The oxygen reduction reaction (ORR) catalyzed by transition-metal single-atom catalysts (SACs) is promising for practical applications in energy-conversion devices, but great challenges still remain due to the sluggish kinetics of O═O cleavage. Herein, a kind of high-density iron network-like sites catalysts are constructed with optimized intermetallic distances on an amino-functionalized carbon matrix (Fe-HDNSs). Quasi-in situ soft X-ray absorption spectroscopy and in situ synchrotron infrared characterizations demonstrate that the optimized intermetallic distances in Fe-HDNSs can in situ activate the molecular oxygen by fast electron compensation through the hybridized Fe 3d‒O 2p, which efficiently facilitates the cleavage of the O═O bond to *O species and highly suppresses the side reactions for an accelerated kinetics of the 4e ORR.
View Article and Find Full Text PDFNon-noble metal oxides have emerged as potential candidate electrocatalysts for acidic oxygen evolution reactions (OERs) due to their earth abundance; however, improving their catalytic activity and stability simultaneously in strong acidic electrolytes is still a major challenge. In this work, we report CoO@carbon core-shell nanoparticles on 2D graphite sheets (CoO@C-GS) as mixed-dimensional hybrid electrocatalysts for acidic OER. The obtained CoO@C-GS catalyst exhibits a low overpotential of 350 mV and maintains stability for 20 h at a current density of 10 mA cm in HSO (pH = 1) electrolyte.
View Article and Find Full Text PDFThe development of two-dimensional (2D) magnetic semiconductors with room-temperature ferromagnetism is a significant challenge in materials science and is important for the development of next-generation spintronic devices. Herein, we demonstrate that a 2D semiconducting antiferromagnetic Cu-MOF can be endowed with intrinsic room-temperature ferromagnetic coupling using a ligand cleavage strategy to regulate the inner magnetic interaction within the Cu dimers. Using the element-selective X-ray magnetic circular dichroism (XMCD) technique, we provide unambiguous evidence for intrinsic ferromagnetism.
View Article and Find Full Text PDFSynthesis of highly active and durable oxygen evolution reaction (OER) catalysts applied in acidic water electrolysis remains a grand challenge. Here, we construct a type of high-loading iridium single atom catalysts with tunable d-band holes character (h-HL-Ir SACs, ∼17.2 wt % Ir) realized in the early OER operation stages.
View Article and Find Full Text PDFTuning the local reaction environment is an important and challenging issue for determining electrochemical performances. Herein, we propose a strategy of intentionally engineering the local reaction environment to yield highly active catalysts. Taking Pt nanoparticles supported on oxygen vacancy enriched MgO nanosheets as a prototypical example, we have successfully created a local acid-like environment in the alkaline medium and achieve excellent hydrogen evolution reaction performances.
View Article and Find Full Text PDFObjective: To evaluate the effect of periodontal treatment on combined periodontal-pulpal lesions.
Methods: A total of 327 patients with periodontal-pulpal lesions (360 affected teeth) were selected, and all affected teeth were treated with a complete root canal, and assigned into group A (periodontal treatment group, 180 affected teeth) and group B (non-periodontal treatment group, 180 affected teeth). Group A received periodontal basic treatment for 2 weeks after the completion of root canal treatment; 6 weeks later, if there were still more than 5 mm periodontal pockets and bleeding after detection, flap treatment was performed.
Iridium-based perovskites show promising catalytic activity for oxygen evolution reaction (OER) in acid media, but the iridium mass activity remains low and the active-layer structures have not been identified. Here, we report highly active 1 nm IrO particles anchored on 9R-BaIrO (IrO/9R-BaIrO) that are directly synthesized by solution calcination followed by strong acid treatment for the first time. The developed IrO/9R-BaIrO catalyst delivers a high iridium mass activity (168 A g), about 16 times higher than that of the benchmark acidic OER electrocatalyst IrO (10 A g), and only requires a low overpotential of 230 mV to reach a catalytic current density of 10 mA cm.
View Article and Find Full Text PDFUncovering the dynamics of active sites in the working conditions is crucial to realizing increased activity, enhanced stability and reduced cost of oxygen evolution reaction (OER) electrocatalysts in proton exchange membrane electrolytes. Herein, we identify at the atomic level potential-driven dynamic-coupling oxygen on atomically dispersed hetero-nitrogen-configured Ir sites (AD-HN-Ir) in the OER working conditions to successfully provide the atomically dispersed Ir electrocatalyst with ultrahigh electrochemical acidic OER activity. Using in-situ synchrotron radiation infrared and X-ray absorption spectroscopies, we directly observe that one oxygen atom is formed at the Ir active site with an O-hetero-Ir-N structure as a more electrophilic active centre in the experiment, which effectively promotes the generation of key *OOH intermediates under working potentials; this process is favourable for the dissociation of HO over Ir active sites and resistance to over-oxidation and dissolution of the active sites.
View Article and Find Full Text PDFACS Appl Mater Interfaces
July 2021
Two-dimensional (2D) materials with intrinsic magnetic properties are intensively explored due to their potential applications in low-power-consumption electronics and spintronics. To date, only a handful of intrinsic magnetic 2D materials have been reported. Here, we report a realization of intrinsic ferromagnetic behavior in 2D VC MXene nanosheets through layer mismatch engineering.
View Article and Find Full Text PDFGraphene is extremely promising for next-generation spintronics applications; however, realizing graphene-based room-temperature magnets remains a great challenge. Here, we demonstrate that robust room-temperature ferromagnetism with T up to ∼400 K and saturation magnetization of 0.11 emu g (300 K) can be achieved in graphene by embedding isolated Co atoms with the aid of coordinated N atoms.
View Article and Find Full Text PDFMetal-oxide/hydroxide hybrid nanostructures provide an excellent platform to study the interfacial effects on tailoring the catalysis of metal catalysts. Herein, a hybrid nanostructure of Pt@Co(OH)2 supported on SiO2 was synthesized by incipient wetness impregnation of Co(OH)2 with the aid of H2O2 and successive urea-assisted deposition-precipitation of platinum nanoparticles. The Fenton-like reaction between Co2+ and H2O2 during the impregnation process facilitates the formation of active interfacial sites.
View Article and Find Full Text PDFSingle-atom-layer catalysts with fully activated basal-atoms will provide a solution to the low loading-density bottleneck of single-atom catalysts. Herein, we activate the majority of the basal sites of monolayer MoS , by doping Co ions to induce long-range ferromagnetic order. This strategy, as revealed by in situ synchrotron radiation microscopic infrared spectroscopy and electrochemical measurements, could activate more than 50 % of the originally inert basal-plane S atoms in the ferromagnetic monolayer for the hydrogen evolution reaction (HER).
View Article and Find Full Text PDFACS Appl Mater Interfaces
August 2019
The activation and modulation of the magnetism of MoS nanosheets are critical to the development of their application in next-generation spintronics. Here, we report a synergetic strategy to induce and modulate the ferromagnetism of the originally nonmagnetic MoS nanosheets. A two-step experimental method was used to simultaneously introduce substitutional V dopants and sulfur vacancy (V) in the MoS nanosheet host, showing an air-stable and adjustable ferromagnetic response at room temperature.
View Article and Find Full Text PDFUnderstanding the variation of active structure during the hydrogen evolution reaction (HER) process is of great importance for aiding in the design of optimized electrocatalysts. Herein, we present a composite material of FeP nanoparticles coated by N-doped carbon (FeP@NC) as an efficient HER electrocatalyst, synthesized by a pyrolysis and equivalent-volume impregnation method. The as-prepared FeP@NC catalyst can accelerate the HER at a small overpotential of 135 mV with a current density of 10 mA cm in acidic medium and also shows a robust long-term stability with a minor decay of about 10% of the initial current density after 15 h.
View Article and Find Full Text PDFACS Appl Mater Interfaces
September 2018
Reversible manipulation of the magnetic behavior of two-dimensional van der Waals crystals is crucial for expanding their applications in spin-based information-processing technologies. However, to date, most experimental approaches to tune the magnetic properties are single way and have very limited practical applications. Here, we report an interface charge-transfer method for obtaining a reversible and air-stable magnetic response at room temperature in Mn-doped MoS nanosheets.
View Article and Find Full Text PDFTongue squamous cell carcinoma (TSCC) is highly malignant and poorly differentiated, resulting in a high frequency of local recurrence and distant metastases. Sox2 (Sry‑box2), an important factor in embryonic development and cell differentiation, has been shown to associate with malignant phenotypes and epithelial‑mesenchymal transition (EMT) progression in numerous types of human tumors. However, the clinical relevance and molecular mechanisms of Sox2 in TSCC remain unclear.
View Article and Find Full Text PDFExploration of the biological effects of transition metal ions in acupuncture points is essential to clarify the functional mechanism of acupuncture treatment. Here we show that in the SP6 acupuncture point (Sanyinjiao) the Fe ions are in a high-spin state of approximately te in an Fe-N(O) octahedral crystal field. The Fe K-edge synchrotron radiation X-ray absorption fine structure results reveal that the Fe-N and Fe-O bond lengths in the SP6 acupuncture point are 2.
View Article and Find Full Text PDFProline rich 11 (PRR11) serves an important role in the development and progression of a number of types of human cancer. However, the clinical role of PRR11 in tongue squamous cell carcinoma (TSCC) remains unknown. The present study aimed to investigate the expression and clinicopathological significance of PRR11 in TSCC.
View Article and Find Full Text PDFDirect and scalable synthesis of monodisperse gold nanoclusters is highly desired but remains a great challenge due to the complexity of chemical reactions. In this regard, a suitable precursor is important as it can simplify the synthesis processes and offer controllability in tuning the product. In this study, we found that Au(PPh)Cl could be used as an effective precursor for the direct synthesis of atomically monodisperse [Au(PPh)] nanoclusters without the need of tedious post-synthetic purification steps.
View Article and Find Full Text PDFAccumulating data suggest that microRNAs (miRNAs) play a pivotal role in the regulation of tumor cell sensitivity to chemotherapeutic agents. Although the roles of a few miRNAs have been identified in cisplatin resistance, little is known in regards to the concerted contribution of miRNA‑mediated biological networks. In the present study, we demonstrated that microRNA-218 (miR-218) was significantly upregulated in cisplatin-resistant oral cancer cells.
View Article and Find Full Text PDFDoping atomically thick nanosheets is a great challenge due to the self-purification effect that drives the precipitation of dopants. Here, a breakthrough is made to dope Mn atoms substitutionally into MoS nanosheets in a sulfur-rich supercritical hydrothermal reaction environment, where the formation energy of Mn substituting for Mo sites in MoS is significantly reduced to overcome the self-purification effect. The substitutional Mn doping is convincingly evidenced by high-angle annular dark-field scanning transmission electron microscopy and X-ray absorption fine spectroscopy characterizations.
View Article and Find Full Text PDFACS Appl Mater Interfaces
August 2017
Developing efficient and durable oxygen evolution electrocatalyst is of paramount importance for the large-scale supply of renewable energy sources. Herein, we report the design of significant surface hydrophilicity based on cobalt oxyhydroxide (CoOOH) nanosheets to greatly improve the surface hydroxyl species adsorption and reaction kinetics at the Helmholtz double layer for high-efficiency water oxidation activity. The as-designed CoOOH-graphene nanosheets achieve a small surface water contact angle of ∼23° and a large double-layer capacitance (C) of 8.
View Article and Find Full Text PDFDirect and efficient photocatalytic water splitting is critical for sustainable conversion and storage of renewable solar energy. Here, we propose a conceptual design of two-dimensional CN-based in-plane heterostructure to achieve fast spatial transfer of photoexcited electrons for realizing highly efficient and spontaneous overall water splitting. This unique plane heterostructural carbon ring (C)-CN nanosheet can synchronously expedite electron-hole pair separation and promote photoelectron transport through the local in-plane π-conjugated electric field, synergistically elongating the photocarrier diffusion length and lifetime by 10 times relative to those achieved with pristine g-CN.
View Article and Find Full Text PDFAbnormal expression of β-catenin contributes to tumor development, progression, and metastasis in various cancers. However, little is known about the relationship between abnormal expression of β-catenin and cisplatin chemotherapy in oral squamous cell carcinoma (OSCC). The present study aimed to investigate the effect of β-catenin on OSCC cisplatin resistance and evaluated the drug susceptibility of stable cell lines with β-catenin knockin and knockdown.
View Article and Find Full Text PDFThis retrospective study aimed to identify if the existence of the accessory parotid gland correlated with the etiology of parotitis. This may aid the development of better treatment strategies in the future. Sialographic features of cases with parotitis and healthy subjects were reviewed.
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