JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
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2022
·
IF 6.76
Junfeng Yang,Yuyang Wu,Yanhui Dong,Hao Cui,Chenyang Shi,Hang Sun,Shengyan Yin
Herein, a ternary Bi@H-TiO 2 /B-C 3 N 4 type II heterostructure is successfully designed and prepared via metal Bi as cocatalyst for photocatalytic H 2 generation. As expected, under λ > 300 nm light, the highest photocatalytic hydrogen production rate (HPR) of Bi@H-TiO 2 /B-C 3 N 4 is up to 223.08 μmol g −1 h −1 . Excitingly, under visible light (λ > 400 nm), the highest HPR of Bi@H-TiO 2 /B-C 3 N 4 is increased to 18.84 μmol g −1 h −1 , which is about 67.3 times, 37.7 times and 6.8 times as high as that of H-TiO 2 , B-C 3 N 4 and H-TiO 2 /B-C 3 N 4 under the same conditions, respectively. Moreover, the electrochemical impedance spectroscopy and transient photocurrent tests manifest that the interface resistance of Bi@H-TiO 2 /B-C 3 N 4 composite decreases and the photocurrent density increases after loading metal Bi. These results indicate that loading metal Bi as cocatalyst (providing more electron trapping sites) is beneficial to improve photocatalytic activity in the type II heterostructure composite. And the electron transfer directions (B-C 3 N 4 → H-TiO 2 → Bi or B-C 3 N 4 → Bi) are proved by ultraviolet photoelectron spectroscopy test. Therefore, the Bi@H-TiO 2 /B-C 3 N 4 photocatalyst with strong visible light absorption is expected to be a promising candidate in photocatalytic fields under visible light.
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INDUSTRIAL CROPS AND PRODUCTS
·
2022
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IF 6.449
Yachong Zhu,Yehong Chen,Chaojun Wu,Dongmei Yu,Qijun Ding,Ronggang Li
In this study, cellulose nanofibrils (CNFs) were directly prepared after autohydrolysis of eucalyptus raw materials. The effect of different autohydrolysis times on the hydrogen bond structure, micro-structure and properties of CNFs were analyzed by FTIR peak fitting, two-dimensional infrared, TGA, TEM and X-ray diffractometer. The results showed that the autohydrolysis treatments could obviously lead to the sequence of hydrogen bond changes in CNFs as follows: v (weak hydrogen bond) > v (free hydroxyl) > v (O(3)H.O(5)) > v (O(2)H.O(6)) > v (O(6)H.O(3′)), and further impact in crystallite size of CNFs. With the increase of the autohydrolysis strength, the crystallite size of CNFs on the 1 1 ¯ 0 crystal plane could be reduced by up to 26%, but the crystallite size on the 110 crystal plane and the 200 crystal plane increased by 24.5% and 22.6%, respectively. These microstructure changes finally increased the crystallinity index of CNFs, and then resulted in their high thermal stability.
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ADVANCED SYNTHESIS & CATALYSIS
·
2022
·Vol. 364
·期 8
·1450-1459
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IF 5.981
Feng Cheng,Jia-Min Zhang,Zhen-Tao Jiang,Xiao-Hu Wu,Ya-Ping Xue,Yu-Guo Zheng
Chiral amino acids are extensively applied in the pharmaceutical, food, cosmetic, and agricultural industries. As a representative example, l -phosphinothricin ( l -PPT, a chiral non-natural amino acid) is a broad-spectrum herbicide. An NAD(H)-driven biocatalytic system for the asymmetric synthesis of chiral amino acids (focused on l -PPT) with high efficiency and low cost is highly desired. The key for the development of such biocatalytic system is to obtain an NADH-dependent biocatalyst with high catalytic performance toward l -PPT pro-ketone PPO. Herein, an engineered glutamate dehydrogenase from Lysinibacillus composti ( Lc GluDH) with desired activity was obtained by gene mining and protein engineering. In silico analyses suggested that the volume of substrate-binding pocket was substantially enlarged from 330.5 Å 3 to 409.6 Å 3 . The stability of Lc GluDH was increased ( T m value increased from 47.3 °C to 65.3 °C) by introducing positively charged amino acids or aromatic amino acids at position 375. The desired biocatalytic system was constructed by coupling the engineered Lc GluDH and an NAD + -dependent FDH. Through this biocatalytic system, the batch production of l -PPT exhibited high space-time yield (207.3 g ⋅ L −1 ⋅ day −1 ) with strict stereoselectivity ( ee of l -PPT>99%). Furthermore, eight other chiral amino acids were synthesised by the developed NAD(H)-driven biocatalytic system with high ee values.
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Nature Communications
·
2023
·Vol. 14
·期 1
·1-12
·
IF 16.6
Meng Hao,Yang Yusen,Shen Tianyao,Yin Zhiming,Wang Lei,Liu Wei,Yin Pan,Ren Zhen,Zheng Lirong,Zhang Jian,Xiao Feng-Shou,Wei Min
Copper-based catalysts serve as the predominant methanol steam reforming material although several fundamental issues remain ambiguous such as the identity of active center and the aspects of reaction mechanism. Herein, we prepare Cu/Cu(Al)O x catalysts with amorphous alumina-stabilized Cu 2 O adjoining Cu nanoparticle to provide Cu 0 −Cu + sites. The optimized catalyst exhibits 99.5% CH 3 OH conversion with a corresponding H 2 production rate of 110.8 μmol s −1 g cat −1 with stability over 300 h at 240 °C. A binary function correlation between the CH 3 OH reaction rate and surface concentrations of Cu 0 and Cu + is established based on kinetic studies. Intrinsic active sites in the catalyst are investigated with in situ spectroscopy characterization and theoretical calculations. Namely, we find that important oxygen-containing intermediates (CH 3 O* and HCOO*) adsorb at Cu 0 −Cu + sites with a moderate adsorption strength, which promotes electron transfer from the catalyst to surface species and significantly reduces the reaction barrier of the C−H bond cleavage in CH 3 O* and HCOO* intermediates.
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JACS Au
·
2023
·
IF 8
Qi Yang,Xiujuan Gao,Faen Song,Xiaoxing Wang,Tao Zhang,Pan Xiong,Yunxing Bai,Xingchen Liu,Xiaoyan Liu,Junfeng Zhang,Gang Fu,Yisheng Tan,Yizhuo Han,Qingde Zhang
Selective oxidation of C–H bonds under mild conditions is one of the most important and challenging issues in utilization of energy-related molecules. Molybdenum oxide nanostructures containing Mo5+ species are effective for these reactions, but the accurate identification of the structure of active Mo5+ species and the catalytic mechanism remain unclear. Herein, unsaturated penta-coordinated Mo5c5+ with a high fraction in MoOx fabricated by the hydrothermal method were identified as the active sites for low-temperature oxidation of dimethyl ether (DME) by the deep correlation of characterizations, density functional theory calculations, and activity results, giving a methyl formate selectivity of 96.3% and DME conversion of 12.5% at unreported 110 °C. Low-temperature electron spin resonance (ESR) and quasi in situ X-ray photoelectron spectra (XPS) with the designed experiments confirm that the Mo5c5+ species can be formed in situ. Molybdenum located at the pentachronic site is preferable to significantly promote the oxidation of the C–H bond in CH3O* at lower temperatures.
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Nature Communications
·
2023
·Vol. 14
·期 1
·1-12
·
IF 16.6
Li Guowei,Jiang Shihui,Liu Aijun,Ye Lixiang,Ke Jianxi,Liu Caiping,Chen Lian,Liu Yongsheng,Hong Maochun
Crystal-field perturbation is theoretically the most direct and effective method of achieving highly efficient photoluminescence from trivalent lanthanide (Ln 3+ ) ions through breaking the parity-forbidden nature of their 4 f -transitions. However, exerting such crystal-field perturbation remains an arduous task even in well-developed Ln 3+ -doped luminescent nanocrystals (NCs). Herein, we report crystal-field perturbation through interstitial H + -doping in orthorhombic-phase NaMgF 3 :Ln 3+ NCs and achieve a three-orders-of-magnitude emission amplification without a distinct lattice distortion. Mechanistic studies reveal that the interstitial H + ions perturb the local charge density distribution, leading to anisotropic polarization of the F − ligand, which affects the highly symmetric Ln 3+ -substituted [MgF 6 ] 4− octahedral clusters. This effectively alleviates the parity-forbidden selective rule to enhance the 4 f –4 f radiative transition rate of the Ln 3+ emitter and is directly corroborated by the apparent shortening of the radiative recombination lifetime. The interstitially H + -doped NaMgF 3 :Yb/Er NCs are successfully used as bioimaging agents for real-time vascular imaging. These findings provide concrete evidence for crystal-field perturbation effects and promote the design of Ln 3+ -doped luminescent NCs with high brightness.
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INTERNATIONAL JOURNAL OF PHARMACEUTICS
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2023
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IF 5.8
Shuai Zhang,Quanzhi Zhang,Runmei Xu,Junyao Ma,Liang Fang
Transdermal drug delivery system (TDDS) was an effective way to realize controlled drug delivery. However, realizing zero-order controlled drug skin delivery was still challenging in the drug-in-adhesive patch. This study provided a strategy to accomplish this delivery form by stabilizing the drug concentration in adhesive through concentration-dependent competitive interaction. Clonidine (CLO) and Granisetron (GRA) were chosen as the model drugs which were of high skin permeability, and polydimethylaminoethyl acrylate (EA) as an excipient to interact with hydroxyphenyl adhesive (HP). Drug release, permeation and pharmacokinetic study were conducted to evaluate the controlled effect of HP-EA. The molecular interaction was characterized by FT-IR, 1 H NMR and XPS. Dynamic simulation and molecular docking further clarified the competitive interaction involved in the release process. Both the drug skin permeation study of CLO and GRA patch based on the HP-EA adhesive showed good zero-order fitting with r of 0.994 and 0.998, compared with non-functional adhesive (0-PSA). Furthermore, the pharmacokinetic study of the CLO patch showed a plateau phase for around 52 h without influencing the area under concentration–time curve ( AUC ), indicating that the HP-EA could realize zero-order drug skin delivery. The mechanism study revealed that EA serving as a ‘buffer component’ promoted the conversion of the ionic CLO to the neutrals the as the neutrals released, which stabilized ‘1% neutrals CLO concentration’. In conclusion, the drug delivery system based on the concentration-dependent competitive interaction broadened our understanding of the molecular mechanisms involved in zero-order controlled release in transdermal patches which would promote the development of zero-order drug delivery in TDDS.
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ChemCatChem
·
2021
·Vol. 13
·期 14
·3312-3318
·
IF 5.686
Ding Ding,Bing Yan,Yang Wang,An-Hui Lu
Graphical Nanofiber Catalysis : Hexagonal boron nitride has been regarded as a potential inorganic nonmetallic catalyst for the oxidative dehydrogenation of propane. Herein, a novel nanofiber catalyst consisting of hexagonal boron nitride/silica oxide ( h -BN/SiO 2 ) was prepared via electrospinning method, which exhibited remarkable 24.9 g olefins ⋅ g BN −1 ⋅ h −1 productivity of olefins in oxidative dehydrogenation of propane. Fibrous nanomaterials have drawn considerable attention in the field of catalysis due to the promoted utilization of the surface and facilitated mass transfer process. In this study, we prepared one-dimensional nanofiber catalysts consisting of hexagonal boron nitride/silica oxide ( h -BN/SiO 2 ) via electrospinning method. The key is to prepare uniform sols consisting of exfoliated h -BN. The diameters of the nanofiber catalysts can be tuned in the range of 150–300 nm through h -BN loading change. When used in oxidative dehydrogenation of propane (ODHP), the obtained nanofibrous catalysts exhibited a 12.4 % conversion of propane and 85.1 % selectivity towards propylene, with remarkable olefins productivity of 24.9 g olefins ⋅ g BN −1 ⋅ h −1 , which is more than 5 times higher than that of bulk ODHP catalysts reported to date. This study shines light on the specific one-dimensional fibrous structure containing dispersed h -BN as well as a new strategy of preparing more efficient boron-based catalysts in the ODHP process.
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Journal of Composites Science
·
2021
·Vol. 5
·期 8
·207
·
IF 0
Ying Zhou,Cuihuan Song,Zhixiang Chen,Qixin Zhou
In this study, we prepared a novel coating composed of hexagonal molybdenum oxide (h-MoO3) nanofiller and waterborne epoxy resin (WEP) to provide corrosion protection. We optimized the h-MoO3nanorod synthesis methodology first by changing different parameters (pH, temperature, etc.). Furthermore, the as-prepared h-MoO3rods were characterized using a scanning electron microscope (SEM) and X-ray diffraction (XRD). Finally, the electrochemical impedance spectroscopy (EIS) test results verified that the anticorrosive performance of the composite coatings was improved by incorporation of low content of MoO3nanofiller (0.5 wt.%) compared to pure WEP sample. This developed composite will provide a new insight for the design and fabrication of one-dimensional (1D) nanomaterial (e.g., nanorod) reinforced epoxy coating and other polymeric coating processes.Keywords:waterborne epoxy;molybdenum trioxide nanorod;composites
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PESTICIDE BIOCHEMISTRY AND PHYSIOLOGY
·
2019
·
IF 2.87
Jiang Zhu,Kai Tian,Christopher A. Reilly,Xinghui Qiu
Helicoverpa armigera and H. assulta are two of the few insects that can feed on hot pepper fruits. Capsaicin and dihydrocapsaicin ( i.e. , capsaicinoids) are the principal pungent compounds in hot peppers. To explore possible molecular mechanisms of adaptation that allow these two species to consume capsaicinoids, the capacity of the three detoxification tissues (fat body, midgut, and Malpighian tubule) of the two pests, to metabolically degrade capsaicin and dihydrocapsaicin, was compared. The results showed that capsaicin and dihydrocapsaicin were metabolized by crude enzyme preparations from all three tissues of the two pests. Five metabolites of capsaicin, and five metabolites of dihydrocapsaicin were identified. Tissue and species differences in the degree of capsaicin and dihydrocapsaicin metabolism were observed. The specialist H. assulta had an overall greater capacity to degrade the capsaicinoids compared to the generalist H. armigera. Further, the midgut was the most significant contributor to capsaicinoid metabolism. The notably high specific activity in Malpighian tubules of H. armigera also further highlights the significance of this organ in xenobiotic detoxification. Alkyl hydroxylation and dehydrogenation were the main pathways for the oxidative biotransformation of both capsaicin and dihydrocapsaicin by cytochrome P450s. This study provides evidence that enhanced metabolic decomposition of capsaicinoids may be an adaptation explaining dietary preferences for Capsicum fruits by these two pests.
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PROGRESS IN ORGANIC COATINGS
·
2019
·
IF 3.42
Bingjie Zou,Xijiang Chang,Jingxia Yang,Shuchuan Wang,Jingli Xu,Shirong Wang,Seiji Samukawa,Lidong Wang
h-BN nanoflakes were treated in three plasma gases (Ar、Ar+H 2 (4:1)、Ar + NH 3 (4:1)) for surface modification. The structure characterization (XRD, IR, XPS etc.) of h-BN indicated that the plasma treatment not only enlarged the interlayer distance of h-BN, but also increased the NH/OH surface groups and the ratio of exfoliated h-BN planes. The plasma treated h-BN exhibited better dispersion and stronger Fe 2+ holding ability in acrylic resin than the pristine h-BN, resulting in smaller corrosion current density (i corr ) and larger charge transfer resistance for the acrylic coating on low carbon steel, especially treated in Ar + NH 3 (4:1).
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Journal of Chemistry
·
2019
·
IF 1.727
Song-qi Hu,Yin Wang,Lin-lin Liu
Hexagonal boron nitride (h-BN) powders were fabricated by the combustion synthesis with B/KNO3/HMX (octogen) mixtures as reactants. X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) were adopted to investigate the phase composition and the chemical composition of the products, respectively. The morphology and resistance to oxidation were studied by scanning electron microscopy (SEM) and thermogravimetry (TGA), respectively. The characterization results showed that the h-BN which was produced through this method has high purity and exhibits excellent resistance to oxidation. The purity of h-BN is improved with the increasing content of HMX in reactants with boron carbide (B4C) and boron oxide (B2O3) as main impurity, but conversely, the yields are obviously decreased. Taking the comprehensive consideration of the purity and the yields together, the optimal molar ratio of B/KNO3/HMX is 10 : 1 : 4. In addition, the experimental results indicated that the crystalline grain size grows with the increasing content of HMX. The method explored in this study does not need expensive processing facilities and equipment, which is a preferable approach for the laboratory to prepare h-BN of high purity.
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