Catalysts
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2023
·Vol. 13
·期 4
·717
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IF 3.9
Kechen Zhang,Changxin Liu,Qiang Liu,Zheyang Mo,Dawei Zhang
Molten salts-assisted synthesis is widely used in the construction of high efficiency graphitic carbon nitride (g-C3N4) photocatalysts, and two isotypes of g-C3N4have been synthesized by such method, namely poly (heptazine imide) (PHI) and poly (triazine imide) (PTI). However, the understanding of the structural changes taking place during the molten salt process and the structure–activity relationship of g-C3N4polymorphs remain blurred. Herein, by regulating the treatment duration of g-C3N4nanosheets (melon) in molten salts, we successfully synthesized g-C3N4with phases of PHI, PHI/PTI and PTI. A continuous structural transformation induced by ions, in which melon transforms to a stable phase PTI via PHI, an intermediate state, was unveiled for the first time. In addition, results reveal that atomic configurations play a vital role in photo absorption, and charge carrier transfer and surface reaction, leading to significant differences in photocatalytic degradation. Among them, PHI with K+and cyan groups modification, as well as high crystallinity, exhibits remarkable degradation efficiency, with 90% removal of tetracycline in 10 min and 80% removal of phenol in 60 min. This study sheds light on a deeper understanding for the molten salt-assisted synthesis and provides new ideas for preparing efficient organic semiconductor photocatalysts.Keywords:graphitic carbon nitride;molten salts;structural transformation;intermediate;photocatalytic degradation
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Fermentation-Basel
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2023
·Vol. 9
·期 4
·322
·
IF 3.7
Jian Wang,Quanjin Jiang,Zhenyu Huang,Yan Wang,Hynek Roubik,Kai Yang,Ming Cai,Peilong Sun
Soybean meal is a class of by-products obtained from the processing of soybean products. Despite its high nutritional value, the presence of glycoside isoflavones limits human use of soybean meal. This study evaluated the effect of solid-state fermentation (SSF) with different edible mushroom mycelia (Pleurotus ostreatus,Hericium erinaceus, andFlammulina velutipes) on the proximate composition, antioxidant properties, and physicochemical properties of fermented soybean meal powder (SP). The results revealed that fermented SP had a higher nutritional value when compared to SP.P. ostreatuswas the most pronounced among the three species. Crude protein content was found to have increased by 9.49%, while the concentration of glutamate and aspartic acid increased by 23.39% and 23.16%, respectively. SSF process significantly increased the total polyphenol content (TPC) and aglycone isoflavone content by 235.9% and 324.12%, respectively, resulting in increased antioxidant activity (evaluated by the DPPH, •OH, ABTS+assays). Microstructural changes in fermented SP and nutrient degradation and utilization were observed. Thus, fermented SP can be used as a raw material with enhanced nutritional properties to develop new functional foods, such as plant-based foods represented by plant meat. It provides a promising approach for increasing the added value of soybean meal.Keywords:soybean meal;solid-state fermentation;edible mushrooms;nutritional value
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Molecular Catalysis
·
2023
·
IF 4.6
Haoquan Guo,Xinyu Lu,Yue Yang,Jinhe Wei,Lizhi Wu,Li Tan,Yu Tang,Xiaoli Gu
Alkyl phenol is an essential chemical intermediate that is in high demand in the chemical industry. The synthesis of alkyl phenols from lignin-derived molecules is one of the most promising routes for utilizing biomass resources. Herein, we report the catalytic hydrodeoxygenation (HDO) of dihydroeugenol (DHE) to alkyl phenols over a highly dispersed Pd/α-MoC catalyst with a substrate conversion of 98% and a selectivity of 96% to alkyl phenols. The Pd/α-MoC catalyst prepared by co-precipitation and temperature-programmed carbonization exhibits exceptional HDO activity under mild conditions with a low H 2 pressure (1–10 bars). The characterizations of the catalyst suggest that Pd are highly dispersed on the α-MoC matrix. The reaction mechanism was investigated using the substrate scope experiments. Under ambient pressure, the abundant oxygen vacancies and acidity sites on Pd/α-MoC enable the selective hydrodeoxygenation of lignin monomers.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2023
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IF 4.4
Boyuan Pan,Mingxiu Lv,Heng Du,Dongxin Zhao,Kui Lu
Various peptide drugs have entered the market with the development of molecular biology. Peptide drugs are used for treat diseases such as diabetes, breast cancer, and HIV infection. In this study, three nicotinamide–modified peptides were synthesized by modifying the N–terminus of BRCA1 (856–871, Y856R, K862Y, R866W) peptide with three nicotinic acid derivatives using solid–phase peptide synthesis. The results of calf thymus DNA (ctDNA) binding activity indicated that binding constants of BRCA1 (856–871, Y856R, K862Y, R866W) (P0) and three nicotinamide–modified peptides (P1, P2, and P3) to ctDNA were 1.89 × 10 3 , 2.97 × 10 4 , 7.61 × 10 4 , and 8.09 × 10 4 L·mol −1 , respectively. The binding affinity of the modified peptides was superior to that of BRCA1 (856–871, Y856R, K862Y, R866W). ΔH θ < 0 and ΔS θ < 0 indicated that van der Waals force and hydrogen bond contributed most to peptide–ctDNA binding. Results obtained by Circular dichroism (CD) indicated that peptide binding interaction led to conformational changes in ctDNA. Ultraviolet–visible (UV) spectroscopy, ethidium bromide (EB) competition experiments, DNA melting experiments, and viscosity measurements verified that peptides interacted with ctDNA via groove binding. Ionic strength experiments manifested that electrostatic binding was also involved in peptide–ctDNA binding.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2023
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IF 4.2
Junxin Chen,Caijin Zhou,Bingqi Xie,Jisong Zhang
Counter-current operation has been widely applied to enhance the extraction efficiency for systems with low distribution coefficients, which was hindered in microextraction because viscous force and surface tension dominate over gravity and inertial force. In this study, a novel design of a tube-in-tube microextractor relying on a poly tetra fluoroethylene membrane to construct a stable interface was proposed to conduct continuous counter-current extraction. Extraction kinetics for two systems with different distribution coefficients, membranes with different pore radii, and three flow rate ratios were measured as a function of residence time. For the system that toluene was used to extract 0.06 wt % phenol in water, 4.1 stages of extraction efficiency were achieved at a residence time of 9.8 min. A challenging case study (50 wt % acetone–water–toluene) was subsequently conducted to prove the high applicability for emulsion systems of this special microextractor. Lastly, a mathematical model was established and the predicted results of three flow rate ratios are in good agreement with experimental results.
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NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 11
·5420-5430
·
IF 3.3
Qi Guo,Jihong Xu,Rui Tang,Yulin Min,Zhenhu Hu,Penghui Shi
In the degradation process of organic pollutants, compared with the free radical pathway, the non-radical pathway shows the advantages of mild oxidation ability, strong anti-interference, and adaptation to different pH values. In this study, a manganese–nitrogen co-doped porous carbon (Mn–N@C-1) with high nitrogen content was prepared to improve the contribution rate of non-radical pathways to the degradation process of organic pollutants. The high performance of Mn–N@C-1 is attributed to the formation of Mn–Nx sites between Pyridine N and Mn, which can effectively oxidize organic pollutants in water (phenol, bisphenol A, 2,4-dichlorophenol). In addition, the catalyst exhibits high catalytic activity over a wide pH range (pH = 3–9) and has good immunity to inorganic anions. Moreover, the Mn–Nx site and graphitic-N are considered to be the generation sites of singlet oxygen, and the role of metastable Mn–N@C-1/PMS* complexes in the electron transfer process is explored. Overall, this study explores the crucial role of non-radical pathways in the degradation of organic pollutants by carbon-based materials.
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MOLECULES
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2023
·Vol. 28
·期 5
·2021
·
IF 4.6
Ran Wei,Yuanhua Mo,Duojiao Fu,Hongqin Liu,Baocai Xu
The discharge of industrial phenol pollutants causes great harm to the natural environment and human health. In this study, phenol removal from water was studied via the adsorption of Na–montmorillonite (Na–Mt) modified by a series of Gemini quaternary ammonium surfactants with different counterions [(C11H23CONH(CH2)2N+(CH3)2(CH2)2N+(CH3)2(CH2)2NHCOC11H23·2Y−, Y = CH3CO3−, C6H5COO−and Br−, 12–2–12·2Y−]. The results of the phenol adsorption indicated that MMt–12–2–12·2Br−, MMt–12–2–12·2CH3CO3−and MMt–12–2–12·2C6H5COO−reached the optimum adsorption capacity, which was 115.110 mg/g, 100.834 mg/g and 99.985 mg/g, respectively, under the conditions of the saturated intercalation concentration at 2.0 times that of the cation exchange capacity (CEC) of the original Na–Mt, 0.04 g of adsorbent and a pH = 10. The adsorption kinetics of all adsorption processes were in good agreement with the pseudo-second-order kinetics model, and the adsorption isotherm was better modeled by Freundlich isotherm. Thermodynamic parameters revealed that the adsorption of phenol was a physical, spontaneous and exothermic process. The results also showed that the counterions of the surfactant had a certain influence on the adsorption performance of MMt for phenol, especially the rigid structure, hydrophobicity, and hydration of the counterions.Keywords:modified montmorillonite;Gemini surfactant;counterions;adsorption;phenol
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JOURNAL OF SUPERCRITICAL FLUIDS
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2023
·
IF 3.9
Fan Yang,Pengfei Zhu,Haiqing Zheng,Wei Yang,Shengji Wu,Huajian Ye,Lei Che
The interactions between cellulose and lignin, and the hydrolysis behavior of cellulose, lignin and cellulose-lignin mixtures with mass ratios of 25/75, 50/50, 75/25 in subcritical water were investigated in this study. Cellulose and lignin interactions greatly promoted the hydrolysis of lignin during hydrolysis of the cellulose-lignin mixture with a mass ratio of 25/75, whereas they accelerated and suppressed lignin hydrolysis in the other cellulose-lignin mixtures at reaction temperatures under and above 257 °C, respectively. The cellulose and lignin interactions presented negative effects on cellulose hydrolysis in all the samples at reaction temperatures higher than 257 °C. However, they showed positive and negative effects in the cellulose-lignin mixture with a mass ratio of 25/75, and the cellulose-lignin mixtures with mass ratios of 50/50 and 75/25, respectively, at reaction temperatures under 257 °C. The cellulose and lignin interactions also suppressed the heat-related reactions and the glucose and aromatic-linked polymer char formation reactions.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
·
IF 9.9
He Zhao,Huarou Zeng,Ting Chen,Xiaoying Huang,Yuepeng Cai,Renfeng Dong
A catalytic micromotor-based (MIL-88B@Fe 3 O 4 ) colorimetric detection system which exhibit rapid color reaction for quantitative colorimetry and high-throughput testing for qualitative colorimetry have been successfully developed. Taking the advantages of the micromotor with dual roles (micro-rotor and micro-catalyst), under rotating magnetic field, each micromotor represents a microreactor which have micro-rotor for microenvironment stirring and micro-catalyst for the color reaction. Numerous self-string micro-reactions rapidly catalyze the substance and show the corresponding color for the spectroscopy testing and analysis. Additionally, owing to the tiny motor can rotate and catalyze within microdroplet, a high-throughput visual colorimetric detection system with 48 micro-wells has been innovatively conducted. The system enables up to 48 microdroplet reactions based on micromotors run simultaneously under the rotating magnetic field. Multi-substance, including their species difference and concentration strength, can be easily and efficiently identified by observing the color difference of the droplet with naked eye after just one test. This novel catalytic MOF-based micromotor with attractive rotational motion and excellent catalytic performance not only endowed a new nanotechnology to colorimetry, but also shows hold great potentials in other fields, such as refined production, biomedical analysis, environmental governance etc., since such micromotor-based microreactor can be easily applied to other chemical microreactions.
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ACS Applied Nano Materials
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2023
·
IF 5.9
Wujiayue Luo,Junjie Chen,Yutong Sun,Zhenglin He,Yunzhang Li,Guosheng Shi
Ultrafast molecular-sieving graphene-based membranes with selective separation of volatile aromatic compounds (VACs) have great potential in environmental protection, reutilization of expensive materials, and industrial separation processes. However, current graphene-based absorbents suffer from slow removal speed and limited adsorption capacity for VACs. Herein, pristine and Ni2+-controlled graphene oxide membranes (GOMs) with a permeance up to ∼8.0 × 10–6 mol m–2 s–1 Pa–1, being 1–2 orders of magnitude higher than those of previously reported membranes. The GOMs selectively separate VACs from N2 is achieved on ceramic substrates via the size-exclusion effect for the first time. At a high VACs feed concentration, such GOMs show high rejection rates of 99.8, 99.4, 95.9, and 97.3% for phenol, benzaldehyde, benzoic acid, and benzylamine, respectively. X-ray diffraction (XRD) results show the two-dimensional (2D) channel size for gas transportation within the GOMs is 0.44 nm, which can reject the transportation of VACs but have no effect on N2. Interestingly, using improved Ni2+-controlled GOMs, the rejection rates of benzoic acid and benzylamine rejection rates increased from 95.9 to 98.6% and from 97.3 to 99.4%, respectively. Our finding provides a fast and efficient way to filter VACs in air and has potential applications in air purification and industrial processes.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2023
·
IF 6.2
Xiaoxi Yu,Xiaocui Wu,Fang Guo,Jingping Liu,Qingshan Zhao
As a promising advanced oxidation process , photo-assisted peroxymonosulfate (PMS) activation for wastewater treatment has attracted widespread attentions. However, rational design of synergetic and recyclable catalysts for PMS photo-activation remains a big challenge. In this study, a carbon layer-coated amorphous CoO x supported on graphitic carbon nitride (CoO x @C/g-C 3 N 4 ) composite was fabricated to drive visible-light-assisted activation of PMS for efficient organic pollutant degradation. Amorphous CoO x nanoparticles were in-situ grown on two-dimensional g-C 3 N 4 substrate, among which a carbon layer serves as a high-speed electron transmission channel, facilitating the separation of photogenerated electron-hole pairs and accelerating the Co 3+ /Co 2+ redox cycle. Simultaneously, the carbon layer provides a protective film to suppress Co leaching, thereby improving the catalytic activity and reusability. Owing to the unique heterostructure and synergetic effect, the optimized 6% CoO x @C/g-C 3 N 4 composite exhibits superior catalytic efficiency and excellent cycling stability towards the degradation of various organic pollutants, which displays nearly 100% elimination of tetracycline (TC) within 80 mins. The h + , SO 4 •- and •OH are determined as the main contributors in the visible light-assisted PMS activation system, and the possible catalytic mechanism is also proposed. This work demonstrates a feasible strategy for constructing synergetic and effective photo-activation PMS catalysts for water remediation.
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Jingxuan Yang,Dongxu Qu,Jue Wang,Yangtao Wu,Lingjun Bu,Yuanxi Huang,Shiqing Zhou
The N-Br bond in monobromoamine (NH 2 Br) can be cleaved by UV irradiation to generate Br • and subsequently HO • , resulting in an advanced oxidation condition (i.e., UV/NH 2 Br). This study investigated the degradation of six contaminants of emerging concern (CECs) in the UV/NH 2 Br process, including the phenolic hydrocarbons phenol and bisphenol A (BPA), the amines aniline and sulfadiazine (SDZ), and the persistent organic pollutants ibuprofen (IBP) and carbamazepine (CBZ). The results showed that UV/NH 2 Br process significantly improved the degradation of CECs following pseudo-first order kinetics, and the degradation of CECs was enhanced with the increase of NH 2 Br dosage. UV/NH 2 Br was more efficient in degrading CECs containing phenolic hydroxyl groups (100 %), followed by those containing amine groups (> 95 %). The degradation efficiency was influenced by the pH value and was highest at pH 7. It was found that low concentrations of Cl − (< 0.5 mM ) and HCO 3 − (< 0.5 mM) promoted the degradation of SDZ and IBP, but further increases in Cl − and HCO 3 − (0.5 ∼ 5.0 mM) resulted in inhibition. SDZ and IBP degradation was inhibited by photo absorption competition and free radical depletion in natural organic matter and actual water. Probe experiments showed that reactive bromine species (RBS), reactive nitrogen species (RNS), and hydroxyl radical (HO • ) played a dominant role in CEC degradation. During the degradation of IBP by UV/NH 2 Br, hydroxylation, bromination , and quinylation were proposed as the primary reaction mechanisms. As compared to HOCl disinfection, NH 2 Cl disinfection after the UV/NH 2 Br process produced lower concentrations of disinfection by-products (DBPs).
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