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2,669 result(s) for "Li, Yaping"
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Pinpointing the axial ligand effect on platinum single-atom-catalyst towards efficient alkaline hydrogen evolution reaction
Developing active single-atom-catalyst (SAC) for alkaline hydrogen evolution reaction (HER) is a promising solution to lower the green hydrogen cost. However, the correlations are not clear between the chemical environments around the active-sites and their desired catalytic activity. Here we study a group of SACs prepared by anchoring platinum atoms on NiFe-layered-double-hydroxide. While maintaining the homogeneity of the Pt-SACs, various axial ligands (−F, −Cl, −Br, −I, −OH) are employed via a facile irradiation-impregnation procedure, enabling us to discover definite chemical-environments/performance correlations. Owing to its high first-electron-affinity, chloride chelated Pt-SAC exhibits optimized bindings with hydrogen and hydroxide, which favor the sluggish water dissociation and further promote the alkaline HER. Specifically, it shows high mass-activity of 30.6 A mgPt −1 and turnover frequency of 30.3  H 2 s −1 at 100 mV overpotential, which are significantly higher than those of the state-of-the-art Pt-SACs and commercial Pt/C catalyst. Moreover, high energy efficiency of 80% is obtained for the alkaline water electrolyser assembled using the above catalyst under practical-relevant conditions. Establishing robust structure/performance correlations is critical for the development of single-atom-catalysts with improved activity. Here, the axial ligand on Pt single-atom-catalyst is precisely adjusted and studied, showing that the ligand’s first electron affinity is crucial for the catalysis.
Phosphorus oxoanion-intercalated layered double hydroxides for high-performance oxygen evolution
Rational design and controlled fabrication of efficient and cost-effective electrodes for the oxygen evolution reaction (OER) are critical for addressing the unpre- cedented energy crisis. Nickel-iron layered double hydroxides (NiFe-LDHs) with specific interlayer anions (i.e. phosphate, phosphite, and hypophosphite) were fabricated by a co-predpitation method and investigated as oxygen evolution electrocatalysts. Intercalation of the phosphorus oxoanion enhanced the OER activity in an alkaline solution; the optimal performance (i.e., a low onset potential of 215 mV, a small Tafel slope of 37.7 mV/dec, and stable electrochemical behavior) was achieved with the hypophosphite-intercalated NiFe-LDH catalyst, demonstrating dramatic enhancement over the traditional carbonate-intercalated NiFe-LDH in terms of activity and durability. This enhanced performance is attributed to the interaction between the intercalated phosphorous oxoanions and the edge-sharing MO6 (M = Ni, Fe) layers, which modifies the surface electronic structure of the Ni sites. This concept should be inspiring for the design of more effective LDH-based oxygen evolution electrocatalvsts.
Indole-3-acetic acid improves drought tolerance of white clover via activating auxin, abscisic acid and jasmonic acid related genes and inhibiting senescence genes
Background Auxin may have a positive effect on plants under drought stress. White clover is widely cultivated and often prone to water shortages. In the present study, we investigated the effects of exogenous indole − 3-acetic acid (IAA) on growth and physiological changes of white clover under drought stress condition. The contents of endogenous IAA and other hormones including ABA, CTK, JA, GA, IAA, and SA were assayed. Moreover, expressions of auxin-responsive genes, drought-responsive genes and leaf senescence-associated genes were detected in response to exogenous IAA. Results Compared to control, drought stress alone significantly diminished stem dry weigh, relative water content (RWC) and total chlorophyll content (Chl). Exogenous IAA treatment significantly increased RWC and Chl, whereas L-AOPP treatment drastically decreased stem dry weight, RWC and Chl under drought stress condition. Additionally, exogenous IAA treatment significantly increased ABA content and JA content, up-regulated expression of auxin responsive genes ( GH3.1 , GH3.9 , IAA8 ), drought stress responsive genes ( bZIP11 , DREB2 , MYB14 , MYB48 , WRKY2 , WRKY56 , WRKY108715 and RD22 ), and down-regulated expressions of auxin-responding genes ( GH3.3 , GH3.6 , IAA27 ) and leaf senescence genes ( SAG101 and SAG102 ) in the presence of PEG. Contrarily, L-AOPP treatment significantly reduced contents of ABA, GA3 and JA, down-regulated expressions of GH3.1 , GH3.9 , IAA8 , bZIP11 , DREB2 , MYB14 , MYB48 , WRKY2 , WRKY56 , WRKY108715 , ERD and RD22 , and up-regulated SAG101 and SAG102 . Conclusions Exogenous IAA improved drought tolerance of white clover possibly due to endogenous plant hormone concentration changes and modulation of genes involving in drought stress response and leaf senescence. These results provided useful information to understand mechanisms of IAA improved drought tolerance in white clover.
Boosting oxygen evolution of single-atomic ruthenium through electronic coupling with cobalt-iron layered double hydroxides
Single atom catalyst, which contains isolated metal atoms singly dispersed on supports, has great potential for achieving high activity and selectivity in hetero-catalysis and electrocatalysis. However, the activity and stability of single atoms and their interaction with support still remains a mystery. Here we show a stable single atomic ruthenium catalyst anchoring on the surface of cobalt iron layered double hydroxides, which possesses a strong electronic coupling between ruthenium and layered double hydroxides. With 0.45 wt.% ruthenium loading, the catalyst exhibits outstanding activity with overpotential 198 mV at the current density of 10 mA cm −2 and a small Tafel slope of 39 mV dec −1 for oxygen evolution reaction. By using operando X-ray absorption spectroscopy, it is disclosed that the isolated single atom ruthenium was kept under the oxidation states of 4+ even at high overpotential due to synergetic electron coupling, which endow exceptional electrocatalytic activity and stability simultaneously. While water splitting offers a carbon-neutral means to store energy, water oxidation is sluggish and corrosive over earth-abundant electrocatalysts. Here, authors show single ruthenium atoms over cobalt-iron layered double hydroxides to be effective and stable oxygen evolution electrocatalysts.
A cancer vaccine-mediated postoperative immunotherapy for recurrent and metastatic tumors
Vaccines to induce effective and sustained antitumor immunity have great potential for postoperative cancer therapy. However, a robust cancer vaccine simultaneously eliciting tumor-specific immunity and abolishing immune resistance continues to be a challenge. Here we present a personalized cancer vaccine (PVAX) for postsurgical immunotherapy. PVAX is developed by encapsulating JQ1 (a BRD4 inhibitor) and indocyanine green (ICG) co-loaded tumor cells with a hydrogel matrix. Activation of PVAX by 808 nm NIR laser irradiation significantly inhibits the tumor relapse by promoting the maturation of dendritic cells and eliciting tumor infiltration of cytotoxic T lymphocytes. A mechanical study reveals that NIR light-triggered antigen release and JQ1-mediated PD-L1 checkpoint blockade cumulatively contribute to the satisfied therapeutic effect. Furthermore, PVAX prepared from the autologous tumor cells induces patient-specific memory immune response to prevent tumor recurrence and metastasis. The PVAX model might provide novel insights for postoperative immunotherapy. Cancer vaccines represent a promising personalized therapeutic approach to treating cancer. Here, the authors report the efficacy in a metastatic model of a cancer vaccine-mediated postoperative immunotherapy, based on the coencapsulation of the JQ1 and a photosensitizer ICG together with inactivated tumor cells into a hydrogel matrix.
Combining gut microbiota modulation and chemotherapy by capecitabine-loaded prebiotic nanoparticle improves colorectal cancer therapy
Colorectal cancer (CRC) therapy efficiency can be influenced by the microbiota in the gastrointestinal tract. Compared with traditional intervention, prebiotics delivery into the gut is a more controllable method for gut microbiota modulatory therapy. Capecitabine (Cap), the first-line chemotherapeutic agent for CRC, lacks a carrier that can prolong its half-life. Here, we construct a Cap-loaded nanoparticle using the prebiotic xylan-stearic acid conjugate (SCXN). The oral administration of SCXN delays the drug clearance in the blood and increases the intra-tumoral Cap concentration in the CRC mouse model. SCXN also facilitates the probiotic proliferation and short chain fatty acid production. Compared with free Cap, SCXN enhances the anti-tumor immunity and increases the tumor inhibition rate from 5.29 to 71.78%. SCXN exhibits good biocompatibility and prolongs the median survival time of CRC mice from 14 to 33.5 d. This prebiotics-based nanoparticle provides a promising CRC treatment by combining gut microbiota modulation and chemotherapy. Gut microbiota regulates colorectal cancer (CRC) progression and respond to therapy. Here the authors generate nanoparticles using prebiotic micelles and loaded with the chemo drug capecitabine that boost gastrointestinal probiotic response, increase anti-tumour immunity and improve survival when provided orally in CRC preclinical murine models.
Curcumin inhibits proliferation, migration, invasion and promotes apoptosis of retinoblastoma cell lines through modulation of miR-99a and JAK/STAT pathway
Curcumin, a primary active ingredient extracted from the Curcuma longa, has been recently identified as a potential anti-tumor agent in multiple kinds of cancers. However, the effect of curcumin on retinoblastoma (Rb) is still unclear. Therefore, we attempted to reveal the functional impacts and the underlying mechanisms of curcumin in Rb cells. Two Rb cell lines SO-Rb50 and Y79 were pre-treated with various doses of curcumin, and then cell proliferation, apoptosis, migration, and invasion were assessed, respectively. Further, regulatory effects of curcumin on miR-99a expression, as well as the activation of JAK/STAT pathway were studied. Data showed that curcumin significantly inhibited the viability, colony formation capacity, migration and invasion, while induced apoptosis of SO-Rb50 and Y79 cells. Up-regulation of miR-99a was observed in curcumin-treated cells. Curcumin suppressed the phosphorylation levels of JAK1, STAT1, and STAT3, while curcumin did not inhibit the activation of JAK/STAT pathway when miR-99a was knocked down. Curcumin inhibited proliferation, migration, invasion, but promoted apoptosis of Rb cells. The anti-tumor activities of curcumin on Rb cells appeared to be via up-regulation of miR-99a, and thereby inhibition of JAK/STAT pathway.
Dynamic chloride ion adsorption on single iridium atom boosts seawater oxidation catalysis
Seawater electrolysis offers a renewable, scalable, and economic means for green hydrogen production. However, anode corrosion by Cl - pose great challenges for its commercialization. Herein, different from conventional catalysts designed to repel Cl - adsorption, we develop an atomic Ir catalyst on cobalt iron layered double hydroxide (Ir/CoFe-LDH) to tailor Cl - adsorption and modulate the electronic structure of the Ir active center, thereby establishing a unique Ir-OH/Cl coordination for alkaline seawater electrolysis. Operando characterizations and theoretical calculations unveil the pivotal role of this coordination state to lower OER activation energy by a factor of 1.93. The Ir/CoFe-LDH exhibits a remarkable oxygen evolution reaction activity (202 mV overpotential and TOF = 7.46 O 2 s −1 ) in 6 M NaOH+2.8 M NaCl, superior over Cl - -free 6 M NaOH electrolyte (236 mV overpotential and TOF = 1.05 O 2 s −1 ), with 100% catalytic selectivity and stability at high current densities (400-800 mA cm −2 ) for more than 1,000 h. The seawater oxidation reaction faces challenges from competitive chloride oxidation reaction. Herein, the authors have utilized chlorine adsorption to modulate the single-atom Ir coordination state and promote seawater oxidation and catalyst stability.
Bioinspired lipoproteins-mediated photothermia remodels tumor stroma to improve cancer cell accessibility of second nanoparticles
The tumor stromal microenvironments (TSM) including stromal cells and extracellular matrix (ECM) form an abominable barrier hampering nanoparticles accessibility to cancer cells, significantly compromising their antitumor effects. Herein, we report a bioinspired lipoprotein (bLP) that can induce efficient photothermia to remodel TSM and improve second bLP accessibility to cancer cells for antitumor therapy. The multiple stromal cells and ECM components in TSM are remarkably disrupted by bLP-mediated photothermal effects, which cause a 4.27-fold enhancement of second bLP accumulation in tumor, deep penetration in whole tumor mass and 27.0-fold increase of accessibility to cancer cells. Of note, this bLP-mediated TSM-remodeling to enhance cancer cell accessibility (TECA) strategy produces an eminent suppression of tumor growth and results in a 97.4% inhibition of lung metastasis, which is superior to the counterpart liposomes. The bLP-mediated TECA strategy provides deeper insights into enhancing nanoparticle accessibility to cancer cells for antitumor therapy. The stromal cells and extracellular matrix hamper nanoparticle access to cancer cells and their anti-cancer efficacy. Here, the authors report a bioinspired lipoprotein (bLP) for photothermal remodelling of tumour stroma and show this to improve subsequent bLP accessibility to cancer cells.
Manipulating solvent fluidic dynamics for large-area perovskite film-formation and white light-emitting diodes
Presynthesized perovskite quantum dots are very promising for making films with different compositions, as they decouple crystallization and film-formation processes. However, fabricating large-area uniform films using perovskite quantum dots is still very challenging due to the complex fluidic dynamics of the solvents. Here, we report a robust film-formation approach using an environmental-friendly binary-solvent strategy. Nonbenzene solvents, n-octane and n-hexane, are mixed to manipulate the fluidic and evaporation dynamics of the perovskite quantum dot inks, resulting in balanced Marangoni flow, enhanced ink spreadability, and uniform solute-redistribution. We can therefore blade-coat large-area uniform perovskite films with different compositions using the same fabrication parameters. White and red perovskite light-emitting diodes incorporating blade-coated films exhibit a decent external quantum efficiency of 10.6% and 15.3% (0.04 cm 2 ), and show a uniform emission up to 28 cm 2 . This work represents a significant step toward the application of perovskite light-emitting diodes in flat panel solid-state lighting. Achieving large-area uniform film is the primary challenge to commercialise perovskite LEDs. The authors here employ green binary solvents to regulate the fluidic dynamics in perovskite quantum dot inks during blade-coating to achieve efficient 28 cm2-sized red and white perovskite LEDs.