FUEL
·
2023
·
IF 7.4
Xiao-Yan Zhao,Xue-Yu Ren,Yan-Jun Wang,Jing-Pei Cao,Zi-Meng He,Nai-Yu Yao,Hong-Cun Bai,Hou-Luo Cong
Direct conversion of lignite into light aromatics via catalytic fast pyrolysis is a great challenge because of severe catalyst deactivation and low aromatics yield. The tandem catalysis (1Zn@MCM-41 and ZSM-5) system was employed to promote the conversion of thermally-derived volatiles of lignite into aromatics at 600 °C. The mesoporous Zn-incorporated MCM-41 (xZn@MCM-41) with different doping amount of Zn was prepared with a one-pot hydrothermal procedure. The structure and the dispersion of Zn species of 1Zn@MCM-41 were systematically studied with XRD, SEM, BET, NH 3 -TPD and so on. The presence of 1Zn@MCM-41 significantly expands the lifetime of the microporous ZSM-5. Meanwhile, the yield of aromatics, especially benzene, is also increased to some extent. The content of the long-chain hydrocarbons and the phenolic compounds are decreased significantly after being cracked by the mesoporous 1Zn@MCM-41. More small molecules are able to contact with the active sites located in the micropores of ZSM-5 with the presence of Zn@MCM-41. In addition, the ZSM-5 in the tandem catalysts system presents an excellent stability. Therefore, this meso -microporous tandem catalysis system promotes the preferential cracking of macromolecular compounds, the cracked small molecules generated from which then contact with ZSM-5 to produce aromatics. This work provides a new perspective for the gradient catalyzing lignite-derived volatiles over a tandem catalysis system.
✓ 已验证
产品关联
DOI
高影响因子
BIOCHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 3.9
Siyuan Chang,Bingfeng Li,Tianyi Chen,Leilei Zhang,Yaru Li,Xuejun He,Sen Zhang,Xin Pan
The catalytic transformation of biomass-derived 5-hydroxymethylfurfural (HMF) into value-added chemicals and biofuels has received considerable interest. Previously, we demonstrated that Pseudomonas aeruginosa PC-1 could be used for selective 900 mM HMF oxidation into 5-hydroxymethyl-2-furancarboxylic acid (HMFCA) with over 90% yield. Here, we aimed to mine the potential aldehyde dehydrogenases (ALDHs) for HMF biocatalysis and improved the catalytic activity and tolerance through protein engineering. ALDHs were heterologously expressed in E. coli BL21 (DE3) and subsequently the most efficient HMF oxidation conditions of E. coli /pET -PaALDH70140 were identified. Based on the structural analysis of PaALDH70140 with the HMF and NAD + complexes, the engineering hotspots in the active site architecture were identified and subjected to saturation mutagenesis . The mutant L172R displayed 175% higher HMF catalytic efficiency than PaALDH70140, and the mutant also showed improved HMF-tolerance. Kinetic parameters suggested that L172R had higher HMF affinity and catalytic efficiency, indicating a higher HMF conversion efficiency than the wild-type. Molecular docking revealed that the mutation introduced new hydrogen bonds between the enzyme and HMF, which fixed the spatial position of HMF and shortened the reaction time of the catalysis, thus enhancing the catalytic efficiency of HMF. In the fed-batch process, E. coli /pET -PaALDH70140 - L172R exhibited a 166% increase in the yield of HMFCA within 22 h, proving its potential for HMF bioconversion applications.
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2023
·
IF 7.4
Qiaozhi Ma,Haotong Liang,Jianying Lin,Qiyu Liu
Production of 5-HMF from cellulose is a promising approach for advanced bio-fuels preparation, but the degradation of active 5-hydroxymethylfurfural (5-HMF) is a critical challenge affecting 5-HMF selectivity. To address this issue, biphasic reaction system consisting of water and organic solvent is generally used to in-situ extract 5-HMF into organic phase to inhibit product degradation. Despite the high 5-HMF selectivity achieved in biphasic system, low product concentration and difficulty in separation restrict its industrial applications. Molten salt hydrate (MSH) is unique in cellulose conversion and 5-HMF preservation. In this work, MSH of LiBr was used as monophasic solvent for cellulose conversion and an acidity tunable solid acid AlSiO-x was used as the catalyst. It was found that a relatively high 5-HMF yield of 44.5% together with carbon balance of 75.0% were obtained at 170 °C for 20 min, which is higher than the results ever reported. Importantly, this work proved that the ratio of total Brønsted to Lewis acid sites on solid acid is the key issue affected 5-HMF yield. After reaction, solid acid can be recycled for more than 5 times without catalytic performance decline, and the dissolved 5-HMF can be sufficiently separated from MSH via hyper cross-linked polymer (HCP) adsorption.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF CLUSTER SCIENCE
·
2023
·
IF 2.8
Luo Yun,Hou Min,Yan Yu,Li Wen Ge,Tong Jing
The Schiff base ligand (5-bromosalicylaldehyde)-2-aminophenol (H 2 L) and its complex were synthesized and characterized. The crystal structure was established by single-crystal X-ray diffraction, which showed that the monomer [Ni 4 L 4 (CH 3 CH 2 OH) 4 ]·1.46(CH 3 CH 2 OH) (the Ni(II) complex) crystallized in the tetragonal structure with space group I 4 1 / a . IR, elemental analysis, and thermogravimetric analysis were used to further confirm the structure of the Ni(II) complex. Its independent unit consists of four Ni(II) atoms, four L 2− Schiff base ligands, and four coordinated ethanol molecules. In vitro anticancer activities against the four human cell lines, A-549, MDA-MB-231, SMMC-7721, and CNE-2Z, revealed that the Ni(II) complex exhibited significant anticancer activity. Furthermore, the anticancer activities of the Ni(II) complex on SMMC-7721 and CNE-2Z cells were much better than that of cisplatin. In addition, migration and the Transwell assay illustrated that the Ni(II) complex could inhibit the invasion and cell migration of tumor cells CNE-2Z and SMMC-7721.
✓ 已验证
产品关联
DOI
高影响因子
ENERGY & FUELS
·
2023
·
IF 5.3
Xu Zhang,Haowen Cui,Qinfang Li,Haian Xia
It is of great significance to develop an affordable and environmentally friendly method for producing 5-hydroxymethylfurfural (HMF) and furfural from inexpensive and abundant agricultural waste. Herein, FePO4 combined with organic acids such as mandelic acid were used as catalysts in a one-pot catalytic conversion of untreated wheat straw into HMF and furfural in a two-phase system of THF/H2O saturated by NaCl. H+, Fe(OH)2+, and Fe(OH)2+ originated from partially dissolved FePO4 in hot water together with organic acids provided Brønsted and Lewis acid sites for the cascade conversion of wheat straw. Whereas organic acid could regulate the concentrations of Lewis and Brønsted acid sites to promote the dehydration process of fructose and hinder the production of by-products and humins, boosting the yield of HMF and furfural. The response surface methodology (RSM) was used to optimize the reaction conditions. The highest yield of HMF was 62.9% at 200 °C and 120 min, which is higher than the reported yield of HMF using lignocellulose as raw material in the current literature. Furfural has also achieved a higher yield (93.9%) at 180 °C and 90 min. This study demonstrates the rationality of the deployment of lignocellulose to produce furan compounds by organic acids and FePO4, providing the possibility for efficient production of HMF and furfural from recalcitrant agricultural waste.
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2023
·
IF 7.4
Tingting Liu,Yangyang Guo,Lei Luo,Meng Ye,Wen Liu,Tingyu Zhu
Solid amine adsorbents hold promising application prospects in the realm of industrial flue gas decarbonization. Nevertheless, there remains a need for substantial improvement in the cycling stability of solid amine adsorbents. Additionally, the competitive adsorption mechanism of solid amine adsorbents pertaining to flue gas components lacks thorough verification. In this study, amine-grafted micro-mesoporous ZSM-5/SBA-16 adsorbents were synthesized to improve the CO 2 adsorption capacity and investigate the effect of impurity gases on CO 2 adsorption. Various characterization techniques, including X-ray diffraction (XRD), thermogravimetric analysis (TGA), N 2 adsorption, and elemental analysis, were employed to analyze the properties of the adsorbents. The loading analysis of the micro-mesoporous molecular sieve revealed that ZS-A-2.0 exhibited the highest CO 2 adsorption capacity of 41.39 mg/g. Mass spectrometry was utilized to evaluate the co-adsorption experimentation involving multicomponent gases. The breakthrough curves of CO 2 displayed dual stages at low concentrations, suggesting the simultaneous occurrence of physical and chemical adsorption throughout the entire adsorption process. Based on temperature programming desorption (TPD) and in situ Fourier transform infrared spectroscopy (FTIR), the results indicated a notable enhancement in CO 2 adsorption due to the presence of H 2 O. Conversely, the presence of SO 2 and NO exhibited adverse effects on CO 2 adsorption, consequently hindering the formation of carbamate and (RNH 3 ) 2 CO 3 adsorption products. This study presents, for the first time, a comprehensive investigation into the interactive adsorption mechanism and product distribution between CO 2 and impurity gases. The findings presented herein provide valuable insights and essential support for practical flue gas applications.
✓ 已验证
产品关联
DOI
高影响因子
ANALYST
·
2023
·Vol. 148
·期 16
·3931-3937
·
IF 4.2
Tian-Yuan Guo,Hong-Wei Li,Chun-Xia Zhang,Yuqing Wu
Besides being a luminescent material, cytidine 5′-monophosphate-capped gold nanoclusters (AuNCs@CMP) also show superior peroxidase-like activity which can promote TMB oxidation in the presence of H2O2, causing the solution to turn efficiently from pale to blue. However, the presence of perfluorooctane sulfonate (PFOS) in the above system inhibited TMB oxidation and bluing of the solution, consequently establishing a colorimetric platform of AuNCs/H2O2/TMB for PFOS determination. The results showed that it responded to PFOS over a wide range of 2.0–50 μM, with a limit of detection (LOD) as low as 150 nM. Furthermore, in-depth mechanism investigation revealed that, rather than the active site of the catalyst being occupied by PFOS, such a hypochromatic effect originated from depletion of the reactive oxygen species (ROS) by PFOS degradation, thereby also offering a unique strategy to scavenge the lethal toxicity of PFOS. In addition, the colorimetric response of AuNCs/H2O2/TMB to PFOS was extended to smartphone determination conveniently based on RGB values. Finally, the established platform was applied to PFOS determination both in soil extracts and in tap water with good recovery, which supplies a novel colorimetric platform for visual determination of PFOS in practice. The method has the advantages of being rapid, sensitive and highly selective, which highlight the design and construction of more systems for determination and elimination of lethal pollutants in environmental water.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Surfaces and Interfaces
·
2022
·
IF 6.137
Weiquan Li,Die Hu,Ke Yin,Chenglong Yu,Bichun Huang
A series of hierarchical Ru-Ce/H-ZSM-5 were designed and synthesized using the sol-gel method, and they were applied as catalysts for the catalytic combustion of chlorobenzene. The pore diameter of the catalyst was adjusted using an amount of sodium alginate (SA). Among all of the catalysts synthesized, the 0.8 wt.%Ru-10 wt.%Ce/H-ZSM-5 catalyst with a crystallization recipe of 1SiO 2 : 0.02Al 2 O 3 : 0.15TPAOH: 0.04SA: 40H 2 O (named RCZA-0.04) exhibited the optimal catalytic activity, with the 90% conversion of chlorobenzene at 247 °C. In addition, the RCZA-0.04 catalyst maintained superb stability during a long-term reaction at 325 °C. The results of characterizations demonstrated that RCZA-0.04 possessed the largest mesoporous volume, which reduced the diffusion resistance of chlorobenzene and increased the dispersion of the active components, thereby enhancing the catalytic activities. Moreover, the RCZA-0.04 catalyst possessed a low Brønsted/Lewis ratio, which was conducive to the adsorption of chlorobenzene and the cleavage of the C Cl bond.
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2022
·
IF 4.326
Yuen Bai,Dongyang Liu,Liang Zhao,Jinsen Gao,Chunming Xu,Haitao Pang,Xuhui Gao
The influences of different B (Brønsted) acid site concentrations and the ratio of L (Lewis)/B (Brønsted) on the cracking pathways and product distributions in hexane cracking reactions as a model component of naphtha were investigated. The sodium-modified ZSM-5 catalysts were prepared by the wet impregnation method, and the Si–OH–Al groups of ZSM-5 were broken in the post-treatment process, resulting in a decrease in the number of strong B acid sites (SBAS) and an increase in the number of strong L acid sites (SLAS). The correlations between the n-hexane catalytic cracking reaction pathways and the catalyst acid properties were established. The reduced SBAS inhibits secondary reactions of light olefins such as hydrogen transfer, oligomerization, cyclization, and aromatization, while the increased SLAS and the ratio of SLAS/SBAS promoted the β scission reactions that significantly improved the yields of light olefins. Consequently, the appropriate SBAS and SLAS/SBAS ratios are desirable for the production of ethylene and propylene. The optimal SBAS concentration and SLAS/SBAS ratio ranged from 4.44 to 6.69 μmol/g and 9.18–11.86 for maximum ethylene and propylene yields of 16.14% and 14.63% in hexane catalytic pyrolysis reactions, respectively. Furthermore, the optimally prepared catalysts illustrated superior reactivities and catalytic stabilities in naphtha catalytic pyrolysis reactions under industrial conditions.
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Research and Technology-JMR&T
·
2022
·
IF 6.267
Wei Zhao,Rui-feng Liu,Jie Yan,Xian Wang,Hong-wei Zhang,Wen-xian Wang
The microstructure evolution and mechanical properties of 5 wt% SiC/7075Al composites processed with a combination of three-step spark plasma sintering (SPS), hot rolling (HR), and high-frequency electric pulse assisted treatment (HEAT) processing were investigated herein. It was found that the HEAT tremendously promoted the recrystallization behavior after the hot rolling, leading to grain refinement and residual stress weakening. It can be attributed to the combination of the electrical (Electron wind) and thermal effects (Joule heat) of pulse current. Electron wind promotes the expansion of the movement of dislocations, providing the material basis for recrystallization. Joule heat and residual stress within the matrix provide the substance conditions. There was a remarkable improvement in strength and ductility, among which the increase in strength was mainly due to the combined effect of phase precipitation strengthening and grain refinement, while the increase in elongation was mainly attributed to grain refinement and residual stress weakening. Compared to those of the untreated samples, the average grain size decreased by 18.3%, residual stresses reduced by 70%, and tensile strength improved by 37.3%. High-frequency assisted treatment has a comprehensive improvement on the microstructure and mechanical properties of SiC/7075Al composites.
✓ 已验证
产品关联
DOI
高影响因子
Frontiers in Chemistry
·
2022
·
IF 5.545
Li-Na Ke,Ling-Qi Kong,Xiu-Lian Zhu,Feng-Xu Wu,Qin-Hua Chen,Bin Li,Yun Dong,Hong-Mei Wang,Xiao-Hua Zeng
We have synthesized Rhopaladins’ analog (2E,4E)-4-chlorobenzylidene-2-(4-chlorostyryl)-N-cyclohexyl-1-(4-fluorophenyl)-5-oxopyrrolidine-2-carboxamide (RPDPRH) via a highly facile, inexpensive and green approach and verified the structural superiority of compound RPDPRH through molecular docking. Moreover, we further detected the anti-proliferation, apoptosis and HPV E6/E7 effects of RPDPRH on CaSki cells. Finally, we confirmed that compared with the previous compound (E)-N-(tert-butyl)-2-(4-chlorobenzoyl)-4-(4-fluorobenzylidene)-1-isopropyl-5-oxopyrrolidine-2-carboxamide (RPDPB), RPDPRH could better inhibit proliferation, induce apoptosis, and down-regulate HPV E6/E7 mRNA expression on Caski cells. And preliminary RT-PCR experiments have demonstrated that RPDPRH also could affect the expression of Bcl-2, Bax and Caspase-3 mRNA in Caski cells. In summary, RPDPRH has potential as an effective agent against cervical cancer and will play an important role in our subsequent research.Keywords: 4-arylidene-5-oxopyrrolidine, green synthesis, molecular docking, anti-tumor activity, apoptosis
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
·
2022
·
IF 6.437
Bingbing Luo,Kai Wu,Jiajun Yu,Siyu Wang,Yihan Wang,Chenyang Chu,Huiyan Zhang
Catalytic pyrolysis of biomass for efficient N-heterocycles production is highly promising but extremely challenging. Herein, catalytic co-pyrolysis of glycerol and cellulose under ammonia atmosphere was proposed to enhance the N-heterocycles yield. First, a solvolysis effect of glycerol, which could improve the thermal depolymerization of cellulose, was observed in thermogravimetric analysis (TGA). After that, the major influential factors, including Si/Al ratio, reaction temperature, and glycerol-to-cellulose (Gly:Cel) ratio, were investigated systematically. The N-heterocycles yield, as well as the comprehensive synergies of feedstocks, reached their maximum value under the conditions of Si/Al = 85, 550 ℃, and Gly:Cel = 5:1. The best synergistic extents for pyrroles , pyridines, and indoles were 105.3%, 71.3%, and 38.8%, respectively. The mechanism insight showed that, the thermal decomposition of cellulose was promoted while the coking of oxygenated molecules was suppressed during the catalytic co-pyrolysis process. Consequently, more oxygenated molecules were generated and retained for further catalytic conversion into imine intermediates and N-heterocycles.
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）