GREEN CHEMISTRY
·
2021
·Vol. 23
·期 21
·8458-8467
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IF 10.182
Shanshan Xiong,Chao Luo,Zhihao Yu,Na Ji,Lingjun Zhu,Shurong Wang
The isomerization–dehydration cascade conversion on the saccharide platform is a pivotal route for biomass valorization, although it exhibits a specific reaction complexity that makes achieving an efficient conversion a highly technical challenge. The rational design of novel versatile solid acids is deemed to be the key to improving the cascade catalytic performance. In this paper, a dual-functional carbon-based solid acid catalyst (DFCSA) with tunable Brønsted/Lewis acid sites was developed for the cascade conversion of saccharides. The combined modification of H3PO4 and HNO3 on the carbon substrate contributed to the grafting of protonated moieties with a reasonably porous structure. With the aid of AlPO4, which has an orthorhombic crystal structure, the newly developed catalyst was able to achieve good performance for the subsequent hydrothermal conversion. Under optimal conditions, glucose and xylose were transformed with high product yields: 38.2 mol% levulinic acid and 69.7 mol% furfural, respectively. In addition, the catalyst displayed excellent hydrothermal stability, with only a slight degradation in activity after 10 cycles, which was ascribed mainly to the high thermal stability of AlPO4 and the firm grafting of the surface functional groups. As shown by the kinetic analysis, the DFSCA catalyst had a higher conversion rate and lower activation energy in the cascade conversion of xylose than that of glucose, leading to a better yield of furfural.
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Food & Function
·
2021
·Vol. 12
·期 20
·9912-9921
·
IF 5.396
Mohan Zhang,Shuai Chen,Yuhua Dai,Ting Duan,Yuying Xu,Xiaolin Li,Jun Yang,Xinqiang Zhu
Aspartame (ASP) and sucralose (SUC) are non-nutritive sweeteners which are widely consumed worldwide. They are considered safe for human consumption, but their effects on certain physiological aspects, such as the lifespan or health status, of the organism have not yet been studied in depth and only limited data are available in the literature. The objectives of this study were to evaluate the effects of ASP and SUC on the lifespan and health indexes using Caenorhabditis elegans (C. elegans) as a model system. Interestingly, it was shown that at the concentrations tested, ASP (0.03–3 mg mL−1) showed an increasing trend of the mean lifespan of C. elegans, with a significant increase of 27.6% compared to the control at 3 mg mL−1. Similarly, SUC (ranging from 0.03 to 10 mg mL−1) also significantly increased the mean lifespan by 20.3% and 22.3% at 0.03 and 0.3 mg mL−1, respectively. However, 10 mg mL−1 SUC had a negative effect on the lifespan, though it did not reach a statistically significant level. In addition, ASP and SUC decreased lipofuscin accumulation and transiently improved motility, indicating improved health status. Nonetheless, they had different effects on food intake and intestinal fat deposition (IFD) at different intervals of time. Taken together, our findings revealed that ASP and SUC can prolong the lifespan and improve the health status of C. elegans.
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Journal of Cleaner Production
·
2021
·
IF 9.297
Fengjiao Lai,Feng Yan,Pengju Wang,Chunyan Li,Xuehua Shen,Zuotai Zhang
The development of heterogeneously functional catalysts is of great significance in selective catalysis for biomass valorization. Herein, we report for the first time the applicability of chitin/Ag co-modified H 3 PW 12 O 40 composites (Chx-AgPW) as catalysts for producing valuable furans from carbohydrates and biomass. The as-prepared Ch15-AgPW catalyst exhibited the best catalytic performance, due to the dual Brǿnsted-Lewis acidity and appropriate chitin content. When the amount of Ch15-AgPW catalyst was 0.25 mmol, an excellent 5-hydroxymethylfurfural (HMF) yield of 78.3% could be achieved at 150 °C for 3 h with nearly 100% glucose conversion in the H 2 O/MIBK (V H2O:MIBK = 4:6) solvent system. Furthermore, high-yield HMF could also be obtained from other carbohydrates such as fructose (85.3%), sucrose (72.3%), cellobiose (65.6%), starch (52.7%) and inulin (43.5%). Additionally, corn stover , rice straw and sugarcane bagasse under typical reaction conditions simultaneously produced furfural and HMF in yields of 64.6%–72.2% and 18.5%–25.6%, respectively. Combined with the characterization, mechanism study demonstrated that the surface functional groups in chitin were conductive to rapid absorption of the substrates; the Brǿnsted acid sites from heteropoly anion (H 2 [PW 12 O 40 ] - ) promoted the initial depolymerization of biomass and the final dehydration to furans; the introduction of Ag + favored the isomerization of intermediates. After reaction finished, the Ch15-AgPW catalyst could be easily recovered by filtration and effectively reused at least eight cycles without substantial loss in catalytic activity . This work provides a novel strategy to synthesize stable heterogeneous catalysts with tunable acidity for producing bio-based fuels and chemicals from renewable resources .
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FUEL
·
2021
·
IF 6.609
Xin Yu,Lincai Peng,Jun Dai,Hui Li,Chaonan Tao,Fa Yang,Junhua Zhang
Conversion of carbohydrates at concentrated feeds represents highly desirable for the industrial deployment of biobased fuels and chemicals but challenging. One key bottleneck is that the excessive formation of polymeric humins greatly diminishes the utilization rate of feedstocks and the destination product yield. We report that the use of ethylene glycol as co-solvent for acid-catalyzed conversion of concentrated sugars enhances desirable alkyl levulinate (AL) production compared to reactions carried out in single monohydric alcohols (e.g., methanol, ethanol). Ethylene glycol served not only as a solubilizer of sugars in the reaction medium to lessen their tendency to polymerize by protecting reactive hydroxyl groups in sugars with alcohols, but also as a supporter to restrain the condensation of furan intermediates. With 10 vol% ethylene glycol as the co-solvent of ethanol, an improved yield of ethyl levulinate (EL) from 45% to 56% was accomplished from concentrated feeds of glucose (200 g/L). In particular, high space time yield and EL concentration respectively up to 30 kg/m 3 ·h and 90 g/L were obtained in a batch reactor. The solvents and catalyst could be isolated from the products, and showed good reusability. This contribution opens a reliable avenue for converting highly concentrated feeds of biomass-related sugars to oxygenated liquid fuels and versatile chemicals.
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NEW JOURNAL OF CHEMISTRY
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2021
·Vol. 45
·期 37
·17576-17583
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IF 3.591
Lijun Xu,Lu Yang,Aihua Liu
One-pot synthesis of Mn3O4 nanorods is reported for the first time by the oxidation of manganese metal resulting from reducing Mn2+ by NaBH4 at room temperature. The resultant Mn3O4 nanorods were 10–70 nm in width and up to hundreds of nanometers in length, and were very stable in aqueous solution. The Mn3O4 nanorods can oxidize H2O2 under acidic conditions quickly accompanying their decomposition. Using 3,3′,5,5′-tetramethylbenzidine (TMB) as a competitive chromogenic substance, colorimetric methods were developed for the sensitive detection of H2O2 and glucose. The methods exhibited a linear range of 2–100 μM with a limit of detection (LOD) of 1.7 μM for detecting H2O2, and a linear range of 5–200 μM with a LOD of 4.4 μM for detecting glucose. The application in analyzing glucose in human serum samples demonstrates its practicability.
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JOURNAL OF MEMBRANE SCIENCE
·
2021
·
IF 8.742
Chao Yang,Ya Li,Mengying Long,Pengfei Yang,Yafei Li,Yu Zheng,Runnan Zhang,Yanlei Su,Hong Wu,Zhongyi Jiang
Embedding nanofillers into the selective layer to creating moderate nanopores is a promising strategy to obtain high-performance nanofiltration membranes. Herein, we synthesized polyethyleneimine (PEI) functionalized graphene quantum dots (GQDs) as the water phase monomers and prepared an ultrathin desalination membrane through interfacial polymerization (IP). The in situ embedded GQDs with superiorly uniform dispersion generate abundant nanopores in the membrane, and PEI chains fill the introduced nanopores, avoiding the formation of overlarge nanopores. Besides, the PEI-grafted GQDs (NGQDs) display a reduced diffusion rate during IP, rendering an ultrathin selective layer. Benefiting from the ultrathin thickness (∼6.5 nm), the abundant water pathways (specific surface area: 6.73 m 2 /g), and the increased pore size (∼0.82 nm), the PA-NGQD 600 membrane exhibits competitive pure water permeance (38.5 L m -2 h -1 bar -1 ) and inorganic salt rejection (95.5% for Na 2 SO 4 ). The permeance exceeds those of the most desalination membranes reported so far and is ∼3 times higher than that of the reported GQD-based desalination membrane. This work provides a facile strategy for creating abundant nanopores in membranes with ultrathin thickness by interfacial polymerization.
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Biology-Basel
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2021
·Vol. 10
·期 10
·1038
·
IF 5.079
Haodong Cui,Min Jiang,Wenhua Zhou,Ming Gao,Rui He,Yifan Huang,Paul K. Chu,Xue-Feng Yu
Simple SummaryCRISPR/Cas9 system as a potential gene editing platform has been widely applied in biological engineering and disease therapies. To achieve precise gene targeting, active CRISPR/Cas9 components must be efficiently transported to targeted cells. As a simple and effective strategy, Cold Atmospheric Plasma (CAP) treatment has been demonstrated for the transmembrane delivery of various exogenous materials. In comparison with carrier-dependent delivery methods, this carrier-free platform provides a promising alternative to circumvent the obstacles of biosafety and complicated preparation processes. In this work, a CAP-based CRISPR/Cas9 carrier-free delivery platform has been established and corresponding mechanism related to efficient transportation has been explored. Briefly, the efficient production of bioactive species in culture media after CAP treatment alters cell membrane potential and permeability, which facilitates cytosolic delivery of active CRISPR/Cas9 components via passive diffusion and ATP-dependent endocytosis pathways, resulting in efficient genome editing and gene silencing. This carrier-free strategy using CAP-based transportation may also be extended to other active biomolecules in drug delivery and gene therapy.AbstractA carrier-free CRISPR/Cas9 ribonucleoprotein delivery strategy for genome editing mediated by a cold atmospheric plasma (CAP) is described. The CAP is promising in many biomedical applications due to efficient production of bioactive ionized species. The MCF-7 cancer cells after CAP exposure exhibit increased extracellular reactive oxygen and nitrogen species (RONS) and altered membrane potential and permeability. Hence, transmembrane transport of Ca2+into the cells increases and accelerates ATP hydrolysis, resulting in enhanced ATP-dependent endocytosis. Afterwards, the increased Ca2+and ATP contents promote the release of cargo into cytoplasm due to the enhanced endosomal escape. The increased membrane permeability also facilitates passive diffusion of foreign species across the membrane into the cytosol. After CAP exposure, the MCF-7 cells incubated with Cas9 ribonucleoprotein (Cas9-sgRNA complex, Cas9sg) with a size of about 15 nm show 88.9% uptake efficiency and 65.9% nuclear import efficiency via passive diffusion and ATP-dependent endocytosis pathways. The efficient transportation of active Cas9sg after the CAP treatment leads to 21.7% and 30.2% indel efficiencies in HEK293T and MCF-7 cells, respectively. This CAP-mediated transportation process provides a simple and robust alternative for the delivery of active CRISPR/Cas9 ribonucleoprotein. Additionally, the technique can be extended to other macro-biomolecules and nanomaterials to cater to different biomedical applications.Keywords:cold atmospheric plasma;CRISPR/Cas9;carrier-free transport;genome editing
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高影响因子
JOURNAL OF DENTISTRY
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2021
·
IF 4.379
Rui Guo,Wenan Peng,Hongye Yang,Chenmin Yao,Jian Yu,Cui Huang
Objectives This paper aimed to evaluate the influence of resveratrol-doped adhesive on the durability and antibiofilm capability of dentin bonding . Methods Experimental adhesives were prepared by incorporating resveratrol into a universal adhesive at concentrations of 0 (control), 0.1, 1, and 10 mg/mL. The microtensile bond strength, fracture modes, and adhesive–dentin interface nanoleakage were assessed after 24 h of water storage, 10,000 times of thermocycling or 1-month of collagenase ageing. Relevant antibiofilm capability on Streptococcus mutans ( S. mutans ), in situ zymography , degree of conversion, and cytotoxicity of resveratrol-doped adhesives were also determined. Results Irrespective of thermocycled or collagenase ageing, the resveratrol-doped adhesive (1 mg/mL) maintained the bond strength and reduced the nanoleakage expression. Meanwhile, the inhibitory ability on endogenous protease activity and S. mutans biofilm formation with acceptable biocompatibility were obtained. Conclusions This study suggested that the resveratrol-doped adhesive achieved effective improvement on dentin bond durability and secondary caries management. Clinical significance The application of the resveratrol-doped adhesive indicates promising benefits to increase the lifetime of composite restorations.
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MICROCHIMICA ACTA
·
2019
·Vol. 186
·期 12
·1-10
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IF 5.479
Gan Xiaorong,Zhao Huimin,Schirhagl Romana,Quan Xie
A non-enzymatic fluorometric assay is described for the determination of glucose. The method is based on the use of g-C 3 N 4 quantum dots (QDs) that have good water solubility. The QDs were synthesized by a one-step solvothermal process using formamide as precursor. The QDs possess an average size of ~5 nm, a band gap of 3.0~3.5 eV, and strong blue fluorescence (with excitation/emission maxima at 400/447 nm). Fluorescence is quenched by glucose (which acts as the electron acceptor) via an electron transfer mechanism. Comprehensive spectroscopy and density functional theory calculations show that the selectivity of the fluorescent probe can be attributed to the presence of N-H bonds that are formed between the QDs (mainly at plane edges) and glucose. The interaction forces lead to the formation of localized states for capturing hot electrons. This results in a decrease in the band gap and a reduction in fluorescence intensity. The probe is selective over some typical interfering species (such as cysteine and albumin) which often are present in the urine of diabetics. The method has a linear response in the 0.2 to 5.0 mM glucose concentration range and a 0.2 mM detection limit.
Schematic representation of the synthesis of g-C 3 N 4 quantum dots (QDs) as a fluorescent nanoprobe for selective detection of glucose.
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CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Xue Zhong,Huan Xia,Wenquan Huang,Zhixian Li,Yanbin Jiang
The combination of chemo- and enzyme catalysis for multi-step tandem reactions has presented great challenges for decades. Herein, glucose oxidase (GOx) and a metal-organic framework MOF-545(Fe), which possessed peroxidase-like activity, were combined to construct a mimic multi-enzyme system for tandem catalysis. MOF-545(Fe) not only served as a support for the enzyme immobilization, but also contributed its catalytic activity to co-operate with natural enzymes for the cascade reactions. Based on the prepared mimic multi-enzyme system GOx@MOF-545(Fe), a colorimetric biosensor for glucose rapid detection was achieved with a low limit of detection (0.28 μM) and high specificity. Meanwhile, due to the protection of MOF-545(Fe), the immobilized enzyme exhibited excellent reusability and stability, e.g. long-term stability, thermal stability and anti-organic solvent stability. After being stored at room temperature for 7 days, the immobilized enzyme retained 92% of activity, while only 40% of activity of free enzyme was retained. And the immobilized enzyme maintained 71% of its initial activity after 5 cycles. This strategy of combining MOF mimics and natural enzymes for tandem catalysis may provide a novel and facile approach to design a highly efficient, stable, functional chemo-enzyme composites catalyst, which holds great promise for applications in biosensing, biopharmaceutical and industrial catalysis.
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AGRONOMY JOURNAL
·
2019
·Vol. 111
·期 5
·2341-2349
·
IF 1.805
Jing Li,Yin Min Htwe,Yong Wang,Yaodong Yang,Yi Wu,Dongxia Li,Abdul Kareem,Rencai Wang
Haustorium absorbs energy from the endosperms (liquid and solid) and plays a key role in nutrient mobilization during coconut germination and seedling growth. This study was conducted to shed light on possible interactions between haustorium and endosperms during this process. Germination rates and morphological changes of coconut cultivars Hainan Tall (HT) and Red Dwarf (RD), as well as the profiles of sugars and fatty acids in endosperms and haustorium were also analyzed. Results showed that liquid and solid endosperm inside the coconut exhausts successively, while haustorium occupies the nut gradually. Haustorium had significant positive correlation with seedling, while it had significant negative correlation with liquid and solid endosperms. Sugars in liquid endosperm continuously decreased, whereas in solid endosperm and haustorium accumulated at early stages and decreased later along with the aggressive seedling growth. Fatty acids in solid endosperm shared a very similar trend with sugars. In conclusion, haustorium development and seedling growth mainly depend on the nutrients stored in the liquid endosperm at early stages and then depend on the solid endosperm, in which fatty acids degrade rapidly to sugar so as to provide enough energy. These findings could be applicable in coconut germination and seedling propagation. Core Ideas Relative cool season (25–29°C) is more suitable for coconut germination and local variety (HT) is more adaptable. Development mainly depends on stored nutrients in liquid endosperm at early stages and then on solid endosperm. Fatty acids in solid endosperm degrade rapidly to sugars since liquid endosperm almost exhausted. Conversion of fatty acids to sugars helps provide enough energy for rapidly growing haustorium and seedling.
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ENERGY & FUELS
·
2019
·
IF 3.021
Yuan Zhao,Kaifeng Lu,Hao Xu,Yang Qu,Lingjun Zhu,Shurong Wang
5-Hydroxymethylfurfural (HMF), a well-known value-added platform chemical, can be produced by biomass dehydration for the synthesis of bio-based liquid fuels. In this study, several kinds of saccharides that are widely available from biomass resources, namely, sucrose, maltose, cellobiose, lactose, inulin, and cellulose, were selected as feedstocks. A sulfonated ionic liquid catalyst was employed for the production of HMF from the selected saccharides in a renewable butanone–water solvent mixture. The yields of primary dehydration products versus time on stream from the saccharides were comparatively studied, and the distribution of the liquid-phase product was also analyzed. Results showed that the proposed reaction system could achieve fast conversion of disaccharides and polysaccharides with high selectivity toward HMF. Complete conversion of disaccharide and up to 65.1% yield of HMF were achieved within 1 min. Sucrose and inulin, which are rich in the fructose unit, showed the highest HMF selectivity. The next were maltose, cellobiose, and cellulose, which mainly consist of the glucose unit. They produced more oxygenated aliphatics than sucrose and inulin via side reactions. Lactose had the lowest HMF selectivity and tended to be converted into furan byproducts during the dehydration process.
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