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1.
J Colloid Interface Sci ; 668: 161-170, 2024 Aug 15.
Article in English | MEDLINE | ID: mdl-38677205

ABSTRACT

CO2-to-high value-added chemicals via a photocatalytic route is of interest but strangled by the low efficiency. Herein, a novel Fe-TiO2-x/TiO2 S-scheme homojunction was designed and constructed by using a facile surface modification approach whereby oxygen vacancy (OV) and Fe introducing on the TiO2 nanorod surface. The as-synthesized Fe-TiO2-x/TiO2 S-scheme homojunction exhibits positive properties on promoting photocatalytic CO2 reduction: i) the nanorod structure provides numerous active sites and a radical charge transfer path; ii) the doped Fe and OV not only synergistically enhance light utilization but also promote CO2 adsorption; iii) the Fe-TiO2-x/TiO2 S-scheme homojunction benefits photoexcited charge separation and retains stronger redox capacity. Thanks to those good characters, the Fe-TiO2-x/TiO2 homojunction exhibits superior CO2 reduction performances with optimized CO/CH4 generation rates of 122/22 µmol g-1h-1 which exceed those of pure TiO2 by more than 9.4/7.3 folds and most currently reported catalytic systems. This manuscript develops a facile and universal approach to synthesize well-defined homojunction and may inspire the construction of other more high-efficiency photocatalysts toward CO2 reduction and beyond.

2.
Langmuir ; 40(12): 6363-6374, 2024 Mar 26.
Article in English | MEDLINE | ID: mdl-38470241

ABSTRACT

The programmed self-assembly of patchy nanoparticles (NPs) through a bottom-up approach is an efficient strategy for producing highly organized materials with a predetermined architecture. Herein, we report the preparation of di- and trivalent silica NPs with polystyrene (PS)/poly(4-vinylbenzyl azide) (PVBA) patches and assemble them in a THF mixture by lowering the solvent quality. Silica-PS/PVBA colloidal hybrid clusters were synthesized through the seeded growth emulsion copolymerization of styrene and 4-vinylbenzyl azide (VBA) in varying ratios. Subsequently, macromolecules on silica NPs originating from the copolymerization of growing PS or PVBA chains with the surface-grafted MMS compatibilizer are engineered by fine-tuning of polymer compositions or adjustment of solvent qualities. Moreover, multistage silica regrowth of tripod and tetrapod allowed a fine control of the patch-to-particle size ratio ranging from 0.69 to 1.54. Intriguingly, patchy silica NPs (1-, 2-, 3-PSNs) rather than hybrid clusters are successfully used as templates for multistep regrowth experiments, leading to the formation of silica NPs with a new morphology and size controllable PVBA/PS patches. Last but not least, combined with mesoscale dynamics simulations, the self-assembly kinetics of 2-PSN and 3-PSN into linear colloidal polymers and honeycomb-like lattices are studied. This work paves a new avenue for constructing colloidal polymers with a well-defined sequence and colloidal crystals with a predetermined architecture.

3.
Molecules ; 29(4)2024 Feb 07.
Article in English | MEDLINE | ID: mdl-38398515

ABSTRACT

Much experimental work has been contributed to all-metal σ, π and δ-aromaticity among transition metals, semimetallics and other metals in the past two decades. Before our focused investigations on the properties of triangular and sandwich-shaped all-metal aromatics, A. I. Boldyrev presented general discussions on the concepts of all-metal σ-aromaticity and σ-antiaromaticity for metallo-clusters. Schleyer illustrated that Nucleus-Independent Chemical Shifts (NICS) were among the most authoritative criteria for aromaticity. Ugalde discussed the earlier developments of all-metal aromatic compounds with all possible shapes. Besides the theoretical predictions, many stable all-metal aromatic trinuclear clusters have been isolated as the metallic analogues of either the σ-aromatic molecule's [H3]+ ion or the π-aromatic molecule's [C3H3]+ ion. Different from Hoffman's opinion on all-metal aromaticity, triangular all-metal aromatics were found to hold great potential in applications in coordination chemistry, catalysis, and material science. Triangular all-metal aromatics, which were theoretically proved to conform to the Hückel (4n + 2) rule and possess the smallest aromatic ring, could also play roles as stable ligands during the formation of all-metal sandwiches. The triangular and sandwich-shaped all-metal aromatics have not yet been specifically summarized despite their diversity of existence, puissant developments and various interesting applications. These findings are different from the public opinion that all-metal aromatics would be limited to further applications due to their overstated difficulties in synthesis and uncertain stabilities. Our review will specifically focus on the summarization of theoretical predictions, feasible syntheses and isolations, and multiple applications of triangular and sandwich shaped all-metal aromatics. The appropriateness and necessities of this review will emphasize and disseminate their importance and applications forcefully and in a timely manner.

4.
iScience ; 27(1): 108774, 2024 Jan 19.
Article in English | MEDLINE | ID: mdl-38261948

ABSTRACT

In the winter months, the temperature in most of the Earth stays below 0°C; the average temperature in winter at the South Pole is about -60°C. Therefore, it is urgent to develop efficient catalytic systems for selective and efficient H2 evolution upon NH3BH3 hydrolysis at subzero temperatures. For solving the freezing issue of water at below 0°C, herein, we have employed a facile and surfactant-free approach to synthesize M-Pt/C nanocomposites (M = Pd, Rh, Ru, Ni, Cu, or Fe), by the alloying of commercial Pt/C with Pd, Rh, Ru, Cu, Ni, or Fe for selective and efficient H2 evolution upon NH3BH3 hydrolysis in saline solution at below 0°C, even at -15°C. In addition, NH3BH3 hydrolysis over Pd-Pt/C in the saturated NaCl solution is utilized not only for safe hydrogen production but also for its in situ hydrogenation reduction in organic chemistry, which could avoid using dangerous hydrogen cylinders.

5.
Adv Sci (Weinh) ; 11(12): e2306893, 2024 Mar.
Article in English | MEDLINE | ID: mdl-38225898

ABSTRACT

H2 generation from methanol-water mixtures often requires high pressure and high temperature (200-300 °C). However, CO can be easily generated and poison the catalytic system under such high temperature. Therefore, it is highly desirable to develop the efficient catalytic systems for H2 production from methanol at room temperature, even at sub-zero temperatures. Herein, carbon nanotube-supported Pt nanocomposites are designed and synthesized as high-performance nano-catalysts, via stabilization of Pt nanoparticles onto carbon nanotube (CNT), for H2 production upon methanol dehydrogenation at sub-zero temperatures. Therein, the optimal Pt/CNT nanocomposite presents the superior catalytic performance in H2 production upon methanol dehydrogenation at the expense of B2(OH)4, with the TOF of 299.51 min-130 oC. Compared with other common carriers, Pt/CNT exhibited the highest catalytic performance in H2 production, emphasizing the critical role of CNT in methanol dehydrogenation. The confinement of Pt nanoparticles by CNTs is conducive to inhibiting the aggregation of Pt nanoparticles, thereby significantly increasing its catalytic performance and stability. The kinetic study, detailed mechanistic insights, and density functional theory (DFT) calculation confirm that the breaking of O─H bond of CH3OH is the rate-controlling step for methanol dehydrogenation, and both H atoms of H2 are supplied by methanol. Interestingly, H2 is also successfully produced from methanol dehydrogenation at -10 °C, which absolutely solves the freezing problem in the H2 evolution upon water-splitting reaction.

6.
Nanoscale ; 15(39): 15975-15981, 2023 Oct 12.
Article in English | MEDLINE | ID: mdl-37782093

ABSTRACT

Although sodium formate is widely used as a conventional additive to enhance selective H2 evolution from HCOOH dehydrogenation, this leads to a waste of resources and an increase in the cost of H2 production. For this reason, N-doped carbon nanospheres with abundant graphitic C/N have been designed to enrich the electron cloud density of the Pd atom for improving its catalytic activity in H2 generation upon additive-free HCOOH dehydrogenation. Herein, we have synthesized N-doped carbon nanosphere-stabilized Pd nanoparticles (Pd/NCSs) as high-efficiency nano-catalysts, via fixation of Pd nanoparticles onto N-doped carbon nanospheres (NCSs), for selective and controlled H2 generation upon additive-free HCOOH dehydrogenation. Pd/NCS-800 (1640 h-1) provided a 12 times larger TOF than commercial Pd/C (134 h-1) in H2 generation upon additive-free HCOOH dehydrogenation. It seemed that graphitic N/C of NCS-800 enriched the electron cloud density of the Pd atom, which was favorable for the cleavage of C-H bonds in HCOOH dehydrogenation. In addition, the selective H2 evolution from additive-free HCOOH dehydrogenation over Pd/NCS-800 is successfully controlled by adjusting the pH.

7.
RSC Adv ; 13(42): 29689-29694, 2023 Oct 04.
Article in English | MEDLINE | ID: mdl-37822652

ABSTRACT

A series of sulfonate anions paired aromatic triangular palladium clusters 3-7, abbreviated as [Pd3]+[ArSO3]-, were synthesized using a simple "one pot" method, and gave excellent isolated yields (90-95%). Their structures and properties have been fully characterized and further investigated by fluorescence, single crystal X-ray Diffraction (XRD) and X-ray Photoelectron Spectroscopy (XPS). In varying organic solvents, they presented apparently stronger absorption and emission in MeOH, driven by the combined interactions of hydrogen bonds and polarity. The crystallographic data demonstrated that the methyl orange ion stabilized complex 7 possessed a D3h symmetric metallic core which was still coplanar and almost equilateral, jointly influenced by the giant hindrance and milder donating effect from the sulfonate. The binding energies for Pdn+ 3d5/2 and Pdn+ 3d3/2 measured by XPS presented at 336.55 and 342.00 eV, respectively. These data were much lower than that of a usual Pd2+ 3d and significantly higher than that of a Pd0 species, further proving the unified palladium valence state (+4/3) in the tri-palladium core and its aromaticity featured by the cyclic electron delocalization.

8.
Inorg Chem ; 62(42): 17555-17564, 2023 Oct 23.
Article in English | MEDLINE | ID: mdl-37822237

ABSTRACT

Although a range of noble metal catalysts, including Ru, Rh, Pd, Pt, and Au, have been developed for efficient H2 generation upon NH3BH3 hydrolysis at room temperature, this is a highly urgent need for exploring earth-abundant metal nanocatalysts for H2 generation upon NH3BH3 hydrolysis. Herein, a NaBH4 reduction strategy was developed to boost the catalytic performance of NiMoO4 nanorods in H2 generation upon NH3BH3 hydrolysis. Indeed, the pristine NiMoO4 nanorods were catalytically inert in NH3BH3 hydrolysis. Significantly, the reduced NiMoO4 nanorods presented excellent catalytic activity in H2 generation upon NH3BH3 hydrolysis, with a turnover frequency (TOF) of 31.2 L(H2)·gcat-1·h-1. Interestingly, the TOF of NH3BH3 hydrolysis over reduced NiMoO4 nanorods significantly increased from 31.2 to 53.6 L(H2)·gcat-1·h-1 under 0.3 M NaOH. The boosting catalytic performance of NiMoO4 nanorods via NaBH4 reduction in H2 generation might be attributed to the higher content of Oads and the formation of nickel boride in the reduced NiMoO4 nanorods. In this work, NH3BH3 hydrolysis over reduced NiMoO4 nanorods was not only used for safe H2 generation but also for its in situ tandem hydrogenation in organic chemistry.

9.
Molecules ; 28(9)2023 May 06.
Article in English | MEDLINE | ID: mdl-37175337

ABSTRACT

The burgeoning need to study the applications of nanoparticles (NPs) in biomedical and pharmaceutical fields requires an understanding of their interactions with lipid membranes for further in vivo studies. In this paper, negatively charged egg yolk lecithin liposome (EYL) has been prepared and used as model lipid membranes. Positively charged Mg3Al-layered double hydroxides (LDHs) are viewed as models of clay particles. The ability of the LDH NPs, a two-dimensional nanostructure with an average diameter of 100 nm (LDHs-100) or 500 nm (LDHs-500) to cross the membranes, has been thoroughly investigated via (high-resolution) transmission electron microscopy (TEM), optical microscopy (OM), scanning electron microscopy (SEM), confocal fluorescence microscopy (CLSM), and dynamic light scattering (DLS). The liposomes with an average diameter of 1.5 µm were prepared by the thin-film rehydration method followed by an extrusion technique. A calcein leakage assay and steady-state fluorescence measurement displayed the variation of membrane integrity and polarity of the pyrene-located microenvironment during the interaction between EYL and calcein-interacted LDH NPs (CE-LDHs) or LDH NPs, respectively. These results imply that not only spherical particles but also even more sophisticated nanostructured materials are able to effectively cross the lipid bilayers, thereby engineering new compounds that may be encapsulated for safe and potential use in biomedical applications.


Subject(s)
Liposomes , Nanoparticles , Liposomes/chemistry , Lecithins , Egg Yolk , Hydroxides/chemistry , Nanoparticles/chemistry
10.
RSC Adv ; 13(21): 14060-14064, 2023 May 09.
Article in English | MEDLINE | ID: mdl-37179997

ABSTRACT

Carbon anions formed via the addition of Grignard reagents to SP-vinyl phosphinates were modified with electrophilic reagents to afford organophosphorus compounds with diverse carbon skeletons. The electrophiles included acids, aldehydes, epoxy groups, chalcogens and alkyl halides. When alkyl halides were used, bis-alkylated products were afforded. Substitution reactions or polymerization occurred when the reaction was applied to vinyl phosphine oxides.

11.
iScience ; 26(4): 106504, 2023 Apr 21.
Article in English | MEDLINE | ID: mdl-37091254

ABSTRACT

Sodium formate (SF) is regarded as a technological additive to improve H2 generation upon HCOOH dehydrogenation. The development of SF as a hydrogen storage material is still a challenge. Herein, we report the design and synthesis of carbon nanosphere-stabilized Pd nanoparticles (Pd/CNS) for the direct H2 generation upon SF hydrolysis in the presence of Fe3+. The tandem reaction, isotopic mass spectrometry, and gas chromatograms result confirmed that SF hydrolysis generates H2 with one H atom provided by SF and other H by H2O. The kinetic study and detailed mechanistic investigations have demonstrated that the concerted process between the cleavage of O-H bond in H2O and -O2C-H bond oxidative addition is the rate-controlling step in SF hydrolysis. This work offers a new chemical hydrogen storage material (HCOONa) for the high-efficiency generation, transport, and storage of H2.

12.
Inorg Chem ; 62(11): 4598-4605, 2023 Mar 20.
Article in English | MEDLINE | ID: mdl-36893321

ABSTRACT

In spite of the fact that remarkable developments are achieved in the design and development of novel nanocatalysts for H2 release upon dimethylamineborane hydrolysis, the development of an "on-off" switch for demand-based H2 evolution upon dimethylamineborane hydrolysis is still a matter of supreme importance, however. Herein, we synthesized a string of MoS2 nanosheet-supported RuNi bimetallic nanohybrids (RuxNi1-x/MoS2), by fixation of RuNi nanoparticles at the MoS2 surface, for the H2 evolution upon the hydrolysis of dimethylamineborane at 30 °C. For safely and effectively generating, transporting, and storing H2 gas, the selective "on-off" switch for on-demand H2 evolution upon dimethylamineborane hydrolysis over the Ru0.8Ni0.2/MoS2 nanohybrid has been successfully realized by the Zn2+/EDTA-2Na system. In particular, the H2 evolution is totally switched off by adding Zn(NO3)2. It seems that Zn2+ ions are attached and anchored at the Ru0.8Ni0.2/MoS2 surface, inhibiting their surface-active sites, leading to the termination of H2 evolution. Then, the H2 generation is subsequently reactivated by adding the EDTA-2Na solution because of its excellent coordination ability with Zn2+ ions. This study not only offers a new and efficient RuNi nanocatalyst for dimethylamineborane hydrolysis but also proposes a new method for the demand-based H2 production.

13.
Adv Healthc Mater ; 12(17): e2300064, 2023 07.
Article in English | MEDLINE | ID: mdl-36854114

ABSTRACT

Insufficient angiogenesis frequently occurs after the implantation of orthopedic materials, which greatly increases the risk of bone defect reconstruction failure. Therefore, the development of bone implant with improved angiogenic properties is of great importance. Mimicking the extracellular matrix clues provides a more direct and effective strategy to modulate angiogenesis. Herein, inspired by the bioelectrical characteristics of the bone microenvironment, a piezoelectric bioactive glasses composite (P-KNN/BG) based on the incorporation of polarized potassium sodium niobate is constructed, which could effectively promote angiogenesis. It is found that P-KNN/BG has exceptional wireless electrical stimulation performance and sustained active ions release. In vitro cell experiments reveal that P-KNN/BG enhances endothelial cell adhesion, migration, and differentiation via activating the eNOS/NO signaling pathway, which might be contributed to cell membrane hyperpolarization induced by wireless electrical stimulation increase the influx of active ions into the cells. In vivo chick chorioallantoic membrane experiment demonstrates that P-KNN/BG shows excellent pro-angiogenic capacity and biocompatibility. This work broadens the current understanding of bioactive materials with bionic electrical properties, which brings new insights into the clinical treatment of bone defect repair.


Subject(s)
Bone and Bones , Neovascularization, Physiologic , Endothelial Cells , Cell Adhesion , Ions/pharmacology , Osteogenesis , Glass
14.
Chemistry ; 29(26): e202203772, 2023 May 08.
Article in English | MEDLINE | ID: mdl-36746746

ABSTRACT

Although remarkable progresses are achieved in the design and development of the mono-shift in photoluminescence for mechanofluorochromic materials, it is still a severe challenge to explore the opposite mechanofluorochromic materials with both blue- and red-shifted photoluminescence. Herein, two unprecedented 4,5-bis(TPE)-1H-imidazole fused pyridine or quinoline-based fluorophores X-1 and X-2 were designed and synthesized, and X-1 and X-2, exhibit completely opposite mechanofluorochromic behavior. Under UV lamp, the color of pristine X-1 changed from blue to green with reversible redshifted 27 nm in fluorescence emission spectra after ground, while the color of pristine X-2 changed from red to yellow with reversible blue-shifted 74 nm after ground. The detailed characterizations (including PXRD, SEM and DSC) confirmed that this opposite mechanofluorochromism was attributed to the transformation of order-crystalline and amorphous states. The crystal structure analysis and theoretical calculation further explain that opposite mechanofluorochromic behavior take into account different π-π stacking mode by induced π-extended systems. In addition, these TPE-based fluorophores (X-1 and X-2) exhibited excellent bio-compatibility and fluorescence properties for bio-imaging, writable data storage and anti-counterfeiting materials.

15.
J Org Chem ; 88(5): 2898-2907, 2023 Mar 03.
Article in English | MEDLINE | ID: mdl-36802599

ABSTRACT

An efficient triflic anhydride promoted phosphorylation of ketone was disclosed, and vinylphosphorus compounds were prepared under solvent- and metal-free conditions. Both aryl and alkyl ketones could perform smoothly to give vinyl phosphonates in high to excellent yields. In addition, the reaction was easy to carry out and easy to scale up. Mechanistic studies suggested that this transformation might involve nucleophilic vinylic substitution or a nucleophilic addition-elimination mechanism.

16.
J Org Chem ; 87(21): 14093-14102, 2022 Nov 04.
Article in English | MEDLINE | ID: mdl-36281070

ABSTRACT

The visible-light-promoted difunctionalization of alkenyl ketones has been developed for easy access of various tetralones, cyclopropane, or alkenyl migration compounds. With fac-[Ir(ppy)3] as the photocatalyst, alkenyl ketones captured the α-carbonyl alkyl radical and evolved through intramolecular cyclization and the elimination of a proton to give the difunctionalized products. This strategy is characterized by good yields, mild reaction conditions, and outstanding functional group tolerance.

17.
Nat Commun ; 13(1): 5707, 2022 09 29.
Article in English | MEDLINE | ID: mdl-36175442

ABSTRACT

Rice bean (Vigna umbellata) is an underexploited domesticated legume crop consumed for dietary protein in Asia, yet little is known about the genetic diversity of this species. Here, we present a high-quality reference genome for a rice bean landrace (FF25) built using PacBio long-read data and a Hi-C chromatin interaction map, and assess the phylogenetic position and speciation time of rice bean within the Vigna genus. We sequence 440 landraces (two core collections), and GWAS based on data for growth sites at three widely divergent latitudes reveal loci associated with flowering and yield. Loci harboring orthologs of FUL (FRUITFULL), FT (FLOWERING LOCUS T), and PRR3 (PSEUDO-RESPONSE REGULATOR 3) contribute to the adaptation of rice bean from its low latitude center of origin towards higher latitudes, and the landraces which pyramid early-flowering alleles for these loci display maximally short flowering times. We also demonstrate that copy-number-variation for VumCYP78A6 can regulate seed-yield traits. Intriguingly, 32 landraces collected from a mountainous region in South-Central China harbor a recently acquired InDel in TFL1 (TERMINAL FLOWER1) affecting stem determinacy; these materials also have exceptionally high values for multiple human-desired traits and could therefore substantially advance breeding efforts to improve rice bean.


Subject(s)
Vigna , Chromatin , Genomics , Humans , Phylogeny , Plant Breeding , Vigna/genetics
18.
Chemosphere ; 308(Pt 3): 136521, 2022 Dec.
Article in English | MEDLINE | ID: mdl-36169050

ABSTRACT

Although remarkable progresses have been achieved in the exploration of new and efficient catalytic systems for efficient degradation of estriol, there are only very few available reports providing high mineralization of estriol. Hence, it is still a serious challenge to develop the novel and efficient methods for enhanced degradation and mineralization of estriol due to its serious threat to environment and human health. Herein, this study proposes a series of ZrO2 modified manganese oxide octahedral molecular sieve (ZrO2/OMS-2) nanocomposites as efficient catalysts for enhanced degradation and mineralization of estriol via PMS activation at 30 °C. Among them, ZrO2/OMS-2-27% provided the highest degradation efficiency (95%) and mineralization degrees (70.1%), which exceeded most reported catalytic systems, in the catalytic degradation of estriol. These quenching tests and EPR analysis had confirmed that O2•- and 1O2 were primary reactive oxygen species (ROS) in the ZrO2/OMS-2-27%/PMS system, contrary to the OMS-2/PMS system for which SO4•- and OH• are primary ROS. This might be due to the abundant O-containing surface functional groups of ZrO2/OMS-2-27%. This work not only provides a facile and high-efficiency methodology for the construction of Mn-based nanomaterial, but also proposes a new and efficient nano-catalyst for estriol removal.


Subject(s)
Nanocomposites , Peroxides , Catalysis , Estriol , Humans , Reactive Oxygen Species
19.
Dalton Trans ; 51(29): 11125-11134, 2022 Jul 26.
Article in English | MEDLINE | ID: mdl-35797528

ABSTRACT

The active sites of [FeFe]-hydrogenase promoted by Fe/E (E = S, Se) clusters have attracted considerable interest due to their significance in understanding the interconversion of hydrogen with protons and electrons. As an extension of the study on Fe/Se clusters related to H-cluster model compounds of [FeFe]-hydrogenase, a series of tertiary phosphine substituted Fe/Se carbonyls were successfully prepared. The treatment of Fe2(µ-SePh)2(CO)6 (A) and excess PR3 resulted in the ferrous bis(selenolate) carbonyls Fe(SePh)2(CO)2(PR3)2 (PR3 = PPhMe2, 1; PMe3, 2) in moderate yields. In striking contrast, the reaction of Fe2(µ-SeCH2Ph)2(CO)6 (B) with the same PR3 ligand resulted in the PR3-disubstituted models Fe2(µ-SeCH2Ph)2(CO)4(PR3)2 (PR3 = PPhMe2, 3; PMe3, 4) as the principal products. The more interesting finding is that two independent isomers (anti- and syn-) can be isolated according to different reaction temperatures. Further reactions of 3 or 4 with PR3 under UV irradiation afforded the first PR3-trisubstituted 2Fe2Se derivatives Fe2(µ-SeCH2Ph)2(CO)3(PR3)3 (PR3 = PPhMe2, 5; PMe3, 6). 6 could be further converted into the tetrasubstituted product Fe2(µ-SeCH2Ph)2(CO)2(PMe3)4 (7), while no further substitution was observed with 5 and excess of PPhMe2. All the prepared compounds were fully characterized by elemental analysis, various spectroscopic techniques and X-ray crystallography. In addition, some electrochemical properties of these models were studied by cyclic voltammetry (CV) in MeCN. Compounds 4, 6 and 7 were found to be catalysts for the H2 evolution reaction under electrochemical conditions.


Subject(s)
Hydrogenase , Iron-Sulfur Proteins , Crystallography, X-Ray , Hydrogen/chemistry , Hydrogenase/chemistry , Iron-Sulfur Proteins/chemistry , Models, Molecular , Protons
20.
Clin Transl Immunology ; 11(5): e1393, 2022.
Article in English | MEDLINE | ID: mdl-35582627

ABSTRACT

Objectives: Temozolomide (TMZ) resistance is a key factor that restricts the therapeutic effect of glioblastoma (GBM). YTH-domain family member 2 (YTHDF2) is highly expressed in GBM tissues, while the mechanism of YTHDF2 in TMZ resistance in GBM remains not fully elucidated. Methods: The YTHDF2 expression in TMZ-resistant tissues and cells was detected. Kaplan-Meier analysis was employed to evaluate the prognostic value of YTHDF2 in GBM. Effect of YTHDF2 in TMZ resistance in GBM was explored via corresponding experiments. RNA sequence, FISH in conjugation with fluorescent immunostaining, RNA immunoprecipitation, dual-luciferase reporter gene and immunofluorescence were applied to investigate the mechanism of YTHDF2 that boosted TMZ resistance in GBM. Results: YTHDF2 was up-regulated in TMZ-resistant tissues and cells, and patients with high expression of YTHDF2 showed lower survival rate than the patients with low expression of YTHDF2. The elevated YTHDF2 expression boosted TMZ resistance in GBM cells, and the decreased YTHDF2 expression enhanced TMZ sensitivity in TMZ-resistant GBM cells. Mechanically, YTHDF2 bound to the N6-methyladenosine (m6A) sites in the 3'UTR of EPHB3 and TNFAIP3 to decrease the mRNA stability. YTHDF2 activated the PI3K/Akt and NF-κB signals through inhibiting expression of EPHB3 and TNFAIP3, and the inhibition of the two pathways attenuated YTHDF2-mediated TMZ resistance. Conclusion: YTHDF2 enhanced TMZ resistance in GBM by activation of the PI3K/Akt and NF-κB signalling pathways via inhibition of EPHB3 and TNFAIP3.

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