INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
·
2023
·Vol. 24
·期 14
·11480
·
IF 5.6
Wei Mao,Jiawen Hao,Lingyu Zeng,Hao Wang,Hao Xu,Jinghong Zhou
Herein, we report the synthesis of bimetal–organic frameworks (BMOFs) with both Brønsted and Lewis acidities, in which phosphotungstic acid (PTA) was encapsulated in BMOFs. It is efficient in converting starch to 5-hydroxymethyl-furfural (HMF) in deep eutectic solvents (DESs) such as choline chloride and formic acid. The highest yield of HMF (37.94%) was obtained using P0.5/BMOFs1.0to catalyze starch in a mixed solvent system comprising DESs and ethyl acetate (EAC) (v/v; 2:3) at 180 °C and a reaction time of 10 min. Employing a DES as a cocatalyst and solvent reduced the use of organic solvents. The catalyst showed adequate reusability, and the HMF yield only decreased by 2.88% after six cycles of reuse compared with that of the initial catalyst. This study demonstrates the application potential of BMOFs in the conversion of biomass to useful molecules with commercial and/or research value.Keywords:bimetal–organic frameworks;phosphotungstic acid;loading;cassava starch;catalysis
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INORGANICA CHIMICA ACTA
·
2023
·
IF 2.8
Ruiqin Huang,Wei Li,Xiaoling Luo,Zheng Liu,Guo-Cheng Han,Runzhi Wei
2,5-bis(trifluoromethyl)terephthalic acid (H 2 L 1 ) as the main ligand and 1,10′-phenanthroline (L 2 ) as the co-ligand were reacted with manganese chloride tetrahydrate (MnCl 2 ·4H 2 O), nickel sulfate hexahydrate (NiSO 4 ·6H 2 O) and cobalt nitrate hexahydrate (Co(NO 3 ) 2 ·6H 2 O) by solvothermal reaction to give the manganese complex [Mn 2 (L 1 ) 2 (L 2 ) 2 ] n ( 1 ), the nickel complex {[Ni 3 (L 1 ) 3 (L 2 ) 2 (H 2 O) 4 ]·2DMF} n ( 2 ) and the cobalt complex {[Co 2 (L 1 ) 2 (DMF) 2 ]·H 2 O} n ( 3 ). The structures were characterized and their properties studied by means of single-crystal X-ray diffraction, infrared spectroscopy, elemental analysis, ultraviolet spectroscopy, fluorescence spectroscopy, thermogravimetric analysis. The single-crystal structure analysis showed that the complexes 1 – 3 are infinitely extended three-dimensional network-like structures of space groups P 1 - , P 1 - , P 2 1 / n , respectively. The results of fluorescence analysis and thermogravimetric analysis showed that complexes 1 – 3 have good thermal stability and fluorescence properties, respectively. Complex 3 can also maintain good thermal stability at 230 °C, and the maximum fluorescence emission wavelength is 370 nm.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Yongzhuo Yu,Wei Li,Huixing Yang,Qiuming Wei,Linlin Hou,Zhiliang Wu,Yangyang Jiang,Chaoyu Lv,Yuxin Huang,Jiyu Tang
The construction of heterojunction systems is an effective way to efficiently generate hydrogen by water photolysis. In this work, Ni-MOF (trimesic acid, (BTC)) and g-C 3 N 4 (denoted as CN) were combined, and then Ni-MOF/CN was modified by 4-Methyl-5-vinyl thiazole (denoted as MVTh). Finally, CdS was loaded on the surface of Ni-MOF/CN/MVTh to prepare the photocatalyst Ni-MOF/g-C 3 N 4 /MVTh/CdS (denoted as Ni/CN/M/Cd) with a triangular closed-loop path heterojunction for the first time. As a photocatalyst without precious metal cocatalysts, Ni/CN/M/Cd displayed high H 2 evolution (17.844 mmol·g −1 ·h −1 ) under an optimum CdS loading of 40 wt%. The H 2 evolution rate was approximately 79 times that of Ni-MOF/CN and exceeded those of almost all catalysts based on MOF/CN in the literature. The triangular closed-loop heterojunction formed between Ni-MOF, g-C 3 N 4 , and CdS could realize the directional migration of photocarriers and significantly diminished the transfer resistance of carriers. The Ni 2+ in Ni-MOF provided many cocatalytic sites for H 2 evolution via g-C 3 N 4 and CdS. Furthermore, charge carrier separation in Ni-MOF/CN/CdS improved after the innovative addition of MVTh. This study provides a reference for the construction of a closed-loop heterojunction system without precious metal cocatalysts.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Materials Chemistry A
·
2022
·Vol. 10
·期 39
·21135-21141
·
IF 14.511
Lifang Gao,Xin Wen,Shipeng Liu,Dongyang Qu,Yingming Ma,Jianhui Feng,Zhiwei Zhong,Hongyu Guan,Li Niu
Electrocatalytic preparation of 2,5-furancarboxylic acid (FDCA) from biomass-derived 5-hydroxymethylfurfural (HMF) is a highly attractive strategy for the development of the bio-renewable polymer industry. However, developing highly efficient catalysts with sufficient oxidation current density and durability remains a challenge. Introducing heteroatoms into layered double hydroxides (LDHs) can modulate the electrocatalysis behavior effectively. Herein, vanadium and cobalt were co-doped into nickel (oxy)hydroxide to construct a NiVCo-LDHs catalyst. With the diatomic synergetic modulation, the as-designed NiVCo-LDHs can electrosynthesize FDCA from HMF at a low potential of 1.376 V vs. RHE and achieve a 93.2–99.7% yield and 86.5–97.8% faradaic efficiency of FDCA during ten consecutive cycles. Such performance is superior to those of most reported nickel-based LDHs for HMF oxidation. Further studies indicate that the introduction of V can provide high intrinsic catalytic activity, mainly due to the enhanced specific surface area, facile electron transfer and abundant active sites.
✓ 已验证
产品关联
DOI
高影响因子
Catalysts
·
2022
·Vol. 12
·期 10
·1086
·
IF 4.501
Byu Ri Sim,Jie Gu,Yvette Ley,Shenggan Luo,Yihan Liu,Qin Chen,Yao Nie,Yi-Lei Zhao
Candida parapsilosiscarbonyl reductases (CpRCR) have been widely used for the reductive conversion of ketone precursors and chiral alcohol products in pharmaceutical industries. The enzymatic enantioselectivity is believed to be related to the shape complementation between the cavities in the enzymes and the substitutions of the ketone substrates. In this work, we reported an unexpected enantioselectivity in the enzyme reductions of dihydrofuran-3(2H)-one (DHF) to (S)-tetrahydrofuran-3-ol (DHF-ol, enantiomeric excess: 96.4%), while dihydrothiophen-3(2H)-one substrate (DHT) was unproductive under the same experimental conditions. To rationalize the exclusiveS-configuration and the specific reactivity ofDHF, we carried out molecular dynamics simulations for the reacting complexations ofDHFwithCpRCR, andDHTwithCpRCR. Our calculations indicate thatDHFpreferentially binds to the small cavity near L119, F285, and W286, while the large cavity near theα1helix was mainly occupied by solvent water molecules. Moreover, the pre-reaction state analysis suggests that thepro-Sconformations were more abundant than thepro-R, in particular forDHF. This suggests that the non-polar interaction of substrate C4-C5 methylene contacting the hydrophobic side-chains of L119-F285-W286, and the polar interaction of funanyl oxygen exposing the solvent environment play important roles in the enantioselectivity and reactivity. The phylogenetic tree ofCpRCR homologues implies that a variety of amino acid combinations at positions 285 and 286 were available and thereby potentially useful for redesigning enantioselective reductions of 5-membered-ring heterocyclic ketones.Keywords:carbonyl reductases;enantioselectivity;heterocyclic ketone;molecular modelling
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ENZYME INHIBITION AND MEDICINAL CHEMISTRY
·
2022
·
IF 5.756
Jinhua Zhu,Danyang Zhou,Dandan Wu,Wei Liu,Xiuhua Liu
In this work, a highly effective separation approach mediated by 5-Lipoxygenase (5-LOX) was established for screening and isolation of anti-inflammatory ingredients from leaves of Lonicera japonica Thunb. (LLJT). Using 5-LOX immobilised on TiO2 nanotubes as a microreactor, the targeted screening was exploited by combining with HPLC-MS system. Four compounds confirmed as luteolin, luteoside, lonicerin, and isochlorogenic acid C and a fraction (M1) were screened out to be potent inhibitors of 5-LOX. Their anti-inflammatory activities were further investigated and confirmed by RAW 264.7 cells inflammation model and rat foot swelling model. Furthermore, M1 was prepared by MCI GEL CHP20P column chromatography, and further separated by Pre-HPLC. One new compound confirmed to be 5,7,3′,4′-tetrahydroxyflavone-7-O-sambubioside was first isolated from LLJT. The results provide a new method for the effective separation of active components derived from natural products.HighlightsA 5-LOX mediated separation method was established for isolation of anti-inflammatory compounds.An anti-inflammatory ingredient was separated by MCI GEL CHP20P column chromatography.One new compound was first isolated from leaves of Lonicera japonica Thunb.5-LOX was immobilised on TiO2 nanotubes and exploited by combining with HPLC-MS system.The anti-inflammatory activity of screened components was evaluated.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Omega
·
2022
·
IF 4.132
Wen He,Fuwei Li,Yufei Gu,Xiaofeng Wang,Hengshuo Gu,Hongbing Fu,Xiumei Liang,Zhixia Li
Chainlike ZSM-5 was synthesized in a tetrapropylammonium hydroxide (TPAOH) and poly(diallydimethylammonium chloride) (PDDA) dual-template system. The synthesis parameters and formation mechanism of chainlike zeolites were investigated. The optimized composition of the synthesis mixture was as follows: the PDDA/SiO2, TPAOH/SiO2, SiO2/Al2O3, and H2O/SiO2 molar ratios are, respectively, 0.16, 0.4, 50, and 40, with tetraethyl orthosilicate and aluminum nitrate as silicon/aluminum sources. The resultant ZSM-5 showed a cross-linked chainlike morphology, mesopore-dominated pore structure, and mild acidity. The formation of the chainlike zeolite was attributed to synergistic actions between PDDA and TPAOH. TPAOH acted as an alkali source and helped to induce nucleation and control the crystal size. PDDA acted as a soft template to promote crystal nucleation, and a hard template to form a three-dimensional mesoporous structure. Light olefin (C2–4=) selectivities from cracking of ethanol and oleic acid over the present chainlike ZSM-5 at 400 °C reached 90 and 75.7%, respectively, which were much higher than those from commercial ZSM-5 (75 and 52.3%, respectively), demonstrating the excellent hydrothermal stability and catalytic performance of the synthesized chainlike zeolite.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Analytical Methods
·
2022
·Vol. 14
·期 26
·2586-2595
·
IF 3.532
Mingshu Song,Qin Wu,Beibei Liu,Pan Li,Lan Jiang,Yulong Wang,Sa Dong,Yonghua Xiong,Bruce D. Hammock,Cunzheng Zhang
In this study, a designed hapten possessing the classic structure of PDE-5 inhibitors was synthesized. A monoclonal antibody (mAb) with broad recognition for six PDE-5 inhibitors was further produced. For the determination of lodenafil, methisosildenafil, mirodenafil, udenafil and tadalafil, the limit of detection (LOD) and IC50 ranged from 1.01 to 26.91 ng mL−1 and 12.75 to 278 ng mL−1, respectively. Thereafter, a quantum dot bead-based lateral flow immunoassay (QB-LFIA) was developed, which improved the LOD and IC50 to 0.32–6.52 ng mL−1 and 7.45–133.8 ng mL−1, respectively. Method validation was conducted using honey and capsule samples spiked with PDE-5 inhibitors, and the recoveries of the intra- and inter-assays ranged from 81.01% to 108.16%, with coefficients of variation below 12.71%. In addition, the validity and the consistency have been confirmed with a comparison between QB-LFIA and HPLC-MS/MS (R2 = 0.9957). Furthermore, the developed QB-LFIA was employed for the inspection of real products, and several samples were found to be adulterated with lodenafil and methisosildenafil.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INDUSTRIAL CROPS AND PRODUCTS
·
2022
·
IF 6.449
Shaoqing Wang,Zhihe Li,Weiming Yi,Peng Fu,Xueyuan Bai
Catalytic pyrolysis of corn cob lignin were preformed using a tailored HZSM-5 @Al-SBA-15 hierarchical zeolite for the production of value-added aromatic hydrocarbon. Resulted showed that the highly ordered two-dimensional p6mm mesoporous shell could uniformly form on the surface of HZSM-5 core phase. The porosity and acidity of the HZSM-5 @Al-SBA-15 could be tailored by adjusting the TEOS/HZSM-5 mass ratio in the synthesis process. The aromatic hydrocarbon components regulated due to pre-cracking and enhanced diffusion via the mesoporous shell, as well as the retained shape-selectivity of the HZSM-5 core. Herein, the relative content of MAHs reached 45.02% with fewer poly-aromatic hydrocarbons (PAHs) of 25.91% when the TEOS/HZSM-5 mass ratio of 1.0. However, the length of the diffusion path had a certain impact on the anti-coking behavior. The catalytic stability of the hierarchical zeolites was also improved, with less coke formation than HZSM-5 alone. This work demonstrates that using a tailored hierarchical zeolite to regulate aromatic hydrocarbon components is feasible, and provide a reference for the practical application of agricultural crop wastes.
✓ 已验证
产品关联
DOI
高影响因子
Frontiers in Chemistry
·
2022
·
IF 5.545
Duan Ying,Wang Rui,Liu Qihang,Qin Xuya,Li Zuhuan
The conversion of 5-hydroxymethylfurfural (HMF) to 1-hydroxy-2,5-hexanedione (HHD) represented a typical route for high-value utilization of biomass. However, this reaction was often catalyzed by the noble metal catalyst. In this manuscript, W promoted Ni/Al2O3 was prepared as a noble-metal-free catalyst for this transformation. The catalysts were characterized by XRD, XPS, NH3-TPD, TEM, and EDS-mapping to study the influence of the introduction of W. There was an interaction between Ni and W, and strong acid sites were introduced by the addition of W. The W promoted Ni/Al2O3 showed good selectivity to HHD when used as a catalyst for the hydrogenation of HMF in water. The influences of the content of W, temperature, H2 pressure, reaction time, and acetic acid (AcOH) were studied. NiWOx/Al2O3-0.5 (mole ratio of W:Ni = 0.5) was found to be the most suitable catalyst. The high selectivity to HHD was ascribed to the acid sites introduced by W. This was proved by the fact that the selectivity to HHD was increased a lot when AcOH was added just using Ni/Al2O3 as catalysts. 59% yield of HHD was achieved on NiWOx/Al2O3-0.5 at 393 K, 4 MPa H2 reacting for 6 h, which was comparable to the noble metal catalyst, showing the potential application in the production of HHD from HMF.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Cleaner Production
·
2022
·
IF 11.072
Yibing Xie,Mengyu Wang,Xueqian Wang,Langlang Wang,Ping Ning,Yixing Ma,Jichang Lu,Rui Cao,Yu Xue
The traditional way for arsine (AsH 3 ) removal from the reducing exhaust gas by catalytic oxidation undershot the expect goal in pollutant emission control. This laboratory scale work used magnetic field to improve the chemical environment of AsH 3 catalytic oxidation over magnetic response catalyst Fe/HZSM-5. After introducing external magnetic field at a magnetic field intensity of 0.1 T, the catalytic performance of Fe/HZSM-5 for AsH 3 removal was improved by 52%, and the turnover frequency (TOF) value increased from 4.65 × 10 −3 s −1 to 5.73 × 10 −3 s −1 . The structure–activity relationship of the catalyst in the presence of magnetic field was investigated. The characterization results showed that Fe is mainly anchored onto the surface of Fe/HZSM-5 catalyst through an oxygen bridge, while a small proportion of Fe exists in the form of iron oxides . The Fe species and surface labile oxygen (O − ) in the aluminum tetrahedra are the magnetic active sites of Fe/HZSM-5, magnetic field promotes the reaction by increasing the activity of them. It was discovered that paramagnetic O − increased by 50% in the presence of magnetic field compared with that in its absence. Therefore, a magnetic-field-assisted oxygen cycling process is proposed. In terms of the stability of catalyst, formation of more amorphous oxidized arsenic after reaction in the presence of magnetic field reduced the toxicity to the strong acid sites of the catalyst, and the holding time of excellent AsH 3 removal efficiency was prolonged from 23 h to 35 h. These results provide new insights into magnetic-field-assisted zeolite catalysis.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF DAIRY SCIENCE
·
2022
·
IF 4.225
Yuanjia Chen,Lin Luo,Peiyan Feng,Baojun Xu,Xiaoqun Wei
ABSTRACT A robust method using HPLC-UV was developed to improve the accuracy and repeatability of a quantitative method to detect 5 nucleotides (cytidine-monophosphate, uridine monophosphate, adenosine monophosphate, guanine monophosphate, and inosine monophosphate) in infant formulas. The results showed that efficient separation could not be achieved without strict conditions. The proposed method displayed a strong linear relationship (R 2 > 0.9999) of single nucleotide in infant formula milk powder in the range of 10 to 1,000 mg/kg, a steady recovery (80.0% ∼110.0%) with relative standard deviation from 0.5% to 3.5%, under strict conditions of hydrophilic C 18 column with di-isopropyl at 62.5 ± 2.5°C (± standard deviation), 0.65 ± 0.1 mg/mL tetrabutylammonium bisulfate, and mobile phase of pH of 2.75 ± 0.02. By applying this method on a series of milk products in the Chinese market, we found a few of them exceeded the legal limits of nucleotides.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）