathione (GSH) and near infrared (NIR) light. Specifically, after uptaking by cancer cells, local GSH attacked coordination bond within NCu-FleCP, resulting in the release of Cu(I) and free Fle. The CC bond of Fle is cleavage under NIR light to release CO for gas therapy, and Cu(I) reacts with local H O through Fenton like reaction to generate hydroxyl radicals ( OH) for chemodynamic therapy. Detailed in vitro and in vivo experiments demonstrate that the CO prodrug system in generating a sufficient quantity of CO and OH offers remarkable destructive effects against cancer cells without causing toxicity to surrounding normal tissues. The study provides a solid foundation to develop smart coordination polymer CO prodrugs with on-demand CO release, enhanced permeability and retention effect, and biodegradability for multimodal synergistic therapy.
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http://dx.doi.org/10.1002/adhm.202001728DOI Listing
April 2021

Photoacoustic Cavitation-Ignited Reactive Oxygen Species to Amplify Peroxynitrite Burst by Photosensitization-Free Polymeric Nanocapsules.

Angew Chem Int Ed Engl 2021 02 7;60(9):4720-4731. Epub 2021 Jan 7.

Guangdong Provincial Key Laboratory of Laser Life Science, MOE Key Laboratory of Laser Life Science & Institute of Laser Life Science, College of Biophotonics, South China Normal University, Guangzhou, 510631, China.

Photoacoustic (PA) technology can transform light energy into acoustic wave, which can be used for either imaging or therapy that depends on the power density of pulsed laser. Here, we report photosensitizer-free polymeric nanocapsules loaded with nitric oxide (NO) donors, namely NO-NCPs, formulated from NIR light-absorbable amphiphilic polymers and a NO-releasing donor, DETA NONOate. Controlled NO release and nanocapsule dissociation are achieved in acidic lysosomes of cancer cells. More importantly, upon pulsed laser irradiation, the PA cavitation can excite water to generate significant reactive oxygen species (ROS) such as superoxide radical (O ), which further spontaneously reacts with the in situ released NO to burst highly cytotoxic peroxynitrite (ONOO ) in cancer cells. The resultant ONOO generation greatly promotes mitochondrial damage and DNA fragmentation to initiate programmed cancer cell death. Apart from PA imaging, PA cavitation can intrinsically amplify reactive species via photosensitization-free materials for promising disease theranostics.
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http://dx.doi.org/10.1002/anie.202013301DOI Listing
February 2021

A regenerable ion-imprinted magnetic biocomposite for selective adsorption and detection of Pb in aqueous solution.

J Hazard Mater 2021 04 28;408:124410. Epub 2020 Oct 28.

Collaborative Research Center, Shanghai University of Medicine and Health Sciences, Pudong, Shanghai 201318, China. Electronic address:

A regenerable ion-imprinted magnetic biocomposite (IIMB) was successfully synthesized for simultaneous removal of Pb using Serratia marcescens and carboxymethyl chitosan (CMC) as functional carriers, Pb was utilized as the imprinted ion, while FeO served as the magnetic component. The structure and properties of IIMB were characterized by various techniques. The adsorption kinetics, isotherms and thermodynamics were applied to interpret the Pb adsorption process on IIMB. The results showed the IIMB possessed prominent uptake ability toward Pb. The pseudo-second-order kinetic (R = 0.9989) and Langmuir models (R = 0.9555) fitted the data well. Adsorption thermodynamics revealed that the adsorption was a spontaneous endothermic reaction. The possible adsorption mechanisms involved physical adsorption, electrostatic attraction and complexing. Moreover, because Pb can be specifically and strongly adsorbed on IIMB, a simple method for detection of Pb was established by coupling IIMB with flame atomic absorption spectrometry (IIMB-FAAS). The developed IIMB-FAAS assay can sensitively detect Pb with a linear range from 5.0 to 500.0 μg/L. The detection limit (LOD) of 0.95 μg/L as well as a quantification limit (LOQ) of 3.20 μg/L were obtained. This work proved that the IIMB could selective and efficient adsorb Pb, which provided some insights into wastewater treatment, water quality inspection and environmental remediation.
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http://dx.doi.org/10.1016/j.jhazmat.2020.124410DOI Listing
April 2021

Electrochemical non-enzymatic glucose sensors: recent progress and perspectives.

Chem Commun (Camb) 2020 Dec 29;56(93):14553-14569. Epub 2020 Oct 29.

Key Laboratory of Magnetic Molecules and Magnetic Information Materials (Ministry of Education), School of Chemistry and Material Science, Shanxi Normal University, Linfen 041004, Shanxi, China.

The detection of glucose has important significance in clinical medicine and the food industry, especially in the diagnosis of diabetes. In recent years, electrochemical non-enzymatic glucose sensors have attracted intensive attention to detect the glucose level with great progress. In this review, we summarize a variety of non-enzymatic glucose sensor materials, including precious metals Pt, Au and their alloy metals, non-precious transition metals and their metal oxides, composites and other functional materials. Moreover, fundamental insights into the reaction mechanism and influencing factors of materials are given. Finally, this review discusses the perspectives and challenges of future developments in electrochemical non-enzymatic glucose detection.
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http://dx.doi.org/10.1039/d0cc05650bDOI Listing
December 2020

Exploiting Ru-Induced Lattice Strain in CoRu Nanoalloys for Robust Bifunctional Hydrogen Production.

Angew Chem Int Ed Engl 2021 Feb 8;60(6):3290-3298. Epub 2020 Dec 8.

Green Catalysis Center, and College of Chemistry, Zhengzhou University, Zhengzhou, 450000, China.

Designing bifunctional catalysts capable of driving the electrochemical hydrogen evolution reaction (HER) and also H evolution via the hydrolysis of hydrogen storage materials such as ammonia borane (AB) is of considerable practical importance for future hydrogen economies. Herein, we systematically examined the effect of tensile lattice strain in CoRu nanoalloys supported on carbon quantum dots (CoRu/CQDs) on hydrogen generation by HER and AB hydrolysis. By varying the Ru content, the lattice parameters and Ru-induced lattice strain in the CoRu nanoalloys could be tuned. The CoRu /CQDs catalyst with an ultra-low Ru content (1.33 wt.%) exhibited excellent catalytic activity for HER (η=18 mV at 10 mA cm in 1 M KOH) and extraordinary activity for the hydrolysis of AB with a turnover frequency of 3255.4 mol  mol  min or 814.7 mol  mol  min at 298 K, respectively, representing one of the best activities yet reported for AB hydrolysis over a ruthenium alloy catalyst. Moreover, the CoRu /CQDs catalyst displayed excellent stability during each reaction, including seven alternating cycles of HER and AB hydrolysis. Theoretical calculations revealed that the remarkable catalytic performance of CoRu /CQDs resulted from the optimal alloy electronic structure realized by incorporating small amounts of Ru, which enabled fast interfacial electron transfer to intermediates, thus benefitting H evolution kinetics. Results support the development of new and improved catalysts HER and AB hydrolysis.
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http://dx.doi.org/10.1002/anie.202013985DOI Listing
February 2021

Enhanced electrocatalytic N-to-NH fixation by ZrS nanofibers with a sulfur vacancy.

Chem Commun (Camb) 2020 Nov;56(90):14031-14034

Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 610054, Sichuan, China.

Industrially, large-scale NH3 production is achieved by the Haber-Bosch process, which operates under harsh reaction conditions with abundant energy consumption and CO2 emission. Electrochemical N2 reduction is an eco-friendly and energy-saving method for artificial N2 to NH3 fixation under ambient reaction conditions. Herein, we demonstrate that ZrS2 nanofibers with a sulfur vacancy (ZrS2 NF-Vs) behave as an efficient electrocatalyst for ambient N2 reduction to NH3 with excellent selectivity. In 0.1 M HCl, this ZrS2 NF-Vs catalyst attains a large NH3 yield of 30.72 μg h-1 mgcat.-1 and a high faradaic efficiency of 10.33% at -0.35 V and -0.30 V vs. reversible hydrogen electrode, respectively. It also shows high electrochemical and structural stability. The density functional theory calculations reveal that the introduction of Vs facilitates the adsorption and activation of N2 molecules.
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http://dx.doi.org/10.1039/d0cc05917jDOI Listing
November 2020
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