Surface-Casting Synthesis of Mesoporous Zirconia with a CMK-5-Like Structure and High Surface Area.

About 15 years ago, the Ryoo group described the synthesis of CMK-5, a material consisting of a hexagonal arrangement of carbon nanotubes. Extension of the surface casting synthesis to oxide compositions, however, was not possible so far, in spite of many attempts. Here it is demonstrated, that crystalline mesoporous hollow zirconia materials with very high surface areas up to 400 m2 g-1 , and in selected cases in the form of CMK-5-like, are indeed accessible via such a surface casting process. The key for the successful synthesis is an increased interaction between the silica hard template surface and the zirconia precursor species by using silanol group-rich mesoporous silica as a hard template. The surface areas of the obtained zirconias exceed those of conventionally hard-templated ones by a factor of two to three. The surface casting process seems to be applicable also to other oxide materials.

Catalysis Meets Nonthermal Separation for the Production of (Alkyl)phenols and Hydrocarbons from Pyrolysis Oil.

A simple and efficient hydrodeoxygenation strategy is described to selectively generate and separate high-value alkylphenols from pyrolysis bio-oil, produced directly from lignocellulosic biomass. The overall process is efficient and only requires low pressures of hydrogen gas (5 bar). Initially, an investigation using model compounds indicates that MoCx /C is a promising catalyst for targeted hydrodeoxygenation, enabling selective retention of the desired Ar-OH substituents. By applying this procedure to pyrolysis bio-oil, the primary products (phenol/4-alkylphenols and hydrocarbons) are easily separable from each other by short-path column chromatography, serving as potential valuable feedstocks for industry. The strategy requires no prior fractionation of the lignocellulosic biomass, no further synthetic steps, and no input of additional (e.g., petrochemical) platform molecules.

Nitrogen-Doped Ordered Mesoporous Carbon Supported Bimetallic PtCo Nanoparticles for Upgrading of Biophenolics.

Hydrodeoxygenation (HDO) is an attractive route for the upgrading of bio-oils produced from lignocellulose. Current catalysts require harsh conditions to effect HDO, decreasing the process efficiency in terms of energy and carbon balance. Herein we report a novel and facile method for synthesizing bimetallic PtCo nanoparticle catalysts (ca. 1.5 nm) highly dispersed in the framework of nitrogen-doped ordered mesoporous carbon (NOMC) for this reaction. We demonstrate that NOMC with either 2D hexagonal (p6m) or 3D cubic (Im3‾ m) structure can be easily synthesized by simply adjusting the polymerization temperature. We also demonstrate that PtCo/NOMC (metal loading: Pt 9.90 wt %; Co 3.31 wt %) is a highly effective catalyst for HDO of phenolic compounds and "real-world" biomass-derived phenolic streams. In the presence of PtCo/NOMC, full deoxygenation of phenolic compounds and a biomass-derived phenolic stream is achieved under conditions of low severity.

A mixed ionic and electronic conducting dual-phase membrane with high oxygen permeability.

To combine good chemical stability and high oxygen permeability, a mixed ionic-electronic conducting (MIEC) 75 wt% Ce(0.85)Gd(0.1)Cu(0.05)O(2-δ)-25 wt% La(0.6)Ca(0.4)FeO(3-δ)(CGCO-LCF) dual-phase membrane based on a MIEC-MIEC composite has been developed. Copper doping into Ce(0.9)Gd(0.1)O(2-δ) (CGO) oxide enhances both ionic and electronic conductivity, which then leads to a change from ionic conduction to mixed conduction at elevated temperatures. For the first time we demonstrate that an intergranular film with 2-10 nm thickness containing Ce, Ca, Gd, La, and Fe has been formed between the CGCO grains in the CGCO-LCF one-pot dual-phase membrane. A high oxygen permeation flux of 0.70 mL min(-1) cm(-2) is obtained by the CGCO-LCF one-pot dual-phase membrane with 0.5 mm thickness at 950 °C using pure CO2 as the sweep gas, and the membrane shows excellent stability in the presence of CO2 even at lower temperatures (800 °C) during long-term operation.

Omni-dimensional dynamic convolution feature coordinate attention network for pneumonia classification.

Pneumonia is a serious disease that can be fatal, particularly among children and the elderly. The accuracy of pneumonia diagnosis can be improved by combining artificial-intelligence technology with X-ray imaging. This study proposes X-ODFCANet, which addresses the issues of low accuracy and excessive parameters in existing deep-learning-based pneumonia-classification methods. This network incorporates a feature coordination attention module and an omni-dimensional dynamic convolution (ODConv) module, leveraging the residual module for feature extraction from X-ray images. The feature coordination attention module utilizes two one-dimensional feature encoding processes to aggregate feature information from different spatial directions. Additionally, the ODConv module extracts and fuses feature information in four dimensions: the spatial dimension of the convolution kernel, input and output channel quantities, and convolution kernel quantity. The experimental results demonstrate that the proposed method can effectively improve the accuracy of pneumonia classification, which is 3.77% higher than that of ResNet18. The model parameters are 4.45M, which was reduced by approximately 2.5 times. The code is available at https://github.com/limuni/X-ODFCANET .

Natural gas to fuels and chemicals: improved methane aromatization in an oxygen-permeable membrane reactor.

Adding value with membranes: Improved methane aromatization was achieved by using an oxygen-permeable membrane. The resulting membrane reactor shows a superior methane conversion and a higher resistance towards catalyst deactivation.

Realization of Quantum Secure Direct Communication with Continuous Variable.

With the progress of theoretical and applied technologies, the communication system based on the classical encryption is seriously threatened by quantum computing and distributed computing. A communication method that directly loads confidential information on the quantum state, quantum secure direct communication (QSDC), came into being for resisting security threats. Here, we report the first continuous-variable QSDC (CV-QSDC) experimental demonstration for verifying the feasibility and effectiveness of the CV-QSDC protocol based on Gaussian mapping and propose a parameter estimation for signal classification under the actual channels. In our experiment, we provided 4 × 102 blocks, where each block contains 105 data for direct information transmission. For the transmission distance of 5 km in our experiment, the excess noise is 0.0035 SNU, where SNU represents the unit of shot-noise units. The 4.08 × 105 bit per second experimental results firmly demonstrated the feasibility of CV-QSDC under the fiber channel. The proposed grading judgment method based on parameter estimation provides a practical and available message processing scheme for CV-QSDC in a practical fiber channel and lays the groundwork for the grading reconciliation.

Hydrogenation of different carbon substrates into light hydrocarbons by ball milling.

The conversion of carbon-based solids, like non-recyclable plastics, biomass, and coal, into small molecules appears attractive from different points of view. However, the strong carbon-carbon bonds in these substances pose a severe obstacle, and thus-if such reactions are possible at all-high temperatures are required1-5. The Bergius process for coal conversion to hydrocarbons requires temperatures above 450 °C6, pyrolysis of different polymers to pyrolysis oil is also typically carried out at similar temperatures7,8. We have now discovered that efficient hydrogenation of different solid substrates with the carbon-based backbone to light hydrocarbons can be achieved at room temperature by ball milling. This mechanocatalytic method is surprisingly effective for a broad range of different carbon substrates, including even diamond. The reaction is found to proceed via a radical mechanism, as demonstrated by reactions in the presence of radical scavengers. This finding also adds to the currently limited knowledge in understanding mechanisms of reactions induced by ball milling. The results, guided by the insight into the mechanism, could induce more extended exploration to broaden the application scope and help to address the problem of plastic waste by a mechanocatalytic approach.

Flexibilization of Biorefineries: Tuning Lignin Hydrogenation by Hydrogen Partial Pressure.

The present study describes an interesting and practical catalytic system that allows flexible conversion of lignin into aromatic or aliphatic hydrocarbons, depending on the hydrogen partial pressure. A combination of experiment and theory shows that the product distribution between aromatics and aliphatics can be simply tuned by controlling the availability of hydrogen on the catalyst surface. Noticeably, these pathways lead to almost complete oxygen removal from lignin biomass, yielding high-quality hydrocarbons. Thus, hydrogen-lignin co-refining by using this catalytic system provides high flexibility in hydrogen storage/consumption towards meeting different regional and temporal demands.

Effects of simulated saliva-gastrointestinal digestion on the physicochemical properties and bioactivities of okra polysaccharides.

This study was to investigate the effects of in vitro simulated saliva-gastrointestinal digestion on the physicochemical properties and bioactivities of okra polysaccharides (OPS). Results showed that the digestibilities of OPS were about 5.1%, 37.5%, and 41.3% after saliva digestion (SD), saliva-gastric digestion (SGD), and saliva-gastrointestinal digestion (SGID), respectively. The SGID significantly changed the physicochemical properties of OPS, such as total uronic acids, total flavonoids, monosaccharide composition, rheological properties, and molecular weights (Mw). Especially, Mw changes resulted in the breakdown of glycosidic bonds during SGD, and the degradation of OPS during SGID was mainly caused by disrupting aggregates. Furthermore, the bioactivities of OPS were also affected by SGID. After SGID, OPS still possessed strong antioxidant activities, binding capacities, and prebiotic activities, but the α-glucosidase inhibitory effect was obviously decreased. Overall, results can provide valuable and scientific support on the oral administration of OPS as functional foods and medicines in the future.

Influences of different drying methods on the structural characteristics and multiple bioactivities of polysaccharides from okra (Abelmoschus esculentus).

In this study, in order to evaluate the influences of drying methods on the chemical structures and bioactivities of polysaccharides from okra (OPPs), four drying methods, including microwave drying at 400 W, 600 W, and 800 W, freezing drying, hot air drying, and vacuum drying, were applied to dry okra fruits. Six different OPPs were extracted from okra dried by different drying methods. Results showed that physicochemical characteristics and bioactivities of OPPs varied by different drying methods. Noticeable variations in extraction yields, molecular weights, rheological properties, molar ratios of constituent monosaccharides, contents of uronic acids, degrees of esterification, and contents of total phenolics were observed in OPPs obtained by different drying methods. In addition, results showed that OPPs, especially OPP-H and OPP-V obtained by hot air drying and vacuum drying, respectively, exhibited remarkable antioxidant activities (ABTS, DPPH, and nitric oxide radical scavenging activities, and ferric reducing antioxidant powers), strong in vitro binding capacities (fat, cholesterol, and bile acids binding capacities), and obvious inhibitory activities on α-amylase and α-glucosidase. Results suggested that the hot air and vacuum drying techniques could be appropriate drying methods before extraction of OPPs with high bioactivities for applications in the functional food and medicine industries.

Analysis of Methanolic Extracts and Crude Polysaccharides from the Leaves of Chuanminshen violaceum and Their Antioxidant Activities.

The root of Chuanminshen violaceum is used as an important edible and medicinal plant in China. However, its leaves are generally considered byproducts, and therefore do not have a use. Thus, the phenolic compounds in the methanolic extracts (CVLMs) and the chemical characteristics of crude polysaccharides (CVLPs) from the leaves of C. violaceum and their in vitro antioxidant activities were explored. The results showed that chlorogenic acid and rutin were the major individual phenolic compounds in the leaves, which ranged from 1.22 ± 0.03 to 2.87 ± 0.04 mg/g DW, and from 2.25 ± 0.04 to 4.03 ± 0.05 mg/g DW, respectively. Meanwhile, the extraction yields of CVLPs from the leaves ranged from 4.73% to 5.41%. The CVLPs consisted of mannose, rhamnose, galacturonic acid, glucose, galactose, and arabinose, suggesting the existence of pectic polysaccharides. Furthermore, both CVLMs and CVLPs exhibited strong antioxidant activities. Chlorogenic acid and rutin were major contributors to the antioxidant activities of CVLMs, and the antioxidant activities of CVLPs were closely correlated to their α-1,4-D-galactosiduronic linkages. The results are beneficial for understanding the chemical properties and in vitro antioxidant activities of CVLMs and CVLPs. The leaves of C. violaceum have potential to be developed as natural antioxidants.

Learning to Map Social Network Users by Unified Manifold Alignment on Hypergraph.

Nowadays, a lot of people possess accounts on multiple online social networks, e.g., Facebook and Twitter. These networks are overlapped, but the correspondences between their users are not explicitly given. Mapping common users across these social networks will be beneficial for applications such as cross-network recommendation. In recent years, a lot of mapping algorithms have been proposed which exploited social and/or profile relations between users from different networks. However, there is still a lack of unified mapping framework which can well exploit high-order relational information in both social structures and profiles. In this paper, we propose a unified hypergraph learning framework named unified manifold alignment on hypergraph (UMAH) for this task. UMAH models social structures and user profile relations in a unified hypergraph where the relative weights of profile hyperedges are determined automatically. Given a set of training user correspondences, a common subspace is learned by preserving the hypergraph structure as well as the correspondence relations of labeled users. UMAH intrinsically performs semisupervised manifold alignment with profile information for calibration. For a target user in one network, UMAH ranks all the users in the other network by their probabilities of being the corresponding user (measured by similarity in the subspace). In experiments, we evaluate UMAH on three real world data sets and compare it to state-of-art baseline methods. Experimental results have demonstrated the effectiveness of UMAH in mapping users across networks.

A Convergent Approach for a Deep Converting Lignin-First Biorefinery Rendering High-Energy-Density Drop-in Fuels.

Herein, a lignin-centered convergent approach to produce either aliphatic or aromatic bio-hydrocarbons is introduced. First, poplar or spruce wood was deconstructed by a lignin-first biorefining process, a technique based on the early-stage catalytic conversion of lignin, yielding lignin oils along with cellulosic pulps. Next, the lignin oils were catalytically upgraded in the presence of a phosphidated Ni/SiO2 catalyst under H2 pressure. Notably, selectivity toward aliphatics or aromatics can simply be adjusted by changes in H2 pressure and temperature. The process renders two distinct main cuts of branched hydrocarbons (gasoline: C6-C10, and kerosene/diesel: C14-C20). As the approach is H2-intensive, we examined the utilization of pulp as an H2 source via gasification. For several biomass sources, the H2 obtainable by gasification stoichiometrically meets the H2 demand of the deep converting lignin-first biorefinery, making this concept plausible for the production of high-energy-density drop-in biofuels.

A novel CO2-stable dual phase membrane with high oxygen permeability.

By cobalt-doping of the mixed conducting phase PSFC, a good combination of high CO2 stability and high oxygen permeability is obtained for the 60 wt% Ce(0.9)Pr(0.1)O(2-δ)-40 wt% Pr(0.6)Sr(0.4)Fe(0.5)Co(0.5)O(3-δ) (CP-PSFC) dual phase membrane, which suggests that CP-PSFC is a promising membrane for industrial applications in the oxyfuel process for CO2 capture.