Abstract
Glucose electrolysis offers a prospect of value-added glucaric acid synthesis and energy-saving hydrogen production from the biomass-based platform molecules. Here we report that ...nanostructured NiFe oxide (NiFeO
x
) and nitride (NiFeN
x
) catalysts, synthesized from NiFe layered double hydroxide nanosheet arrays on three-dimensional Ni foams, demonstrate a high activity and selectivity towards anodic glucose oxidation. The electrolytic cell assembled with these two catalysts can deliver 100 mA cm
−2
at 1.39 V. A faradaic efficiency of 87% and glucaric acid yield of 83% are obtained from the glucose electrolysis, which takes place via a guluronic acid pathway evidenced by in-situ infrared spectroscopy. A rigorous process model combined with a techno-economic analysis shows that the electrochemical reduction of glucose produces glucaric acid at a 54% lower cost than the current chemical approach. This work suggests that glucose electrolysis is an energy-saving and cost-effective approach for H
2
production and biomass valorization.
Environmental issues triggered by increasing nitrate in agricultural river has become global concern. Identifying nitrate sources and transformation are crucial for water sources protection and ...eliminating nitrate contamination in an agricultural watershed. In this study, chemical and dual isotopic compositions of nitrate were employed to trace the nitrate sources and transformation processes, and proportional contribution of NO3− source were estimated by SIAR based on Bayesian model. NH4+ concentrations in middle Mun and lower Mun in wet season were significantly higher than NO3−, suggesting enhanced runoff processes by flood promote agricultural fertilized NH4+ leaching into the river. Higher Cl− concentration and NO3−/Cl− indicated that manure and sewage was the dominate nitrate source in the Lam Takhong River and the upper Mun. The overall values of δ15N-NO3− and δ18O-NO3− ranged from −3.9‰ to +16.6‰ and from −5.2‰ to +40.0‰, respectively. The results of nitrate isotopes indicated that NO3− mainly originated from soil N nitrogen, chemical fertilizer, and manure and sewage wastes. Spatially, soil N and chemical fertilizer contributed the most nitrate in the mainstream of lower Mun, middle Mun, and the Lam Takhong River; whereas over 60% of nitrate was derived from manure and sewage in the upper Mun. The spatial variation of water discharge and rainfall, together with the nitrate concentration and isotopes inferred that the nitrate sources and transformations in rain-fed river in tropical zone were distinguished from other rivers. High water discharge driven by rainfall events accelerated the nitrate export and the contribution of atmospheric deposition in wet season, and enlarged the contribution of manure and sewage in dry season. This study provided an example for further researches and approaches to assess the effects of tropical climate and agriculture on nitrate accumulation in watershed.
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•NO3−/Cl− variations suggested that NO3− mainly from manure and sewage in the upper Mun.•Theoretical and measured δ18O suggested nitrification was the dominate processes.•Denitrification proved to dominate the nitrate transformation in middle and lower Mun.•Chemical fertilizer, soil N and Manure and sewage contributed more than 90% of nitrate inputs.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UILJ, UL, UM, UPCLJ, UPUK, ZAGLJ, ZRSKP
Efficient recruitment and angiogenesis of endothelial progenitor cells (EPCs) are critical during a thrombus event. However, the details of EPC recruitment and the regulation of angiogenesis have not ...been fully determined. The aim of this study was to determine the role of the long noncoding (lnc)RNA Wilms tumor 1 associated protein pseudogene 1 (WTAPP1) in regulation of the migration and angiogenesis of EPCs. EPCs were isolated from human peripheral blood and characterized by flow cytometry, after which lentivirus‐mediated lncRNA WTAPP1 overexpression and knockdown were performed. Scratch assay, Transwell assay, and in vitro and in vivo tube formation assays were performed to measure cell migration, invasion, and angiogenic abilities, respectively. Moreover, a microarray screen, bioinformatic prediction, and quantitative PCR and Western blot of miRNAs interacting with lncRNA WTAPP1 were conducted. Western blot was carried out to elucidate the relationship among WTAPP1, miR‐3120‐5P, and MMP‐1 in the autophagy pathway. WTAPP1 positively regulated migration, invasion, and in vitro and in vivo tube formation in EPCs by increasing MMP‐1 expression and activating PI3K/Akt/mTOR signaling. Furthermore, WTAPP1 contains a putative miR‐3120‐5P binding site. Suppression of WTAPP1 by miR‐3120‐5P decreased the level of MMP‐1. In addition, we demonstrated that suppression of the autophagy pathway is involved in the effects of WTAPP1 on EPC migration and angiogenesis. The lncRNA WTAPP1, a molecular decoy for miR‐3120‐5p, regulates MMP‐1 expression via the PI3K/Akt and autophagy pathways, thereby mediating cell migration and angiogenesis in EPCs. Acting as a potential therapeutic target, the lncRNA WTAPP1 may play an important role in the pathogenesis of DVT. Stem Cells 2018;36:1863–12
The long noncoding RNA Wilms tumor 1 associated protein pseudogene 1, a molecular decoy for miR‐3120‐5p, regulates MMP‐1 expression via the PI3K/Akt and autophagy pathways, thereby mediating cell migration and angiogenesis in endothelial progenitor cells.
A visible‐light photocatalytic generation of N‐centered hydrazonyl radicals has been accomplished for the first time. This approach allows efficient intramolecular addition of hydrazonyl radical to ...terminal alkenes, thus providing hydroamination and oxyamination products in good yields. Importantly, the protocol involves deprotonation of an NH bond and photocatalytic oxidation to an N‐centered radical, thus obviating the need to prepare photolabile amine precursors or the stoichiometric use of oxidizing reagents.
Centered on N: A visible‐light‐induced photocatalytic generation of N‐centered hydrazonyl radicals has been accomplished for the first time. This approach allows efficient intramolecular addition of hydrazonyl radical to terminal alkenes, thus providing hydroamination and oxyamination products in good yields. Importantly, the protocol involves direct NH oxidation under mild reaction conditions. Ts=4‐toluenesulfonyl.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SBCE, SBMB, UL, UM, UPUK
This study aims to evaluate the effects of cold atmospheric plasma (CAP) treatment on the bonding of resin cement to high-translucency zirconia. Zirconia specimens were subjected to different ...treatments: no treatment (ZrT), 10-methacryloyloxydecyl dihydrogen phosphate (MDP)-containing primer (ZrT-M), alumina particle air-abrasion with/without MDP-containing primer (ZrT-AM/ZrT-A), CAP with/without MDP-containing primer (ZrT-PM/ZrT-P). The surface topography, wettability, and chemical composition were evaluated. The shear bond strength (SBS) was tested before and after thermocycling. CAP did not alter the morphology, increased the wettability, and decreased the carbon/oxygen ratio of zirconia surface. The SBSs of ZrT-PM and ZrT-P were significantly higher than the other groups. After thermocycling, ZrT-A, ZrT-M, ZrT-AM, and ZrT-P showed comparable SBSs, all of which were lower than ZrT-PM. It was concluded that CAP improved the bonding performance of high-translucency zirconia without damaging its surface. The combination of CAP with MDP further enhanced the bond strength and may enable durable bonding.
Organic azides are highly reactive, which have long established as versatile building blocks in the assembly of structurally diverse N‐containing heterocycles. The conversion of organic azides into ...high‐value compounds is of great importance and a subject of enormous current interest. Transition metal‐catalyzed C(sp2)−H amination/annulation of organic azides provides a powerful tool for the transformation of organic azides into a wide range of biologically important heterocyclic frameworks. In this review, we aim to summarize the recent progress on organic azides‐mediated C(sp2)−H amination/annulation for N‐heterocycle synthesis enabled by transition metal catalysts. Representative strategies are discussed in detail, including catalytic systems, reaction scopes, limitations and mechanisms.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SBCE, SBMB, UL, UM, UPUK
Inspired by the efficient modular design of contemporary engineering, a design philosophy is proposed for the construction of molecular building blocks. Here, modular design of supramolecular organic ...frameworks (SOFs) for image‐guided photodynamic therapy (PDT) in vivo is presented. The closo‐dodecaborate cluster (B12) can selectively bind with the convex exterior of cucurbit8uril (CB8) with a molar ratio of 1:3 through chaotropic effect, which enables the CB8‐B12 based SOFs with exchangeable units/functions. After the B12 is modified with polyethylene glycol (PEG) and RGD sequence as target ligand and the CB8 is loaded with methylene blue (MB) as supramolecular photosensitizer, the SOFs can be easily prepared with wide engineering range. A uniform nanoshuttle (NanoSOF) with excellent water dispersibility and bioavailability can be prepared by simply mixing the B12‐PEG‐RGD and MB@CB8 in aqueous solution. As a proof of concept, the NanoSOF is applied as smart nanomedicine for targeted tumor imaging and PDT of tumor, and excellent tumor targeting ability as well as tumor ablation ability can be achieved in vivo. This work highlights the modular design of SOFs with exchangeable units/functions based on chaotropic effect, which may arouse research interests in many other fields.
Inspired by the modular design of contemporary engineering, the chaotropic effect between B12 and CB8 is applied as an assembling motif to construct supramolecular organic frameworks (SOFs) with exchangeable units/functions. Nanosized SOFs functionalized with a targeting ligand and loaded with photosensitizers can be easily prepared by modular design, and are successfully applied as smart nanomedicine for image‐guided photodynamic therapy in vivo.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SBCE, SBMB, UL, UM, UPUK
The radio-frequency atmospheric-pressure glow discharge (RF-APGD) plasma is a novel cold atmospheric plasma (CAP) source, which has low energy characteristic. This study investigated the effect of ...RF-APGD plasma on the mechanical properties of dentin collagen and resin-dentin bonding. The scanning electron microscopy analysis was performed before and after a novel RF-APGD plasma and a conventional CAP treatment and a tensile test was carried out for the stiffness of dentin collagen. The microtensile resin-dentin bond strength was tested either immediately or after a 50,000-cycle thermocycling process. Dentin collagen maintained an intact structure after a 45-s RF-APGD plasma treatment, whereas even a 10-s treatment with the conventional CAP collapsed the collagen scaffold. When compared with control groups, the RF-APGD plasma treatment showed: (i) an improved stiffness of dentin collagen; (ii) a significant improvement in the bonding strength before/after artificial aging. Thus, RF-APGD plasma treatment has excellent prospects as a resin-dentin bonding protocol.
Organic Fenton-like catalysis has been recently developed for water purification, but redox-active compounds have to be ex situ added as oxidant activators, causing secondary pollution problem. ...Electrochemical oxidation is widely used for pollutant degradation, but suffers from severe electrode fouling caused by high-resistance polymeric intermediates. Herein, we develop an in situ organic Fenton-like catalysis by using the redox-active polymeric intermediates, e.g., benzoquinone, hydroquinone, and quinhydrone, generated in electrochemical pollutant oxidation as H₂O₂ activators. By taking phenol as a target pollutant, we demonstrate that the in situ organic Fenton-like catalysis not only improves pollutant degradation, but also refreshes working electrode with a better catalytic stability. Both ¹O₂ nonradical and ·OH radical are generated in the anodic phenol conversion in the in situ organic Fenton-like catalysis. Our findings might provide a new opportunity to develop a simple, efficient, and cost-effective strategy for electrochemical water purification.
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BFBNIB, NMLJ, NUK, PNG, SAZU, UL, UM, UPUK
Coronavirus can cross the species barrier and infect humans with a severe respiratory syndrome. SARS-CoV-2 with potential origin of bat is still circulating in China. In this study, a prediction ...model is proposed to evaluate the infection risk of non-human-origin coronavirus for early warning.
The spike protein sequences of 2666 coronaviruses were collected from 2019 Novel Coronavirus Resource (2019nCoVR) Database of China National Genomics Data Center on Jan 29, 2020. A total of 507 human-origin viruses were regarded as positive samples, whereas 2159 non-human-origin viruses were regarded as negative. To capture the key information of the spike protein, three feature encoding algorithms (amino acid composition, AAC; parallel correlation-based pseudo-amino-acid composition, PC-PseAAC and G-gap dipeptide composition, GGAP) were used to train 41 random forest models. The optimal feature with the best performance was identified by the multidimensional scaling method, which was used to explore the pattern of human coronavirus.
The 10-fold cross-validation results showed that well performance was achieved with the use of the GGAP (g = 3) feature. The predictive model achieved the maximum ACC of 98.18% coupled with the Matthews correlation coefficient (MCC) of 0.9638. Seven clusters for human coronaviruses (229E, NL63, OC43, HKU1, MERS-CoV, SARS-CoV, and SARS-CoV-2) were found. The cluster for SARS-CoV-2 was very close to that for SARS-CoV, which suggests that both of viruses have the same human receptor (angiotensin converting enzyme II). The big gap in the distance curve suggests that the origin of SARS-CoV-2 is not clear and further surveillance in the field should be made continuously. The smooth distance curve for SARS-CoV suggests that its close relatives still exist in nature and public health is challenged as usual.
The optimal feature (GGAP, g = 3) performed well in terms of predicting infection risk and could be used to explore the evolutionary dynamic in a simple, fast and large-scale manner. The study may be beneficial for the surveillance of the genome mutation of coronavirus in the field.