ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Wanzhen Zhu,Yu Meng,Chaoxin Yang,Jun Zhao,Hongliang Wang,Wei Hu,Guangqiang Lv,Yingxiong Wang,Tiansheng Deng,Xianglin Hou
As the frontier in heterogeneous catalyst, a monomer and positively charged active sites in the single-atom catalyst (SAC), anchored by high electronegative N, O, S, P, etc., atoms, may not be active for the multispecies (O2, substrates, intermediates, solvent etc.) involved liquid-phase aerobic oxidation. Here, with catalytic, aerobic oxidation of 5-hydroxymethylfurfural as an example, Pt SAC (Pt1-N4) was synthesized and tested first. With commercial Pt/C (Pt loading of 5 wt %) as a benchmark, 2,5-furandicarboxylic acid (FDCA) yield of 97.6% was obtained. Pt SAC (0.56 wt %) gave a much lower FDCA yield (28.8%). By changing the coordination atoms from highly electronegative N to low electronegative Co atoms, the prepared Pt single-atom alloy (SAA, Pt1-Co3) catalyst with ultralow Pt loading (0.06 wt %) gave a much high FDCA yield (99.6%). Density functional theory (DFT) calculations indicated that positively charged Pt sites (+0.712e) in Pt1-N4 almost lost the capability for oxygen adsorption and activation, as well as the adsorption for the key intermediate. In Pt1-Co3 SAA, the central negatively charged Pt atom (−0.446e) facilitated the adsorption of the key intermediate; meanwhile, the nearby Co atoms around the Pt atom constituted the O2-preferred adsorption/activation sites. This work shows the difference between the SAC with NPs and the SAA during liquid-phase oxidation of HMF and gives a useful guide in the future single-atom catalyst design in other related reactions.
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高影响因子
Molecular Catalysis
·
2019
·
IF 2.938
Liqin Wang,Heqin Guo,Qiang Wang,Bo Hou,Litao Jia,Jinglei Cui,Debao Li
Furfural, generally achieved from hemicelluloses and its derived pentose, is a high value-added product. The formation of furfural from cellulose and hexose remains challenging. The acid sites in zeolites are the major active sites for preparing furfural from hexose. The catalytic performance of zeolites can be improved by increasing the number of active sites for the preparation of furfural. In this work, HZ-Na free-m and HZ-Na-m zeolites were prepared through without or with adding Na + ions in the mother gels, respectively. GHB (hydrolysate of GBL) was the active site for the formation of acyclic fructose precursor (Intermediate 2). Acyclic fructose production and the following dehydration for producing furfural were favored by the middle strong and strong Brønsted acids in the channels of HZSM-5. Meanwhile, middle strong and strong Brønsted acids were favored the production of HMF from fructose and furfural from xylose. The exterior weak Lewis acid of HZSM-5 could promote the formation of soluble oligomers. The soluble oligomers were composed by HMF and furfural through condensation, etherification, nucleophilic attack and electrophilic attack. HMF molecule was easy to participate in the production of soluble oligomers than furfural molecule over exterior weak Lewis acid of HZSM-5.
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高影响因子
Journal of Biobased Materials and Bioenergy
·
2017
·Vol. 11
·期 5
·414-423
·
IF 0.975
Liu Chenlu,Liao Longfei,Li Zengyong,Liu Ying,Wu Shubin,Zhuang Junping
Mesoporous MCM-41 was amino-functionalized to immobilize cupric (Cu2+) and vanadyl (VO2+) for preparing MCM–NH2–Cu2+ and MCM–NH2–VO2+ co-catalysts. The as-prepared two catalysts had been characterized
by XRD, N2 adsorption–desorption, FT-IR, XPS and TEM. The catalytic performance of MCM–NH2–VO2+ in HMF oxidation could be significantly promoted by using MCM–NH2–Cu2+ as the co-catalysts. Several critical
reaction parameters had been investigated, and it indicated that the highest conversion of 5-hydroxymethylfurfural (HMF) obtained was 98.1% at 110 °C in toluene with an optimal 2,5-diformylfuran (DFF) yield of 61.2%. Particularly, the MCM–NH2–Cu2+ and
MCM–NH2–VO2+ catalyst exhibited great stability and can be reused and showed no significant loss of their catalytic activities.
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DOI
高影响因子
NANO
·
2018
·
IF 1.1
Yunlei Zhang,Pei Jin,Minjia Meng,Lin Gao,Meng Liu,Yongsheng Yan
The direct synthesis of metal-organic frameworks (MOFs) with acidic and basic active sites is challenging due to the introduction of functional groups by post-functionalization method often jeopardize the framework integrity. Herein, we report the direct synthesis of acid-base bi-functional MOFs with tuning acid-base strength. Employing modulated hydrothermal (MHT) approach, microporous MOFs named UiO-66-NH 2 was prepared. Through the ring-opening reaction of 1,3-propanesultone with amino group, UiO-66-NH 2 -SO 3 H-type catalysts can be obtained. The synthesized catalysts were well characterized and their catalytic performances were evaluated in one-pot glucose to 5-HMF conversion. Results revealed the acid-base bi-functional catalyst possessed high activity and excellent stability. This work provides a general and economically viable approach for the large-scale synthesis of acid-base bi-functional MOFs for their potential use in catalysis field.
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高影响因子
Journal of Sustainable Metallurgy
·
2023
·Vol. 9
·期 3
·1303-1314
·
IF 2.4
Lv Ningning,Qiu Yuchao,Hu Yiming,Shi Hangkai,Shi Junjie,Ding Xiang,Li Haolun
It has been proved that Cr 2 O 3 is favorable to promote the crystallization of perovskite in the Selective Crystallization and Phase Separation (SCPS) process. However, the related thermodynamic data of equilibrium phase relations was quite limited. In the present work, the equilibrium phase relations of CaO-SiO 2 -TiO 2 system with the addition of 5 wt% Cr 2 O 3 were experimentally carried out using the high temperature equilibration-quenching technique followed by X-Ray Diffraction (XRD), Scanning Electron Microscopy-Energy Dispersive X-Ray Spectroscopy (SEM–EDS), as well as thermodynamic calculation. More attention has been focused on the influence of 5 wt% Cr 2 O 3 addition on the liquid-perovskite two-phase coexisting region. The results indicated that the crystallization of perovskite was promoted by Cr 2 O 3 addition by expanding the primary phase of perovskite toward higher SiO 2 areas. Meanwhile, distinct discrepancies were found when the present experimental results were compared with the data from the literature and the isotherms calculated by FactSage, indicating that the present results are not only meaningful for the improvement of the SCPS process, but also important for the optimization of titania related oxide thermodynamic database. Graphical Abstract
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高影响因子
CATALYSIS LETTERS
·
2022
·Vol. 152
·期 11
·3427-3436
·
IF 2.936
Xu Siquan,Xing Xinyi,Wu Han,Shi Xian,Zhang Zongqi,Gao Hui
5-Hydroxymethylfurfural (HMF) is a biomass-derived platform compound with great application potential. Herein, the efficient NbW-SBA-15 series catalysts were prepared by incorporating the niobium and tungsten into the pore wall of SBA-15 mesoporous silica. The physico-chemical features of NbW-SBA-15 catalysts with different proportions of niobium and tungsten were analyzed through ICP-AES, Low/Wide-angle XRD, N 2 adsorption–desorption, SEM, TEM, UV–Vis DRS, Raman spectroscopy, NH 3 -TPD, and Py-FTIR technologies. It was discovered that by changing the incorporating ratio of niobium and tungsten in the pore wall, the acidic nature (acid strength, acid density, and acid ratio) of the catalyst was adjusted, which in turn affected the catalytic performance. As the introduction molar ratio of niobium to tungsten is 1:1, the corresponding [1:1]NbW-SBA-15 catalyst occupied the highest acid density and stronger acid sites, showing the best catalytic activity. A desired HMF yield of 64% was obtained under optimal reaction conditions. Furthermore, after five consecutive testing cycles, the performance of [1:1]NbW-SBA-15 catalyst was maintained, confirming its outstanding hydrothermal stability. Graphical Abstract
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INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
·
2024
·Vol. 25
·期 5
·2693
·
IF 4.9
Xiaofan Liu,Huihui Zhao,Jiatao Xie,Yanping Fu,Bo Li,Xiao Yu,Tao Chen,Yang Lin,Daohong Jiang,Jiasen Cheng
Phytopathogenic fungi normally secrete large amounts of CWDEs to enhance infection of plants. In this study, we identified and characterized a secreted glycosyl hydrolase 5 family member inSclerotinia sclerotiorum(SsGH5,Sclerotinia sclerotiorumGlycosyl Hydrolase 5).SsGH5was significantly upregulated during the early stages of infection. Knocking outSsGH5did not affect the growth and acid production ofS. sclerotiorumbut resulted in decreased glucan utilization and significantly reduced virulence. In addition,Arabidopsis thalianaexpressing SsGH5 became more susceptible to necrotrophic pathogens and basal immune responses were inhibited in these plants. Remarkably, the lost virulence of theΔSsGH5mutants was restored after inoculating ontoSsGH5transgenicArabidopsis. In summary, these results highlight thatS. sclerotiorumsuppresses the immune responses ofArabidopsisthrough secreting SsGH5, and thus exerts full virulence for successful infection.
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DOI
PubMed
高影响因子
BULLETIN OF THE CHEMICAL SOCIETY OF JAPAN
·
2021
·Vol. 95
·期 1
·116-120
·
IF 5.488
Zhu Xin Yi,Yang Xi Nan,Wu Heng,Tao Zhu,Xiao Xin
The interaction between pyridine pillar[5]arene (PyP5) and 2-naphthol with the former as the host molecule and the latter as the guest molecule is studied by fluorescence spectroscopy and NMR techniques, and the results show that PyP5 forms a 1:1 host-guest inclusion complex with 2-naphthol. Although free 2-naphthol has strong fluorescence, it is quenched in 2-naphthol@PyP5. Experiments were conducted with 2-naphthol@PyP5 as a fluorescent probe to detect different anions with results showing that only CO32− causes a significant enhancement of the fluorescence of the fluorescent probe. Due to this high selectivity and high sensitivity, the fluorescent probe 2-naphthol@PyP5 may open up an effective way for the detection of CO32−.
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高影响因子
Journal of Energy Chemistry
·
2013
·
IF 0
Xiuquan Jia,Jiping Ma,Penghua Che,Fang Lu,Hong Miao,Jin Gao,Jie Xu
Direct conversion of fructose-based carbohydrates to 5-ethoxymethylfurfural (EMF) catalyzed by Lewis acid in ethanol was investigated. It was found that BF 3 ·(Et) 2 O was favorable for 5-hydroxymethylfurfural (HMF) etherification to EMF. BF 3 ·(Et) 2 O combination with AlCl 3 ·6H 2 O with the molar ratio of 1 was an effective catalyst system for synthesis of EMF from fructose-based carbohydrates. 55.0%, 45.4% and 23.9% of EMF yields were obtained from fructose, inulin and sucrose under optimized conditions, respectively.
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DOI
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2025
·
IF 8.5
Yan Li,Fan Yang,Xuemei Tan,Yitong Li,Chunjie Gong,Huanan Li,Wanli Cheng,Wenjing Xiao,Jiashu Liu,Zhengbing Jiang
2.5-Furandicarboxylic acid (FDCA) is considered a next-generation bio-based platform chemical that can serve as a precursor to polyethylene furanoate. This study established a dual-enzyme cascade system for FDCA production utilizing lipase from Burkholderia sp. RF7-non_BP1 ( BP 1-Lip) and alcohol oxidase from Colletotrichum gloeosporioides ( Cgl AlcOx). The reaction was carried out in two steps, the molar yield of 5-hydroxymethyl-2-furancarboxylic acid (HMFCA) reached 94.44 ± 3.02 %% after 24 h, and the molar yield of FDCA reached 100 ± 1.96 % after 84 h, with a productivity of 9.29 mg/L/h. In addition, the conversion of 50 mM HMF was successfully achieved by feeding batch substrate addition strategy. After a total reaction time of 264 h, the FDCA concentration reached 41.03 mM, with an FDCA productivity of 24.26 mg/L/h. Molecular docking analysis of BP 1-Lip with HMF showed that the aldehyde group is easily oxidized and can form multiple hydrogen bonds with residues such as Asn110, Lys127, and Asn130. etc.; Lys127 enhances binding stability by localizing substrates through salt bridges and π-cation interactions; Hydrophobic residues Val131 and Tyr292 stabilize the furan ring localization and maintain the ideal conformation of the substrate; The electronic/spatial effects of hydroxymethyl and furan conformations make it difficult for HMFCA and DFF to effectively bind, inhibiting further oxidation.
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DOI
PubMed
高影响因子
CytoJournal
·
2025
·
IF 3.1
Xunjia Li,Zhixin Xu,Ying Li,Yan Luo,Jie Zhou,Deyu Zuo,Weijian Xiong
Objective:
Patients with chronic kidney disease (CKD) exhibit increased vascular calcification (VC) risks, worsened by high-dose erythropoietin (EPO). While EPO treats anemia, its role in VC pathogenesis remains unclear. Ginsenoside Rb1 (Rb1), a Panax ginseng compound with anti-calcification properties, may counteract EPO-induced VC through the GATA binding protein 6 (GATA6)/bone morphogenetic protein 2 (BMP2)/Smad1/5/9 pathway. This article aims to explore whether Rb1 could counteract EPO-induced VC through the GATA6/BMP2/Smad1/5/9 pathway.
Material and Methods:
Adenine-induced CKD rats and b-glycerophosphate-treated vascular smooth muscle cells (VSMCs) received EPO ± Rb1. Calcification was assessed through von Kossa/alizarin red staining. Smooth muscle protein 22-a (SM22a)/a-Smooth muscle actin (a-SMA) expression was measured by immunofluorescence and real-time-quantitative polymerase chain reaction (RT-qPCR). GATA6/BMP2/Smad1/5/9 activation was analyzed using RT-qPCR/Western blot. Rb1-BMP2 interactions were tested through biotin pulldown, micro-thermophoresis, and Co-immunoprecipitation (Co-IP). GATA6 knockdown validated pathway roles.
Results:
High-dose EPO significantly worsened CKD-associated calcification and VSMC calcification (P < 0.01), suppressed SM22a and a-SMA expression levels, and activated the GATA6/BMP2/Smad1/5/9 pathway (P < 0.01). GATA6 knockdown reduced EPO-exacerbated calcification and modulated BMP2/Smad1/5/9 signaling (P < 0.01). Rb1 increased SM22a and a-SMA expression levels and inhibited Smad 1/5/9 phosphorylation (P < 0.01), without affecting GATA6 or BMP2 expression (P > 0.05). Molecular docking and Co-IP experiments revealed that Rb1 binds directly to BMP2, blocking its interaction with bone morphogenetic protein receptor and inhibiting Smad 1/5/9 phosphorylation (P < 0.01).
Conclusion:
Rb1 mitigates EPO-aggravated VC in CKD by disrupting BMP2/Smad1/5/9 signaling, positioning it as a promising molecular intervention strategy to reduce EPO-induced vascular toxicity.
Keywords: Bone morphogenetic protein 2/Smad1/5/9 signaling pathway, Chronic kidney disease, Erythropoietin, Ginsenoside Rb1, Vascular calcification
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PubMed
高影响因子
ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Xu Chen,Wenjun Zhang,Yanmei Zheng,Lin Dong,Zupeng Chen
The photocatalytic oxidation of 5-hydroxymethylfurfural (5-HMF) to 2,5-furandicarboxylic acid (FDCA) represents a sustainable strategy for the conversion of biomass-based platform compounds into high-value chemicals. In this work, a supramolecular self-assembly strategy is employed to synthesize tubular carbon nitride (T-MCN), and sodium ion-doped carbon nitride (Na-T-MCN) is obtained via sodium chloride-assisted thermal polymerization. The optimized catalyst demonstrates superior activity in the oxidation of 5-HMF, achieving a high yield of FDCA (90%) within 8 h. The exceptional photocatalytic performance of Na-T-MCN is attributed to the incorporation of Na+ ions and cyanamide groups, which facilitate the separation of photogenerated charges and holes. To elucidate the underlying mechanism, intermediate trapping experiments and electron paramagnetic resonance (EPR) spectroscopy are employed to investigate the dynamics of photoinduced charge separation, electron transfer, and the reaction pathway of photocatalytic oxidation of 5-HMF. The findings reveal that the key active species in the oxidation reaction are the •O2– and h+ species. This study provides a viable and efficient strategy for converting biomass platform compounds into high-value-added products.
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