The sluggish polysulfide redox kinetics and the uncontrollable sulfur speciation pathway, leading to serious shuttling effect and high activation barrier associated with sulfur cathode. We describe here the use of cor...
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The sluggish polysulfide redox kinetics and the uncontrollable sulfur speciation pathway, leading to serious shuttling effect and high activation barrier associated with sulfur cathode. We describe here the use of core–shell structured composite matrixes containing abundant catalytic sites for nearly fully reversible cycling of sulfur cathodes for Na-S batteries. The bidirectional tandem electrocatalysis provide successive reversible conversion of both long- and short-chain polysulfides, whereas Fe 2 O 3 accelerates Na 2 S 8 /Na 2 S 6 to Na 2 S 4 conversion and the redox-active Fe(CN) 6 4− -doped polypyrrole shell catalyzes Na 2 S 4 reduction to Na 2 S. The electrochemically reactive Na 2 S can be readily charged back to sulfur with minimal overpotential. Simultaneously, stable cycling of Na-S pouch cell with a high reversible capacity of 696 mAh g −1 is also demonstrated. The bidirectional confined tandem catalysis renders the manipulation of sulfur redox electrochemistry for practical Na-S cells.
Intramolecular Cl−S non-covalent interaction is introduced to modify molecular backbone of a benzodithiophene terthiophene rhodamine (BTR) benchmark structure, helping planarize and rigidify the molecular framework fo...
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Intramolecular Cl−S non-covalent interaction is introduced to modify molecular backbone of a benzodithiophene terthiophene rhodamine (BTR) benchmark structure, helping planarize and rigidify the molecular framework for improving charge transport. Theoretical simulations and temperature-variable NMR experiments clearly validate the existence of Cl−S non-covalent interaction in two designed chlorinated donors and explain its important role in enhancing planarity and rigidity of the molecules for enhancing their crystallinity. The asymmetric isomerization of side-chains further optimizes the molecular orientation and surface energy to strike a balance between its crystallinity and miscibility. This carefully manipulated molecular design helps result in increased carrier mobility and suppressed charge recombination to obtain simultaneously enhanced short-circuit current ( J sc ) and fill factor (FF) and a very high efficiency of 15.73 % in binary all-small-molecule organic solar cells.
The classic solvent system can't sufficiently separate one-dimensional edge-sharing SnI 2 crystals in solution, which severely restricts the fabrication of high-quality tin-based perovskite film. Herein, a strong ...
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The classic solvent system can't sufficiently separate one-dimensional edge-sharing SnI 2 crystals in solution, which severely restricts the fabrication of high-quality tin-based perovskite film. Herein, a strong Lewis base (hexamethylphosphoramide, HMPA) has been introduced to coordinate Sn 2+ to modulate solvation behaviours on perovskite precursor and regulate crystallization kinetics. The large molecular volume of HMPA and stronger bind energy of SnI 2 ⋅ 2HMPA (−0.595 eV vs −0.118 eV for SnI 2 ⋅ 2DMSO) change the solvation structure of SnI 2 from edge-sharing cluster to monodisperse adduct, which contributes to uniform nucleation sites and prolongs crystal growth process. Delightfully, a fully-covered perovskite film is formed on the large-area substrate and tin-based perovskite solar cells processed with HMPA exhibit an excellent efficiency of 13.46 %. This research provides novel insights and directions for the solution preparation of smooth and uniform large-area tin-based perovskite film.
The deficient catalytic activity of nanozymes and insufficient endogenous H 2 O 2 in the tumor microenvironment (TME) are major obstacles for nanozyme-mediated catalytic tumor therapy. Since electron transfer is the b...
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The deficient catalytic activity of nanozymes and insufficient endogenous H 2 O 2 in the tumor microenvironment (TME) are major obstacles for nanozyme-mediated catalytic tumor therapy. Since electron transfer is the basic essence of catalysis-mediated redox reactions, we explored the contributing factors of enzymatic activity based on positive and negative charges, which are experimentally and theoretically demonstrated to enhance the peroxidase (POD)-like activity of a MoS 2 nanozyme. Hence, an acidic tumor microenvironment-responsive and ultrasound-mediated cascade nanocatalyst (BTO/MoS 2 @CA) is presented that is made from few-layer MoS 2 nanosheets grown on the surface of piezoelectric tetragonal barium titanate (T-BTO) and modified with pH-responsive cinnamaldehyde (CA). The integration of pH-responsive CA-mediated H 2 O 2 self-supply, ultrasound-mediated charge-enhanced enzymatic activity, and glutathione (GSH) depletion enables out-of-balance redox homeostasis, leading to effective tumor ferroptosis with minimal side effects.
BACKGROUND:To facilitate advances in personalized medicine, it is important to detect predictive, stable and interpretable biomarkers related with different clinical characteristics. These clinical characteristics may...
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BACKGROUND:To facilitate advances in personalized medicine, it is important to detect predictive, stable and interpretable biomarkers related with different clinical characteristics. These clinical characteristics may be heterogeneous with respect to underlying interactions between genes. Usually, traditional methods just focus on detection of differentially expressed genes without taking the interactions between genes into account. Moreover, due to the typical low reproducibility of the selected biomarkers, it is difficult to give a clear biological interpretation for a specific disease. Therefore, it is necessary to design a robust biomarker identification method that can predict disease-associated interactions with high reproducibility.
RESULTS:In this article, we propose a regularized logistic regression model. Different from previous methods which focus on individual genes or modules, our model takes gene pairs, which are connected in a protein-protein interaction network, into account. A line graph is constructed to represent the adjacencies between pairwise interactions. Based on this line graph, we incorporate the degree information in the model via an adaptive elastic net, which makes our model less dependent on the expression data. Experimental results on six publicly available breast cancer datasets show that our method can not only achieve competitive performance in classification, but also retain great stability in variable selection. Therefore, our model is able to identify the diagnostic and prognostic biomarkers in a more robust way. Moreover, most of the biomarkers discovered by our model have been verified in biochemical or biomedical researches.
CONCLUSIONS:The proposed method shows promise in the diagnosis of disease pathogenesis with different clinical characteristics. These advances lead to more accurate and stable biomarker discovery, which can monitor the functional changes that are perturbed by diseases. Based on these predictions, researche
Wide-band gap (1.68 eV) perovskite solar cells (PSCs) are important components of perovskite/Si tandem devices. However, the efficiency of wide band gap PSCs has been limited by their huge open-circuit voltage ( V oc ...
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Wide-band gap (1.68 eV) perovskite solar cells (PSCs) are important components of perovskite/Si tandem devices. However, the efficiency of wide band gap PSCs has been limited by their huge open-circuit voltage ( V oc ) deficit due to non-radiative recombination. Deep-level acceptor defects are identified as the major killers of V oc , and they can be effectively improved by passivation with ammonium salts. Theoretical calculation predicts that increasing the distance between F and −NH 3 + of fluorinated ammonium can dramatically enhance the electropositivity of −NH 3 + terminals, thus providing strong adsorption onto the negatively charged I A and I Pb anti-site defects. Characterizations further confirm that surface gradient passivation employing p -FPEAI demonstrates the most efficient passivation effect. Consequently, a record-efficiency of 21.63 % with the smallest V oc deficit of 441 mV is achieved for 1.68 eV-band gap inverted PSCs. Additionally, a flexible PSC and 1 cm 2 opaque device also deliver the highest PCEs of 21.02 % and 19.31 %, respectively.
This study investigated the dynamic changes in NiFe (hydr)oxide and identified the role of high-valent Fe in the oxygen-evolution reaction (OER) within alkaline media via in situ techniques. Several high-valent Fe ion...
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This study investigated the dynamic changes in NiFe (hydr)oxide and identified the role of high-valent Fe in the oxygen-evolution reaction (OER) within alkaline media via in situ techniques. Several high-valent Fe ions were found to remain considerably stable in the absence of potential in NiFe (hydr)oxide, even 96 hours after the OER. For Ni 2+ hydroxide treated with 57 Fe ions, where Fe sites are introduced onto the surface of Ni 2+ hydroxide, no Fe 4+ species were detected at the rate-determining step (RDS). The findings of this study suggested that the oxidation of bulk Fe ions, similar to Ni ions, to high valent forms, is charge accumulation without a direct role in OER; these results offered a novel perspective on manipulating Fe states to optimize OER efficacy. The prevailing hypothesis suggested that trace amounts of high-valent Fe ions, notably those on the surface, directly participate in OER.
The development of oxidation catalysts that are resistant to sulfur poisoning is crucial for extending the lifespan of catalysts in real-working conditions. Herein, we describe the design and synthesis of oxide-metal ...
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The development of oxidation catalysts that are resistant to sulfur poisoning is crucial for extending the lifespan of catalysts in real-working conditions. Herein, we describe the design and synthesis of oxide-metal interaction (OMI) catalyst under oxidative atmospheres. By using organic coated TiO 2 , an oxide/metal inverse catalyst with non-classical oxygen-saturated TiO 2 overlayers were obtained at relatively low temperature. These catalysts were found to incorporate ultra-small Pd metal and support particles with exceptional reactivity and stability for CO oxidation (under 21 vol % O 2 and 10 vol % H 2 O). In particular, the core (Pd)-shell (TiO 2 ) structured OMI catalyst exhibited excellent resistance to SO 2 poisoning, yielding robust CO oxidation performance at 120 °C for 240 h (at 100 ppm SO 2 and 10 vol % H 2 O). The stability of this new OMI catalyst was explained through density functional theory (DFT) calculations that interfacial oxygen atoms at Pd−O−Ti sites (of oxygen-saturated overlayers) serve as non-metal active sites for low-temperature CO oxidation, and change the SO 2 adsorption from metal(d)-to-SO 2 (π*) back-bonding to much weaker σ(Ti−S) bonding.
Low-temperature photothermal therapy (PTT), which circumvents the limitations of conventional PTT (e.g., thermotolerance and adverse effects), is an emerging therapeutic strategy which shows great potential for future...
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Low-temperature photothermal therapy (PTT), which circumvents the limitations of conventional PTT (e.g., thermotolerance and adverse effects), is an emerging therapeutic strategy which shows great potential for future clinical applications. The expression of heat shock proteins (HSPs) can dramatically impair the therapeutic efficacy of PTT. Thus, inhibition of HSPs repair and reducing the damage of nearby normal cells is crucial for improving the efficiency of low-temperature PTT. Herein, we developed a nanobomb based on the self-assembly of NIRII AIE polymer PBPTV and carbon monoxide (CO) carrier polymer mPEG(CO). This smart nanobomb can be exploded in a tumor microenvironment in which hydrogen peroxide is overexpressed and release CO into cancer cells to significantly inhibit the expression of HSPs and hence improve the antitumor efficiency of the low-temperature PTT.
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