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Herein, well-defined hollow dendritic AuPtAg alloyed nanocrystals (ANCs) were synthesized by a simple L -proline-mediated one-pot aqueous method. More importantly, the synthesized hollow dendritic architectures provide a suitable platform for immobilization of anti-prostate specific antigen (PSA). The resultant label-free immunosensor exhibited the improved performance for highly sensitive detection of PSA based on the enhanced catalytic currents of K 3 [Fe(CN) 6 ] as a signal probe. Impressively, the immunosensor showed the wide linear range of 0.05–50 ng mL –1 and low detection limit of 0.017 ng mL –1 under optimal conditions for the assay of PSA, couple with the improved stability, reproducibility and selectivity. It provides a promising platform for clinical research and diagnosis. [ABSTRACT FROM AUTHOR]

[Display omitted] [ABSTRACT FROM AUTHOR]

Nowadays, novel and efficient signal amplification strategy in electrochemiluminescence (ECL) platform is urgently needed to enhance the sensitivity of biosensor. In this work, the dual ECL signal enhancement strategy was constructed by the interactions of Pd nanoparticles attached covalent organic frameworks (Pd NPs@COFs) with tris (bipyridine) ruthenium (RuP) and Exonuclease III (Exo.III) cycle reaction. Within this strategy, the COFs composite was generated from the covalent reaction between 2-nitro-1,4-phenylenediamine (NPD) and trialdehyde phloroglucinol (Tp), and then animated by glutamate (Glu) to attach the Pd NPs. Next, the "signal on" ECL biosensor was constructed by the coordination assembly of thiolation capture DNA (cDNA) onto the Pd NPs@COFs modified electrode. After the aptamer recognition of progesterone (P4) with hairpin DNA 1 (HP1), the Exo. III cycle reaction was initiated with HP2 to generate free DNA, which hybridized with cDNA to form double-stranded DNA (dsDNA). For that, the RuP was embedded into the groove of dsDNA and achieved the ultrasensitive detection of P4 with a lower limit of detection (LOD) down to 0.45 pM, as well as the excellent selectivity and stability. This work expands the COFs-based materials application in ECL signal amplification and valuable DNA cyclic reaction in biochemical testing field. [Display omitted] • The Pd NPs were in situ produced on the COFs for signal enhancement of RuP. • The Exo. III assisted cyclic reaction was initiated by P4 to generate more DNA. • The dual signal amplification strategy was designed for the detection of P4. [ABSTRACT FROM AUTHOR]

Lignin is continuously investigated by various techniques for valorization due to its high content of oxygen-containing functional groups. Catalytic systems employing hydrolysis‑hydrogenolysis, leveraging the synergistic effect of redox metal sites and acid sites, exhibit efficient degradation of lignin. The predominance of either hydrolysis or hydrogenolysis reactions hinges upon the relative activity of acid and metal sites, as well as the intensity of the reductive atmosphere. In this study, the Pd-MoO x /TiO 2 catalyst was found to primarily catalyze hydrolysis in the lignin depolymerization process, attributed to the abundance of moderate acidic sites on Pd and the redox-assisted catalysis of MoO x under inert conditions. After subjecting the reaction to 240 °C for 30 h, a yield of 48.22 wt% of total phenolic monomers, with 5.90 wt% consisting of diphenols, was achieved. Investigation into the conversion of 4-propylguaiacol (4-PG), a major depolymerized monomer of corncob lignin, revealed the production of ketone intermediates, a phenomenon closely linked to the unique properties of MoO x. Dehydrogenation of the propyl is a key step in initiating the reaction, and 4-PG could be almost completely transformed, accompanied by an over 97 % of 4-propylcatechol selectivity. This distinctive system lays a new theoretical groundwork for the eco-friendly valorization of lignin. • 4-PG could be nearly full converted into 4-propylcatechol with over 97% selectivity. • Hydrolysis by Pd acidic catalysis is the dominant reaction over hydrogenolysis. • Redox-assisted catalysis of MoO x produced from hexaammonium heptamolybdate tetrahydrate plays an important role. • Ketones found in the reaction are special intermediates. • 48.22 wt% of phenols are yielded from corncob lignin depolymerization. [ABSTRACT FROM AUTHOR]

Continuous visbreaking of heavy oil in a tubular reactor was studied under pressurized steam environments at 10 MPa (MPS) and 18 MPa (HPS). Within the operating range considered, heavy oil and pressurized steam exhibit a liquid-vapor two-phase structure. During the transition from the MPS environment to the HPS environment, the dissolution of water into the oil phase is promoted, thereby reducing the viscosity of the oil phase. According to the lumped reaction kinetics analysis, the reaction behavior of the lumped component VR2 with a boiling point higher than 700 °C determines the visbreaking efficiency in the early visbreaking stage to a large extent. Dealkylation of VR2 and condensation of the lightest lumped component show sensitive responses to improved diffusion in the oil phase. At 400 °C and a space time of 37 min, visbreaking in HPS environment can achieve a viscosity reduction rate of 90%. Meanwhile, the asphaltene content of the product is lower than the feedstock value. • Continuous heavy oil visbreaking was investigated in pressurized steam environments. • Visbreaking products with reduced viscosity and asphaltene content can be obtained. • Dissolution of water in heavy oil reduces the viscosity of the oil phase. • Reaction kinetics of visbreaking respond sensitively to diffusion improvement. • Dealkylation of heaviest components determines initial visbreaking efficiency. [ABSTRACT FROM AUTHOR]

Self-assembled pectin nanoparticles was prepared and evaluated for delivering the hydrophobic drug, honokiol (HK), to HepG2 cells. These hydrophobic drug-loaded nanoparticles were developed without using any surfactant and organic solvent. Hydroxypropyl-β-cyclodextrin (HCD) was used to fabricate an inclusion complex with HK (HKHCD) to increase the solubility of the drug and thus facilitate its encapsulation and dispersion in the pectin nanoparticles. Investigation of the in vitro release indicated that the drug-loaded nanoparticles exhibited a higher drug release rate than free honokiol and an effective sustained-release. Cytotoxicity, cell apoptosis and cellular uptake studies further confirmed that the pectin nanoparticles with galactose residues generated higher cytotoxicity than free honokiol on HepG2 cells which highly expressed asialoglycoprotein receptors (ASGR). Nevertheless, these findings were not observed in ASGR-negative A549 cells under similar condition. Therefore, pectin nanoparticles demonstrated a specific active targeting ability to ASGR-positive HepG2 cells and could be used as a potential drug carrier for treatment of liver-related tumors. [ABSTRACT FROM AUTHOR]

• Key AWG design parameters for AWG based FBG interrogating system. • Effect of the key AWG parameters on AWG's bandwidth. • Experimental study of 5 different AWG transmission spectra. • Experimental study on AWG-based FBG interrogating system performance. Fiber Bragg Grating or FBG sensors are widely adopted in fields of structural health and temperature monitoring. The increasing demand for compact, high-performance FBG interrogators is highly desired. We have designed and fabricated high-performance arrayed waveguide gratings or AWGs using SOI technology with different parameters in FBG interrogator systems applications. Key parameters that affect FBG interrogating performance during AWG design are theoretically investigated and experimentally demonstrated. Using our proposed and optimized parameters, our fabricated AWGs have up to 2.88 dB of bandwidth, with low crosstalk and low on-chip loss. With custom supporting circuit, our proposed optimized AWG can keep the comparable interrogation accuracy and resolution performance to the previous best reported AWG based FBGI system while having four-time larger measuring dynamic range of 2 nm. This paper also provides guidance for optimizing the AWG-based FBG interrogation system during the AWG designing phase. [ABSTRACT FROM AUTHOR]

Four new diarylheptanoid glycosides (1 – 4), (1 S ,3 R ,5 S)-2-(4-hydroxy-3- methoxyphenyl)-6-[2-(4-hydroxyphenyl)ethyl]-tetrahydropyran-4-ol-4 ' - O - β -D-glucopyranoside (1), (1 S ,3 R ,5 S)-2-(4,5-dihydroxy-3-methoxyphenyl)-6-[2-(4-hydroxyphenyl) ethyl]-tetrahydropyran-4-ol-4 ' - O - β -D-glucopyranoside (2), (1 S ,3 R ,5 S)-2-(4-hydroxy- 3,5-dimethoxyphenyl)-6-[2-(4-hydroxy-3-methoxyphenyl)ethyl]-tetrahydropyran-4-ol-4 ' - O - β -D-glucopyranoside (3), and (1 R ,3 R ,5 R)-2-(4-hydroxy-3,5-dimethoxyphenyl)- 6-[2-(4-hydroxy-3-methoxyphenyl)ethyl]-tetrahydropyran-4-ol-3- O - β -D-glucopyranoside (4) were isolated from the 50% ethanol extract of Zingiber officinale peel. The structures of the isolated compounds were determined by HR-ESI-MS and extensive spectroscopic techniques (UV, IR, 1D-NMR, and 2D-NMR). Compounds 1 – 4 significantly increased the survival rate of human normal lung bronchial epithelial cells (BEAS-2B) induced by lipopolysaccharide (LPS) at the concentration of 10 μM. Four new diarylheptanoid glycosides (1 – 4), were isolated from the 50% ethanol extract of Zingiber officinale peel. The structures of the isolated compounds were determined by HR-ESI-MS and extensive spectroscopic techniques (UV, IR, 1D-NMR, and 2D-NMR). Compounds 1 – 4 significantly increased the survival rate of human normal lung epithelial cells (BEAS-2B) induced by LPS at the concentration of 10 μ M. [Display omitted] [ABSTRACT FROM AUTHOR]

Zhengzhou of Henan province is an important agricultural production base. To improve the performance of the combined drying system and promote the development of agricultural products in Zhengzhou area, a solar assisted multi-source heat pump (SMSHP) drying system was proposed based on a traditional solar assisted air source heat pump (SASHP) drying system. The simulation models were developed for the air source heat pump (ASHP), SASHP, and SMSHP drying system respectively. The coefficient of performance, energy consumption and specific moisture extraction rate of the drying systems under different seasons were analyzed. Moreover, to validate the simulation models, an experimental platform of the combined drying system was designed and set up, and the experimental tests were carried out on the ASHP, SASHP, and SMSHP drying system. The simulation results revealed that the SMSHP drying system had lower energy consumption, higher coefficient of performance and specific moisture extraction rate than that of the SASHP drying system. The most significant performance enhancement was observed in spring, where the SMSHP system demonstrated a 22.69 % increase in coefficient of performance, a 19.2 % increase in specific moisture extraction rate, and a 16.11 % decrease in energy consumption compared to the SASHP drying system. Comparing with the experimental data, the simulation model errors of the energy consumption, coefficient of performance, and specific moisture extraction rate of the SMSHP drying system were 3.19 %, 0.28 %, and 2.27 %, respectively. Therefore, the accuracy of the simulation results was confirmed. To better calculate the heat provided by the solar collection system, the concept of the tank heating guarantee rate was first introduced, and it was found to be more scientific than the solar energy guarantee rate. At last, The economic and environmental benefit of the drying systems were analyzed during the life cycle, and the SMSHP drying system exhibited better comprehensive performance than the SASHP drying system. This paper provides valuable insights into the comprehensive utilization of solar energy and the control logic of solar assisted air source heat pump combined drying system under different seasons. [ABSTRACT FROM AUTHOR]

Abstract: In this paper, the effect of the back panel structure on the performance of fluid flow and heat transfer of vertical open refrigerated display cabinets (VORDC) is presented by experiments and numerical simulation. Experimental tests are performed to validate the accuracy of numerical predictions. The characteristics of heat transfer and fluid flow of VORDC are investigated at the different locations of the perforations of back panel at the same porosity and the different flow ratios between back panel and air curtain at different porosities. By comparing numerical results with experimental results, the predictive abilities of the computational model have been revealed. Further computational results have also shown that less than 3% porosities can provide a better performance in the VORDC; the location of perforations has a minor influence on the temperature distribution of products. Furthermore, the suitable porosities in the back panel among the shelves are more likely to improve the uniformity of products temperature in the VORDC. As a result, the overall uniformity of product temperature inside the refrigerated display cabinet and the maximum deviation values of product temperature have been improve to 41% and 49%, respectively. The present study can provide the theoretical guide for the design of the narrow VORDC. [Copyright &y& Elsevier]

[Display omitted] • Ni 2 P/Al 2 O 3 with small nanoparticles and pure phase was controllably synthesized. • Ni 2 P/Al 2 O 3 shows excellent hydrogenation and desulfurization activities. • Nanoflower-like structure improves dispersion and accessibility of active sites. • The outstanding performance can be attributed to the rich Niδ+ active sites. The hydrogenation of unsaturated bonds and elimination of sulfur impurities in C 9 petroleum resin (C 9 PR) are crucial for improving its quality and performance. In this study, we prepared a nanoflower-like Ni 2 P/Al 2 O 3 catalyst using an in-situ synthesis combined with liquid-phase phosphidation strategy and applied for the production of value-added hydrogenated C 9 PR. In-situ synthesis of Ni-Al hydrotalcite anchors and disperses Ni nanoparticles, while liquid-phase phosphidation introduces high-content Niδ+ and Pδ− active sites and prevents the formation of inactive AlPO 4 , synergistically enhancing both hydrogenation and desulfurization activities. The synthesized Ni 2 P/Al 2 O 3 catalyst achieves a 99.6 % hydrogenation degree and reduces sulfur content from 137 ppm to 0 ppm, much better than the catalysts prepared by conventional impregnation and metal phosphate reduction methods. These results give valuable insights for designing efficient catalysts and advancing single-step hydrorefining processes to generate high-quality, value-added hydrogenated petroleum resins. [ABSTRACT FROM AUTHOR]

Photoelectrochemical (PEC) analysis has attracted accumulated attention on diagnosis of diseases and high-efficiency photosensitizers are urgently needed. In this work, N-doped sheet-like porous carbon (N-PC) was prepared by thermal stripping of Zn2+ from zeolitic imidazole framework-8 (ZIF-8), followed by in situ formation of gold nanoparticles (Au NPs) embedded in the N-PC (termed Au NPs@N-PC). Also, the zinc meso-tetra (4-carboxyphenyl) porphine (ZnP) behaved as photosensitizer, which was covalently linked with Au NPs@N-PC (ZnP-Au NPs@N-PC), achieving the 9.2-fold enhancement in the photocurrents by using dopamine (DA) as donor. Next, the PEC mechanism was strictly discussed by UV–vis diffuse reflectance (DLS) spectroscopy, fluorescence (FL) and density functional theory (DFT) calculations. By virtue of the excellent PEC property, a label-free "signal off" PEC aptasensor was constructed based on the ZnP-Au NPs@N-PC for ultrasensitive detection of protein tyrosine kinase (PTK-7). The established biosensor showed a wider linear range of 10.00 pg mL−1 to 1.00 μg mL−1 (R 2 = 0.99) and a lower limit of detection (LOD, 1.42 pg mL−1), coupled by showing acceptable results for diagnosis of gliomas. Hence, this research opens a valuable avenue for synthesis of advanced photosensitizer and holds huge potential in biomedical field. • The Au NPs were in situ embedded on the pores of the N-PC. • The Au NPs@N-PC promoted photoelectron transfer of ZnP for signal enhancement. • The PEC biosensor was built for the detection of PTK-7 in glioma samples. [ABSTRACT FROM AUTHOR]

Atomic doping plays an important role in the fabrication of electronic devices. However, the atomic doping of two-dimensional materials is challenging as the thickness approaches the nanoscale. Self-doping, achieved through an asymmetric structure, can simplify the fabrication of electronic devices. In this study, the electronic properties of the F-GaN-H/SiC hetero-structures are investigated based on the first principles. The intrinsic polarization of the F-GaN-H leads to charge transfer resulting in self-doping. The spatial distribution of carriers in the F-GaN-H/SiC hetero-structures is reversed with polarization reversal. And p -type doped F-GaN-H and n -type doped SiC are achieved in polarization-down (P d) hetero-structures, which is contrary to polarization-up (P u) hetero-structures. The band gaps of the F-GaN-H/SiC hetero-structures are smaller than the intrinsic materials, and the band structures are modulated by polarization direction. For the P u hetero-structures, a high hole mobility of 8.87 × 103 cm2 V−1 s−1 is achieved. The self-doping and the excellent transport properties of the F-GaN-H/SiC hetero-structures, with the tunable bandgap structures to polarization direction, not only simplify the fabrication of electronic devices but also demonstrate the potential application for optoelectronic and high-speed electronic devices. • The p -doped F-GaN-H and n -doped SiC are achieved in P d hetero-structures. • The n -doped F-GaN-H and p -doped SiC are achieved in P u hetero-structures. • The band structures are tunable to polarization direction. • The large hole mobility of 8.87 × 103 cm2 V−1 s−1 is obtained in hetero-structure. [ABSTRACT FROM AUTHOR]

Carbon adsorbents have been widely used to remove indoor volatile organic compounds (VOCs), however, the proliferation of bacteria on the carbon adsorbents may deteriorate the indoor air quality and thus pose a serious threat to human health. Herein, we report the synthesis of antibacterial porous carbon spheres (carbonized aminophenol-formaldehyde resin, CAF) with well-dispersed Cu species via an in situ incorporation of Cu2+ during the polymerization of 3-aminophenol-formaldehyde resin followed by a thermal carbonization and reduction process. Compared with CAF, the Cu/CAF- x nanocomposites with Cu loading show a much higher specific surface area (>700 m2 g−1 vs. 569 m2 g−1 for CAF). In addition, the pore size of Cu/CAF- x is ranging from 0.7 to 1.68 nm, which is exactly conducive to adsorb the toluene molecules. As a result, the toluene adsorption capacity is improved from 123.50 mg g−1 for CAF to >170 mg g−1 for Cu/CAF- x. More importantly, such adsorbents possess excellent antibacterial performance, the Cu/CAF-10 (10 wt% of Cu loading) with a concentration of 50 μg mL−1 can completely kill the E. coli within 30 min. Our work paves the way to the development of bifunctional adsorbents with both efficient VOCs adsorption and excellent antibacterial performance. [Display omitted] • An in situ complexation strategy is developed to prepare Cu loaded carbon composite. • Cu/CAF- x show higher toluene adsorption capacity than porous carbon adsorbent. • Cu/CAF-10 with a low concentration of 50 μg mL-1 can kill 100% E. coli within 30 min. • The in situ complexation strategy can be extended to prepare other metal-carbon composites. [ABSTRACT FROM AUTHOR]

Abstract: The binary Cu–Zr system is an important material for various implementations. The copper–zirconium alloy is one of the best known transition metal–metal binary system which may be obtained in a glassy state by conventional melt-spinning technique over a wide range of composition. On other hand, substitution of Zr for Al in the CuZnAl oxide system was found to improve the catalytic performance during oxidative steam reforming of methanol. In these cases the knowledge of phase equilibria and thermodynamic properties of the binary Cu–Zr system seems to be important for an industry. A new thermodynamic description of this system was proposed based on Calphad method. A good agreement between experimental information and calculation was found. [Copyright &y& Elsevier]

[Display omitted] • A new method allows Al 2 O 3 to simultaneously expose {111} facets with strong acidity and {110} facets with moderate basicity. • MoS 2 and NiS on this Al 2 O 3 works by cooperative action on the newly exposed facets. • The catalyst is used in the thio-etherification of ethanethiol and isoamylene to thioethers. • The combined use of two advanced techniques, crystal facet engineering and cooperative catalysis, is demonstrated. In alumina-based catalysts the properties of the alumina support directly influence the structure (size, morphology, orientation, etc.) of the resulting active phase and ultimately determine the performance of the final catalysts. This paper presents a facile and efficient method for γ-Al 2 O 3 to simultaneously expose {111} facets with strong acidity and {110} facets with moderate basicity. It is shown that the metal oxides NiO x and MoO x can be selectively deposited and subsequently sulfided on the respective facets to form a NiS 2 -MoS 2 /Al 2 O 3 catalyst with substantially enhanced activity for thio-etherification reaction. By cooperative action of the active sites on the newly exposed facets, the catalyst is shown to have superior activity over a conventional NiMoS/Al 2 O 3 catalyst in the thio-etherification reaction between ethanethiol and isoamylene (2-methyl-2-butene) to yield ethylamyl thioethers. Our findings show that tuning the physicochemical properties via crystal facet engineering and inducing cooperative catalysis via preferential deposition of active metals open a novel avenue for the rational design and synthesis of high performance catalysts. [ABSTRACT FROM AUTHOR]

Abstract: Successive treatment of γ,δ-unsaturated β-ketoesters and nitroalkenes with a bifunctional thiourea and TMG promoted the tandem Michael addition, giving rise to highly functionalized cyclohexanones in good yields. The three contiguous stereogenic centers of the obtained products were constructed with high diastereo- and enantioselectivity (up to >99% de and 92% ee). The reaction was successfully applied to the asymmetric synthesis of (−)-epibatidine, which was synthesized from the cyclohexanone derivative in seven steps in 30% overall yield. [Copyright &y& Elsevier]

SBA-15, possessing uniform mesopore system and large specific surface area, shows a tremendous mass transfer advantage in the reactions involving reactant, intermediate or product whose dynamic diameter is larger than the pore size of microporous zeolites, but the low acidity greatly limits its application in acid-catalyzed reactions (e.g., hydroisomerization). Herein, we report an Al-functionalized SBA-15 molecular sieve (Al-SBA-15) with enhanced acidity obtained via a pH-adjusted prehydrolysis synthesis approach for hydroisomerization. Its physicochemical properties and catalytic performance were carefully characterized, evaluated in hydroisomerization of n-octane after loading active component Pt, and compared with a pure silica SBA-15 and two Al-containing samples (AlSBA-15 and Al/SBA-15) produced through direct synthesis and wetness impregnation, respectively. The results show that the acidity of three Al-functionalized samples is prominently improved, and thus the conversion of n-octane over them is greatly increased when compared with siliceous SBA-15. Moreover, among three Al-containing SBA-15 materials, Al-SBA-15 with the largest pore diameter and moderate acidity exhibits relatively high n-octane conversion and di-branched isomers selectivity but minimal cracking selectivity. These results demonstrate that pH-adjusted prehydrolysis is an effective route to preparing Al-functionalized SBA-15 with suitable acidity for the hydroisomerization of alkanes. Unlabelled Image • Three Al-functionalized SBA-15 materials were prepared by using different methods. • The acidity is greatly improved after introducing Al into the siliceous SBA-15. • Al-SBA-15 prepared via pH-adjusted prehydrolysis has suitable pores and acidity. • Al-SBA-15 shows good catalytic performance in n-octane hydrosiomerization. [ABSTRACT FROM AUTHOR]

With the increasing application of crop straw, the greenhouse gas emissions caused due to crop straw have received increasing attention. However, the current studies have not explored the greenhouse gas emissions from on-farmland consumption of returned straw. Based on a long-term positioning experiment, three treatments were set up in double-cropping rice fields: chemical fertilizer (CF), straw replacing 1/3 nitrogen fertilizer (MS), and straw replacing 2/3 nitrogen fertilizer (HS). We measured the biomass, soil properties, and greenhouse gas emissions of double-cropping rice and then comprehensively evaluated the global warming potential, carbon footprint, and net ecological and economic benefits. The straw treatments (MS and HS) increased the cumulative annual emissions of CH 4 (98.44% and 261.23%), CO 2 (30.85% and 122.29%), and N 2 O (7.37% and 52.50%), the cumulative annual global warming potential (74.15% and 206.12%), average GHG intensity (43.26% and 138.07%), and the annual cumulative net ecosystem carbon budget (52.96% and 100.97%) in the early and late rice growing seasons, respectively. We observed that the real-time greenhouse gas emissions were significantly correlated to the soil microbial functional genes and total carbon, NH 4 +-N, and NO 3 −-N. The results of the random forest model showed that total carbon (13.87%) and nirK abundance (9.80%) were the highest predictors of global warming potential at the booting and maturity stages, respectively during rice growing season. Combining the resource inputs for agricultural production and the greenhouse gas emission potential of the returned straw on its own, MS showed the lowest net greenhouse gas emission, and MS and HS showed significantly increased annual cumulative net ecological economic benefits (38.08% and 34.30%). Overall, MS showed the lowest net greenhouse gas emission and the highest net ecological economic benefits, which is a straw-returning measure with low environmental impact and high economic returns. [Display omitted] • The straw replacing chemical fertilizers increased greenhouse gas emissions. • Straw treatments increased global warming potential and greenhouse gas intensity. • Straw replaced 1/3 nitrogen fertilizer had the lowest net greenhouse gas emissions. • Straw treatments have higher rice yield and agricultural economic benefits. • Straw treatments have higher net ecological economic benefits. [ABSTRACT FROM AUTHOR]

The WS 2 /WSSe and WSSe/WS 2 bilayers are constructed using single-layer WS 2 and WSSe with a lattice mismatch rate of only 1.85 %, and their structural properties, carrier mobility, electrical properties, and photocatalytic performance are performed using density functional theory. The carrier mobility of WS 2 /WSSe and WSSe/WS 2 bilayers is better than that of single-layer WS 2. And the conductivity of the WSSe/WS 2 bilayer in the Zigzag direction is superior to that in the Armchair direction. The results of band structure using the HSE06 method demonstrate that the most stable WS 2 /WSSe and WSSe/WS 2 bilayers are type-II band alignment. WS 2 /WSSe and WSSe/WS 2 bilayers can undergo redox reactions at pH = 0 and pH = 7 respectively. And they all emerge a built-in electric field to cause photo-generated carriers to recombine between the layers to upgrade the photocatalytic performance of the bilayer, which is a typical S-scheme heterojunction. And the power conversion efficiency (PCE) of the WS 2 /WSSe and WSSe/WS 2 bilayers are 15.5 % and 15.7 % respectively, so the utilization rate of sunlight is relatively high. In general, WS 2 /WSSe and WSSe/WS 2 bilayers are ideal materials in the field of photocatalytic water splitting. [Display omitted] • The hole mobility in the zigzag direction of the WS 2 /WSSe can reach 2278 cm2/Vs. • The WS 2 /WSSe and WSSe/WS 2 bilayers are S-scheme heterojunction. • The PCE of WS 2 /WSSe and WSSe/WS 2 bilayers can reach 15.5% and 15.7%. [ABSTRACT FROM AUTHOR]

• Detailed characterization of ionic liquid drops impacting on heated porous surfaces. • Increased temperature and velocity accelerate the droplet penetration. • Ionic liquid drop exhibits smaller diameter, height, and more stability than water. • Evaporation alters the relationship between residual volume and contact time. The impingement dynamics of a promising ionic liquid absorbent, namely, 1-ethyl-3-methylimidazolium acetate ([EMIm]Ac) in droplet falling film flow modes on heated porous surfaces in absorption refrigeration were investigated experimentally. The influences of impact velocity and surface temperature on the ionic liquid droplet spreading diameter, dynamic contact angle, spreading height, and residual volume against the heated porous surfaces were explored. The results indicated that the residual volume generally decreased in linear with increasing contact time at 323.15 K, while the dependence exhibited a polynomial behavior at higher heating temperatures. Compared to the impingement behaviors of deionized water droplets, such as oscillations and capillary waves were not observed in [EMIm]Ac droplets. The residual volume of the deionized water droplets varied exponentially with the contact time owing to the combined effects of the evaporation, penetration, and variation of the thermophysical properties of the droplet. Moreover, increases in the impact velocity and surface temperature enlarge the spreading diameter and accelerate the droplet penetration for the ionic liquid. [ABSTRACT FROM AUTHOR]

• High-efficiency ZnMOF(Ru) was obtained via a simple solvothermal method. • The unique ZnMOF(Ru) increased the mass loading and utilization efficiency of Ru(dcbpy) 3 2+ effectively. • ZnMOF(Ru)-based coreactant-free ECL biosensor was fabricated for ultrasensitive detection of BRCA1. Nowadays, serious restriction by aggregation quenching and proton attack in aqueous media, electrochemiluminescence (ECL) signals of emitter hardly match the requirement of ultrasensitive biomedical detection in practice. In this work, a novel flower-like metal-organic framework microsphere was formed by chelating Zn ion with carboxyl-rich tris(4,4′-dicarboxylic acid-2,2′-bipyridyl) ruthenium(II) (Ru(dcbpy) 3 2+) in the presence of cetyltrimethylammonium bromide (CTAB), defined as ZnMOF(Ru) for simplicity. For that, the obtained ZnMOF(Ru) as a high-performance ECL emitter displayed 53-fold amplification in aqueous solution without any coreactant alternative to that of Ru(dcbpy) 3 2+, coupled with the dramatically enhanced fluorescence quantum yield and stability of the intermediates. Thus, a "sandwich"-like ECL biosensor was developed for detecting breast cancer 1 gene (BRCA1), showing the wide linear range (1.0 fM–0.1 nM) and ultralow limit of detection (LOD) down to 0.71 fM. Hence, this work provides a universal and robust pattern to develop advanced ECL luminophores and exploit their potential applications in bioanalysis. [ABSTRACT FROM AUTHOR]

Abstract: Periodic mesoporous organosilica (PMO) materials with large pores have been successfully synthesized using a combinational strategy by decreasing both the synthesis temperature and acidity. Herein, we use a tri-block copolymer EO106PO70EO106 [Pluronic F127, where EO is poly(ethylene oxide) and PO is poly(propylene oxide)] as the template, bis(trimethoxysilyl)ethane (BTME) as a silica source and 1,3,5-trimethylbenzene (TMB) as a pore expander. The PMO material synthesized in this approach has a face-centered cubic (fcc) structure. When the synthesis temperature is 0°C and the acidity is 0.1M HCl, the pore diameter of the PMO material reaches 33.6nm, which is the largest among cubic PMO materials to our knowledge. [ABSTRACT FROM AUTHOR]

Development of ultra-sensitive and high specific aptasensors is important for early diagnosis of prostate cancer. Herein, ultrasensitive detection of prostate specific antigen (PSA) aptasensor was realized based on the "on-off-on" model via fluorescence (FL) covalent energy transfer between g-C 3 N 4 quantum dot (g-CNQDs) and palladium triangular plates (Pd TPs). Specifically, the Pd TPs were primarily linked with PSA aptamer (PA) as the reporter probe, followed by attaching them onto the g-CNQDs surfaces, causing the highly enlarged FL quenching rate (ca. 75%). After the introduction of PSA, the FL intensities recovered again because of the distinctively stronger affinity of PA to PSA than that of g-CNQDs. The bond of pyridine N with Pd was identified as efficient energy transfer pathway through the X-ray photoelectron spectroscopy (XPS) and FL measurements. The surface plasmon resonance (SPR) experiments certified the remarkably different affinity of PA towards g-CNQDs and PSA. The as-constructed FL aptasensor can accurately quantify PSA with wide linear range of 10 pg mL−1-50 ng mL−1 and ultra-low limit of detection (LOD, 4.2 pg mL−1), indicating the promising applications in clinical assay and biological detection. Image 1 • Pd TPs were synthesized under solvothermal conditions and acted as effective fluorescent quencher. • The Pd TPs-PA behaved as signal reporter for constructing a FL aptasensor. • The aptasensor was applied for PSA detection with low detection limit and high specificity. [ABSTRACT FROM AUTHOR]

• No chemical agents or surfactants are involved in the preparation process. • Simple synthesis and low cost make QUT/HA-NF a good clinical application potential. • The nanoformulation can be targeted to tumor cells via CD44 receptor mediation. In this study, a novel hyaluronic acid-based quercetin nanoformulation (QUT/HA-NF) was constructed for targeted tumor therapy. QUT/HA-NFs have the advantages of simple operation steps, low production cost and good industrialization prospects. Moreover, surfactants, solvents and chemicals are not involved in the preparation process, which avoid the cumbersome extraction of surfactants and the side effects caused by residual solvents or chemicals. The QUT/HA-NFs we prepared have small particle size and high drug loading. In vitro studies have shown that QUT/HA-NFs can significantly enhance tumor cell uptake and tumor cell killing through CD44 receptor mediation. In a xenograft mouse model of 4T1 tumor, QUT/HA-NFs showed stronger inhibition of tumor growth compared with quercetin alone. The QUT/HA-NFs proposed in this study are expected to provide a potential candidate for the treatment of tumors. [ABSTRACT FROM AUTHOR]

A biomimetic assembly of per-O-methylated-cyclodextrin dimer with cobalt proto-porphyrin (CoIII-PPIX@Py2CD) was achieved via covalent linkage between CoIII of CoIII-PPIX and pyridine N of Py2CD (primarily synthesized by the acyl chlorination reaction of two β-CDs monomers with 3,5-bis (bromomethyl) pyridine). Ultraviolet–visible (UV–vis) and circular dichroism (CD) absorption spectroscopy, and NMR hydrogen spectroscopy (H1-NMR) were adopted to carefully characterize the structure of Py2CD and its functional assembly with CoIII-PPIX. X-ray photoelectron spectroscopy (XPS) was employed to affirm the binding of the as-obtained CoIII-PPIX@Py2CD, whose electrochemical kinetics were extensively studied to validate the feasibility in the catalytic reduction of hydrogen peroxide (H 2 O 2). The developed sensor displayed the wide linear range for H 2 O 2 detection and the low detection limit of 2.47 × 10−7 M. This work sheds some constructive lights on rational design and synthesis of preeminently biomimic carrier and high cost-effectiveness catalyst for (bio)analytical applications. Image 1 • Py2CD was obtained by the covalent linkage of two β-CDs monomers with 3,5-bis (bromomethyl) pyridine. • The CoIII-PPIX@Py2CD were prepared by acyl chlorination reaction between the CoIII of CoIII-PPIX and pyridine N of Py2CD. • The catalyst dramatically improved the electronic conductivity and amplified the catalytic signals towards H 2 O 2 reduction. • An ultrasensitive chronoamperometric sensor was developed for H 2 O 2 detection. [ABSTRACT FROM AUTHOR]

The effect of the timing of adding 1 wt% decalin as a hydrogen donor on heavy oil visbreaking was studied. Experiments show that either premixing decalin with heavy oil or adding decalin during the reaction accelerates the formation of light distillates and improves the efficiency of viscosity reduction. Premixing with heavy oil is an appropriate way to add decalin. After 10 min of reaction at 400 ℃, the viscosity reduction rate of the product reaches 90% and the asphaltene content of the product is 1.8 wt% lower than that of the raw heavy oil. According to theoretical calculations, the active hydrogens of decalin preferentially saturate the aromatic C radicals that are critical for condensation. The equilibrium constant of the H-donation reaches the order of 105, while the activation energy of the reaction is only about 26 kJ/mol. The thermal cracking of decalin itself releases active and small-sized radicals, which accelerate visbreaking by participating in the dealkylation network of heavy oil molecules. • Decalin cracking releases radicals with high activity and diffusivity. • Addition of decalin in visbreaking greatly accelerates viscosity reduction. • Decalin selectively saturates aromatic C radicals vital for condensation. • Premixing decalin with heavy oil inhibits condensation in early reaction stage. • Premixing decalin as a hydrogen donor with heavy oil in visbreaking is recommended. [ABSTRACT FROM AUTHOR]

Nowadays, synthesis of novel organic photosensitizer is imperative but challenging for photoelectrochemical (PEC) assay in analytical and biomedical fields. In this work, the PEC responses enhanced about 4.3 folds after in situ electrostatic assembly of 1-butyl-3-methylimidazole tetrafluoroborate ([BIm][BF 4 ]) on meso-tetra (4-carboxyphenyl) porphine (TP), which was first covalently linked with NH 2 modified indium tin oxide electrode ([BIm]+-–TP-NH 2 -ITO). Moreover, the [BIm]+-–TP-NH 2 -ITO showed a much larger photocurrent in a water/dimethyl sulfoxide (DMSO) binary solvent with a water fraction (f w) of 90%, which displayed 6.7-fold increase over that in pure DMSO, coupled by discussing the PEC enhanced mechanism in detail. Then, the PEC signals were sharply quenched via a competitive reaction between magnetic bead linked dsDNA (i.e., initial hybridization of aptamer DNA with linking DNA) and HCT-116 cells (closely associated with CRC), where the liberated L-DNA stripped the [BIm]+ from [BIm]+-–TP-NH 2 -ITO. The PEC detection strategy exhibited a wider linear range (30 ∼ 3 × 105 cells mL–1) and a lower limit of detection (6 cells mL–1), achieving single-cell bioanalysis even in diluted human serum sample. The in situ assembly strategy offers a valuable biosensing platform to amplify the PEC signals with advanced organic photosensitizer for early diagnosis of tumors. [ABSTRACT FROM AUTHOR]

• A US-responsive CO release system was constructed for the first time. • The Fenton-like effect of VS 4 was reported for the first time. • The GSH-depleting effect of Mn(CO) 5 Br was first discovered. • CaCO 3 shell layer can achieve tumor microenvironment responsive drug release and lead to Ca2+ overload. • Generation of multiple mitochondrial apoptosis-based therapeutic molecules such as ROS, CO, and Ca2+. Mitochondria, the energy suppliers of cells, are crucial for cell survival and proliferation. Tumor therapy based on mitochondrial apoptosis holds good promise. Currently utilized strategies, such as the production of CO and ROS and Ca2+ overload, are not highly selective and have limited effectiveness. In this study, a smart nanoplatform (V-Mn@Ca) controlled by ultrasound (US) and with high therapeutic efficacy was designed, which can specifically target the tumor site and activate mitochondrial apoptosis at multiple levels. Specifically, VS 4 , featuring a narrow band gap, are utilized to generate a Fenton-like effect. Loading Mn(CO) 5 Br enables a US-induced release of CO and depletion of GSH, which would further enhance ROS-mediated mitochondrial apoptosis. Finally, an encapsulated CaCO 3 shell layer disrupts Ca2+ homeostasis in tumor cells. Overall, our study shows that the V-Mn@Ca platform triggers CO, ROS, and Ca2+ production in a controlled manner. Thus, providing sonodynamic therapy and CO therapy on a timed-targeted basis for enhanced mitochondrial apoptosis and subsequent tumor cell death, which inhibits tumor growth. [ABSTRACT FROM AUTHOR]

• ZnPPIX-Pd NCs work as an ECL emitter with high ECL intensity and lower excitation potential. • The ECL was irradiated from single oxygen via electrocatalytic reduction of ZnPPIX-Pd NCs. • A fast and ultrasensitive ECL sensor was constructed for Zn2+ detection based on "signal on" mode. Zinc ions (Zn2+) act as a transcription factor in eukaryotic cells for mediating protein-protein interactions in human healthy. The simple and sensitive detection of Zn2+ is the crucial mission in analytical field. This work demonstrated a novel and fast Zn2+ detection strategy based on "signal on" mode with electrochemiluminescence (ECL) luminophore, in which singlet oxygen was generated via electrocatalytic reduction of zinc proto-porphyrin IX grafted onto Pd nanocubes (ZnPPIX-Pd NCs). In protocol, Pd NCs were synthetized under hydrothermal conditions and aminated through thermal oxidative polymerization of 3-aminopropyltriethoxysilane (APTES), followed by further linking with PPIX via amide reaction. The resulting PPIX-Pd NCs effectively captured Zn2+ in chelation and monitored by Fourier transform infrared (FTIR) spectroscopy and ultraviolet-visible (UV-vis) absorption spectroscopy. By virtue of the metal resonance responses of Pd NCs, an intense monochromic, potential shuffling and enhanced ECL irradiation shows up for the hybrid nanocomposite with H 2 O 2 as the coreactant. To this end, an ultrasensitive method based on the nanocomposite with a "signal-on" model was developed for Zn2+ detection with a low detection limit down to 0.38 nM (based on a S / N = 3), excellent precision and high stability. The ECL strategy reveals the potential application in molecular diagnosis and offers a new avenue for bioassay of structural Zn(II) proteins and zinc finger-binding nucleotides. [ABSTRACT FROM AUTHOR]

Highlights • Hyaluronic acid is modified on its surface to actively target tumor cells. • It has a synergistic effect of photothermal chemotherapy. • Laser irradiation increases its temperature and accelerates drug release. Abstract This study has developed a versatile nano-system with the combined advantages of photothermal effect, active tumor-targeting, temperature-sensitive drug release, and photoacoustic imaging. The nano-system consists of the core of the phase change material (PCM), the outer polypyrrole (PPY) shell and the hyaluronic acid (HA) modified in the PPY shell. The obtained composite nanoparticles (denoted as DTX/PPN@PPY@HA) were spherical with a mean diameter of about 232.7 nm. In vivo and in vitro photoacoustic imaging experiments show that DTX/PPN@PPY@HA is an effective photoacoustic contrast agent, which can be used for accurate localization of tumor region and real-time guidance of photothermal chemotherapy. DTX/PPN@PPY@HA shows good photothermal effects and temperature-sensitive drug release. In addition, cellular experiments showed that DTX/PPN@PPY@HA could be efficiently internalized into tumor cells and produce significant cytotoxicity with the help of near-infrared (NIR) laser. Furthermore, the remarkable inhibition of DTX/PPN@PPY@HA against tumor growth was achieved in 4T1 tumor-bearing mice model. [ABSTRACT FROM AUTHOR]

Graphical abstract Highlights • Cu 3 Pt NFs were prepared via a theobromine- and CTAC-mediated hydrothermal method. • The architectures displayed dramatically boosted ORR activity. • A novel immunosensor was constructed based on the enlarged ORR signals. • The immunosensor showed great enhancement for detection of AFP. Abstract Herein, rhombic dodecahedral Cu 3 Pt nanoframes (Cu 3 Pt NFs) were prepared via solvothermal strategy using theobromine as the reductant and structure-directing agent, coupled with cetyltrimethylammonium chloride (CTAC) as the co-structure-director. The samples showed dramatically boosted catalytic performance for oxygen reduction reaction (ORR), owing to their highly open structures with enlarged specific surface areas. Using Cu 3 Pt NFs catalyzed ORR as signal amplification platform, a novel electrochemical immunosensor was constructed to monitor alpha-fetoprotein (AFP). The as-fabricated immunosensor displayed a wide linear range of 0.1–104 pg mL–1 and a low detection limit of 0.033 pg mL–1. [ABSTRACT FROM AUTHOR]

Graphical abstract By the differences in heavy oil composition and thermodynamic state of water applied, the oil-in-water emulsion structure of heavy oil/SCW systems may transit to the condensed emulsion or pseudo single-phase structure, determining their feasible application in upgrading of heavy oil. Highlights • MD simulation on dissolution of PAHs or PAH mixtures in sub-CW/SCW was applied. • Dissolution of heavy PAHs in sub-CW/SCW is sensitive to thermodynamic state of water. • Preferential dissolution of light PAHs occurs during dissolution of PAH mixtures. • Electrostatic interaction promotes the dissolution of PAHs in sub-CW/SCW. • Heavy oil/SCW could exist in condensed emulsion or pseudo single-phase structure. Abstract To get a better understanding of the upgrading of heavy oil under severe hydrothermal environment, a molecular dynamics simulation on the dissolution of oil droplets containing polycyclic aromatic hydrocarbons (PAHs) or PAH mixtures in subcritical or supercritical water (sub-CW/SCW) was applied. Being the representative of light PAHs, naphthalene dissolves readily into sub-CW/SCW. The dissolution of heavy PAHs, like benzo[α]pyrene and benzo[ghi]perylene however is sensitive to the thermodynamic state of water. During the dissolution of PAH mixtures, a preferential dissolution of light PAHs into the water phase occurs, leaving heavy PAHs concentrated in the oil droplets. With the simultaneous increase in water density and temperature, the miscibility of PAHs with sub-CW/SCW is improved by the enhanced attractive electrostatic interaction between PAHs and hydrothermal environment and the weakened interaction between PAHs. By the differences in heavy oil composition and the thermodynamic state of water, the upgrading of heavy oil in sub-CW/SCW could be run in the condensed emulsion or pseudo single-phase structure. [ABSTRACT FROM AUTHOR]

Graphical abstract Highlights • Well-defined Pd nanocones were facilely obtained by the PLL-mediated one-pot hydrothermal method. • Pd nanocones were firstly employed as an anodic ECL emitter, where TPA served as the coreactant. • An ultrasensitive ECL sensor was constructed for DA detection with a wider linear range and the lower detection limit. Abstract Electrochemiluminescence (ECL) has attracted significant interest because of its superior properties and potential applications in bioanalysis, and therefore many luminescent nanomaterials have been developed. Herein, well-defined Pd nanocones (Pd NCs) were facilely obtained by a one-pot hydrothermal method with poly- l -lysine (PLL) as a green protecting ligand, which were mainly characterized by transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS). Then, the as-obtained Pd NCs were first explored as an anodic ECL emitter, where tripropylamine (TPA) worked as the coreactant to boost the ECL emission. The possible ECL mechanism of Pd NCs/TPA system was extensively explored by ECL and electrochemical techniques. Briefly, the ECL emission underwent the oxidation-reduction route, in which both Pd NCs and TPA were initially oxidized, and then the oxidized TPA lost an proton to form reducing agent (TPA·) strongly reacted with the oxidized Pd NCs generating Pd NCs* for the emission. Furthermore, using dopamine (DA) as an ECL quencher, an ultrasensitive sensor was constructed for DA detection. The fabricated ECL sensor shows high sensitivity and selectivity, good stability, and wide linear range with the low detection limit of 0.46 pM. It offers a new avenue to exploit ECL illuminant and enriches the ECL emission theory. [ABSTRACT FROM AUTHOR]

[Display omitted] • A series of Pd/SiO 2 catalysts with graded pore sizes were successfully prepared. • Macroporous catalysts facilitate NBR diffusion and improve metal utilization. • The correlation between D cat /D NBR with HD and Weisz modulus Φ were revealed. • Pd/N-SiO 2 -70 shows excellent activity (96.7%) and selectivity (100 %) to C = C. Pore diffusion effect plays a crucial role in heterogeneous hydrogenation of unsaturated polymers. However, how large pore size can eliminate the pore diffusion limitation remains a controversial issue. Herein, we prepared a series of Pd/SiO 2 catalysts with graded pore sizes and investigated the effect of pore size on hydrogenation activity of nitrile butadiene rubber (NBR). It is found that when the catalyst pore size (D cat) is 7 times of the diameter of NBR chains (D NBR), the Weisz modulus Φ can be reduced to < 0.3 thus the internal mass transfer limitation can be eliminated, making NBR easier to approach the active sites. Consequently, the catalysts with the D cat /D NBR > 7 exhibit excellent catalytic activity (96.7%) and selectivity (100%) to C = C. This work emphasizes that the pore size of catalysts can regulate the pore transfer limitation and the accessibility of internal active sites, providing useful guidance for the design of efficient macromolecular hydrogenation catalysts. [ABSTRACT FROM AUTHOR]

The hydrothermal synthesis of zeolite from chemical Al/Si source in the presence of structure directing agent is considered to be a resource extensive, energy consuming, and environmental unfriendly process. Herein, we report a novel, cost-effective, and eco-friendly synthesis for the preparation of ZSM-5 zeolite from silicon-rich diatomite and aluminum-rich rectorite minerals in the absence of organic structure-directing agent and chemical Al/Si source. Synthesis factors (SiO 2 /Al 2 O 3 , Na 2 O/SiO 2 , and H 2 O/SiO 2 molar ratios along with seed content) and crystallization behavior were systematically investigated, providing fundamental knowledges on the formation of ZSM-5 from natural minerals. Synthesis under the optimized conditions (SiO 2 /Al 2 O 3 ratio of around 38, Na 2 O/SiO 2 ratios of 0.12–0.15, H 2 O/SiO 2 ratios of 15–25, and seed content above 0.5%) led to production of highly crystalline ZSM-5 zeolite with hexagonal prism morphology and large surface area. Various characterization techniques tracking the products at different crystallization times revealed that the crystallization process consisted of three stages: short induction stage (0–6 h), rapid growth stage (6–18 h), and stable growth stage (18–36 h). Moreover, the synthesized ZSM-5 crystals can be used as effective seed for producing the next generation of ZSM-5 zeolite. [ABSTRACT FROM AUTHOR]

Slurry-phase hydrocracking (SPHC) of unconventional heavy feedstocks is considered as a promising process to fill the gap between the ever-increasing demand for vehicle fuels and the fast-depleting supply of conventional crude oil. The one-through nature of SPHC processes requires low-cost yet high-performance catalyst. This article reports a simple but effective hydrothermal modification strategy to treat a cheap natural bauxite mineral as a support (HMB) to prepare SPHC catalyst (HMBC) with outstanding catalytic performance. For comparison, an acid-modified bauxite (AMB) derived catalyst (AMBC) was also prepared. The physicochemical properties of HMB, HMBC, AMB and AMBC were systematically characterized, and the catalytic performance of HMBC and AMBC was assessed in the SPHC of a high temperature coal tar (HTCT). The results showed that HMBC exhibited HTCT hydrocracking activity superior to AMBC, attributed to the more suitable acidity of the support HMB and the weaker interaction between MoO 3 and HMB that results in the higher sulfidation degree of molybdenum oxide species and thereby provides more active MoS 2 phases for hydrocracking. Furthermore, compared with the acid treatment previously reported, the hydrothermal modification is simpler, more energy-saving, and more environment-friendly and therefore is feasible for industrial application. [ABSTRACT FROM AUTHOR]

Supported Pd catalyst with an enhanced catalytic performance for polystyrene hydrogenation was successfully prepared by using macroporous silica microspheres (MSM) as the support. In order to eliminate the macromolecular diffusion limitation and improve the metal utilization, MSM was treated with steam at 800 °C first to remove mesopores and then refluxed with aqueous solutions to increase Si OH groups on the surface for Pd immobilization. The optimum support was obtained after the steam treatment for 2 h and using ammonia solution as reflux liquors, and the corresponding catalyst showed superior hydrogenation activity with a high conversion of 95%. [ABSTRACT FROM AUTHOR]

Herein, bimetallic core-shell Au@Pt nanocrystals (Au@Pt NCs) were prepared by a simple one-pot aqueous method using 2-pyrrolidone-5-carboxylic acid sodium salt (PCA-Na) as a new and green growth-directing agent. The obtained architectures displayed excellent catalytic activity towards oxygen reduction reaction (ORR) compared with commercial Pt/C catalyst. A novel immunosensor was constructed via assembly prostate specific antibody on the surface of Au@Pt NCs. It was found that the ORR currents were significantly suppressed due to the specific antigen-antibody reaction. The ultra-sensitive determination of prostate specific antigen (PSA) was realized on account of the immunocomplex impeding the redox probe accessible to the electrode. The immunosensor exhibited good analytical performance for the assay of PSA with the wide linear range of 0.1 ~ 50 ng mL –1 and low detection limit of 0.018 ng mL –1 ( S / N = 3), coupled with the improved stability, reproducibility and selectivity. [ABSTRACT FROM AUTHOR]

Introduction Anaplastic lymphoma kinase ( ALK ) rearrangements are present in approximately 5% of non-small-cell lung cancers (NSCLCs). NSCLCs with ALK -rearrangement can be effectively treated with crizotinib. However, magnitude and duration of responses are found to be heterogeneous. This study explored the clinical efficacy of crizotinib in different ALK variants. Methods Among 96 ALK -rearrangement patients treated with crizotinib, 60 patients were identified with tumor specimens that could be evaluated by next-generation sequencing (NGS). We retrospectively evaluated the efficacy of crizotinib in different ALK variants. Results The median Progression-free survival (PFS) of the 96 ALK -rearrangement patients was 14.17 months. Among the 60 patients with NGS results, the most frequent variants were variant 3a/b (33.33%), variant 1 (23.33%) and variant 2 (15.00%). The percentage of rare EML4 - ALK variants and non EML4 - ALK variants were 10.00% and 18.33%. Survival analysis showed that patients with variant 2 appeared to have longer PFS than others (P = .021); also, patients with TP53 mutation seemed to have an unfavorable PFS than those with TP53 wild-type with a borderline p value (P = .068). After adjusting for other baseline characteristics, EML4 - ALK variant 2 was identified as an important factor for a better PFS of crizotinib. We also found that patients with variant 3a/b had shorter duration of response to crizotinib; however, no significant difference of PFS was observed between the PFS of variant3a/b and non-v3 EML4 - ALK variants. Conclusions Our results indicate prolonged PFS in patients with EML4 - ALK variant 2. [ABSTRACT FROM AUTHOR]

• A novel posture mapping method is proposed in to avoid the incorrect mapping. • The kinematics solution for SRS 7-DOF robot with posture constraints is derived. • The structure transformation method is modified to reduce the loss of workspace. • An explicit posture mapping and teleoperation framework is proposed. In most industrial robot applications, on-site robot operation is required. However, this is not feasible for certain harsh operating conditions, such as high temperatures and intense radiation. In such instances, teleoperation based on machine vision can be applied, and adding posture constraints helps control the robot to complete more complex tasks. The general idea is to use quadratic programming or other optimization methods to solve the problem. In order to improve accuracy and ensure real-time performance, a real-time explicit mapping and teleoperation control (REMTC) is proposed. Based on the principle of "included angle minimization" (IAM), the incorrect mapping problem which might be caused by the traditional method is solved. In addition, considering that the analytical inverse solution algorithm is not as universal as the general optimization framework, an improved structure transformation method is proposed, so that the algorithm can be applied to both Spherical- Revolute-Spherical (SRS) and non-SRS robots. Finally, the experiment verifies the effectiveness of the algorithm in real-time performance, accuracy and reliability. [ABSTRACT FROM AUTHOR]

[Display omitted] • WS 2 with W defect can be used to capture NO and as the NO 2 sensor. • Adsorption of NO 2 can alter the band gap type of WS 2 for intrinsic and S defect. • WS 2 with W defect makes an ideal reversible sensor for detecting CO and NH 3. The magnetic and electronic behaviors of four toxic gas molecules (CO, NH 3 , NO, and NO 2) adsorbed on intrinsic and defective (V W /WS 2 or V S /WS 2) WS 2 are systematically discussed using density functional theory. The adsorption energy of NO-V W /WS 2 is reduced more compared to that of NO adsorbed on intrinsic WS 2 , indicating that V W /WS 2 can be used to capture NO. The adsorption of the four toxic gas molecules shortens the band gap of the defective WS 2. The introduction of the S defect changes the type of band gap of the system. More interestingly, the adsorption of NO 2 (NO) changes the system from a direct bandgap for intrinsic WS 2 (V W /WS 2) to an indirect bandgap, while the introduction of NO 2 changes the system from an indirect bandgap for V S /WS 2 to a direct bandgap. Finally, the shorter recovery times for CO and NH 3 -V W /WS 2 compared to CO and NH 3 adsorbed on intrinsic WS 2 suggest that V W /WS 2 makes an ideal reversible sensor for detecting CO and NH 3. In conclusion, the adsorption of gas molecules and the defect can modulate the magnetic and electronic properties of WS 2. Importantly, intrinsic and defective WS 2 will facilitate gas sensing and detection of toxic gases. [ABSTRACT FROM AUTHOR]

The strategy of adding tetralin as a H-donor in the thermal processing of heavy oil was investigated by experimental characterization and theoretical calculations. According to the experiments, the timing of adding 1 wt% of tetralin has a great influence on the visbreaking performance of heavy oil. Calculations based on density functional theory showed that benzyl radicals released from the thermal cracking of tetralin accelerate the dealkylation that determines the heavy oil upgrading. Meanwhile, H α provided by tetralin is able to selectively saturate aromatic C radicals which are essential for condensation. Compared with the conventional H-donor addition, i.e., pre-mixing of tetralin with heavy oil, a similar viscosity reduction rate of about 98% can be obtained during the visbreaking with delayed tetralin addition. Furthermore, the addition of tetralin before the significant occurrence of condensation further increases the conversion of vacuum residue fraction by 3.4% and reduces the asphaltene content of the product by 2.6 wt%. [Display omitted] • Tetralin cracking releases benzyl radicals which accelerate heavy oil upgrading. • H α provided by tetralin selectively saturates aromatic C radicals. • Pre-mixing of tetralin with heavy oil affects sufficient condensation inhibition. • In visbreaking tetralin should be added before apparent occurrence of condensation. • In delayed coking the addition of tetralin is not recommended. [ABSTRACT FROM AUTHOR]

• The mesoporous iron oxide was successfully synthesized by using the waste wood powder as a template. • The alkali concentration had an effect on the physicochemical properties and performance of the synthesized iron oxides. • The iron oxide catalyst with larger surface area and pore volume exhibited higher yield of gasoline and diesel distillates. • The perfect performance of mesoporous iron oxide catalyst is ascribed to the presence of more exposure Fe active sites. In order to develop a high-efficiency iron oxide catalyst for the slurry-phase hydrocracking of poor heavy oil, the mesoporous iron oxide was successfully synthesized by using the waste wood powder as a template, and the influence of alkali concentration in the resulting solution on crystal phase, morphology and pore structure of the synthesized samples was investigated. The crystal phase of the synthesized iron oxide transfers from α-Fe 2 O 3 to γ-Fe 2 O 3 , and their crystal sizes gradually decrease with an increase of alkali concentration based on the XRD and HRTEM results. Additionally, the iron oxide with mesoporous structure, larger surface area and pore volume is obtained at the higher concentration of alkali in solution confirmed by N 2 adsorption-desorption analysis. The assessment result of the iron oxide catalyst employed in the slurry-phase hydrocracking of vacuum residue (VR) illustrates that the yields of gasoline and diesel distillates obtained over Fe-O-B 20 , Fe-O-B 24 and Fe-O-B 30 catalysts are higher compared with those over Fe-O-B 2 and Fe-O-B 14 catalysts, it can be attributed that more exposure Fe active sites derived from their larger surface area and pore volume availably improve the catalyst hydrogenation activity, which can inhibit the over-cracking reaction of intermediate products and the condensation of polycyclic aromatic hydrocarbon in VR to enhance the yields of gasoline and diesel distillates. [ABSTRACT FROM AUTHOR]

Autism spectrum disorders (ASDs) have tremendous medical and social problems in the world, which have attracted accumulated attention on the related microRNAs (miRNAs) detection by photoelectrochemical (PEC) method. Herein, 1,2,4,5-benzenetetramine tetrahydrochloride (BTA) behaved as ideal ligand to chelate with chloroauric (AuCl 4 -) for forming two-dimensional (2D) sheet-like metal organic frameworks (MOFs) (termed AuCl 4 --MOFs), followed by in situ formation of gold nanoparticles (Au NPs) embedded in metal organic frameworks (defined as MOFs@Au NPs). The resulted MOFs@Au NPs showed 5.3-time increase in the anode photocurrent over Au NPs alone by using ascorbic acid (AA) as electron donor. Then, the PEC mechanism was strictly studied by electron paramagnetic resonance (EPR) and electrochemistry. Next, a label-free "signal on" model PEC biosensor was constructed based on MOFs@Au NPs as photosensitizer to detect miRNA-23a-3p (related with ASDs), integrated by a competitive reaction associated with magnetic bead (MB) linked double-stranded DNA (dsDNA). The sensor showed a wider linear range of 200 fM ∼ 2.00 nM (R 2 = 0.99) and a limit of detection (LOD) down to 78.9 fM. This analytical strategy holds huge potential for blood-based RNA detection in biomedical field. • MOFs@Au NPs were obtained via the in-situ reduction of AuCl 4 --MOFs with BTA ligand. • The MOFs@Au NPs obviously accelerated the oxidation reaction of AA and boosted the photocurrent sharply. • The label-free PEC biosensor was fabricated for sensitive detection of miRNA-23a-3p via a MB linked dsDNA competitive reaction. [ABSTRACT FROM AUTHOR]

In this work, we consider the fluid/gravity correspondence for general rotating black holes. By using the suitable boundary condition in near horizon limit, we study the correspondence between gravitational perturbation and fluid equation. We find that the dual fluid equation for rotating black holes contains a Coriolis force term, which is closely related to the angular velocity of the black hole horizon. This can be seen as a dual effect for the frame-dragging effect of rotating black hole under the holographic picture. [ABSTRACT FROM AUTHOR]

[Display omitted] • The flower-like nickel phosphide catalysts were prepared by a hydrotalcite strategy. • Ni 2 P/Al 2 O 3 catalyst showed excellent catalytic activity and desulfurization ability. • The outstanding performance ascribed to the rich active Niδ+ species. • The enhanced stability was due to strong interaction between active sites and support. The catalytic hydrogenation of petroleum resin (PR) to high value-added hydrogenated PR (HPR) represents a forward-looking technology for upgrading the pyrolysis petroleum by-product. Herein, flower-like and pure-phase supported nickel phosphide catalysts were controllably fabricated through a hydrotalcite strategy with red phosphorous as the P source. The PR hydrogenation activity of the catalysts followed the order of Ni 2 P/Al 2 O 3 > NiP 2 /Al 2 O 3 > Ni/Al 2 O 3 > imp-Ni 2 P/Al 2 O 3 catalysts (prepared by the impregnation method). Such enhanced performance of Ni 2 P/Al 2 O 3 could be ascribed to small nickel phosphide particle size and rich active Niδ+ species. Notably, the sulfur contents of PR were effectively reduced from 55.4 (C 5 PR) and 72.3 ppm (C 9 PR) to 3.8 and 7.9 ppm after hydrogenation by Ni 2 P/Al 2 O 3. Meanwhile, Ni 2 P/Al 2 O 3 also exhibited good stability with the hydrogenation degree of HC 5 PR maintaining at 94.39 % after 100 h. Our work provides a promising nickel phosphide catalyst with outstanding hydrogenation activity, hydrodesulfurization ability, and stability toward PR hydrogenation. [ABSTRACT FROM AUTHOR]

The impact dynamics of water drops on porous surfaces wetted by a hygroscopic ionic liquid aqueous solution are investigated. Firstly, to better illustrate the different dynamic characteristics of water drops on ionic liquid-wetted porous surfaces, it is compared with that on the dry and water-wetted porous surfaces. The results indicate that, the water drop barely penetrates on the dry porous surface at ambient temperature, but penetrate when the surface temperature is raised or the surface is pre-wetted. The maximum spreading and penetration of the droplet on the ionic liquid-wetted surface is larger and faster than that on the water-wetted surface. Then, the effect of the mass fraction of aqueous ionic liquid, impact velocity, porosity on the spreading and penetration is explored. The larger the mass fraction of aqueous ionic liquid on the porous surface, the faster the droplet spreading factor, height, and residual volume decrease. The effect of impact velocity is even more pronounced for the water droplets impacting on pure ionic liquid-wetted porous surfaces. A higher porosity contributes to a smaller spreading diameter but a larger volume decreasing rate on the wetted porous surface. [ABSTRACT FROM AUTHOR]

Molecular dynamics simulations were applied to characterize the dissolution of subcritical water (Sub-CW) in polycyclic aromatic hydrocarbons (PAHs). The phase equilibria of Sub-CW/PAHs are characterized by the dissolution of Sub-CW in PAHs. The solubility of Sub-CW increases with temperature but is relatively insensitive to pressure changes. Furthermore, an increase in PAH scale leads to a decrease in Sub-CW solubility. The PAH-rich phase can be divided into an interface region and a bulk region, and the water concentrations in the two regions differ greatly. The Hansen solubility parameters of PAHs and Sub-CW exhibit opposite distributions, hindering the mutual solubility between the two. The dissolution of Sub-CW is promoted by the destruction of intermolecular hydrogen bonds of water at increasing temperature, but is ultimately inhibited by the difference in dispersion properties between PAHs and Sub-CW. According to the Gibbs solvation free energy, the electrostatic interaction between PAHs and Sub-CW favors the dissolution of Sub-CW. Meanwhile, the van der Waals interaction shows different effects. • Phase equilibria of PAHs and Sub-CW were studied by MD simulation. • Phase equilibria of PAHs and Sub-CW feature dissolution of Sub-CW in PAHs. • Solubility of Sub-CW in PAHs is sensitive to temperature change. • Opposite distributions of Hansen HSP hinder dissolution of Sub-CW in PAHs. • Electrostatic interaction promotes dissolution of Sub-CW in PAHs. [ABSTRACT FROM AUTHOR]

The phase equilibria of subcritical water (Sub-CW) and four-ring N-, S-containing heterocyclic aromatic hydrocarbons (hetero-PAHs) were investigated by molecular dynamics simulation. In a temperature range of 250–350 °C and a pressure range of 4.2–21 MPa, the mixture of hetero-PAHs and Sub-CW shows an equilibrium between water-rich and oil-rich liquid phases, characterized by a significant dissolution of water in the oil phase. The solubility of Sub-CW is 1.9–3.8 wt% in N-containing hetero-PAHs and 1.0 to 2.7 wt% in S-containing hetero-PAHs. Compared with polycyclic aromatic hydrocarbons (PAHs) with the same ring number, the presence of the thiophenic ring in hetero-PAHs leads to a decrease in the solubility of Sub-CW. The particularity of N-containing hetero-PAHs lies in the hydrogen bond between the pyridinic ring and water molecules, which increases the solubility of Sub-CW at temperatures below 300 °C. The solubility of Sub-CW in hetero-PAHs/PAHs can be correlated with the Gibbs solvation free energy of water dissolved in the oil phase and the cohesive energy density of the oil phase as parameters. • Phase equilibria of hetero-PAHs and Sub-CW were studied by MD simulation. • Phase equilibria feature dissolution of Sub-CW in hetero-PAHs rich phase. • The presence of thiophenic rings in hetero-PAHs decreases Sub-CW solubility. • The presence of pyridinic rings in hetero-PAHs increases Sub-CW solubility. • Hydrogen bonds play vital roles in Sub-CW solubility in N-containing hetero-PAHs. [ABSTRACT FROM AUTHOR]