FUEL
·
2025
·
IF 7.5
Wenqian Song,Yuxin Wen,Guojun Kang,Wenqing Lv,Dekang Li,Haoquan Hu,Lijun Jin,Shijian Lu,Zhong Yan,Pengfei Liu
Amine-based solution absorption as the most promising and commercialized CO 2 capture method, attracted the increasing attention. However, its key lies in improving the CO 2 desorption performance while reducing the energy consumption in desorption. In this paper, HZSM-5 was dealuminated by sulfuric acid, further loaded by Fe 2 O 3 , Co 3 O 4 , NiO and ZnO via impregnation method and used in catalytic desorption of the blended amine solution of N-methyl-diethanolamine and piperazine. Results indicated that sulfuric acid leaching increased the number of acid sites and mesoporous surface area. When sulfuric acid reached 0.8 mol/L, the resultant catalyst (0.8H 2 SO 4 -HZ) improved the amount of the desorbed CO 2 by 10.26% and decreased the heat duty to 2128 kJ/mol CO 2 , with a reduction of 17.01% compared to non-catalytic system. The loading of metal oxides on 0.8H 2 SO 4 -HZ decreased surface area and changed acidity of catalysts. CO 2 desorption amount under catalysis of metal oxide modified M /0.8H 2 SO 4 -HZ followed the order of Fe/0.8H 2 SO 4 -HZ > Zn/0.8H 2 SO 4 -HZ > Ni/0.8H 2 SO 4 -HZ > Co/0.8H 2 SO 4 -HZ, whereas the relative heat duty was in order of Zn/0.8H 2 SO 4 -HZ > Co/0.8H 2 SO 4 -HZ > Ni/0.8H 2 SO 4 -HZ > Fe/0.8H 2 SO 4 -HZ. Fe/0.8H 2 SO 4 -HZ exhibited excellent catalytic performance, along with 12.82% increase in amount of CO 2 desorbed and reduction in heat duty to 2039 kJ/mol CO 2 , with a 20.49% decrease. Meanwhile, Fe/0.8H 2 SO 4 -HZ showed good stability after ten cycles and the addition of Fe/0.8H 2 SO 4 -HZ promoted CO 2 absorption. Suitable pore structure and abundant acid sites of the modified catalyst contributed to proton transfer and decomposition of carbamate. A possible mechanism for catalytic desorption over modified HZSM-5 was proposed. The work indicates that catalytic desorption by modified HZSM-5 catalyst is a promising way to decrease the energy consumption of amine solution regeneration.
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高影响因子
Journal of Water Process Engineering
·
2019
·
IF 3.173
Senlin Ma,Xingtao Zuo,Juan Xiong,Cong Ma,Zhongbing Chen
An ozonation process combined with hydrophobic adsorbent high silica ZSM-5 (HSZSM-5) was designed to enhance sulfamethoxazole (SMX) removal and reduce the ozone consumption. The promoted effect of HSZSM-5 on SMX removal was investigated in terms of SMX removal and TOC removal efficiency as well as the ozone consumption. The impacts of pH and CO 3 2− /HCO 3 - were also analyzed. The presence of HSZSM-5 helped to increase the SMX degradation and TOC removal efficiency and their kinetics rate constants. HSZSM-5 adsorption behaviors for SMX and its degradation intermediates were responsible for the findings. Direct ozone oxidation was the main mechanism of SMX removal as HZSM-5 could not contribute to producing H 2 O 2 and •OH. Much higher CO 3 2− /HCO 3 - concentration (≥10 mM) and pH value (>7) were in favor of SMX degradation. HSZSM-5 had a positive contribution to SMX removal. The mass ratio of ozone consumption to the removed SMX reduced to 0.63 g O 3 /g SMX. This system of introducing high silica zeolite in the ozonation/adsorption process is an environmentally and economically sound technology to removal micropollutants.
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高影响因子
RUSSIAN JOURNAL OF GENERAL CHEMISTRY
·
2021
·Vol. 90
·期 12
·2376-2380
·
IF 0.868
Abbas N.,Shabir G.,Saeed A.,Tirmizi S. A.,Echeverría G. A.,Piro O. E.,Erben M. F.
Abstract The present study is devoted to the synthesis of 4-chloro-2-{[5-(diethylamino)-2-hydroxybenzylidene]amino}phenol and its transition metal complexes. Synthesis of the ligand has been achieved by the condensation reaction of N,N -diethylsalicylaldehyde with 4-chloro-2-aminophenol in acidic medium. Metals complexes of the ligand with different transition metal ions [M 2+ = Mn(II), Fe(II), Co(II), Ni(II), Cu(II), Zn(II), Cd(II), Hg(II), and Pd(II)] have been accumulated in alcoholic media and characterized by spectroscopic methods. UV-Vis analysis of the complexes indicates the ligand coordination to the metal ions via both OH groups and the azomethine nitrogen atom, acting as a tridentate ligand. Anticancer tests of selected complexes demonstrate moderate in vitro activity of Cu(II) complex against HeLa cell line.
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高影响因子
ChemSusChem
·
2022
·Vol. 15
·期 13
·e202200233
·
IF 9.14
Zuojun Wei,Yuran Cheng,Hao Huang,Zhihe Ma,Kuo Zhou,Yingxin Liu
Graphical Simply the best : 14 Secondary metals and 6 catalytic supports are screened to fabricated Ni-based 10NiMn(4 : 1)/γ-Al 2 O 3 catalyst with improved activity and stability for the reductive amination of 5-hydroxymethylfurfural to 2,5-bis(aminomethyl)furan, which is attributed to the electron transfer effect between active Ni particles and the well-dispersed MnO x on the γ-Al 2 O 3 support. Mono- and bimetallic Ni-based catalysts were prepared by screening 6 supports and 14 secondary metals for reductive amination of 5-hydroxymethylfurfural (5-HMF) into 2,5-bis(aminomethyl)furan (BAMF), among which γ-Al 2 O 3 and Mn were the best candidates. By further optimization of the reaction conditions at 0.4 g catalyst loading for 0.5 g substrate of 5-HMF and 160 °C of reaction temperature, 10Ni/γ-Al 2 O 3 and 10NiMn(4 : 1)/γ-Al 2 O 3 achieved the highest BAMF yields of 86.3 and 82.1 %, respectively. Although the BAMF yield values were comparable with that over Raney Ni, the turnover frequencies based on the initial BAMF yield and unit weight of Ni for 10NiMn(4 : 1)/γ-Al 2 O 3 , 10Ni/γ-Al 2 O 3 , and Raney Ni were calculated as 0.41, 0.09, and 0.04 h −1 , respectively. X-ray diffraction, transmission electron microscopy, and X-ray photoelectron spectroscopy showed that the existence of MnO x well dispersed on the γ-Al 2 O 3 support and its electron transfer effect with Ni particles on the surface of the support contributed to the high efficiency and better recyclability for the five-time reused 10NiMn(4 : 1)/γ-Al 2 O 3 catalyst.
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PubMed
高影响因子
SOLID STATE SCIENCES
·
2019
·
IF 2.155
Yisong Wang,Tao Du,He Jia,Ziyang Qiu,Yanli Song
ZSM-5 zeolite with high aluminum content (Si/Al = 25) was synthesized and then cation-exchanged with alkali metal , alkaline earth metal , transition metal and rare earth metal cations (Li + , Mg 2+ , Ca 2+ , Cu 2+ , Zn 2+ , La 3+ and Ce 3+ ). Crystal structure and physicochemical properties were characterized by XRD , FTIR , TGA/DTG, XRF and nitrogen adsorption-desorption measurement. CO 2 adsorption isotherms of all samples were recorded approximately 0–120 kPa at 0 °C, 30 °C and 60 °C, and they were all successfully fitted by the Toth model. The N 2 adsorption isotherm presented an approximate straight rising line, and it was perfectly fitted by the Langmuir model. In addition, the CO 2 /N 2 adsorption selectivity, Henry's law constant and the working adsorption quantity were calculated by single component CO 2 and N 2 adsorption testing. Transition metal cations Cu 2+ and Zn 2+ type ZSM-5 had the maximum adsorption quantity of 0 °C (70.24 and 74.38 cm 3 /g), and they had the maximum adsorption selectivity under high pressure and adsorption saturation conditions. The adsorption heat of all ion-exchanged samples was lower than Na-ZSM-5, and it had the approximate value at high loadings (in the range of 15.46–17.65 kJ/mol).
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高影响因子
Catalysis Science & Technology
·
2022
·Vol. 12
·期 21
·6437-6443
·
IF 6.177
Xingyu Lu,Ke Qi,Di Wang,Xueya Dai,Wei Qi
2,5-Furandicarboxylic acid (FDCA) is a high-value platform molecule that can replace the fossil derivative terephthalic acid in the synthesis of important chemicals. FDCA can be synthesized from the oxidation of the biomass derivative 5-hydroxymethylfurfural (HMF). In this study, we loaded Cu-based catalysts with different morphologies and chemical states on carbon paper, and it was found that the Cu nanocrystalline/carbon paper catalyst with a thin and scattered dendrite structure (Cu(NSD)/CP) exhibits the best performance for the electrooxidation of HMF (96% yield and 100% selectivity for FDCA), which is attributed to the fact that the Cu0 and Cu1+ species in the catalyst are easily oxidized in situ to Cu2+ species, showing high catalytic activity during the reaction process. This paper highlights the importance of the identification of active sites and the rational design of catalysts based on structure–function relations.
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高影响因子
PHARMACEUTICAL RESEARCH
·
2021
·Vol. 38
·期 4
·693-706
·
IF 4.2
Xu Wenhao,Su Wenjing,Xue Zhencheng,Pu Faxiang,Xie Zhangfu,Jin Kongliang,Polyakov Nikolay E.,Dushkin Alexander V.,Su Weike
Purpose This study aims to overcome the challenges of the current oral targeted drug delivery system, such as the complex preparation process, poor biocompatibility, and delayed drug release. Methods Here, a non-covalent polymer hydrogel was prepared using the mechanochemical method, and the solid phase loading of 5-amino salicylic acid (5-ASA) was realized. Results The results obtained from the thermodynamics study, particle size analysis, and electron microscopy show that chitosan (CS) and sodium alginate (SA) form a pH-sensitive hydrogel under the mechanochemical force and also maintain good stability in aqueous solution. Fluorescent tracers study showed that the pH-sensitive hydrogel could achieve the targeted drug release in the colon and the retention time was over 12 h. Next, in vivo efficacy studies, change in mice body weight, DAI (disease activity index) score, thymus, and spleen index, and the diseased state of the mice colon revealed that the pH-sensitive hydrogel is an improved drug delivery system over 5-ASA API commercial preparations as observed in the efficacy and toxicological studies. Conclusion This method uses an innovative preparation technology that without the need of cross-linking agent to produce an efficient colon-targeted drug delivery system for the treatment of ulcerative colitis.
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PubMed
高影响因子
RSC Advances
·
2018
·Vol. 8
·期 57
·32423-32433
·
IF 2.936
Guo Qiu,Xincheng Wang,Chongpin Huang,Yingxia Li,Biaohua Chen
The efficient conversion of carbohydrates to 5-hydroxymethylfurfural (5-HMF) under mild conditions represents a very attractive and promising method of producing important building blocks. In this work, niobium phosphotungstates, with Nb/P molar ratios of 0.6, 1.0, 2.0 and 4.0 (NbPW-06, NbPW-1, NbPW-2, and NbPW-4, respectively) have been prepared by a facile, one-pot, alcohol-mediated thermal process and used for the direct conversion of fructose to 5-HMF. By adding a certain amount of Nb, the surface of the catalyst became enriched in P, and this enrichment was associated with the presence of surface P–OH groups that offered Brønsted acid sites that can activate superficial hydrogen species to facilitate 5-HMF generation. Pyridine-FTIR confirmed the presence of Brønsted and Lewis acid sites, which might play important roles in the dehydration of fructose to 5-HMF. Furthermore, polar aprotic solvents were well-suited for the conversion, and higher yields of 5-HMF were obtained in polar aprotic solvents than in nonpolar solvents. A 5-HMF yield of 96.7% with complete fructose consumption was obtained over NbPW-06 in DMSO at 80 °C after 90 min. In addition, NbPW-06 could be recycled several times without a significant decrease in the catalytic activity. A catalytic mechanism for this reaction was proposed. Moreover, this catalytic system can also be utilized for the dehydration of sucrose and inulin to 5-HMF in satisfactory yields. This study establishes an important platform for the further design of Nb-containing catalysts for the production of 5-HMF from carbohydrates under mild conditions.
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PubMed
高影响因子
JOURNAL OF CATALYSIS
·
2019
·
IF 7.723
Rui Chen,Changjun Yang,Quanquan Zhang,Bingguang Zhang,Kejian Deng
A new iron tetra(2,3-bis(butylthio)maleonitrile)porphyrazine (FePz(SBu) 8 ) has been synthesized, then it was loaded on H-ZSM-5 zeolite to obtain a supported biomimetic photocatalyst H-ZSM-5/FePz(SBu) 8 . Using H 2 O 2 as oxidant, the photocatalytic selective oxidation of glucose in water under visible light (λ ≥ 420 nm) irradiation was carried out in presence of H-ZSM-5/FePz(SBu) 8 . Under such conditions, the glucose can be efficiently converted into value-added chemicals such as glucaric acid, gluconic acid, arabinose, glycerol and formic acid . More importantly, in comparison with pure FePz(SBu) 8 and pure H-ZSM-5 zeolite, the H-ZSM-5/FePz(SBu) 8 exhibited a higher photocatalytic activity for glucose oxidation and the formation of glucaric acid was observed only when H-ZSM-5/FePz(SBu) 8 was used, deriving from the synergistic effect between FePz(SBu) 8 and H-ZSM-5 zeolite. Some reaction parameters of glucose oxidation catalyzed by the H-ZSM-5/FePz(SBu) 8 were discussed, such as loading amount of FePz(SBu) 8 , H 2 O 2 :glucose ratio, glucose concentration, and so on. It was demonstrated that the Soret-band of FePz(SBu) 8 contributed more to the visible light photocatalytic activity than the Q-band during the photocatalytic process. The stability of H-ZSM-5/FePz(SBu) 8 during the photocatalytic process was further evaluated by the reusability test. In addition, the generation of reactive oxygen species was determined by electron spin resonance (ESR) technology and scavenger experiments. A possible reaction pathway of glucose oxidation was also discussed.
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高影响因子
GREEN CHEMISTRY
·
2025
·
IF 9.2
Ke Liu,Ling Jiang,Lun Wang,Qunfeng Zhang,Li-Rong Yang,Jianping Wu,Haoran Yu
2,5-furandicarboxylic acid (FDCA) is a potential platform chemical from renewable feedstocks to make various polymers and high-value compounds. Bioconversion of 5-hydroxymethylfurfural (HMF) to FDCA by biocatalysts has the advantages of high selectivity, cost-effectiveness, and eco-friendliness. However, the full oxidation of HMF often requires a combination of two or three enzymes, as the production of FDCA involves three consecutive oxidation steps. In this study, we identified a pyrroloquinoline quinone (PQQ) and lanthanide-dependent alcohol dehydrogenase, PedH, capable of directly converting HMF to FDCA, representing a rare and intriguing discovery. We then engineered the enzyme for improved thermostability and activity against HMF to improve FDCA yield. Using computational design method, the thermostability was first significantly improved, with the 4M variant obtained showing a Tm value increased by 9.6 oC, and a half-life improved by 10.3-fold compared to wild type. With the 4M as the template, potential mutation sites for engineering enzyme activity were identified based on calculation of binding free energy and a deep learning model MutCompute. An automatic high-throughput platform for site-saturation mutagenesis library construction and screening was developed and applied to the identified mutation targets. After five rounds evolution, a variant was obtained that produced FDCA at a yield 474-fold higher than that of 4M. Under optimized reaction conditions, the optimal variant achieved a FDCA yield of 96.4% with 40 mM HMF as the substrate. Molecular dynamics simulations revealed that the mutations expanded the substrate binding pocket and shortened the reaction distances between substrate and cofactors. This study provides a highly efficient evolution approach for PedH, and several variants that are potentially used for high yield production of FDCA in industrial fields.
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高影响因子
ADVANCED POWDER TECHNOLOGY
·
2024
·
IF 4.2
Hu Wen,Yuxin Li,Haitao Yin,Wei Wang,Zhengchao Jin,Shunyu Han,Nanzhe Jiang
The conversion of natural clay to crystalline zeolites has been the subject of considerable interest from both academic and industrial circles. We present an effective strategy for converting kaolin to ZSM-5 zeolite, addressing the issue of reduced mesopore formation in conventional nano-ZSM-5 aggregates due to close-packing. This strategy utilizes kaolin as the sole source of silicon and aluminum, and by decoupling the nucleation and growth of ZSM-5 crystals, loosely stacked nano-H-ZSM-5 aggregates with high crystallinity crystals can be synthesized in a solid-like system by employing a tiny amount of TPAOH (TPAOH/SiO 2 = 0.064). The resulting nano-H-ZSM-5 aggregates exhibited high specific surface area (405.66 m 2 /g), high mesopore volume (0.64 cm 3 /g), and superior catalytic activity. This strategy offers a novel approach to the cost-effective synthesis of nano-H-ZSM-5 aggregates suitable for industrial applications.
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高影响因子
ACS Catalysis
·
2025
·
IF 13.1
Rong Shang,Hao Zhang,Yulong Li,Bang Gu,Qinghu Tang,Feng Qiu,Qiu-E Cao,Wenhao Fang
The synthesis of primary amines from renewable biobased carbonyl compounds via reductive amination has received much attention. Modifying the surface structure of a heterogeneous catalyst may offer prospects to address selectivity maneuvering in this complex amination process. In this work, a metal–organic framework (MOF)-derived carbon-coated strategy was adopted to prepare the Ni@C catalysts with different thicknesses of carbon shells. This type of Ni catalyst achieved 98% yield of (5-(aminomethyl)furan-2-yl)methanol (AMF) at 100 °C under 2 bar of H2 from reductive amination of 5-hydroxymethylfurfural (HMF, an important cellulose-derived platform molecule) with NH3·H2O. In comparison, a Ni-NiO catalyst obtained by reducing NiO with H2 would mainly overhydrogenate AMF to (5-(aminomethyl)tetrahydrofuran-2-yl)methanol (THAMF, 52% in yield) as a byproduct. The modification of the electronic structure of Ni0 active sites with a carbon shell was elucidated, demonstrating electron-rich Ni0 sites for H2 activation. Moreover, different HMF adsorption modes on Ni-NiO and Ni@C surfaces were illustrated, significantly affecting the product distribution. Subsequently, distinctive NH3·H2O activation processes were proposed for both Ni catalysts to understand selective conversion of the Schiff base (i.e., the critical reaction intermediate). The developed Ni@C catalyst with suitable carbon thickness, abundant Ni0 centers, and defective carbon species showed high AMF yield under mild reaction conditions, facile separation–regeneration, and satisfying reusability. In addition, this Ni catalyst can also provide a relatively good substrate scope toward bioamine synthesis via reductive amination.
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