Chemical modification of electrode materials by heteroatom dopants is crucial for improving storage performance in rechargeable batteries. Electron configurations of different dopants significantly ...influence the chemical interactions inbetween and the chemical bonding with the host material, yet the underlying mechanism remains unclear. We revealed competitive doping chemistry of Group IIIA elements (boron and aluminum) taking nickel‐rich cathode materials as a model. A notable difference between the atomic radii of B and Al accounts for different spatial configurations of the hybridized orbital in bonding with lattice oxygen. Density functional theory calculations reveal, Al is preferentially bonded to oxygen and vice versa, and shows a much lower diffusion barrier than BIII. In the case of Al‐preoccupation, the bulk diffusion of BIII is hindered. In this way, a B‐rich surface and Al‐rich bulk is formed, which helps to synergistically stabilize the structural evolution and surface chemistry of the cathode.
A model study has been performed on Group IIIA element (boron and aluminum) co‐doped high‐nickel layered oxide cathode materials to understand competitive doping chemistry. A notable difference between the atomic radii of B and Al accounts for different spatial configurations of the hybridized orbital in bonding with lattice oxygen, resulting in the formation of a B‐rich surface and an Al‐rich bulk.
Spontaneous droplet jumping on micro‐/nano‐structured superhydrophobic surfaces has been exploited as an efficient means for enhancing steam condensation heat transfer. However, the good performance ...of such surfaces quickly decays with raising the degree of subcooling, due to the mismatch between the characteristic length scales and droplet sizes when they grow up. Herein, a novel strategy for multiscale droplet regulation is proposed by combining sub‐millimeter fin structure with a hierarchical microporous superhydrophobic surface. A superior condensation heat transfer performance is attained on such hierarchical superhydrophobic finned tube (F‐SHB), in comparison to the baseline case of superhydrophobic non‐finned (SHB) tube under well‐controlled test conditions. Although the droplet jumping is not as vigorous as that on the SHB tube, the finned geometry of the F‐SHB tube leads to a condensation heat transfer enhancement even under high degrees of subcooling up to 36 K, because of the accelerated departure of large droplets by imposing Laplace force gradient in the presence of V‐shaped sub‐millimeter fins. This multiscale enhancement strategy is shown to enable a cascading regulation over the entire lifespan of condensate droplets. The fabrication of F‐SHB tubes is facile and easy to be scaled up, showing great potential in practical steam condensation applications.
A multiscale strategy is proposed to enable cascading regulation over the entire lifespan of condensate droplets. Combining hierarchical superhydrophobic textures and micro‐fins achieves a miracle enhancement effect on facilitating small droplet jumping at the fin tips under lower subcooling degrees and accelerating large droplet drainage via creating Laplace pressure imbalance over a wide range of subcooling up to 36 K.
This paper examines the impacts of GDP, trade structure, exchange rate and FDI (foreign direct investment) inflows on China's carbon emissions from 1982 to 2016 and verifies the validity of EKC ...(Environmental Kuznets Curve) hypothesis for China. Differentiated from the existing literature which rarely considers services trade and exchange rate, this paper uses the proportion of services trade to measure trade structure, and exchange rate as one of the independent variables. Firstly, the stability of each variable is tested by ADF (Augmented Dickey-Fuller) and NP (Ng-Perron) test. Then, ARDL bound test is used to test the cointegration of the variables as it has better properties than traditional cointegration methods and is more suitable for the model in this paper. Thirdly, Error Correction Model is used to analyze the long-term and short-term dynamic relationship between the variables. Fourthly, the Granger causality test based on the VAR is performed. It is found that during the study period EKC hypothesis was valid for China, and that whilst the impacts of both services trade and exchange rate on China's carbon emissions were negative, the impacts of FDI inflows were positive. Conclusions and policy implications are provided at the end of the paper.
•The impacts of GDP, etc. on China's carbon emissions are examined.•The validity of EKC hypothesis for China is verified;•Trade structure is measured by services trade proportion in total;•Exchange rate is used as one of the independent variables.
Sustainable hydrogen production is an essential prerequisite of a future hydrogen economy. Water electrolysis driven by renewable resource-derived electricity and direct solar-to-hydrogen conversion ...based on photochemical and photoelectrochemical water splitting are promising pathways for sustainable hydrogen production. All these techniques require, among many things, highly active noble metal-free hydrogen evolution catalysts to make the water splitting process more energy-efficient and economical. In this review, we highlight the recent research efforts toward the synthesis of noble metal-free electrocatalysts, especially at the nanoscale, and their catalytic properties for the hydrogen evolution reaction (HER). We review several important kinds of heterogeneous non-precious metal electrocatalysts, including metal sulfides, metal selenides, metal carbides, metal nitrides, metal phosphides, and heteroatom-doped nanocarbons. In the discussion, emphasis is given to the synthetic methods of these HER electrocatalysts, the strategies of performance improvement, and the structure/composition-catalytic activity relationship. We also summarize some important examples showing that non-Pt HER electrocatalysts could serve as efficient cocatalysts for promoting direct solar-to-hydrogen conversion in both photochemical and photoelectrochemical water splitting systems, when combined with suitable semiconductor photocatalysts.
Acute pain is protective and a cardinal feature of inflammation. Chronic pain after arthritis, nerve injury, cancer, and chemotherapy is associated with chronic neuroinflammation, a local ...inflammation in the peripheral or central nervous system. Accumulating evidence suggests that non-neuronal cells such as immune cells, glial cells, keratinocytes, cancer cells, and stem cells play active roles in the pathogenesis and resolution of pain. We review how non-neuronal cells interact with nociceptive neurons by secreting neuroactive signaling molecules that modulate pain. Recent studies also suggest that bacterial infections regulate pain through direct actions on sensory neurons, and specific receptors are present in nociceptors to detect danger signals from infections. We also discuss new therapeutic strategies to control neuroinflammation for the prevention and treatment of chronic pain.
Novel 3D Ni1−xCoxSe2 mesoporous nanosheet networks with tunable stoichiometry are successfully synthesized on Ni foam (Ni1−xCoxSe2 MNSN/NF with x ranging from 0 to 0.35). The collective effects of ...special morphological design and electronic structure engineering enable the integrated electrocatalyst to have very high activity for hydrogen evolution reaction (HER) and excellent stability in a wide pH range. Ni0.89Co0.11Se2 MNSN/NF is revealed to exhibit an overpotential (η10) of 85 mV at −10 mA cm−2 in alkaline medium (pH 14) and η10 of 52 mV in acidic solution (pH 0), which are the best among all selenide‐based electrocatalysts reported thus far. In particular, it is shown for the first time that the catalyst can work efficiently in neutral solution (pH 7) with a record η10 of 82 mV for all noble metal‐free electrocatalysts ever reported. Based on theoretical calculations, it is further verified that the advanced all‐pH HER activity of Ni0.89Co0.11Se2 is originated from the enhanced adsorption of both H+ and H2O induced by the substitutional doping of cobalt at an optimal level. It is believed that the present work provides a valuable route for the design and synthesis of inexpensive and efficient all‐pH HER electrocatalysts.
An integrated electrocatalyst comprising 3D mesoporous Ni0.89Co0.11Se2 nanosheet networks on Ni foam is synthesized, and it demonstrates very high activities and excellent stabilities for hydrogen evolution reaction (HER) in all‐pH conditions. Theoretical calculations verify that electronic structure engineering by optimal Co doping enhances the adsorption of H+ and H2O, leading to the advanced all‐pH HER activity of the catalyst.
Increasing evidence suggests that long noncoding RNAs (lncRNAs) play crucial roles in various biological processes. However, little is known about the effects of lncRNAs on autophagy. Here we report ...that a lncRNA, termed cardiac autophagy inhibitory factor (CAIF), suppresses cardiac autophagy and attenuates myocardial infarction by targeting p53-mediated myocardin transcription. Myocardin expression is upregulated upon H
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and ischemia/reperfusion, and knockdown of myocardin inhibits autophagy and attenuates myocardial infarction. p53 regulates cardiomyocytes autophagy and myocardial ischemia/reperfusion injury by regulating myocardin expression. CAIF directly binds to p53 protein and blocks p53-mediated myocardin transcription, which results in the decrease of myocardin expression. Collectively, our data reveal a novel CAIF-p53-myocardin axis as a critical regulator in cardiomyocyte autophagy, which will be potential therapeutic targets in treatment of defective autophagy-associated cardiovascular diseases.
Conspectus Indole-based chiral heterocycles constitute a class of important heterocyclic compounds that are found in numerous pharmaceuticals, functional materials, and chiral catalysts or ligands. ...Catalytic asymmetric synthesis, for which the 2001 Nobel Prize in Chemistry was awarded, has been demonstrated to be the most efficient method for accessing chiral compounds. Therefore, the catalytic asymmetric synthesis of indole-based chiral heterocycles has attracted great interest from the scientific community. However, the strategies toward this goal are rather limited, and great challenges remain in this field, such as metal contamination in the products, the limited number of platform molecules with versatile reactivity, and the limited number of catalytic asymmetric reactions that offer high step economy, atom economy, and excellent enantiocontrol. Therefore, novel strategies for the catalytic asymmetric synthesis of indole-based chiral heterocycles are urgently needed. To achieve this goal, our group has developed a series of unique strategies, such as designing and developing versatile platform molecules and their corresponding organocatalytic asymmetric reactions to access indole-based chiral heterocycles. In this Account, we describe our efforts to address the remaining challenges in this research field. Namely, we have designed and developed vinylindoles, indolylmethanols, arylindoles and indole derivatives as versatile platform molecules for the construction of indole-based chiral heterocyclic scaffolds with structural diversity and complexity. Based on the reactivities of these platform molecules, we have designed and accomplished a series of organocatalytic asymmetric cycloaddition, cyclization, addition and dearomatization reactions with a high step economy, atom economy and excellent enantiocontrol. Using these strategies, a wide range of indole-based chiral heterocycles, including five-membered to seven-membered heterocycles, axially chiral heterocycles and tetrasubstituted heterocycles, have been synthesized with high efficiency and excellent enantioselectivity. In addition, we have investigated the properties of some indole-based chiral heterocycles, including their bioactivities and catalytic activities, and showed that these chiral heterocycles have potent anticancer activities and promising catalytic activities in asymmetric catalysis. These results help elucidate the potential applications of indole-based chiral heterocycles in drug development and chiral catalysts. The organocatalytic asymmetric synthesis of indole-based chiral heterocycles has undoubtedly become and will continue to be a hot topic in the field of asymmetric catalysis and synthesis. Our efforts, summarized in this Account, will not only open a window for the future development of innovative strategies toward organocatalytic asymmetric synthesis of indole-based chiral heterocycles but also inspire chemists worldwide to confront the remaining challenges in this field and prompt further advances.
Recently, the subradiant states of one-dimensional two-level atom chains coupled to light modes were found to have decay rates obeying a universal scaling, and an unexpected fermionic character of ...the multiply excited subradiant states was discovered. In this Letter, we theoretically obtain the singly excited subradiant states, and by eliminating the superradiant modes, we demonstrate a relation between the multiply excited subradiant states and the Tonks-Girardeau limit of the Lieb-Liniger model which explains the fermionic behavior. In addition, we identify a new family of subradiant states with correlations different from the fermionic ansatz.