Electronics allowing for visible light to pass through are attractive, where a key challenge is to make the core functional units transparent. Here, it is shown that transparent electronics can be ...constructed by epitaxial growth of metal–organic frameworks (MOFs) on single‐layer graphene (SLG) to give a desirable transparency of 95.7% to 550 nm visible light and an electrical conductivity of 4.0 × 104 S m−1. Through lattice and symmetry match, collective alignment of MOF pores and dense packing of MOFs vertically on SLG are achieved, as directly visualized by electron microscopy. These MOF‐on‐SLG constructs are capable of room‐temperature recognition of gas molecules at the ppb level with a linear range from 10 to 108 ppb, providing real‐time gas monitoring function in transparent electronics. The corresponding devices can be fabricated on flexible substrates with large size, 3 × 5 cm, and afford continuous folding for more than 200 times without losing conductivity or transparency.
Transparent electronics can be constructed by epitaxial growth of metal–organic frameworks (MOFs) on single‐layer graphene (SLG) to give desirable transparency. The excellent conductivity of SLG combined with the specific interaction to guest molecules offered by MOFs leads to the accurate detection of gases and distinguishing their types. The corresponding devices can be fabricated on flexible substrates and afford continuous folding.
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FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SAZU, SBCE, SBMB, UL, UM, UPUK
Most deep learning based single image dehazing methods use convolutional neural networks (CNN) to extract features, however CNN can only capture local features. To address the limitations of CNN, We ...propose a basic module that combines CNN and graph convolutional network (GCN) to capture both local and non-local features. The basic module consist of a CNN with triple attention modules (CAM) and a dual GCN module (DGM). CAM that combines the channel attention, spatial attention and pixel attention is designed to earn more weight from important local features. DGM combines spatial coherence computing and channel correlation computing to extract non-local information. The architecture of the network is similar to U-Net, and skip connections used in the symmetrical network can pass the image details from shallow layers to deep layers. Experimental results in several datasets indicate that the proposed method outperforms the state-of-the-arts both quantitatively and qualitatively.
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EMUNI, FIS, FZAB, GEOZS, GIS, IJS, IMTLJ, KILJ, KISLJ, MFDPS, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, SBMB, SBNM, UKNU, UL, UM, UPUK, VKSCE, ZAGLJ
In the synthetic laboratory, researchers typically rely on nuclear magnetic resonance (NMR) spectra to elucidate structures of synthesized products and confirm whether they match the desired target ...compounds. As chemical synthesis technology evolves toward intelligence and continuity, efficient computer-assisted structure elucidation (CASE) techniques are required to replace time-consuming manual analysis and provide the necessary speed. However, current CASE methods typically aim to derive precise chemical structures from spectroscopic data, yet they suffer from drawbacks such as low accuracy, high computational cost, and reliance on chemical libraries. In meticulously designed chemical synthesis reactions, researchers prioritize confirming the attainment of the target product based on NMR spectra, rather than focusing on identifying the specific product obtained. For this purpose, we innovatively developed a binary classification model, termed as MatCS, to directly predict the relationship between NMR spectra image (including 1H NMR and 13C NMR) and the molecular structure of the target compound. After evaluating various feature extraction methods, MatCS employs a combination of the Graph Attention Networks and Graph Convolutional Networks to learn the structural features of molecular graphs and the pretrained ResNet101 network with a Convolutional Block Attention Module to extract features from NMR spectra images. The results show that on a challenging Testsim data set, which poses difficulty in distinguishing spectra of similar molecular structures, MatCS achieves comprehensive evaluation metrics with an F1-score of 0.81 and an AUC value of 0.87. Simultaneously, it exhibited commendable performance on an external SDBS data set containing experimental NMR spectra, showcasing substantial potential for structural verification tasks in real automated chemical synthesis.
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IJS, KILJ, NUK, PNG, UL, UM
Forest management can influence multistakeholders' benefits across the forest-water-energy-food nexus at the watershed scale. However, bringing synergistic gains for multiple stakeholders is still a ...challenge for regional sustainable management. We took the Changhuajiang basin in China's Hainan Island as a case to present the impacts of synergistic management for upstream forest and reservoir optimization on the benefits of downstream hydropower enterprise and different farmers. By multimodel ensembles and scenario analysis, we quantified the relationships among upstream forest ecosystem management (rubber-intercropped), reservoir, water flow and downstream stakeholders' benefits (i.e., hydropower generation for the energy company, and available irrigation water for two downstream sites' farmers). We also adopted the genetic optimization algorithm to obtain the optimal reservoir infrastructure operation rule for the benefit improvement of multiple stakeholders. We found that rubber-intercropped management significantly increased reservoir inflow in the dry seasons (5%–170%) and reduced it in the rainy seasons (0.5%–7%). The irrigation water availability for downstream farmers in the Gao Canal and downstream irrigation areas correspondingly increased by 7% and 24.3% on average, respectively, with a slight change in hydropower production. Further, we found that water regulation by reservoir optimization operation could enhance the irrigation water supply (36.6–92% and 0–100% in Gao Canal and downstream irrigation areas, respectively) and hydropower generation (14.8–28.4%). This study indicates that the effect of upstream forest management on downstream multistakeholders' benefits could be strengthened by reservoir water flow regulation across the forest-water-energy-food nexus, and demonstrates the key role of infrastructure in regulating ecosystem service flow for strengthening the benefits of multistakeholders in the context of ecosystem management.
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•Change in water flow improved irrigated areas' water availability and slightly changed hydropower generation.•Reservoir optimization further improved benefits for farmers and hydropower company by regulating water flow.•Synergistic management of ecosystems and infrastructure can improve multistakeholders' benefits.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UILJ, UL, UM, UPCLJ, UPUK, ZAGLJ, ZRSKP
Background and Aims
During liver fibrosis, liver sinusoidal endothelial cells (LSECs) release angiocrine signals to recruit inflammatory cells into the liver. p300, a master regulator of gene ...transcription, is associated with pathological inflammatory response. Therefore, we examined how endothelial p300 regulates angiocrine signaling and inflammation related to portal hypertension and fibrogenesis.
Approach and Results
CCl4 or partial inferior vena cava ligation (pIVCL) was used to induce liver injury. Mice with LSEC‐specific p300 deletion (p300LSECΔ/Δ) or C‐C motif chemokine ligand 2 (Ccl2) deficiency, nuclear factor kappa B (NFκB)–p50 knockout mice, and bromodomain containing 4 (BRD4) inhibitors in wild‐type mice were used to investigate mechanisms of inflammation regulation. Leukocytes were analyzed by mass cytometry by time‐of‐flight. Epigenetic histone marks were modified by CRISPR endonuclease‐deficient CRISPR‐associated 9‐fused with the Krüppel associated box domain (CRISPR‐dCas9‐KRAB)–mediated epigenome editing. Portal pressure and liver fibrosis were reduced in p300LSECΔ/Δ mice compared to p300fl/fl mice following liver injury. Accumulation of macrophages was also reduced in p300LSECΔ/Δ mouse livers. Ccl2 was the most up‐regulated chemokine in injured LSECs, but its increase was abrogated in p300LSECΔ/Δ mice. While the macrophage accumulation was increased in NFκB‐p50 knockout mice with enhanced NFκB activity, it was reduced in mice with LSEC‐specific Ccl2 deficiency and mice treated with specific BRD4 inhibitors. In vitro, epigenome editing of CCL2 enhancer and promoter regions by CRISPR‐dCas9‐KRAB technology repressed TNFα‐induced CCL2 transcription through H3K9 trimethylation. In contrast, TNFα activated CCL2 transcription by promoting p300 interaction with NFκB and BRD4, leading to histone H3 lysine 27 acetylation at CCL2 enhancer and promoter regions.
Conclusions
In summary, endothelial p300 interaction with NFκB and BRD4 increases CCL2 expression, leading to macrophage accumulation, portal hypertension, and liver fibrosis. Inhibition of p300 and its binding partners might serve as therapy in the treatment of liver diseases.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SAZU, SBCE, SBMB, UL, UM, UPUK
Effective conversion of chitin or its derivatives (i.e., chitosan) to value-added organonitrogen compounds is a promising strategy to valorize chitin. Glucosaminic acid (GlcNA) is an important amino ...acid derived from chitosan. In this work, we demonstrate the feasibility of GlcNA production from chitosan by tandem hydrolysis and oxidation reactions without isolating glucosamine (GlcN) intermediate. The Amberlyst-15 and Au/MgO were identified as suitable catalysts for the hydrolysis and oxidation step, respectively, but the direct employment of hydrolysate from the first step in further oxidation resulted in very low yield of target amino acid. We show that humin-like polymers formed during hydrolysis poisoned Au/MgO, resulting in low GlcNA yield, and subsequently a key detoxication process of the hydrolyzed mixture using activated carbon was developed. It effectively removed the undesired side products that inhibit Au catalyzed oxidation reaction, markedly enhancing the GlcNA yield from 17% for untreated hydrolysate to 63% for preadsorbed sample. As such, a two-step process is developed to produce GlcNA from chitosan with an overall yield of 36%.
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IJS, KILJ, NUK, PNG, UL, UM
We report a novel solid organocatalyst, a double-hydrogen-bonded sulfonated polymer catalyst (D-SPC), for the cascade conversion of fructose to 5-ethoxymethylfurfural (EMF) with a highest yield of ...68.8 mol% and good catalyst recyclability. We demonstrate that the treatment of a sulfonated nitrogen-containing polymer catalyst (SPC) with dihydroxy acetone (DHA) molecules generates new double hydrogen-bonds (H-bonds) between the ring-attached sulfonic acid groups and DHA by deconstructing the existing H-bonds between the sulfonic acid groups and imine/amine nitrogens of the SPC, which is confirmed by FT-IR spectroscopy, elemental analysis,
1
H MAS and
13
C cross-polarization MAS NMR, X-ray photoelectron spectroscopy (XPS), and quantum chemical calculations. The
31
P MAS NMR, pH
surface
, and NH
3
-TPD of the catalysts reveal the weakening of acidity strength due to the stronger double H-bonding on the D-SPC. Notably, we figure out the inverse relationship between the acidity strength of the catalysts and the EMF yield in the one-pot fructose-to-EMF conversion, wherein the use of weaker acid catalysts accelerates the fructose dehydration while decelerating the side-reaction of furan ring opening, therefore avoiding the negative influence of water on the tandem reactions. Moreover, the existence of stable double H-bonds contributes to the good catalyst recyclability due to the stabilization of sulfonic acid groups. The acidic property of the solid catalysts could be adjusted by varying the DHA dosage and the preparation conditions of the SPC (
i.e.
, monomer ratio and oxidant dosage), respectively. We show that the solid acid catalyst with weaker acidity strength and suitable acidity density (
ca.
2.5 mmol g
−1
) is favorable for the one-pot synthesis of EMF directly from fructose. This work highlights the application of novel sulfonated polymer catalysts with adjustable acidic property for the highly selective production of EMF, a liquid biofuel candidate, from biomass-derived carbohydrates.
The removal of volatile organic compounds (VOCs) from flue gas by a tightly coupled catalytic oxidation process in the NH3-SCR unit is a cost-effective approach. A CuCeOx bimetallic mixed oxide ...catalyst prepared by the co-precipitation method has demonstrated the ability to completely convert toluene at 350 ℃ under simulated flue gas conditions. Cu oxide is considered as the main active site for toluene oxidation, and the introduction of Ce induced a synergistic effect which enhanced the surface adsorbed oxygen and oxidation performance. The CuCeOx catalyst was found to outperform commercial VOC catalysts (Pt/Al2O3) and SCR catalysts (V2O5-WO3/TiO2) under the influence of different flue gas components. The negative effect of the flue gas on CuCeOx almost diminished at 350 ℃. The mechanism study showed that toluene on CuCeOx underwent a rapid oxidation pathway, thereby avoiding the potential interaction between intermediates and flue gas components. The superior catalytic performance of CuCeOx in the simulated flue gas conditions were attributed to the higher toluene adsorption efficiency and weaker adsorption towards the flue gas components.
•CuCeOx can completely convert toluene in the simulated fuel gas at 350 ℃.•At 350 ℃, the CO2 selectivity of CuCeOx was almost unaffected by the flue gas.•A rapid oxidation pathway for toluene has minimized flue gas disturbance.•CuCeOx exhibit higher toluene adsorption efficiency under flue gas conditions.
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GEOZS, IJS, IMTLJ, KILJ, KISLJ, NLZOH, NUK, OILJ, PNG, SAZU, SBCE, SBJE, UILJ, UL, UM, UPCLJ, UPUK, ZAGLJ, ZRSKP
We report the preparation of bifunctional hybrid catalysts by supporting H3PMo12O40 (PMo12) heteropolyacid (HPA) on polyaniline (PAN) or formyl-functionalized PAN (F-PAN) for the “one-pot” and ...“one-step” synthesis of 2,5-diformylfuran (DFF) from fructose via 5-hydroxymethylfurfural (HMF) intermediate. We show that the PMo12 HPA is the main active species for both fructose dehydration and HMF oxidation owing to its Brønsted acidic and redox characters. However, the anchoring of PMo12 on PAN reduces the Brønsted acidity by acid–base interaction between protons in HPA and quinoid diimine structure in PAN, thereby reducing the dehydration performance. We demonstrate that the catalytic dehydration performance of the hybrid catalyst could be strengthened by grafting formyl groups on PAN before HPA anchoring. The highest DFF yield of 76.7% is obtained by conducting the “one-pot” reaction over the 40-PMo12/F3-PAN catalyst at 413 K for 7 h in air, wherein the side-reactions of fructose or HMF degradation and HMF rehydration have been significantly reduced. This hybrid catalyst is reusable without significant activity loss, highlighting the designing of stable inorganic–organic hybrid catalysts for producing valuable hexose-derived platform chemicals.
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IZUM, KILJ, NUK, PILJ, PNG, SAZU, UL, UM, UPUK
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