The NiOOH catalyst as obtained dynamically from electrodeposition of Ni2+(aq) in the borate-containing electrolyte was observed to exhibit much higher oxygen evolution activity at a near-neutral pH ...range (7–9) compared to other NiO x -based materials. Here, we demonstrate that this intriguing high activity is owing to the high concentration of Ni cationic vacancy on the nascent ultra-small NiOOH particles (<3 nm). By using first-principles calculations, we compute the thermodynamics of Ni dissolution and clarify the mechanism of oxygen evolution reaction (OER) on the γ-NiOOH surface. We show that (i) ∼4% Ni cations on the surface of γ-NiOOH dissolve at pH = 7 and 1.73 V versus reversible hydrogen electrode; (ii) on the pristine γ-NiOOH surface, OER proceeds via the “lattice peroxide” mechanism (*H2O → *OH → *O–OlattH* → O–Olatt → O2) with an overpotential of 0.70 V; (iii) in the presence of Ni cationic vacancies, OER proceeds via the “hydroperoxide” mechanism (*OH + *H2O → *2OH → *OOH → O2) with an overpotential of 0.40 V. Our electronic structure and geometrical structure analyses demonstrate that the structural flexibility at the four-coordinated Ni site nearby Ni vacancy, featuring the ability to bind two terminal oxo species, is key to boost the activity. Considering the presence of the active OOH intermediate, our theory thus implies that the ultra-small oxide nanoclusters with ample cation vacancies could be a paradigm in catalyst design for oxidation reactions.
The diverse biological effects of nanomaterials form the basis for their applications in biomedicine but also cause safety issues. Induction of autophagy is a cellular response after nanoparticles ...exposure. It may be beneficial in some circumstances, yet autophagy‐mediated toxicity raises an alarming concern. Previously, it has been reported that upconversion nanoparticles (UCNs) elicit liver damage, with autophagy contributing most of this toxicity. However, the detailed mechanism is unclear. This study reveals persistent presence of enlarged autolysosomes in hepatocytes after exposure to UCNs and SiO2 nanoparticles both in vitro and in vivo. This phenomenon is due to anomaly in the autophagy termination process named autophagic lysosome reformation (ALR). Phosphatidylinositol 4‐phosphate (PI(4)P) relocates onto autolysosome membrane, which is a key event of ALR. PI(4)P is then converted into phosphatidylinositol 4,5‐bisphosphate (PI(4,5)P2) by phosphatidylinositol‐4‐phosphate 5‐kinase. Clathrin is subsequently recruited by PI(4,5)P2 and leads to tubule budding of ALR. Yet it is observed that PI(4)P cannot be converted in nanoparticle‐treated hepatocytes cells. Exogenous supplement of PI(4,5)P2 suppresses the enlarged autolysosomes in vitro. Abolishment of these enlarged autolysosomes by autophagy inhibitor relieves the hepatotoxicity of UCNs in vivo. The results provide evidence for disrupted ALR in nanoparticle‐treated hepatocytes, suggesting that the termination of nanoparticle‐induced autophagy is of equal importance as the initiation.
In hepatocytes treated with upconversion nanoparticles (UCN) or nano‐SiO2, loss of phosphatidylinositol‐4‐phosphate 5‐kinase causes the disrupted phospholipid transition from phosphatidylinositol 4‐phosphate to phosphatidylinositol 4,5‐bisphosphate on enlarged autolysosomal membrane and clathrin fails to be recruited to autolysosomes; autophagic lysosome reformation is blocked, leading to enlarged autolysosomes. In the UCN‐treated mice liver, manipulation of autophagy by 3‐methyladenine or trehalose affects liver damage.
Background
Diagnostic criteria for sarcopenia have not been established in Chinese. This study established criteria based on the L3‐skeletal muscle index (L3‐SMI) and assessed its value for outcomes ...predicting in cirrhotic Chinese patients.
Methods
Totally 911 subjects who underwent a CT scan at two centres were enrolled in Cohort 1 (394 male and 417 female subjects, aged 20–80 years). The data of those subjects younger than 60 years (365 male and 296 female subjects) were used to determine the reference intervals of the L3‐SMI and its influencing factors. Cohort 2 consisted of 480 patients (286 male and 184 female patients) from three centres, and their data were used to investigate the prevalence of sarcopenia and evaluate the value of L3‐SMI for predicting the prognosis and complications of cirrhosis.
Results
Age and sex had the greatest effects on the L3‐SMI (P < 0.001). The L3‐SMI scores were clearly higher in male patients than in female patients (52.94 ± 8.41 vs. 38.91 ± 5.65 cm2/m2, P < 0.001) and sharply declined in subjects aged ≥ 60 years. Based on the mean −1.28 × SD among adults aged < 60 years, the L3‐SMI cut‐off value for sarcopenia was 44.77 cm2/m2 in male patients and 32.50 cm2/m2 in female patients. Using these values, 22.5% of the cirrhotic patients (28.7% of male patients and 11.9% of female patients) were diagnosed with sarcopenia. Compared with non‐sarcopenia individuals, sarcopenia patients had lower body mass index (21.28 ± 3.01 vs. 24.09 ± 3.39 kg/m2, P < 0.001) and serum albumin levels (31.54 ± 5.93 vs. 32.93 ± 5.95 g/L, P = 0.032), longer prothrombin times (16.39 ± 3.05 vs. 15.71 ± 3.20 s, P = 0.049), higher total bilirubin concentrations (41.33 ± 57.38 vs. 32.52 ± 31.48 μmol/L, P = 0.039), worse liver function (Child–Pugh score, 8.05 ± 2.11 vs. 7.32 ± 2.05, P = 0.001), higher prevalence of cirrhosis‐related complications (81.82% vs. 62.24%, P < 0.001) and mortality (30.68% vs. 11.22%, P < 0.001). Overall survival was significantly lower in the sarcopenia group risk ratio (RR) = 2.643, 95% confidence interval (CI) 1.646–4.244, P < 0.001, accompanied with an increased cumulative incidence of ascites (RR = 1.827, 95% CI 1.259–2.651, P = 0.002), spontaneous bacterial peritonitis (RR = 3.331, 95% CI 1.404–7.903, P = 0.006), hepatic encephalopathy (RR = 1.962, 95% CI 1.070–3.600, P = 0.029), and upper gastrointestinal varices (RR = 2.138, 95% CI 1.319–3.466, P = 0.002). Subgroup analysis showed sarcopenia shortened the survival of the patients with Model For End‐Stage Liver Disease score > 14 (RR = 4.310, 95% CI 2.091–8.882, P < 0.001) or Child–Pugh C (RR = 3.081, 95% CI 1.516–6.260, P = 0.002).
Conclusions
Sarcopenia is a common comorbidity of cirrhosis and can be used to predict cirrhosis‐related complications and the prognosis.
The recent intensification of the study of contact‐electrification at water‐solid interfaces and its role in physicochemical processes lead to the realization that electron transfers during ...water‐solid contact‐electrification can drive chemical reactions. This mechanism, named contact‐electro‐catalysis (CEC), allows chemically inert fluorinated polymers to act like single electrode electrochemical systems. This study shows hydrogen peroxide (H2O2) is generated from air and deionized water, by ultrasound driven CEC, using fluorinated ethylene propylene (FEP) as the catalyst. For a mass ratio of catalyst to solution of 1:10000, at 20 °C, the kinetic rate of H2O2 evolution reaches 58.87 mmol L−1 gcat−1 h−1. Electron paramagnetic resonance (EPR) shows electrons are emitted in the solution by the charged FEP, during ultrasonication. EPR and isotope labelling experiments show H2O2 is formed from hydroxyl radicals (HO•) or two superoxide radicals (O2•−) generated by CEC. Finally, it is traditionally believed such radicals migrate in the solution by Brownian diffusion prior to reactions. However, ab‐initio molecular dynamic calculations reveal the radicals can react by exchanging protons and electrons through the hydrogen bonds network of water, i.e., owing to the Grotthuss mechanism. This mechanism can be relevant to other systems, artificial or natural, generating H2O2 from air and water.
The present work shows that H2O2 can be produced from water and air through oxidoreduction processes triggered by ultrasound‐driven contact‐electrification at the interface of water and fluorinated ethylene propylene. The performance of the method greatly surpasses present piezocatalysis. This work proposes a clear demonstration of the mechanism and the contribution of the hydrogen bound network to the formation of H2O2.
Graphene oxide (GO), the functionalized graphene with oxygen-containing chemical groups, has recently attracted resurgent interests because of its superior properties such as large surface area, ...mechanical stability, tunable electrical and optical properties. Moreover, the surface functional groups of hydroxyl, epoxy and carboxyl make GO an excellent candidate in coordinating with other materials or molecules. Owing to the expanded structural diversity and improved overall properties, GO and its composites hold great promise for versatile applications of energy storage/conversion and environment protection, including hydrogen storage materials, photocatalyst for water splitting, removal of air pollutants and water purification, as well as electrode materials for various lithium batteries and supercapacitors. In this review, we present an overview on the current successes, as well as the challenges, of the GO-based materials for energy and environmental applications.
A schematic showing the GO/RGO-based hybrid materials for energy and environmental applications along with the SCI-indexed journal publications until now (January, 2015), searched from ISI by the keyword of graphene oxide combined with another one listed in the outer circle (left panel) or the X axis (right panel). Display omitted
•The progresses of GO application in hydrogen storage and photocatalytic water splitting have been elaborately summarized.•The progresses of GO application in lithium batteries and supercapacitors have been systematically discussed.•We summarized the versatile application of GO in air and water purification.
Drug use and relapse involve learned associations between drug-associated environmental cues and drug effects. Extinction procedures in the clinic can suppress conditioned responses to drug cues, but ...the extinguished responses typically reemerge after exposure to the drug itself (reinstatement), the drug-associated environment (renewal), or the passage of time (spontaneous recovery). We describe a memory retrieval-extinction procedure that decreases conditioned drug effects and drug seeking in rat models of relapse, and drug craving in abstinent heroin addicts. In rats, daily retrieval of drug-associated memories 10 minutes or 1 hour but not 6 hours before extinction sessions attenuated drug-induced reinstatement, spontaneous recovery, and renewal of conditioned drug effects and drug seeking. In heroin addicts, retrieval of drug-associated memories 10 minutes before extinction sessions attenuated cue-induced heroin craving 1, 30, and 180 days later. The memory retrieval-extinction procedure is a promising nonpharmacological method for decreasing drug craving and relapse during abstinence.
Polyamide (PA) thin-film composite (TFC) reverse osmosis (RO) membrane has been widely used for desalination to produce fresh water. In order to further enhance the membrane’s water flux without ...sacrificing the salt rejection, in this study, a new kind of three-dimension (3D) multi-layer graphene oxide (mGO) was synthesized through the layer-by-layer (LbL) crosslinking between the sing-layer GO (sGO) nanosheet and 1,3-diamino-2-propanol (DAPL) molecule, and then was introduced into the aqueous phase solution to modify the conventional polyamide TFC RO membrane via interfacial polymerization (IP). The size and structure of mGO were regulated through the optimization of LbL crosslinking techniques, and the effect of mGO on the micro-structure and macro-property of thin-film nanocomposite (TFN) RO membrane was correspondingly investigated. It was found that the mGO made the PA layer surface of RO membrane smoother and more hydrophilic. Most importantly, it increased the water flux of RO membrane, improved the salt rejection above 99.3%, and endowed the RO membrane better long-term stability. Obviously, this is due to that mGO created a certain d-spacing through crosslinking DAPL molecules between sGO nanosheets, which provided channels for water transport across the PA layer and thus accelerated the migration of water molecules in the membrane, ultimately enhancing the water flux of TFN RO membrane. Meanwhile, the DAPL grafted on the outmost surface of mGO enhanced the compatibility between mGO(30) and PA polymeric matrix via the reaction with TMC during the IP, further improving the membrane’s salt rejection. Therefore, this study provides a facile way to improve the comprehensive separation performance of RO membrane.
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•3D mGO was synthesized via LbL crosslinking between sGO nanosheet and DAPL.•The mGO was introduced in aqueous phase to modify the conventional TFC RO membrane.•The PA layer of mGO-based TFN RO membrane become thinner and more hydrophilic.•Flux and rejection of the mGO-based TFN RO membrane were improved concurrently.•Performance improvement is due to the channels in mGO and the DAPL grafted on mGO.
Two new species of the genus Clubiona Latreille, 1804 are described: C. tianpingshan sp. nov. (♂♀) and C. flammaforma sp. nov. (♂♀) from central and south China. The female of C. subcylindrata Wang ...et al., 2018 is described for the first time. Detailed descriptions, photographs of somatic features and copulatory organs, as well as a distribution map of these three species, are provided.
Integrated multi-omics evaluation of 823 tumors from advanced renal cell carcinoma (RCC) patients identifies molecular subsets associated with differential clinical outcomes to angiogenesis blockade ...alone or with a checkpoint inhibitor. Unsupervised transcriptomic analysis reveals seven molecular subsets with distinct angiogenesis, immune, cell-cycle, metabolism, and stromal programs. While sunitinib and atezolizumab + bevacizumab are effective in subsets with high angiogenesis, atezolizumab + bevacizumab improves clinical benefit in tumors with high T-effector and/or cell-cycle transcription. Somatic mutations in PBRM1 and KDM5C associate with high angiogenesis and AMPK/fatty acid oxidation gene expression, while CDKN2A/B and TP53 alterations associate with increased cell-cycle and anabolic metabolism. Sarcomatoid tumors exhibit lower prevalence of PBRM1 mutations and angiogenesis markers, frequent CDKN2A/B alterations, and increased PD-L1 expression. These findings can be applied to molecularly stratify patients, explain improved outcomes of sarcomatoid tumors to checkpoint blockade versus antiangiogenics alone, and develop personalized therapies in RCC and other indications.
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•Genomics of 823 RCC tumors, including 134 sarcomatoid tumors, reveals 7 subtypes•Subtype specific angiogenesis, immune, metabolic, stromal, and cell-cycle profiles•Differential prevalence of PBRM1, KDM5C, CDKN2A/2B, and TP53 alterations in subsets•Differential outcomes to VEGF blockade alone or in combination with anti-PD-L1
Motzer et al. perform integrative multi-omics analyses of 823 renal cancer tumors from a randomized clinical trial. A robust molecular classification scheme, based on transcriptional and gene alteration profiles and differential clinical outcomes to VEGF blockade alone or in combination with anti-PD-L1, informs personalized treatment strategies and future therapeutic development in RCC.
Reminiscence therapy has been reported to improve the well-being in patients with dementia. However, few studies have examined the effects of spiritual reminiscence, which emphasizes on reconnecting ...and enhancing the meaning of one's own experience, on patients with dementia. Therefore, this study aimed to investigate the effects of spiritual reminiscence on hope, life satisfaction, and spiritual well-being in elderly Taiwanese with mild or moderate dementia.
A randomized controlled trial was conducted on 103 patients with mild or moderate dementia recruited from a medical center in central Taiwan. The patients were randomly assigned to either a 6-week spiritual reminiscence group (n = 53) or control group (n = 50). The Herth Hope Index, the Life Satisfaction Scale, the Spirituality Index of Well-Being were administered before and after the 6-week period.
The interaction terms between group and time for the three outcome measures were found to be significant (P < 0.001), indicating that the changes over time in them were different between the intervention and control groups.
Findings of this randomized controlled trial showed that hope, life satisfaction, and spiritual well-being of elderly patients with mild or moderate dementia could significantly be improved with a 6-week spiritual reminiscence intervention.
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