Molecular Catalysis
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2023
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IF 4.6
Ye Tian,Yunchao Feng,Zheng Li,Yi Fan,Jonathan Sperry,Yong Sun,Shuliang Yang,Xing Tang,Lu Lin,Xianhai Zeng
The selective hydrogenation of the C=O group in biomass-derivate furfural (FF) over noble metal-free catalysts is challenging in aqueous. Herein, a CoO x /Nb 2 O 5 nanostructure catalyst was synthesized for the hydrogenation of FF to furfuryl alcohol (FA). Under optimized conditions, a 95.7% yield of FA was obtained with a TOF of 155.7 h −1 , and the kinetic study revealed that the reaction followed a pseudo-first-order pathway with an activation energy of 39.42 kJ mol −1 . The catalyst characterization indicated the interaction between Nb 2 O 5 and CoO via the Nb-O-Co bond in CoO x /Nb 2 O 5 -ctr, which prevented the further reduction of CoO to metal Co in the catalyst's preparation process. The catalytic mechanism suggested CoO was the dominant hydrogenation/adsorption active, whilst Co 3 O 4 and Nb 2 O 5 assisted the adsorption of FF. Further, DFT calculations verified CoO was the main adsorption site for FF adsorption in CoO x /Nb 2 O 5 -ctr. Moreover, CoO x /Nb 2 O 5 -ctr showed outstanding recyclability for the selective hydrogenation of FF to FA ever after five runs. This work provides opportunities for the clean conversion of biomass-based FF to FA and infers potential applications of Co for the large-scale hydrogenation of bio-based platform chemicals.
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BRAZILIAN JOURNAL OF MEDICAL AND BIOLOGICAL RESEARCH
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2023
·
IF 2.3
Wang Yujin,Jiang Hua,Wang Lijun,Gan Huiping,Xiao Xinchun,Huang Liangwu,Li Wenxin,Li Zongrun
Functional constipation (FC) is one of the most common gastrointestinal disorders characterized by hard stools and infrequent bowel movements, which is associated with dysfunction of the enteric nervous system and intestinal motility. Luteolin, a naturally occurring flavone, was reported to possess potential pharmacological activities on intestinal inflammation and nerve injury. This study aimed to explore the role of luteolin and its functional mechanism in loperamide-induced FC mice. Our results showed that luteolin treatment reversed the reduction in defecation frequency, fecal water content, and intestinal transit ratio, and the elevation in transit time of FC models. Consistently, luteolin increased the thickness of the muscular layer and lessened colonic histopathological injury induced by loperamide. Furthermore, we revealed that luteolin treatment increased the expression of neuronal protein HuC/D and the levels of intestinal motility-related biomarkers, including substance P (SP), vasoactive intestinal polypeptide (VIP), and acetylcholine (ACh), as well as interstitial cells of Cajal (ICC) biomarker KIT proto-oncogene, receptor tyrosine kinase (C-Kit), and anoctamin-1 (ANO1), implying that luteolin mediated enhancement of colonic function and contributed to the anti-intestinal dysmotility against loperamide-induced FC. Additionally, luteolin decreased the upregulation of aquaporin (AQP)-3, AQP-4, and AQP-8 in the colon of FC mice. In summary, our data showed that luteolin might be an attractive option for developing FC-relieving medications.
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RADIATION PHYSICS AND CHEMISTRY
·
2023
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IF 2.9
Meng Ren,Jiemin Luo,Duigong Xu,Yakun Guo,Zekun Jing,Hongjun Zhang,Peng Feng,Maobing Shuai
The present work involves the post-irradiation aging of radio-oxidized natural rubber latex (NRL) films irradiated by 60 Co gamma rays . The NRL films underwent the two consecutive processes: irradiation oxidation in air with a dose of 0.1 kGy h −1 (pre-irradiation phase) and radiolysis in argon with a dose of 10 kGy h −1 (post-irradiation phase). The changes of oxygen-containing groups in radio-oxidized NRL films were subsequently analyzed by FTIR (ATR method), XPS, and Raman spectroscopy . Analysis of the EPR spectra of free radicals and macroscope properties (including mechanical and thermodynamic properties) were also carried out. Pre-irradiation of NRL films in air resulted in the rapid formation of various carbonyl and unsaturated carbonyl products related to aliphatic esters, ketones, and carboxylic acids. These were followed by the decomposition of the oxygen-containing functional groups in the post-irradiation phase. In particular, the formation of an enol tautomer of a β-diketone functionality was observed. The increase and decrease of free radicals by EPR analysis were closely related to the crosslinking and degradation of the NRL network structures induced by irradiation. Further analysis indicated that the variations in macroscopic properties of NRL films were attributed to the secondary reactions of free radicals. Mechanistic routes for these irradiation aging processes are proposed and discussed.
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CRYSTENGCOMM
·
2023
·Vol. 25
·期 9
·1365-1373
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IF 3.1
Xin Wu,Xingzhong Zhu,Caixia Kan,Daning Shi
Boosting the electrocatalytic performance of non-Pt catalysts for the hydrogen evolution reaction (HER) is of great importance in the context of the high price and scarcity of Pt. In this work, we successfully synthesized bimetallic core–shell nanostructures with Au nanostars as cores and Rh clusters as shells (Au@Rh nanostars) based on a two-step wet-chemistry strategy. We have demonstrated that the interaction strength between Rh and intermediate(s) involved in the HER could be effectively manipulated due to the existence of a strong electronic effect in bimetallic Au@Rh nanostars. The results from FDTD simulation suggested that the E-M field enhancement of the Au@Rh nanostar is inferior to that of the Au nanostar but there is a more localized distribution between the Au core and Rh shell. Benefiting from the synergistic effect and the plasmon-induced accelerated molecular transformations, the Au@Rh nanostars manifest outstanding plasmon-enhanced electrochemical activity toward the HER with a low overpotential of 28.5 mV for achieving the current density of 10 mA cm−2, which surpasses the commercial Pt/C. Furthermore, the obtained Au@Rh nanostars exhibited remarkable stability during the durability test with only a 3 mV shift in HER polarization curves after 5000 potential cycles. This study provides a versatile strategy for designing bimetallic core–shell nanostructures with plasmon-enhanced electrocatalytic performance.
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EUROPEAN POLYMER JOURNAL
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2022
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IF 5.546
Yaolin Hu,Haina Qi,Liu Yang,Yuqi Sheng,Yunrui Xie,Qianli Ma,Hong Shao,Wensheng Yu,Dan Li,Xiangting Dong
Flexible multiple-functional conductive anisotropic membrane made of one-dimensional directional nanomaterial has the potential applicative prospects in advanced electronic skin and strain sensor. Nevertheless, it is hard to prepare aligned polymeric composites with poly-functional high conductive anisotropy and excellent interface properties, so it has been a vital topic to fabricate and investigate such kind of composites. In this work, the fluorescent anisotropic-conduction Janus-typed nanoribbon array membrane (named as FAJNAM for short) with [Eu(TTA) 3 bipy/polymethylmethacrylate (PMMA)]//[carbon black (CB)/PMMA] Janus-typed nanoribbon as construction unit is prepared by di-axial parallel electrospinning with a di-axial parallel spinneret. Since CB will seriously affect the fluorescence intensity of the Eu(TTA) 3 bipy complex, through using Janus-typed nanoribbon as construction unit, Eu complex and CB can be confined in their own regions, realizing efficacious separation of fluorescent and electrical substances to significantly reduce the adverse effects between the two functions so as to obtain excellent red fluorescence and electrical conduction. The percolation zone of CB in Janus-typed nanoribbons membrane is determined. By adjusting the content of CB, the transition from insulation to conductivity of the FAJNAM can be realized. The highest anisotropic conduction ratio reaches ca. 10 8 when the CB content is 10 %. For the first time, the crucial of critical diffusion concentration of two-phase spinning solutions in the parallel electrospinning process is advanced and studied in depth. Furthermore, the relationship between the critical diffusion concentration and the conductive aeolotropism degree has been explored. The concept of critical diffusion concentration is also applicable to other di-axial parallel electrospinning to prepare multi-functional materials, which will be of great significance to optimize electrospinning conditions. This research provides new technical support for the preparation of highly flexible, conductive anisotropy composite materials.
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CRYSTENGCOMM
·
2022
·Vol. 24
·期 24
·4399-4407
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IF 3.756
Delei Liu,Bing Jiao,Haijun Zhang,Shaowei Zhang,Jianghao Liu
By taking advantage of a microwave and molten-salt co-assisted boro/carbothermal reduction method (MSM-BCTR) and cheap raw materials such as HfO2/ZrO2, B4C and amorphous carbon, three types of (HfxZr(1−x))B2 (x = 0.25, 0.50 and 0.75) solid-solution powders with a single-crystalline rod-like morphology, high compositional uniformity, long lengths of 27.8–41.6 μm and high aspect ratios of 10.1–17.2 were successfully synthesized for the first time. And the required temperature conditions of 1100 °C for 20 min were significantly milder than that required by the molten-salt-assisted reduction method even using strong but high-price elemental boron as a reducing agent. These results demonstrated that the specific MSM-BCTR conditions characterized by molten-salt medium and microwave heating were capable of greatly enhancing not only the kinetics but also the thermodynamic favorabilities of the reactions for synthesizing HfB2 and ZrB2 as well as their solid solutions ((HfxZr(1−x))B2). More interestingly, the investigation on the crystalline growth mechanism of (HfxZr1−x)B2 indicated that under the MSM-BCTR conditions, residual amorphous carbon played an important role in enhancing the oriented growth of (HfxZr(1−x))B2, by preferential adsorption onto their {001} crystal planes and therefore greatly promoting corresponding specific surface energies. This study was expected to provide a feasible way of highly-efficiently and cost-effectively synthesizing ultra-high temperature ceramic powders with a highly-crystalline structure and uniform anisotropic morphology, which were favorable for promoting the oxidation resistance and toughness of their sintered products.
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DESALINATION
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2022
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IF 11.211
Jun Pan,Min Chen,Xianli Xu,Shi-Peng Sun,Zhaohui Wang,Zhaoliang Cui,Weihong Xing,Naser Tavajohi
Large amounts of lignin, hemicellulose , organic matter and inorganic salts are present in pulping and papermaking wastewater. Therefore, the treatment and discharge of pulping wastewater are important issues. We have designed and developed the world's first zero liquid discharge (ZLD) system for it based on pretreatment-membrane-evaporative crystallization integrated technologies . However, for the treatment of high salt reverse osmosis (RO) brine, there are still challenges that need to be addressed. In this work, the feasibility of using a membrane distillation crystallization (MDC) process to treat high saline RO brine was investigated. Two different coating materials , Hyflon AD 40H and perfluoropolyether (PFPE), were applied to improve the membrane surface hydrophobicity for stable and efficient performance. After modification, the water contact angle was up to 138.4 o and 157.7 o for Hyflon/polyvinylidene fluoride (PVDF) and PFPE/PVDF composite membranes, respectively. Moreover, the PFPE/PVDF membrane showed a higher repellency toward RO brine, which is better for the following MDC treatment. During the MDC progress using composite PFPE/PVDF membranes, the salt crystals precipitated and gradually accumulated. More importantly, the final NaCl purity can be up to 94%. Therefore, it is hopeful to improve of the existing ZLD system by MDC operation.
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FUEL
·
2022
·
IF 8.035
Yue-Qin Yang,Ling-Ping Xiao,Wen-Zhe Xiao,Xiao-Ying Li,Qiang Wang,Run-Cang Sun
The development of efficient catalysts is of great significance for the hydrodeoxygenation (HDO) of renewable biomass into value-added biofuel and chemicals to mitigate the environmental and energy menace. Herein, we report a sustainable strategy to fabricate ruthenium nanoparticles (NPs) anchored on defective nitrogen-doped carbon (Ru@NC) via a facile pyrolysis of a mixture of ruthenium trichloride and urea with carbon support. The highly distributed Ru NPs, constituted by N-enriched graphene shells, have been established as an excellent catalyst for the selective HDO of lignin- and furan- derivatives toward biofuel upgrade. Impressively, Ru@NC exhibits enhanced catalytic performance to commercial Ru/C, which could be attributed to the presence of the ensemble effects resulting from defective graphene sheet coverage on the Ru surface. Notably, the prepared catalyst was not affected after five successive reaction cycles, demonstrating superior stability and reproducibility. We envision that this work may pave the way for the development of highly efficient novel metal catalysts for heterogeneous catalytic HDO reactions in sustainable energy conversion.
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ANALYTICAL AND BIOANALYTICAL CHEMISTRY
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2022
·Vol. 414
·期 12
·3593-3603
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IF 4.478
Wu Shuyao,Jiang Meijiao,Mao Hui,Zhao Nan,He Dongqing,Chen Qinan,Liu Daliang,Zhang Wei,Song Xi-Ming
A simple and sensitive electrochemical cholesterol biosensor was fabricated based on ceramic-coated liposome (cerasome) and graphene quantum dots (GQDs) with good conductivity. The cerasome consists of a lipid-bilayer membrane and a ceramic surface as a soft biomimetic interface, and the mild layer-by-layer self-assembled method as the immobilization strategy on the surface of the modified electrode was used, which can provide good biocompatibility to maintain the biological activity of cholesterol oxidase (ChOx). The GQDs promoted electron transport between the enzyme and the electrode more effectively. The structure of the cerasome-forming lipid was characterized by Fourier transform infrared (FT-IR). The morphology and characteristics of the cerasome and GQDs were characterized by transmission electron microscopy (TEM), zeta potential, photoluminescence spectra (PL), etc. The proposed biosensors revealed excellent catalytic performance to cholesterol with a linear concentration range of 16.0 × 10 −6 –6.186 × 10 −3 mol/L, with a low detection limit (LOD) of 5.0 × 10 −6 mol/L. The Michaelis–Menten constant ( K m ) of ChOx was 5.46 mmol/L, indicating that the immobilized ChOx on the PEI/GQDs/PEI/cerasome–modified electrode has a good affinity to cholesterol. Moreover, the as-fabricated electrochemical biosensor exhibited good stability, anti-interference ability, and practical application for cholesterol detection. Graphical abstract
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Peng Wang,Shengyan Pu,Wen Zhang,Lin Shi,Di Zhang
Chemical oxidation is often used to modify the surface properties of carbonaceous materials and improve their environmental benefits in removal of organic pollutants. However, there are some controversial observations and explanations about the influence of chemical oxidation on the adsorption performance of carbonaceous materials that need to be revisited. We studied the influence of chemical oxidation on the adsorption of methylene blue (MB) and bisphenol A (BPA) as model compounds on activated carbon (AC) and carbon nanotubes (CNTs). The kinetics results showed that chemical oxidation prolonged the adsorption of MB and BPA on AC and CNTs, and it accelerated the overall adsorption on CNTs. The adsorption of BPA on oxidized AC was weaker, whereas that of MB was stronger. Furthermore, oxidation treatment of dispersible CNTs greatly increased the adsorption rate and capacity of the CNTs for BPA. The adsorption kinetics and capacity of AC and CNTs are closely related to their structural characteristics (non-dispersibility vs. dispersibility). 1 H NMR relaxation measurements showed that the dispersibility of oxidized CNTs can be increased in a liquid environment. After oxidation, significantly more adsorption sites are exposed, which are responsible for the increased sorption capacity and adsorption rate. This work clarifies the structural dependence of the adsorption performance of modified carbonaceous materials via chemical oxidation.
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Nanomaterials
·
2022
·Vol. 12
·期 2
·244
·
IF 5.719
Qingkai Tang,Xinhua Zhu
The structural, optical, dielectric, and magnetic properties of double perovskite La2FeReO6+δ(LFRO) powders synthesized by solid-state reaction method under CO reduced atmosphere are reported on in this paper. Reitveld refinements on the XRD data revealed that the LFRO powders crystallized in an orthogonal structure (Pbnmspace group) with column-like morphology. The molar ratios of La, Fe, and Re elements were close to 2:1:1. XPS spectra verified the mixed chemical states of Fe and Re ions, and two oxygen species in the LFRO powders. The LFRO ceramics exhibited a relaxor-like dielectric behavior, and the associated activation energy was 0.05 eV. Possible origins of the dielectric relaxation behavior are discussed based on the hopping of electrons among the hetero-valence ions at B-site, oxygen ion hopping through the vacant oxygen sites, and the jumping of electrons trapped in the shallower level created by oxygen vacancy. The LFRO powders display room temperature ferromagnetism with Curie temperature of 746 K. A Griffiths-like phase was observed in the LFRO powders with a Griffiths temperature of 758 K. The direct optical band gap of the LFRO powders was 2.30 eV, deduced from their absorption spectra, as confirmed by their green photoluminescence spectra with a strong peak around 556 nm.Keywords:double perovskite La2FeReO6+δpowders;solid-state reaction;dielectric properties;magnetic properties;optical properties;structural characterization
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JOURNAL OF CATALYSIS
·
2022
·
IF 8.047
Yi Liu,Ying Chen,Yunli Liu,Zewen Chen,Huan Yang,Zhongxiao Yue,Qing Fang,Yunfei Zhi,Shaoyun Shan
Solar energy is considered as the cleanest, cheapest, and most sustainable energy source, and CO 2 cycloaddition that is drove by solar energy has unique advantages in the aspect of energy and environmental. Therefore, Zn and N co-doped porous carbon nanosheets (ZNCs), which were synthesized by a simple one-step pyrolysis method, as catalysts and photothermal material to photothermally drive cycloaddition of CO 2 . The prepared ZNCs show graphene-like layered structure, uniformly distributed Lewis acid (Zn atoms) sites and Lewis base (N atoms) sites, full spectrum absorption and high photothermal conversion efficiency. More importantly, ZNCs have a higher catalytic efficiency than traditional heating methods because it can be quickly in-situ heated by light, hence the yield of cyclic carbonate reached 91.1% (0.1 MPa CO 2 , 1000 mW·cm −2 full-spectrum irradiation, 12 h). ZNCs were recycled five times without significant reduction in catalytic efficiency, and have high activity to other series of epoxides. A possible CO 2 cycloaddition mechanism which is catalyzed by ZNCs is proposed, including the step of adsorption, ring opening, insertion and cyclic carbonates formation.
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