As one of the fascinating high capacity cathodes, O3‐type layered oxides usually suffer from their intrinsic air sensitivity and sluggish kinetics originating from the spontaneous lattice Na ...extraction during air exposure and high tetrahedral site energy of Na+ diffusion transition state. What is worse, the improvement on the two handicaps is hard to simultaneously realize because of the contradiction between Na containment suggested in air stability mechanism and enhanced Na diffusion mentioned in kinetics strategy. Herein, it is shown that a simple strategy of introducing proper Na vacancies into lattice can simultaneously realize a dual performance improvement. Na vacancies decrease the charge density on transitional metal ions and enhance the antioxidative capability of material, ensuring a stable lattice Na containment for Na0.93Li0.12Ni0.25Fe0.15Mn0.48O2 when exposed to air. Additionally, more Na+ diffusional sites and enlarged Na layer spacing are obtained and result in a significantly decreased energy barrier from ≈1000 to 300 meV and a high rate capability of 70.8% retention at 2000 mA g−1. Remarkably, such a strategy can be easily realized by either pre‐ or post‐treating, which exhibits excellent universality for various O3 materials, implying its enormous potential to promote the commercial application of O3‐type cathodes.
A universal strategy of introducing proper Na vacancies into a crystal lattice is proposed to simultaneously improve air‐stability and kinetics of O3‐type layered oxide cathodes. The dual improvement benefits from the multiple effects of Na vacancies on crystalline and electronic structure, namely, decreased charge density on transition metal ions, enhanced antioxidative capability, decreased Na+ diffusion barrier, and optimized migration path.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SBCE, SBMB, UL, UM, UPUK
Age‐associated obesity and muscle atrophy (sarcopenia) are intimately connected and are reciprocally regulated by adipose tissue and skeletal muscle dysfunction. During ageing, adipose inflammation ...leads to the redistribution of fat to the intra‐abdominal area (visceral fat) and fatty infiltrations in skeletal muscles, resulting in decreased overall strength and functionality. Lipids and their derivatives accumulate both within and between muscle cells, inducing mitochondrial dysfunction, disturbing β‐oxidation of fatty acids, and enhancing reactive oxygen species (ROS) production, leading to lipotoxicity and insulin resistance, as well as enhanced secretion of some pro‐inflammatory cytokines. In turn, these muscle‐secreted cytokines may exacerbate adipose tissue atrophy, support chronic low‐grade inflammation, and establish a vicious cycle of local hyperlipidaemia, insulin resistance, and inflammation that spreads systemically, thus promoting the development of sarcopenic obesity (SO). We call this the metabaging cycle. Patients with SO show an increased risk of systemic insulin resistance, systemic inflammation, associated chronic diseases, and the subsequent progression to full‐blown sarcopenia and even cachexia. Meanwhile in many cardiometabolic diseases, the ostensibly protective effect of obesity in extremely elderly subjects, also known as the ‘obesity paradox’, could possibly be explained by our theory that many elderly subjects with normal body mass index might actually harbour SO to various degrees, before it progresses to full‐blown severe sarcopenia. Our review outlines current knowledge concerning the possible chain of causation between sarcopenia and obesity, proposes a solution to the obesity paradox, and the role of fat mass in ageing.
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FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SBCE, SBMB, UL, UM, UPUK
Considerable proportions of rice grains produced in some areas in southern China contain high concentrations of cadmium (Cd), leading to unsafe levels of dietary Cd intake. Cultivars of Indica rice, ...widely grown in southern China, are particularly prone to high Cd accumulation in the grain. Effective methods are needed to decrease Cd accumulation in Indica rice.
OsHMA3, encoding a tonoplast Cd transporter, was overexpressed in an elite Indica rice cultivar (Zhongjiazao 17) driven by CaMV 35S promoter. The effects on Cd translocation, accumulation and tolerance, as well as on the agronomic traits and micronutrient concentrations were evaluated.
OsHMA3 overexpression markedly decreased Cd translocation from roots to shoots and increased Cd tolerance. OsHMA3 overexpression decreased Cd concentrations in brown rice by 94–98%, to levels just above the detection limit, when rice plants were grown in two Cd-contaminated paddy soils. OsHMA3 overexpression generally had no significant effect on grain yield and the concentrations of the essential micronutrients including zinc, iron, copper and manganese in field trials.
Overexpression of OsHMA3 is a highly effective method to reduce Cd accumulation in Indica rice, producing rice grains that were almost Cd free with little effect on grain yield or essential micronutrient concentrations.
•High Cd concentrations of Cd are found in some rice produced in southern China.•Transgenic rice overexpressing OsHMA3 gene was developed in an elite Indica cultivar.•Overexpressing OsHMA3 decreased grain Cd concentration by 94–98%.•Overexpressing OsHMA3 had little effect on grain yield and essential micronutrients.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UILJ, UL, UM, UPCLJ, UPUK, ZAGLJ, ZRSKP
A double functionalization approach was developed to create efficient bifunctional electrocatalysts for electrochemical overall water splitting. Uniform Ni3Co(CN)62·12H2O nanocubes were taken as the ...starting material to fabricate the bifunctional catalysts through ammonia carving, conformal polydopamine coating, precursor metal ion coordination, and thermal phosphorization. N-doped carbon carved hollow nanocubes were loaded with hydrogen evolution reaction (HER) active (Ni-Co) phosphides in the interior cyanide-derived carbon layers and oxygen evolution reaction (OER) active (Ni-Fe) phosphides on the exterior polydopaimne-derived carbon layers. The product catalyst exhibited excellent electrolytic performances, achieving overpotentials of 251 and 142 mV for the OER and HER, respectively and a working cell voltage of 1.63 V for the overall water splitting all at 10 mA/cm2. Holes of several tens nanometers in size located at the eight vertices of the hollow cube allow easy access of the electrolyte to and fast rejection of evolving gas bubbles from the interior of the cube. The N-doped carbon nanocubes, providing fast charge transport pathway, and the positive synergistic effects arising from the mixed metal phosphides, significantly enhanced catalytic performances of the product catalyst. Both quantity and quality of the active sites are largely improved with the doubly functionalized N-doped carbon carved hollow nanocubes, which is a superior catalyst design for all electrocatalytic applications.
Doubly functionalized carbon carved hollow nanocubes, C-(Fe-Ni)P@PC/(Ni-Co)P@CC, were developed and demonstrated as a high performance bifunctional catalyst for electrochemical water splitting. Display omitted
•Double functionalization approach developed for bifunctional electrocatalysts.•N-doped carbon carved hollow nanocube structure increases quantity of active sites.•Well mixed metal phosphides induces synergistic effects to improve quality of active sites.•Require 1.63 V@10 mA cm−2 for full water splitting.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UILJ, UL, UM, UPCLJ, UPUK, ZAGLJ, ZRSKP
The key to develop efficient catalysts is to improve the quantity and activity of catalytic sites of the catalysts through optimal structural and compositional design. Accordingly, open-mouth N-doped ...carbon nanoboxes embedded with mixed metal phosphide nanoparticles are fabricated from monodisperse Ni
3
Fe(CN)
6
2
·H
2
O nanocubes through conformal Ni
3
Co(CN)
6
2
·12H
2
O layer coating, ammonia etching, and thermal phosphorization, sequentially. The product catalyst exhibits highly efficient electrocatalytic performances, achieving low overpotentials of 204 and 129 mV for the oxygen evolution reaction and hydrogen evolution reaction, respectively, and a small working voltage of 1.57 V for the overall water splitting, all at 10 mA cm
−2
. Its long-term electrocatalytic stability is also outstanding, experiencing only minor chronopotentiometric decay after a 24 h operation at 10 mA cm
−2
. The enhanced electrocatalytic performance may be attributed to the synergistic effects between the mixed metal phosphides, the protective function offered by the chainmail catalyst design, and the fast mass transport channels for the electrolyte and gaseous products afforded by the large openings on the nanobox shell, as well as the easy access of the inner active sites of the nanobox. The ingenious open-mouth nanobox structure together with embedded mixed metal phosphide nanoparticles is a unique design for improving the quantity and activity of catalytic sites of the catalyst for high efficiency electrolytic water splitting. The present design concept can be readily applied to the fabrication of other heterogeneous catalysts.
Open-mouth N-doped carbon nanoboxes with embedded mixed metal phosphide nanoparticles, E-(Fe-Ni)P@CC/(Co-Ni)P@CC, were designed and fabricated as highly efficient and durable catalysts for electrolytic water splitting.
Due to the pressure of global ecological degradation, the coordination of economic increase and ecological protection has drawn attention from policymakers and practitioners. Green economic ...efficiency (GEE) is a comprehensive index to measure economic, social, and environmental development. As China is the second-biggest economy in the world with high-energy consumption, it is necessary to investigate its green economy efficiency. In this paper, we innovatively adopt a super-SBM (slacks-based measure) model with undesirable outputs to calculate the GEE in 30 provinces of China between 2008 and 2017, and then comprehensively apply a spatial Dubin model (SDM) to investigated its influencing factors. The results showed that the overall GEE in China during the study period was at a low level with significant regional differences. The inter-regional GEE generally showed a gradient decreasing pattern of “East-Middle-West”, which demonstrates a gradual decline from the East to the West in China. The trend of the national GEE initially dropped and then gradually stabilized over the study period. Foreign trade dependence and direct investment had significant positive effects on the GEE, while the secondary industry and urbanization level had a significant negative effect.
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•Studying the concept of Green Economy Efficiency (GEE)•Coupling the Super-SBM model with the Spatial Dubin Model and Global Moran's I index•Finding the GEE in a gradient decreasing pattern of “East-Middle-West”•Revealing foreign trade dependency and direct investment with positive effects on GEE•Demonstrating secondary industry and urbanization level with significant negative effect
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UILJ, UL, UM, UPCLJ, UPUK, ZAGLJ, ZRSKP
The substantial heterogeneity and hierarchical organization in liver cancer support the theory of liver cancer stem cells (LCSCs). However, the relationship between chronic hepatic inflammation and ...LCSC generation remains obscure. Here, we observed a close correlation between aggravated inflammation and liver progenitor cell (LPC) propagation in the cirrhotic liver of rats exposed to diethylnitrosamine. LPCs isolated from the rat cirrhotic liver initiated subcutaneous liver cancers in nonobese diabetic/severe combined immunodeficient mice, suggesting the malignant transformation of LPCs toward LCSCs. Interestingly, depletion of Kupffer cells in vivo attenuated the LCSC properties of transformed LPCs and suppressed cytokeratin 19/Oval cell 6–positive tumor occurrence. Conversely, LPCs cocultured with macrophages exhibited enhanced LCSC properties. We further demonstrated that macrophage‐secreted tumor necrosis factor‐α triggered chromosomal instability in LPCs through the deregulation of ubiquitin D and checkpoint kinase 2 and enhanced the self‐renewal of LPCs through the tumor necrosis factor receptor 1/Src/signal transducer and activator of transcription 3 pathway, which synergistically contributed to the conversion of LPCs to LCSCs. Clinical investigation revealed that cytokeratin 19/Oval cell 6–positive liver cancer patients displayed a worse prognosis and exhibited superior response to sorafenib treatment. Conclusion: Our results not only clarify the cellular and molecular mechanisms underlying the inflammation‐mediated LCSC generation but also provide a molecular classification for the individualized treatment of liver cancer. (Hepatology 2017;66:1934–1951)
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SBCE, SBMB, UL, UM, UPUK
A highly efficient strategy for the kinetic resolution of axially chiral BINAM derivatives involving a chiral Brønsted acid‐catalyzed imine formation and transfer hydrogenation cascade process was ...developed. The kinetic resolution provides a convenient route to chiral BINAM derivatives in high yields with excellent enantioselectivities.
Chiral BINAMs on demand: A highly efficient strategy for the kinetic resolution of axially chiral BINAM derivatives involving a chiral Brønsted acid catalyzed imine formation and transfer hydrogenation cascade process was developed. The kinetic resolution provides a convenient route to chiral BINAM derivatives in high yields with excellent enantioselectivities.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SBCE, SBMB, UL, UM, UPUK
Layered oxides are the most prevalent cathodes for sodium‐ion batteries (SIBs), but their poor air stability significantly limits their practical application owing to the rapid performance ...degradation of aged materials and the cost increase for material storage and transportation. Here, an effective strategy of constructing stable transition metal (TM) layers with a highly symmetrical six‐TM ring is suggested to enhance structure stability, thus hindering ambient air corrosion. The density functional theory calculations reveal that the higher symmetry ensures a higher thermodynamic energy for H2O insertion into Na layer. The combined analyses of selected area electron diffraction, transmission electron microscopy, X‐ray photoelectron spectroscopy, Fourier transform infrared spectroscopy, thermogravimetric analysis, and chemical titration indicate that the six‐TM ring structure can effectively suppress the series of aging processes including water insertion, the spontaneous loss of lattice sodium, TM valence increment and residual alkali formation. Benefiting from the overall suppression of aging process, the strategy results in an excellent improvement in capacity retention after air exposure from 13.57% to 95.59%, and exhibits a good universality for both P2‐ and O3‐cathodes, which are the two most common structures of Na‐based layered oxides with different aging mechanism. These findings provide new insight to design high‐performance cathodes for SIBs.
An effective strategy of constructing stable transition metal (TM) layers with a highly symmetrical six‐TM ring structure is suggested to enhance the air stability of layered oxide cathodes via increasing the thermodynamic energy for H2O insertion into Na layer and suppressing the spontaneous loss of lattice sodium, and this strategy exhibits a good universality for both P2‐ and O3‐type materials.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SBCE, SBMB, UL, UM, UPUK
Abstract
Chemical modification of transcripts with 5′ caps occurs in all organisms. Here, we report a systems-level mass spectrometry-based technique, CapQuant, for quantitative analysis of an ...organism's cap epitranscriptome. The method was piloted with 21 canonical caps—m7GpppN, m7GpppNm, GpppN, GpppNm, and m2,2,7GpppG—and 5 ‘metabolite’ caps—NAD, FAD, UDP-Glc, UDP-GlcNAc, and dpCoA. Applying CapQuant to RNA from purified dengue virus, Escherichia coli, yeast, mouse tissues, and human cells, we discovered new cap structures in humans and mice (FAD, UDP-Glc, UDP-GlcNAc, and m7Gpppm6A), cell- and tissue-specific variations in cap methylation, and high proportions of caps lacking 2′-O-methylation (m7Gpppm6A in mammals, m7GpppA in dengue virus). While substantial Dimroth-induced loss of m1A and m1Am arose with specific RNA processing conditions, human lymphoblast cells showed no detectable m1A or m1Am in caps. CapQuant accurately captured the preference for purine nucleotides at eukaryotic transcription start sites and the correlation between metabolite levels and metabolite caps.
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