INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2023
·
IF 4.2
Hongdan Zhang,Chunyang Wu,Jialiang Wang,Ying Zhao,Peng Cheng,Zhen Zhao
In recent years, the efficient utilization of light alkanes, especially iso-butane and n-butane, has attracted increasing attention. Here, a series of ZSM-5 zeolite-encapsulated Pt-xZnO (x = 0, 0.05, 0.1, 0.25, 0.5, 1) catalysts were prepared via a one-pot hydrothermal method. The dispersion of metal particles, state of metal species, structure, and acidity of catalysts were confirmed by multiple physical and chemical characterizations. The catalysts were used in the catalytic cracking of iso-butane; the conversion of iso-butane would increase with the increase of ZnO content. However, Pt-0.1ZnO@ZSM-5 presented the best catalytic effect. The yield of ethylene and propylene reached 55% at 625 °C; meanwhile, the total yield of high value-added ethylene, propylene, butene, and BTX was as high as 80%.
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ACS Sustainable Chemistry & Engineering
·
2023
·
IF 8.4
Guoxing Liu,Huai Liu,Junhua Zhang,Rui Zhang,Heng Zhang,Yong Sun,Lincai Peng
Catalytic conversion of concentrated carbohydrates and raw biomass into 5-hydroxymethylfurfural (HMF), an important and value-added platform chemical, is highly desirable for industrial applications but challenging. In this work, the tin pyrophosphate-oxide (SnP2O7–SnO2) catalyst has been designed to efficiently produce HMF from various concentrated carbohydrates and raw biomass. Especially, a high HMF yield of 67.8% was implemented over the SPC4 catalyst from concentrated glucose (36 wt %) in a biphasic solvent system of water and methyl isobutyl ketone. Moreover, the SPC4 catalyst disclosed a wide range of universality for converting various concentrated carbohydrates and raw biomass to HMF with satisfactory yields (45.9–79.5%). To the best of our knowledge, this is the first example of accomplishing appreciable HMF yields from carbohydrates and raw biomass at such a high substrate concentration. It has been demonstrated that the superior catalytic performance of the catalyst should originate from its balanced Lewis and Brønsted acidity and superhydrophilicity property. This work invents a highly promising heterogeneous catalyst for efficiently valorizing renewable lignocellulose-related compounds into versatile furans.
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Foods
·
2023
·Vol. 12
·期 22
·4176
·
IF 5.2
Linlin Wang,Shurong Yang,Chunxia Mei,Nan Tang,Jialiang Wang,Qiangqing Yu,Gang Wang,Gaojue Wu,Jianxin Zhao,Wei Chen
Constipation is a major health concern worldwide and requires effective and safe treatment options. In this study, we selected ten strains of two species of lactobacilli to identify whether they were effective against constipation induced by loperamide administration in BALB/c mice. Monitoring of constipation-related indicators indicated thatLactobacillus paracasei(L. paracasei) mainly acted on the whole intestinal peristalsis to relieve constipation. Furthermore, through the detection of biological, chemical, mechanical, and immune barriers in mice, it was discovered thatL. paracaseichanged the relative abundance of bacteria related to the levels of acetic acid and 5-hydroxytryptamine (5-HT) (such as by increasing the relative abundance ofOdoribacterandClostridium, and reducing the relative abundance ofMucispirillum,Ruminococcus,Coprobacillus, andDorea), increased the concentration of acetic acid in the intestine, which stimulated enterochromaffin cells, promoted 5-HT synthesis in the colon, enhanced intestinal motility, and relieved constipation. In conclusion, this study provides a theoretical foundation for the development of personalized products for the treatment of constipation.Keywords:lactobacilli;constipation;intestinal microbiota;acetic acid;5-HT;gastrointestinal regulatory peptide;inflammatory factors
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Science China-Chemistry
·
2023
·Vol. 66
·期 12
·3636-3644
·
IF 9.6
Wang Shuangyue,Yang Ganceng,Jiao Yanqing,Liu Yue,Tian Chungui,Wu Aiping,Yan Haijing
Electrooxidation of the biomass derivative 5-hydroxymethylfurfural (HMF) is a highly promising approach for attaining versatile value-added chemicals ( e.g. , 2,5-furandicarboxylic acid, FDCA). Ni-based sulfides are promising electrocatalysts for HMF electrooxidation reaction (HMFOR). However, the HMFOR activity of Ni-based catalysts is far from satisfactory due to the unfavorable adsorption of HMF and OH*. Herein, we propose controlled W doping to effectively modify the electronic configuration of nanostructured Ni 3 S 2 to manipulate adsorption of HMF and OH*, for efficiently converting HMF into FDCA. Experimental and theoretical calculations indicate the incorporation of high-valence W results in the upshift of d-band center of Ni 3 S 2 , which facilitates the adsorption and dissociation of water to produce more OH*. Meanwhile, the high-valence W has strong electron-withdrawing ability and attracts electrons from Ni, leading to the elevated Ni valence, which is beneficial to optimizing the adsorption energy of HMF. Both concurrently contribute to the superb HMFOR performance. As a result, W 20 -Ni 3 S 2 @NF with optimal W dopant exhibits a low driving potential (1.34 V vs. RHE at 10 mA cm −2 ), accompanying with the 100% HMF conversion, 99.2% FDCA selectivity, and 97.3% Faraday efficiency. This work provides a design principle for HMFOR electrocatalysts by modulating the adsorption behaviors of HMF and OH* via rational electronic structure engineering.
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EUROPEAN JOURNAL OF MEDICINAL CHEMISTRY
·
2022
·
IF 7.088
Xiaona Sun,Yujin Wang,Zhichao Lei,Shasha Yue,Li Chen,Jianbo Sun
A series of novel 5-hydroxyl-1-azabenzanthrone derivatives were designed, synthesized and evaluated as dual binding site acetylcholinesterase inhibitors for the treatment of Alzheimer's disease (AD). The most effective Compound 16 showed selective inhibition of acetylcholinesterase ( ee AChE IC 50 = 0.045 μM; ee BuChE IC 50 = 19.68 μM; SI = 437.33). Most of the compounds showed cytoprotective effects on PC12 cells damaged by hydrogen peroxide, which might be related to their antioxidant activity . Further experiments confirmed that 16 exhibited anti-apoptotic effects at low concentrations and reduced the relative level of ROS generation in PC12 cells. The expression level of proteins related to antioxidant stress pathway in PC12 cells was relatively increased after administrated with 16 , which may be beneficial to delay the progression of the disease. Moreover, 16 was evaluated to be safe in vivo and in vitro, and showed good overall pharmacokinetic performance and high bioavailability (Foral = 55.5%). Besides, 16 showed comparable performance in ameliorating the scopolamine-induced cognition impairment to donepezil . In addition, in vitro BBB permeability experiments confirmed that 16 had high BBB permeability.
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Processes
·
2023
·Vol. 11
·期 10
·2937
·
IF 3.5
Shuyu Yu,Yibo Lu,Dandan Du,Rankun Wu,Xiang Ji,Hao Li
As the largest group of synthetic dyes, azo dyes can pose various health and environmental risks due to their widespread use and challenging degradation. Laccases are efficient green biocatalysts for the degradation of organic pollutants. Herein, we report thein situpackaging of laccase in copper-doped zeolitic imidazolate framework-8 (ZIF-8) for the decolorization of reactive black 5, which is a model azo dye. The immobilization support (Cu5/mZIF-8) was obtained via lowering the precursor ratio of ZIF-8 and incorporating copper ions during the synthesis process. Cu5/mZIF-8 were found to be nanospheres with an average diameter of around 150 nm. Laccase encapsulated in Cu5/mZIF-8 showed an activity recovery of 75.6%, which was 2.2 times higher than that of the laccase embedded in ZIF-8. Meanwhile, the immobilized laccase (Lac@Cu5/mZIF-8) showed a higher catalytic activity in organic solvents than that of the free enzyme. In the presence of a mediator, Lac@Cu5/mZIF-8 could remove 95.7% of reactive black 5 in 40 min. After four consecutive cycles, the dye decolorization efficiency declined to 28%. About four transformation products of reactive black 5 were identified via LC-MS analysis, and the potential decolorization mechanism was proposed. The results indicated that the immobilized laccase could be used as an efficient biocatalyst in dye decolorization.Keywords:laccase;zeolitic imidazolate framework-8;immobilization;dye decolorization
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ENZYME AND MICROBIAL TECHNOLOGY
·
2021
·
IF 3.493
Rong Wang,Xinqi Xu,Xuemei Yao,Hengtao Tang,Xin Ju,Liangzhi Li
Ribose-5-phosphate isomerase A (RpiA) is of great importance in biochemistry research, however its application in biotechnology has not been fully explored. In this study the activity of RpiA from Ochrobactrum sp. CSL1 (OsRpiA) towards D-allose was engineered based on sequential and structural analyses. Strategies of alanine scanning, rational design and saturated mutagenesis were employed to create three mutant libraries. A single mutant of K124A showed a 45 % activity improvement towards D-allose. The reaction properties of the mutant were analyzed, and a shift of optimal pH and higher thermal stability at low reaction temperatures were identified. The conversion of D-allose was also improved by 40 % using K124A, and higher activities on major substrates were found in the mutant’s substrate scope, implying its application potential in rare sugar preparation. Kinetics analysis revealed that K m of K124A mutant decreased by 12 % and the catalytic efficiency increased by 65 % towards D-allose. Moreover, molecular dynamics simulation illustrated the binding of substrate and K124A was more stable than that of the wild-type. The shorter distance and more relax bond angle between the catalytic residue of K124A and D-allose explained the activity improvement in detail. This study highlights the potential of OsRpiA as a biocatalyst for rare sugar preparation, and provides distinct evidences for its catalytic mechanism.
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Materials Today Chemistry
·
2021
·
IF 8.301
Y. Hu,M. Li,Z. Gao,L. Wang,J. Zhang
Sulfonated carbon dots (SCDs) were synthesized from plant leaves via continuously hydrothermal treatment by hydrogen peroxide and sulfuric acid, used as catalyst for converting fructose to 5-hydroxymethylfurfural (HMF). Owing to nanosize effect and moderate acidic intensity, SCDs could thoroughly distribute in the solvent with an improved interfacial compatibility and selectively convert fructose to HMF. Under the optimal condition, the yield of HMF was 92.6% along with a fructose conversion of 100%, benefiting from a low activation energy of 52.9 kJ/mol when dimethylsulfoxide was used as solvent. The SCDs catalyst can be recovered, after six recycles, the fructose conversion and HMF yield were remained 66.1% and 56.2% under condition with incompletely conversion of fructose, respectively. This work provides a sustainable route to prepare carbon dots with a superior catalytic performance for converting biomass to important biobased platform chemicals.
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ChemCatChem
·
2021
·Vol. 13
·期 13
·3027-3036
·
IF 5.686
Zhijian Wan,Youkun Tao,Hengzhi You,Xiang Zhang,Jing Shao
Graphical Ammonia decomposition : Ni nanoparticles with a mean size of ∼2.3 nm anchored on Na-ZSM-5 nanocrystals were prepared as a catalyst to effectively crack ammonia for CO x -free H 2 production. Ammonia has been increasingly recognised as an effective hydrogen carrier to produce clean hydrogen free of CO x emissions. This study reports the development of Ni-based catalysts to efficiently crack ammonia into hydrogen and nitrogen. A series of catalysts with different Ni loadings supported on Na-ZSM-5 zeolite nanocrystals were prepared with the assistance of 1,10-phenanthroline ligand. The coordination of Ni and the ligand led to the formation of uniform Ni nanoparticles with a mean size of ∼2.3 nm. These small Ni nanoparticles of the catalyst enabled a high activity in ammonia decomposition evaluated using a fixed-bed reactor. Using the zeolite support in its pristine sodium form provided the catalyst with desired basicity. This promotes a strong metal-support interaction, leading the catalyst to have high stability. The catalyst with 5 wt% Ni loading exhibited a high TOF of 3.51 s −1 with no performance degradation at 650 °C for 50 h.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Weiqi Wei,Gaojing Lyu,Weikun Jiang,Zhengyu Chen,Shubin Wu
In this work, a sulfonic acid-functionalized magnetic separable solid acid (Fe 3 O 4 @SiO 2 -SO 3 H) was synthesized, characterized, and tested for fructose conversion to 5-hydroxymethylfurfural (HMF). Results indicated that the prepared catalyst had a good efficacy for fructose dehydration to HMF due to its larger specific surface area, appropriate acid amount and homogeneous acid distribution. The maximum HMF yield of this work was 96.1 mol%. It was obtained at 120 °C for 1.5 h with 100 mol% fructose conversion. More importantly, the produced HMF could be further in-situ oxidized into 2,5-diformylfuran (DFF) after the replacing of the Fe 3 O 4 @SiO 2 -SO 3 H with a ZnFeRuO 4 catalyst, and the highest DFF yield of 90.2 mol% (based on initial fructose) was obtained after reaction another 8.5 h. The production of DFF from fructose through the above two consecutive steps avoids the intermediate HMF separation, which saves time and energy. In addition, both Fe 3 O 4 @SiO 2 -SO 3 H and ZnFeRuO 4 catalysts exhibited satisfied stability in the recycling experiments, which can be reused at least for five times with the HMF and DFF yield loss<5.3% and 3.3%, respectively. Finally, the plausible reaction mechanisms for fructose conversion to HMF or DFF over Fe 3 O 4 @SiO 2 -SO 3 H or/and ZnFeRuO 4 catalysts were also proposed in this work.
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CHEMICAL ENGINEERING SCIENCE
·
2021
·
IF 4.311
Tingting Qi,Yingying Kang,Moses Arowo,Yong Luo,Guang-Wen Chu,Liangliang Zhang,Hai-Kui Zou,Baochang Sun,Jian-Feng Chen
In this study, hierarchical ZSM-5 zeolites are hydrothermally prepared using rotating packed bed (RPB) in premixing process (gelation stage). The impact mechanisms of RPB on the zeolite growth process are investigated. It is found that the zeolite precursor obtained by RPB contains abundant bubbles, and aluminosilicate aggregates in the precursor are broken and dispersed uniformly, which is beneficial for the uniform and fast growth of zeolite. Additionally, the effects of various RPB-premix process parameters, including rotation speed, premixing time, and liquid feed rate on the particle sizes of ZSM-5 are systematically investigated. The prepared ZSM-5 zeolites by RPB-premix route exhibit smaller particle sizes, narrower particle size distributions, larger specific surface areas, richer pore structure, and more acid amount compared with those by traditional premix treatment. Therefore, this study provides a novel approach for the synthesis of high-performance ZSM-5 zeolites.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2021
·
IF 3.764
Xiangbo Song,Jun Yue,Yuting Zhu,Chengyan Wen,Lungang Chen,Qiying Liu,Longlong Ma,Chenguang Wang
Efficient and one-pot conversion of biomass-derived carbohydrate into highly value-added 5-hydroxymethylfurfural (HMF) is a crucial reaction step for the valorization of biomass resources toward bio-based chemicals and fuels. In this work, a series of Sn/SAPO-34 catalysts were prepared through impregnation and evaluated in glucose conversion to HMF. The physicochemical properties of Sn/SAPO-34 catalysts were systematically characterized by SEM, XRD, N2 physisorption, XPS, solid-state 119Sn, 29Si, and 31P NMR, XRF, UV–vis, NH3-TPD, and pyridine-FTIR techniques. It was demonstrated that controlling the Sn loading amount could facilely adjust the acid strength and acid amount of the SAPO-34 zeolite. The incorporation of Sn species could induce the formation of a tetrahedrally coordinated Sn4+ site and Sn-OH site to improve the amounts of Brønsted and Lewis acid sites of the catalyst. However, modification with sufficiently high Sn loading could decrease the acid strength and performance of the catalyst owing to its structure damage. The 5%Sn/SAPO-34 catalyst (i.e., Sn loading calculated based on the mass ratio of SnCl4·5H2O as a precursor to the parent SAPO-34) was found to exhibit the superior catalytic performance under mild conditions and could afford an HMF yield of 64.4% at 98.5% glucose conversion in a biphasic 35 wt % NaCl-H2O/tetrahydrofuran (THF) system at 150 °C within 1.5 h. Additionally, a catalytic reaction pathway was proposed, involving the adsorption of glucose molecules by the −Cl group on the catalyst via a hydrogen bond, followed by glucose isomerization to fructose over the Lewis acid Sn4+ and Al3+ sites and, finally, fructose dehydration to HMF catalyzed by the Brønsted acid Sn-OH and Si-OH-Al sites. The activity of the catalyst decreased due to the leaching of the active site Sn after several consecutive cycles. This work provides insights into the improvement in the Sn-containing zeolite catalyst for tandem conversion of glucose to HMF.
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