ENVIRONMENTAL RESEARCH
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2022
·
IF 8.431
Mingyu Li,Yuhan Ma,Jingjing Jiang,Tianren Li,Chongjun Zhang,Zhonghui Han,Shuangshi Dong
Heterogeneous photo-Fenton technology has drawn tremendous attention for removal of recalcitrant pollutants. Fe-based metal-organic frameworks (Fe-MOFs) are regarded to be superior candidates in wastewater treatment technology . However, the central metal sites of the MOFs are coordinated with the linkers, which reduces active site exposure and decelerates H 2 O 2 activation. In this study, a series of 2, 5-dioxido-1, 4-benzenedicarboxylate (H 2 DOBDC)-functionalized MIL-100(Fe) with enhanced degradation performance was successfully constructed via solvothermal strategy. The modified MIL-100(Fe) displayed an improvement in photo-Fenton behaviors. The photocatalytic rate constant of optimized MIL-100(Fe)-1/2/3 are 2.3, 3.6 and 4.4 times higher compared with the original MIL-100(Fe). The introduced H 2 DOBDC accelerates the separation and transfer in photo-induced charges and promotes Fe(II)/Fe(III) cycle, thus improving the performance. •OH and •O 2 − are main reactive radicals in tetracycline (TCH) degradation. Dealkylation, hydroxylation, dehydration and dealdehyding are the main pathways for TCH degradation.
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FUEL
·
2022
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IF 8.035
Zhe Bai,Luyao Wang,Hongwei Cao,Xiangwen Zhang,Guozhu Li
Hydrodesulfurization (HDS) is an effective way to reduce sulfur content in oil for the enforcement of more stringent environmental regulations. MoS 2 has been widely used as an effective component for catalyzing HDS, and needs to be extensively studied in depth. Herein, MoS 2 nanoflowers with the symbiosis of 1T-2H phases in the basal planes and coexistence of S and Mo vacancies are prepared via the assembly of many nanosheets by a one-pot solvothermal method. The morphology, crystal phase structure and defects of these 1T-2H MoS 2 samples were well characterized. The 1T/2H ratio and the state of vacancies were effectively tuned by changing the solvothermal conditions. Active and stable 1T-2H mixed MoS 2 nanoflowers with high content of 1T phase and moderate S and Mo vacancies were obtained by the regulation of oxalic acid in the mixture of ethanol and water. In the HDS of dibenzothiophene at 300 °C and 4 MPa, the optimal catalyst of MoS 2 -water–ethanol-OA exhibited a substrate conversion of 89.3% in 10 h. Moreover, the activity of MoS 2 -water–ethanol-OA was well retained without any decrease in the recycling experiment.
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REACTIVE & FUNCTIONAL POLYMERS
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2022
·
IF 4.966
Ziqi Zhao,Yulong Liu,Youquan Zhang,Mei Yang,Fang Shen,Zongwu Wei,Kungang Chai,Hongbing Ji
Starch-based urethane polymers hold great potential for adsorptive separation of acetophenone (AP) and 1-phenylethanol (PE), which coexist commonly in the petrochemical by-products. Yet, the overall adsorption performance was restricted due to the poor porosity of adsorbent. We herein applied external crosslinking strategy to fabricate hypercrosslinked aromatic-rich starch urethane polymer (HASUP) with large surface area. The structural evolution, including chemical state, porosity and morphology were observed through various characteristic techniques. The adsorption properties of AP and PE onto HASUP were investigated in both single and binary systems. Compared to its non-porous precursor, HASUP exhibited significantly higher overall adsorption capacity while maintaining the AP selectivity with varying compositions . The further static and dynamic adsorption assessments demonstrated that HASUP showed exceptional performance to separate AP and PE. And HASUP also exhibited excellent anti-interference ability and recyclability for selective adsorption of AP over PE. Furthermore, theoretical results indicated that the multiple interactions including hydrophobic, π-π, and hydrogen bonding interactions account for selective adsorption of AP. In combination with high surface area, this synergistic effect enhanced the adsorption strength , affording a high AP uptake for HASUP. This work may provide an insight for designing novel porous starch-based adsorbents with high performance.
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FUEL
·
2022
·
IF 8.035
Yi Liu,Ying Chen,Shuang Ma,Xianlong Liu,Xiangwen Zhang,Ji-Jun Zou,Lun Pan
High-energy–density (HED) fuels have attracted extensive attention for volume-fixed aerospace vehicles because they can provide more propulsion energy to increase the payload and range of aerospace vehicles. Herein, we report a route for synthesis of HED fuel, pentacyclo[8.2.1.1 4,7 .0 2,9 .0 3,8 ]tetradecane (PCTD) with strained structure, by photoinduced intermolecular [2 + 2] cycloaddition of norbornene (NBE). The triplet quenching and phosphorescence quenching results indicate that NBE cycloaddition is conducted through the photosensitized processes containing triplet–triplet energy transfer, cyclization and relaxation. The reaction conditions are optimized to obtain the high photocatalytic activity, with the NBE conversion and PCTD selectivity reaching 78.7% and 94.4%, respectively. Moreover, a kinetic model is proposed with the reaction rate equation being correlated with the incident light flux, with the pseudo reaction kinetics parameters and reaction rate equations obtained. Importantly, PCTD shows high density of 1.024 g/mL and high volumetric net heat of combustion of 42.98 MJ/L, much higher than those of JP-10. In addition, blending with JP-10 or QC can significantly improve cryogenic properties of blended fuels, which is very promising for the practical application.
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RESEARCH ON CHEMICAL INTERMEDIATES
·
2022
·Vol. 48
·期 3
·983-1001
·
IF 3.134
Zhang Dawei,Ren Lu,Liu Ailing,Zhang Yumin,Lv Yang,Gu Qiang
Abstract An efficient synthesis of 1,3,5-trisubstituted-1 H -pyrazoles was developed via cyclocondensation in 78–92% yields starting from α , β -unsaturated aldehydes/ketones with substituted phenylhydrazine using vitamin B 1 as a catalyst, and was characterized by HR-MS, FT-IR, 1 H NMR and 13 C NMR spectroscopy. The reaction has simple operation, metal-free catalysis, acid or base free catalysis. As a green catalyst, vitamin B 1 was found to possess favorable catalytic activity and reusability for the condensation reaction. 1,3,5-trisubstituted-1 H -pyrazole shows from orange-red to cyan in different solvents when the electron withdrawing group is attached to acetophenone (taking compound 5i as an example). Compound 5i as a metal ion fluorescent probe has excellent selectivity for Ag + detection. The crystal structure of the compound 3-(4-chlorophenyl)-1,5-diphenyl-4,5-dihydro-1 H -pyrazole ( 5b ) in the orthorhombic space group Pca 21 was presented and formed racemic crystals. Graphical abstract
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Bioengineered
·
2022
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IF 6.832
Xiao-Yi Chen,Qian-Long Wang,Wei-Xue Huang,Long-Wei Li,Lan-Cong Liu,Yi Yang,You-Jiao Wu,Shan-Shan Song,Hao Ma,Hua Zhou,Pei Luo
Bacterial peritonitis is a severe disease that diagnosis remains challenging for clinicians. Measuring biomarkers might be a rapid diagnostic method. The objective of this study was to analyze and evaluate the dynamic changes in HIF-1α concentration in serum exosomes during bacterial peritonitis. The pre-clinical application value of serum exosomal HIF-1α was evaluated via imipenem and cilastatin sodium (ICS) intervention in the bacterial peritonitis model. The new colorimetric method to quantitate dynamic expression changes of HIF-1α in serum exosomes during bacterial peritonitis was established by our team via using the gold seed-coated with aptamer-functionalized Au @ Au core-shell peroxidase mimic. The typical inflammatory cytokines of bacterial peritonitis were also measured. Following intramuscular administration with ICS, In-Vivo Xtreme imaging system was used to visualize abdominal infection extent. Meanwhile, HIF-1α concentration in rat serum exosomes and pro-inflammatory factors levels in serum were detected. The serum typical inflammatory cytokines levels were elevated in GFP-labeled E.coli induced bacterial peritonitis. The serum exosomal HIF-1α levels clearly increased at 12 h, reached the peak during 24–48 h, and then gradually decreased at 72 h. Following intramuscular administration with ICS, the abdominal infection extent, HIF-1α concentration in serum exosomes, and the serum pro-inflammatory factors levels were reduced at 24 h in GFP-labeled E. coli induced bacterial peritonitis model. The serum exosomal HIF-1α can be used as a biomarker in the early stage of bacterial peritonitis, which might provide the basic research in the pre-clinical for further predicting and monitoring the pathological process of bacterial peritonitis.
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Natural Product Communications
·
2022
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IF 1.496
Qing Liu,Ying Wei,Yongjia Hao,Jian Yang,Bowen Pan,Xiaosheng Yang,Ying Zhou,Xia Wang
Viral infection imposes a major threat to human health. To develop new potent antiviral agents, Hederagenin (HE), a known inhibitor of HIV-1 and HCV NS3/4A proteases, was used as a starting material to synthesize 4 types of HE derivatives, HE-3,23-diacyl, HES-3,23-diacyl, HES-3-acyl, and HES-3-oxo-23-acyl. We evaluated the in vitro inhibitory activities of the derivatives against HIV-1 and HCV NS3/4A proteases. (3β,23)-Di-O-diglutaryl-hederagenin (1b) and (3β,23)-di-O-(3′,3′-dimethylsuccinyl-hederagenin ethyl ester (2b) exhibited potent inhibitory activities against the HIV-1 and/or HCV NS3/4A proteases with IC50 values < 10 μM, but did not appreciably inhibit general human proteases renin and trypsin. The SARs showed that dicarboxylic acid hemiesters of HE significantly enhance the antiviral activities when C3 or C23 are linked with 6 carbon acyl chains.
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Reaction Chemistry & Engineering
·
2023
·Vol. 8
·期 9
·2342-2352
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IF 3.9
Jia Juan,Xue Ping,Liu Xueping,Xu Chongrui,Gu Yaohua,Li Peng
The co-immobilization of laccase and a mediator is essential for water treatment due to the fact that the free laccase and mediator cannot be recovered and reused simultaneously. Herein, a spherical solid biocatalyst, Lac@Ce-GMA-Cu-DA@AS, was prepared via the co-immobilization of laccase and acetosyringone mediator in a functionalized cellulose composite doped with HKUST-1. The Lac@Ce-GMA-Cu-DA@AS microbeads exhibited higher catalytic activity, better reusability and superior degradation efficiency for the substrate compared to the undoped HKUST-1. Specifically, 96% degradation efficiency of carbazole solution with a concentration of 20 mg L−1 was achieved after treatment with 1.0 g (wet weight) of Lac@Ce-GMA-Cu-DA@AS beads for 8 h under the conditions of 30 °C, pH 5.0, and 20 mM ionic strength. Based on the analysis and identification of the degradation intermediates of carbazole, the possible pathways for the degradation of carbazole by the Lac@Ce-GMA-Cu-DA@AS microbeads were proposed. It was found that the toxicity of the carbazole solution was lower after treatment than the original. Natural polymeric cellulose composite doped with HKUST-1 displayed an excellent performance for co-immobilizing laccase–mediator and can provide a practical new approach for the degradation of carbazole pollutant in water.
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PROCESS BIOCHEMISTRY
·
2023
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IF 4.4
Xiaoxue Zhang,Mengmeng Zhong,Rui Zhou,Wenxiu Qin,Youbin Si
Microbial reduction of Se(IV) to Se(0) is extremely important for the detoxification of selenium oxyanion, but the reductive mechanism is still controversial. In this study, the reduction of Se(IV) by Shewanella oneidensis MR-1 and Shewanella putrefaciens was systematically investigated. The results showed that excessive Se(IV) severely inhibited the growth of microorganisms and Se(IV) reduction. The extracellular accumulation of Nano-Se(0) particles was shown to be approximately 250–650 nm in diameter. Riboflavin facilitated Se(IV) reduction, while rotenone , as an electron inhibitor, could completely inhibit Se(IV) reduction, validating the extracellular electron transport process for biosynthesized Nano-Se(0). Importantly, the amorphous Nano-Se(0) synthesized by S. oneidensis MR-1 were mixtures of helical chains and Se 8 rings, while those synthesized by S. putrefaciens were mainly composed of helical chains. FTIR results demonstrated that Nano-Se(0) particles were wrapped by some proteins, organic substances and lipids , exhibiting superior dispersibility and biocompatibility. Biogenic Nano-Se(0) particles can also be considered for technological applications in various fields.
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JOURNAL OF MOLECULAR LIQUIDS
·
2021
·
IF 6.165
Mingcan Mei,Xutao Hu,Zhen Song,Lifang Chen,Liyuan Deng,Zhiwen Qi
Although chemisorptive ionic liquids (ILs) are widely expected as promising CO 2 absorbents, rigorous thermodynamic analyses for such systems remain challenging due to the inevitable co-existence of chemisorption and physisorption. In this work, an experimental approach combining quantitative NMR (qNMR) spectroscopy and mass balance is proposed to straightforwardly quantify the chemisorption and physisorption of CO 2 in chemisorptive absorbent, and 1-ethyl-3-methylimidazolium acetate ([Emim][OAc]) is selected for an exemplary study. The total CO 2 solubility in [Emim][OAc] is measured by the pressure drop method, of which the chemisorption part is quantified by qNMR and the physisorption part is then determined by mass balance. Correspondingly, a large set of CO 2 solubilities at four temperatures (298.15 K, 313.15 K, 323.15 K, and 348.15 K) covering the low pressure range below 100 kPa are determined, where the chemisorption and physisorption contribution are distinguished quantitatively. Following that, thermodynamic analyses for the CO 2 absorption by [Emim][OAc] are made from chemisorption and physisorption point of view, respectively.
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Nature Biomedical Engineering
·
2021
·Vol. 6
·期 1
·32-43
·
IF 25.671
Zheng Di-Wei,Deng Wei-Wei,Song Wen-Fang,Wu Cong-Cong,Liu Jie,Hong Sheng,Zhuang Ze-Nan,Cheng Han,Sun Zhi-Jun,Zhang Xian-Zheng
Because a host’s immune system is affected by host–microbiota interactions, means of modulating the microbiota could be leveraged to augment the effectiveness of cancer therapies. Here we report that patients with oral squamous cell carcinoma (OSCC) whose tumours contained higher levels of bacteria of the genus Peptostreptococcus had higher probability of long-term survival. We then show that in mice with murine OSCC tumours injected with oral microbiota from patients with OSCCs, antitumour responses were enhanced by the subcutaneous delivery of an adhesive hydrogel incorporating silver nanoparticles (which inhibited the growth of bacteria competing with Peptostreptococcus ) alongside the intratumoural delivery of the bacterium P. anaerobius (which upregulated the levels of Peptostreptococcus ). We also show that in mice with subcutaneous or orthotopic murine OSCC tumours, combination therapy with the two components (nanoparticle-incorporating hydrogel and exogenous P. anaerobius ) synergized with checkpoint inhibition with programmed death-1. Our findings suggest that biomaterials can be designed to modulate human microbiota to augment antitumour immune responses.
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Surfaces and Interfaces
·
2023
·
IF 6.2
Xupeng Zhang,Kaiqian Li,Xianghong Li,Longxin Guo,Shuduan Deng,Zhiping Xu,Gang Zhu
Manufacturing durable wood membranes that demonstrate both high efficiency and ultra-high flux for continuous oil-water separation utilizing scalable and cost-effective processes remains a serious challenge. In this study, a facile two-step approach is employed to prepare a novel superhydrophobic/oleophilic wood-based MOF (metal-organic framework) membrane. This method involves in-situ anchoring of the octahedral Cu-HKUST-1 (copper benzene-1,3,5-tricarboxylate) onto the wood sponge (WS), which inherently features internal micro-channels. The structure is then modified using the eco-friendly hydrophobic long-chain coupling agent dodecyltrimethoxysilane (DTMS). Due to its unique micro/nanoscale rough surface morphology and low surface energy, the functional wood membrane (DTMS/HKUST-1@WS) exhibited a high contact angle of 162.98±1.10° for water and was able to effectively separate various immiscible oil/water mixtures. Notably, the DTMS/HKUST-1@WS membrane can be integrated into a pump drive system, serving as an advanced filter element for the sustained and efficient oil-water constituents. Results showed that this membrane possesses attractive permeability toward CCl 4 (56689.34 L·m −2 ·h −1 ) and toluene (47241.12 L·m −2 ·h −1 ), achieving separation efficiencies over 99.0%. Furthermore, this novel membrane exhibits remarkable resistance to physical damage, high/low temperatures, and corrosive solutions, thereby showcasing stable superhydrophobic and superoleophilic interfaces suitable for oily wastewater treatment in harsh environments. Thus, this work offers an innovative approach for designing functional wood-based MOF membranes to achieve highly efficient continuous oil-water separation.
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