ACS Sustainable Chemistry & Engineering
·
2020
·
IF 7.632
Qian Wang,Zhi Yu,Junting Feng,Paolo Fornasiero,Yufei He,Dianqing Li
The production of biofuel 2,5-dimethylfuran (DMF) from an important biomass platform of 5-hydroxymethyl furfural (HMF) involves a complicated reaction pathway due to the competition of C═O hydrogenation and C–O hydrogenolysis; however, the dependence of formed intermediates and catalytic sites needs to be further identified. Herein, we constructed a highly efficient and selective Cu/ZnO-Al2O3 catalyst via reduction of a CuZnAl-layer double hydroxide (LDH) precursor, aimed for studying the effect of Cu0/Cu+ species on forming different intermediates and their synergetic promotional effect on HMF hydrodeoxygenation. As expected, the dependence of formation of different intermediates on the Cu+/Cu0 ratio was observed; notably, Cu/ZnO-Al2O3 with higher Cu+/Cu0 ratio finally gave 90.1% DMF selectivity at 100% HMF conversion, more selective than CuNi/Al2O3 (59.6%) and Cu/MgO-Al2O3 (75.8%) references. By a combined study of in situ IR experiments, the observed correlation between the reaction intermediates and the Cu0/Cu+ site suggests that Cu0 tends to adsorb the C═O bond as well as hydrogen molecule, while the Cu+ site is preferable to adsorb and activate the C–O bond. With the synergy of dual active sites, the Cu/ZnO-Al2O3 catalyst showed both high activity and selectivity to DMF. This work provides deep insight into the nature of active Cu species in multiple functional group biomass platform transformation.
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ENERGY & FUELS
·
2020
·
IF 3.421
Junhua Zhang,Zhaohua Qi,Yao Liu,Junnan Wei,Xing Tang,Liang He,Lincai Peng
Catalytic transfer hydrogenation (CTH) of 5-hydroxymethylfurfural (HMF) into 2,5-bis(hydroxymethyl)furan (BHMF) is an important method for the catalytic upgrading of biomass-derived platform compounds to fuels and chemicals, and the development of effective and economical catalysts for this purpose is of great significance. In this work, we designed and prepared a new carbon-nanosheets (CNS)-supported Zr/Ca bimetallic catalyst (ZrCa@CNS) with low cost by a “gel-blowing” strategy. Comprehensive studies revealed that ZrCa(2)@CNS-600 exhibited good catalytic activity on the CTH of HMF into BHMF via Meerwein–Ponndorf–Verley (MPV) reduction, and an 84.2% BHMF yield with a 91.2% HMF conversion was obtained in isopropyl alcohol at 190 °C in 10 h. ZrCa(2)@CNS-600 exhibited good heterogeneity, reusability, and stability, and it is readily recovered from the reaction mixture by filtration and consecutively recycled/reused for six times without an obvious loss in its catalytic activity.
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CHEMICAL ENGINEERING RESEARCH & DESIGN
·
2020
·
IF 3.35
Yue Zhou,Huiping Zhang,Ying Yan
CuO/ZSM-5/PSSF was synthesized by a combined wet lay-up papermaking, secondary growth and chemical vapor deposition (CVD) method for the catalytic oxidation of ethyl acetate in the fixed bed reactor. Ethanol and acetaldehyde are found during the oxidation and 3 wt% CuO/ZSM-5/PSSF catalyst exhibited the best performance with 90% conversion of 1500 ppm ethyl acetate at 254 °C with GHSV of 15,000 h −1 , and the CuO/ZSM-5/PSSF exhibits low byproducts selectivity compared to granular CuO/ZSM-5 catalyst. Furthermore, the 3 wt% CuO/ZSM-5/PSSF catalyst exhibits a high stability after being used at 262 °C for 48 h.
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JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
·
2020
·Vol. 95
·期 6
·1748-1755
·
IF 2.75
Ting Wang,Junnan Wei,Yunchao Feng,Huai Liu,Xing Tang,Xianhai Zeng,Yong Sun,Tingzhou Lei,Lu Lin
BACKGROUND Biomass holds the promise to provide a sustainable future for the chemical industry. 2, 5-Bishydroxymethylfuran (BHMF) is a versatile bio-based diol with a broad range of potential applications in many polymeric materials, artificial fibers and drugs. However, the controlling of the BHMF selectivity in hydrogenation of biomass-derived 5-hydroxymethylfurfural (HMF) with complex transformation pathways is always a great challenge especially under solvent-free conditions in which many side reactions may occur due to its rich reducible groups. RESULTS A facile and effective approach was developed for the selective synthesis of BHMF by solvent-free hydrogenation of a deep eutectic mixture consisting of HMF (75 wt%) and choline chloride (ChCl), by which a BHMF selectivity up to 94.6% was gained at full HMF conversion over Raney Co at 100 °C in 4 h. In addition, the HMF conversion and selectivity toward BHMF can be regulated and controlled through altering the strength of hydrogen-bonding interactions of HMF-based deep eutectic mixtures (ChCl–HMF mixtures). CONCLUSION We developed an effective approach that allows the solvent-free synthesis of BHMF via hydrogenation of HMF-based deep eutectic mixtures. The extraordinary BHMF selectivity in the solvent-free hydrogenation of HMF is reasonably attributed to the hydrogen-bonding interactions formed between ChCl and HMF/BHMF which greatly suppresses the side reactions of HMF and the over-reduction of BHMF. © 2020 Society of Chemical Industry
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JOURNAL OF MOLECULAR STRUCTURE
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2020
·
IF 2.463
Fenglan Liang,Deyun Ma
Two nickel (II) based metal-organic frameworks, [Ni(1,4-bib) 1.5 (NO 2 -BDC) (H 2 O)] n ( 1 ) and [Ni(1,4-bimb) (CH 3 O-BDC)] n ( 2 ) (1,4-bib = 1,4-bis(1-imidazolyl)benzene, NO 2 -BDC = 5-nitroisophthalate, 1,4-bimb = 1,4-bis(imidazole-1-ylmethyl)benzene, and CH 3 O-BDC = 5-methoxyisophthalate) have been synthesized and were structurally characterized. Complex 1 is a three-fold interpenetrated 3D framework with 5-connected pcu topology and is comprised of Ni-1,4-bib layers further pillared by 5-nip approximately in the b direction. Complex 2 shows a 2D (4,4) sql network when dinuclear nickel ions and ligands are regarded as nodes and linkers, respectively. Furthermore, the luminescence and catalytic properties of 1 – 2 for the degradation of methyl orange in a Fenton-like process have also investigated.
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RSC Advances
·
2021
·Vol. 11
·期 43
·26908-26914
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IF 3.361
Jingyuan Liu,Xinyi Xue,Xin Zhou,Gang Chen,Wei Liu
3 wt% Ag2S/Zn5In2S8 (3A/Z5) and 3 wt% Ag2S/ZnIn2S4 (3A/Z1) were prepared by a two-step synthesis method. The first-principles calculations revealed that the anisotropic carrier transport property of Zn5In2S8 (Z5) is much stronger than that of ZnIn2S4 (Z1). Furthermore, unsynchronized electron and hole transport leads to higher bulk carrier separation efficiency in Z5. After accelerating the surface photocatalytic reaction rate by Ag2S modification, the differences between 3A/Z5 and 3A/Z1 in the bulk carrier separation were further enlarged. Photoelectrochemical tests confirmed that the bulk charge separation efficiency of 3A/Z5 is 13.70%, which is 7.4 times higher than 3A/Z1 (1.84%). Because of the high bulk carrier separation efficiency, the 3A/Z5 exhibits a promising photocatalytic hydrogen production rate, reaching 3189 μmol h−1 g−1. Through intuitive evidence, this work proves that material with stronger anisotropic conductivity has higher bulk carrier separation efficiency, thus has the potential to exhibit high photocatalytic hydrogen production performance.
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CHEMICO-BIOLOGICAL INTERACTIONS
·
2021
·
IF 5.194
Jing Guan,Xin Tong,Yi Zhang,Fan Xu,Yuxin Zhang,Xiurui Liang,Jiaqi Jin,Hongyan Jing,Liuxian Guo,Xinrui Ni,Jihua Fu
As a widely used anticancer drug in the clinic, cisplatin has obvious side effects, especially nephrotoxicity . Previous studies have suggested that the accumulation of intracellular reactive oxygen species (ROS) is a hallmark of cisplatin-induced acute kidney injury . This study aimed to investigate the relationship between ROS accumulation induced by cisplatin and 5-HT degradation. In vivo, by HE and TUNEL staining, we found that cisplatin-induced renal lesions and apoptotic regions, which were located in proximal tubular epithelial cells, were also the regions in which tryptophan hydroxylase 1 (Tph1), aromatic l -amino acid decarboxylase (AADC), 5-HT 2A receptor (5-HT 2A R) and monoamine oxidase A (MAO-A) were overexpressed, as determined by immunohistochemistry. Notably, the 5-HT 2A R antagonist sarpogrelate hydrochloride (SH) and the AADC inhibitor carbidopa (CDP) significantly attenuated cisplatin-induced increases in serum creatinine and blood urea nitrogen levels, renal ROS levels, oxidative stress (SOD activity and MDA), proinflammatory cytokine levels (NF-κB, TNF-α and IL-1β), proapoptotic factor levels (Bax, Bcl-2, C-caspase 3 and C-caspase 9) and the phosphorylation of p38 and STAT3 , as well as renal lesions and apoptosis . The combination of SH and CDP could almost abolish the effects of cisplatin challenge. In vitro, the effects of cisplatin challenge and the inhibitory effects of SH and CDP were also observed in HK-2 cells. Additionally, similar to the combination of SH and CDP, the MAO-A inhibitor clorgyline could also abolish the effects of cisplatin challenge. More importantly, by western blotting , we detected that the upregulation of Tph1, AADC and MAO-A expression induced by cisplatin both in vivo and in vitro could be obviously suppressed by SH to decrease 5-HT synthesis and mitochondrial 5-HT degradation. Altogether, these findings suggested that cisplatin-induced nephrotoxicity is due to the activation of the 5-HT degradation system in proximal tubular epithelial cells, including 5-HT 2A R and 5-HT synthesis and degradation. 5-HT 2A R plays a role by mediating the expression of MAO-A and the 5-HT synthases Tph1 and AADC.
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PROCESS BIOCHEMISTRY
·
2019
·
IF 2.883
Zhe-Ming Wu,Chang-Ling Hao,Tao Tong,Ren-Chao Zheng,Yu-Guo Zheng
( S )-3-Cyano-5-methylhexanoic acid (( S )-CMHA) is the key chiral intermediate of pregabalin . In this paper, an aqueous two-phase system (ATPS) was developed to extract ( S )-CMHA from nitrilase-catalyzed bioconversion broth. Inorganic salts and hydrophilic solvents were screened to form ATPS, among which an acetone/ammonium sulfate ATPS was investigated in detail, including phase diagram, effect of phase composition and stability of ( S )-CMHA. The maximum product recovery of 99.15% was obtained by an optimized ATPS system composed of 15% (w/w) ammonium sulfate and 35% (w/w) acetone with the removal of 99% cells and 86.27% proteins. The total ( S )-CMHA yield reached 92.11% after back-extraction. The recycling use of ammonium sulfate was investigated, and 93.10% of salt in the salt-rich phase was recovered with the addition of methanol. The results demonstrated the efficiency of the two-step extraction process for separation of ( S )-CMHA.
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RADIOCHIMICA ACTA
·
2019
·Vol. 108
·期 4
·239-247
·
IF 1.339
Quan Gan,Yimin Cai,Kuirong Fu,Lihua Yuan,Wen Feng
The extraction of U(VI) from aqueous nitric acid solutions with pillar[5]arene-based phosphine oxide (L) and [C8mim][NTf 2 ] ionic liquid dissolved in 1,2-dichloroethane was explored. A great positive impact in this system was observed. The effect of IL concentration in the organic phase and HNO 3 concentration in the aqueous phase is considered. The distribution ratios of U(VI) were significantly enhanced upon adding a small amount of ionic liquid as compared with organic diluent. The extraction system was also examined for its ability towards extraction of lanthanides and Th 4+ . The results revealed higher separation factors towards UO 2 2+ over Th 4+ in the presence of ionic liquid compared with organic diluent. Other factors such as C 8 mim + and NTf 2 − have also been considered. This extraction system has shorter equilibrium time as compared with in IL diluent. Stripping experiments showed almost quantitative back extraction of UO 2 2+ within two stages. With high selectivity towards UO 2 2+ and efficient back extraction, this new POP5A-ionic liquid-organic diluent system shows promise for future application of uranium recovery.
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GREEN CHEMISTRY
·
2019
·Vol. 21
·期 7
·1702-1709
·
IF 9.405
Shujing Zhang,Hong Ma,Yuxia Sun,Yang Luo,Xin Liu,Meiyun Zhang,Jin Gao,Jie Xu
The selective hydrogenation and rearrangement of 5-hydroxymethylfurfural (5-HMF) to 3-hydroxymethyl-cyclopentone (HCPN) were studied over a MOF-derived bimetallic nickel–copper catalyst in water. The combination of nickel and copper dramatically improved the efficiency in both the selective hydrogenation of the carbonyl group of 5-HMF and the hydrogenative ring-rearrangement of the C5 ring, affording 70.3% yield for HCPN and 99.8% yield for the rearrangement products. Moreover, it was indicated that water acted as a solvent, reactant, and proton donor by dissociation at an elevated temperature, which supplied slightly acidic conditions and promoted the rearrangement reaction.
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XENOBIOTICA
·
2019
·
IF 1.902
Siyuan Sun,Sisi Zhou,Shaowei Lei,Shujie Zhu,Kai Wang,Huidi Jiang,Hui Zhou
1. Jatrorrhizine is an active ingredient found in various traditional Chinese medicinal plants. Based on our previous finding that jatrorrhizine was a potent inhibitor of OCT2 and OCT3, the aim of the present study was to explore whether jatrorrhizine has an antidepressant-like action action via inhibition of uptake-2 transporters.2. In vitro uptake tests showed that jatrorrhizine strongly inhibited PMAT-mediated MPP+ uptake with an IC50 value of 1.05 μM and reduced 5-HT and NE uptake mediated by hOCT2, hOCT3 and hPMAT with IC50 values of 0.1–1 μM (for OCT2 and OCT3) and 1–10 μM (for PMAT).3. In mouse synaptosomes, jatrorrhizine suppressed 5-HT and NE uptake in a concentration dependently manner, where the role of uptake-2 inhibition is significant.4. The antidepressant-like action of jatrorrhizine was evaluated by mouse tail suspension test (TST). The TST showed that one week of jatrorrhizine (5, 10 and 20 mg/kg, i.p.) or venlafaxine (20 mg/kg, i.g.) can significantly reduce the duration of immobility when compared with vehicle control group.5. The concentration of jatrorrhizine shows a dose-dependent increase in brain tissues.6. Our study suggested that jatrorrhizine might be used as an antidepressant agent via inhibition of uptake-2 transporters.
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JOURNAL OF POLYMER SCIENCE PART B-POLYMER PHYSICS
·
2019
·Vol. 57
·期 11
·713-721
·
IF 2.596
Qiao Wang,Lefan Li,Zongjin Li,Siyao Guo,Guoxing Sun
It remains challenging to satisfy the combined performances for hydrogels with excellent mechanical behavior, high deformability, and super recoverability under harsh environmental conditions. In this study, we first established a strong polymer network via the crosslinking of polymer chains on the surfaces of sub-5-nm calcium hydroxide nanospherulites in ethylene glycol solvent. The organic gel expressed excellent mechanical properties such as a recoverable compressive engineering stress of 249 MPa and an elongation stress of 402 KPa, which was attributed to the uniform nanosized crosslinking structure as characterized by SEM. Moreover, the nonvolatile solvent remained in the gel, meaning that the sample can resist a wide temperature range of −56 to 100 °C without losing the elastic properties. This novel organic gel could provide promising routes to develop the ideal elastic carriers for wearable devices, smart skin sensors, and damping materials. © 2019 Wiley Periodicals, Inc. J. Polym. Sci., Part B: Polym. Phys. 2019 , 57 , 713–721
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