BIOCHEMICAL ENGINEERING JOURNAL
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2023
·
IF 3.9
Siyuan Chang,Bingfeng Li,Tianyi Chen,Leilei Zhang,Yaru Li,Xuejun He,Sen Zhang,Xin Pan
The catalytic transformation of biomass-derived 5-hydroxymethylfurfural (HMF) into value-added chemicals and biofuels has received considerable interest. Previously, we demonstrated that Pseudomonas aeruginosa PC-1 could be used for selective 900 mM HMF oxidation into 5-hydroxymethyl-2-furancarboxylic acid (HMFCA) with over 90% yield. Here, we aimed to mine the potential aldehyde dehydrogenases (ALDHs) for HMF biocatalysis and improved the catalytic activity and tolerance through protein engineering. ALDHs were heterologously expressed in E. coli BL21 (DE3) and subsequently the most efficient HMF oxidation conditions of E. coli /pET -PaALDH70140 were identified. Based on the structural analysis of PaALDH70140 with the HMF and NAD + complexes, the engineering hotspots in the active site architecture were identified and subjected to saturation mutagenesis . The mutant L172R displayed 175% higher HMF catalytic efficiency than PaALDH70140, and the mutant also showed improved HMF-tolerance. Kinetic parameters suggested that L172R had higher HMF affinity and catalytic efficiency, indicating a higher HMF conversion efficiency than the wild-type. Molecular docking revealed that the mutation introduced new hydrogen bonds between the enzyme and HMF, which fixed the spatial position of HMF and shortened the reaction time of the catalysis, thus enhancing the catalytic efficiency of HMF. In the fed-batch process, E. coli /pET -PaALDH70140 - L172R exhibited a 166% increase in the yield of HMFCA within 22 h, proving its potential for HMF bioconversion applications.
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EXPERIMENTAL CELL RESEARCH
·
2023
·
IF 3.7
Zijun Guo,Lin Guo
Gastric cancer (GC) is the 5th most common cancer over the world. Ubiquitin protease 43 (UBP43) is a multifunctional protein with deubiquitinase activities. Abnormal expression of UBP43 has been reported in numerous types of malignancies. Bioinformatic analysis was performed to identify the differentially expressed genes (Fold change ≥2 or ≤ −2 and p < 0.01) in GC from the datasets downloaded from Gene Expression Omnibus and Gene Expression Profiling Interactive Analysis databases, which showed that UBP43 and stress-inducible phosphoprotein 1 (STIP1) were up-regulated in both datasets. Online databases displayed the binding of UBP43 to STIP1 and the positive correlation between the two proteins. This study aims to explore: the role of UBP43 in cell proliferation and apoptosis in GC; the relationship between UBP43 and STIP1; and whether UBP43 exerts its function via STIP1 in GC. Knockdown/overexpression stable GC cell lines were generated by transducing lentivirus carrying coding sequence/short hairpin RNA of UBP43 and puromycin selection. GC patients with higher expressions of UBP43 had poor prognosis. Loss-/gain-of-function experiments revealed that pro-proliferative and anti-apoptotic abilities of UBP43 in GC cells and xenografts. UBP43 could interact with STIP1, inhibit its ubiquitination, and promote its protein stability, thereby enhancing STIP1 expression. Moreover, STIP1 knockdown reversed the pro-proliferative ability of UBP43 in GC cells. Our study uncovers that the pro-proliferative role of UBP43 in GC development is STIP1-dependent and indicates that UBP43 may act as a potent therapeutic target in GC treatment.
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LANGMUIR
·
2023
·
IF 3.9
Yu Zhang,Lu Wang,Ning Ma,Yizhen Wan,Xueyi Zhu,Weiping Qian
Nonspecific adsorption (NSA) seems to be an impregnable obstacle to the progress of the biomedical, diagnostic, microelectronic, and material fields. The reaction path of bioconjugation can alter the surface charge distribution on products and the interaction of bioconjugates, an ignored factor causing NSA. We monitored exacerbated NSA introduced by a 1-ethyl-3-(3-(dimethylamino)propyl) carbodiimide (EDC) addition reaction, which cannot be resistant to bovine serum albumin (BSA) or polyethylene glycol (PEG) antifouling coating and Tween-20. And the negative effects can be minimized by adding as low as 7.5 × 10–6 M N-hydroxysulfosuccinimide (sulfo-NHS). We applied ordered porous layer interferometry (OPLI) to sensitively evaluate the NSA that is difficult to measure on individual particles. Using the silica colloidal crystal (SCC) film with Fabry–Perot fringes as in situ and real-time monitoring for the NSA, we optimized the surface chemistry to yield a conjugate surface without variational charge distribution. In this work, we propose a novel approach from the perspective of the reaction pathway to minimize the NSA of solely EDC-induced chemistry.
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Journal of Materials Chemistry C
·
2023
·Vol. 11
·期 35
·11865-11875
·
IF 6.4
Xiandi Yu,Yuchi Zhang,Le Han,Yan Xu
All-inorganic CsPbBr3 perovskite quantum dots (PQDs) show superior photophysical properties and great potential in various optoelectronic devices, but their low lattice formation energy and high delocalization of surface ions make them susceptible to ambient conditions. In this work, the hierarchical silicalite-1 zeolite co-templated by carbon nanotubes (CNTs) and tetrapropylammonium hydroxide (TPAOH) was applied to encapsulate CsPbBr3 PQDs. Particularly, distinct nanosized CNTs, mass ratios of zeolite to CsPbBr3, and thermal diffusion temperature were systematically studied to optimize the loading capacity and luminescence efficiency of CsPbBr3 PQDs. Consequently, the micro-/mesoporous silicalite-1 confined CsPbBr3 PQD nanocomposite obtained at 700 °C exhibited the best luminescence performance with a full-width at half-maximum (FWHM) of 25 nm, a high PLQY of ∼61.9% and an ultrahigh stability of >100 days in H2O. The CsPbBr3/silicalite-1 nanocomposite shows dual-mode temperature monitoring performance in terms of fluorescence emission intensity and spectral shift, rendering it a promising candidate for credible optical thermometry. Latent fingerprint identification and selective Fe3+ fluorescence sensing applicability of the CsPbBr3/silicalite-1 nanocomposite were then developed. Also, a reversible off/on switching of the green fingerprint image under UV-light irradiation can be easily modulated by spraying Fe3+ aqueous solution and pure H2O, respectively, achieving an effective anti-counterfeiting application.
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JOURNAL OF APPLIED PHYCOLOGY
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2023
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IF 3.3
Tang Tiancheng,Li Chen,Zhu Benwei,Yao Zhong
Ulvan lyase is a useful tool which can degrade ulvan into oligosaccharides with a range of biological activities. In this study, the ulvan lyase ULA-3 from Alteromonas sp. 76–1, which was a 1467-bp encoded 489-amino acid residue protein, has been cloned, heterologously expressed and biochemically characterized. ULA-3 showed the maximum activity at 45 ˚C and pH 9.0. The K m is 1.879 mg mL −1 and V max is 2.597 µmol min −1 mL −1 . Its enzyme activity was outstanding at 11.754 U mg −1 . Moreover, its metal ion stability is exceptionally good and most metal ions at a concentration of 1 mM have no inhibitory effect on its activity. It can endolytically degrade ulvan into oligosaccharides with a degree of polymerization (Dp) of 2–4 and with unsaturated double bond through the β -elimination reaction, which mainly cleaves the glycosidic bond between rhamnose and uronic acids. All in all, our study has increased the ulvan lyase database and offers the opportunity to fully utilize ulvan, a green biomass resource from marine algae.
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Frontiers in Microbiology
·
2022
·
IF 6.064
Zheng Fengzhen,Basit Abdul,Zhuang Huan,Chen Jun,Zhang Jianfen,Chen Weiqing
Acidophilic β-xylanases have attracted considerable attention due to their excellent activity under extreme acidic environments and potential industrial utilizations. In this study, a novel β-xylanase gene (Xyl11) of glycoside hydrolase family 11, was cloned from Trichoderma asperellum ND-1 and efficiently expressed in Pichia pastoris (a 2.0-fold increase). Xyl11 displayed a maximum activity of 121.99 U/ml at pH 3.0 and 50°C, and exhibited strict substrate specificity toward beechwood xylan (Km = 9.06 mg/ml, Vmax = 608.65 μmol/min/mg). The Xyl11 retained over 80% activity at pH 2.0–5.0 after pretreatment at 4°C for 1 h. Analysis of the hydrolytic pattern revealed that Xyl11 could rapidly convert xylan to xylobiose via hydrolysis activity as well as transglycosylation. Moreover, the results of site-directed mutagenesis suggested that the Xyl11 residues, Glu127, Glu164, and Glu216, are essential catalytic sites, with Asp138 having an auxiliary function. Additionally, a high degree of synergy (15.02) was observed when Xyl11 was used in association with commercial β-xylosidase. This study provided a novel acidophilic β-xylanase that exhibits excellent characteristics and can, therefore, be considered a suitable candidate for extensive applications, especially in food and animal feed industries.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
·
IF 9.965
Guoqing An,Chang'an Wang,Hongyi Gao,Ge Wang,Yibin Luo,Zhiyuan Liu,Changjiu Xia,Siqi Liu,Xinxin Peng,Zhixiang Cheng,Xingtian Shu
Titanosilicate-1 zeolites (TS-1) as one of the most commonly used catalysts for alkene epoxidation , construction of hierarchical pores as well as elimination of anatase to promote mass transportation and avoid invalid decomposition of hydrogen peroxide are always desirable yet challenging goals. Here, a novel and unique Ti-based metal organic frameworks (MOFs)-induced synthetic strategy for fabricating anatase-free hierarchical TS-1 was first proposed. All the components of MOFs perform different functions: the uniformly distributed Ti nodes replace conventional tetrabutyl titanate (TBOT) to serve as sole Ti source for constructing zeolite crystal; the separated ligands can be embedded in the zeolite framework and act as template to in situ build hierarchical pore structure ; the coordination interaction between Ti nodes and ligands can efficiently avoid the anatase generation by balancing the forming rates of Ti-OH and Si-OH. This synthetic strategy is of general applicability, and two different synthetic routes including traditional hydrothermal process and steam assisted crystallization (SAC) procedure are successfully adopted. The obtained hydrothermal TS-1 and SAC anatase-free samples all possess abundant intercrystalline mesopores of 20–50 nm and even macropores between 50 and 150 nm, improving the conversion over 25 % for 1‑hexene epoxidation than TS-1 sample prepared by conventional route. The influences of the amount of Ti MOFs precursor and the crystallization process are studied in detail, and possible synthesis mechanisms are proposed. This MOFs-induced strategy might open up an avenue for the rational design of ideal and hierarchical zeolite to boost the catalytic efficiency.
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JOURNAL OF HAZARDOUS MATERIALS
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2022
·
IF 14.224
Xingxing Peng,Tianyu Li,Qihang Zheng,Yingyuan Lu,Yuzhe He,Yetao Tang,Rongliang Qiu
Hexabromocyclododecane (HBCD) is a typical persistent organic pollutant that is widely detected in the environment. Despite the significant efforts put into its mineralisation , there is still a lack of microorganism resources that can completely mineralise HBCD. Stable isotope analysis revealed that the Citrobacter sp . Y3 can use [ 13 C]HBCD as its sole carbon source and degrade or even mineralise it into 13 CO 2 , with a maximum conversion rate of 100% in approximately 14 days. Strain Y3 could completely mineralise HBCD, which it used as its only carbon source, and six debromination enzymes related to HBCD degradation were found in Y3, including haloalkane dehalogenase (DhaA), haloacid dehalogenase (HAD), etc. A functional gene named HBCD-hd-1 , encoding a HAD, was found to be upregulated during HBCD degradation and heterologously expressed in Escherichia coli . Recombinant E. coli with the HBCD-hd-1 gene transformed the typical intermediate 4-bromobutyric acid to 4-hydroxybutanoic acid and showed excellent degradation performance on HBCD, accompanied by nearly 100% bromine (Br) ion generation. The expression of HBCD-hd-1 in Y3 rapidly accelerated the biodegradation of HBCD. With HBCD as its sole carbon source, strain Y3 could potentially degrade HBCD, especially in a low-nutrient environment.
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APPLIED ORGANOMETALLIC CHEMISTRY
·
2022
·Vol. 37
·期 1
·e6935
·
IF 4.072
Yanyun Wang,Jiehua Bao,Changjiang Zuo,Guomeng Dong,Xiaoli Sheng,Yuzhong Huang,Yiwei Zhang,Yuming Zhou
Exploration of levulinic acid (LA) hydrogenation to γ-valerolactone (GVL) contributes to the conversion from carbohydrates to valuable fuels and chemicals. Here, we obtained a series of ultra-small PtNix bimetallic composite catalysts encapsulated in silicalite-1 zeolite (S-1) via a one-pot synthesis strategy protected by tetra(p-carboxyphenyl)porphyrin (TCPP) ligands. The catalytic results showed that PtNi 3 @S-1 (TCPP) exhibited the most active catalytic performance (95.7% LA conversion and 93.8% GVL selectivity) under optimized conditions. The characterization results indicate that ligand modification and bimetallic synergy play an important role in enhancing the catalytic activity. The introduction of TCPP provides a guarantee for the homogeneous encapsulation of PtNi 3 in S-1 zeolite at sub-nanometer size. The electronic interaction of PtNi bimetallic, high dispersibility of active components, improved surface acidity and excellent stability co-contribute to the satisfactory hydrogenation activity.
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POLYMER
·
2022
·
IF 4.432
Jian Xu,Junhao Fei,Tao Tang,Meng Ma,Yanqin Shi,Huiwen He,Si Chen,Xu Wang
In this paper, a bio-based flame retardant PA-AR is synthesized, which endows PLA with good flame retardant and crystallization properties, and at the same time promotes the biodegradability of PLA. Only 1 wt% PA-AR makes the LOI value of PLA reach 26.8% and reaches UL-94 V-0 level. In addition, 1 wt% PA-AR increases the crystallinity of PLA to 23.4%, which increased by 460% compared with PLA. Further, due to the increase of crystallinity, the tensile strength is also improved. Besides, the addition of PA-AR can greatly promote the degradation performance of PLA under specific biological conditions. This work proposed a novel method to obtain completely biodegradable flame retardant composites.
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Advanced Science
·
2022
·Vol. 9
·期 27
·2202744
·
IF 17.521
Songtao Dong,Yuan Zhang,Xiangnan Guo,Chuang Zhang,Zhaomeng Wang,Jiang Yu,Yubo Liu,Chang Li,Yuting Hu,Bingjun Sun,Mengchi Sun,Haotian Zhang,Defang Ouyang,Zhonggui He,Yongjun Wang
Spatiotemporal delivery of nanoparticles (NPs) at the “cellular level” is critical for nanomedicine, which is expected to deliver as much cytotoxic drug into cancer cells as possible when NPs accumulate in tumors. However, macrophages and cancer-associated fibroblasts (CAFs) that are present within tumors limit the efficiency of spatiotemporal delivery. To overcome this limitation, glutathion pulse therapy is designed to promote reduction-sensitive Larotaxel (LTX) prodrug NPs to escape the phagocytosis of macrophages and penetrate through the stromal barrier established by CAFs in the murine triple negative breast cancer model. This therapy improves the penetration of NPs in tumor tissues as well as the accumulation of LTX in cancer cells, and remodels the immunosuppressive microenvironment to synergize PD-1 blockade therapy. More importantly, a method is established that can directly observe the biodistribution of NPs between different cells in vivo to accurately quantify the target drugs accumulated in these cells, thereby advancing the spatiotemporal delivery research of NPs at the “cellular level.”
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JOURNAL OF CHEMICAL SCIENCES
·
2022
·Vol. 134
·期 3
·1-11
·
IF 2.15
LIU XIAOJUAN,LI MINGMING,YANG SHUMING,YANG YAYA,NIE JIANG,XUE YUBING,OUYANG YINGGEN,XIAO SONGTAO
The increasing demand for neodymium (III) and samarium (III) due to their extensive high-tech applications has drawn much attention to their recovery. In this work, the copper-based metal-organic framework HKUST-1 was prepared and used for the adsorption of neodymium (III) and samarium (III) in the media of an aqueous solution. The maximum adsorption capacity of the material for neodymium (III) and samarium (III) was 284.11 and 503.45 mg g −1 at a pH of 5.5, respectively. The adsorption removal rate could achieve nearly 100% at the solid-to-liquid ratio of 1.0 g L −1 , which is relatively excellent among such adsorbents used for rare earth elements uptake. The mechanism and reversibility of neodymium (III) and samarium (III) adsorption were systematically investigated by X-ray diffraction, Fourier transforms infrared spectroscopy, Raman spectra, and X-ray photoelectron spectroscopy, suggesting that the mechanism for the adsorption was ion exchange and complexation between trivalent rare-earth ions and the oxygen atom in the hydroxyl group. The reason behind the material displaying a more robust affinity for samarium (III) may be caused by the energy difference between f n and f n+1 states of samarium (III) was larger than that of neodymium (III), thus forming stronger covalent bonding. Graphical abstract HKUST-1 exhibited high adsorption capacity towards Nd (III) and Sm (III). The reason behind the material displaying a more robust affinity for Sm(III) was caused by that the energy difference between f n and f n+1 states of Sm(III) was larger than that of Nd(III), thus forming stronger covalent bonding.
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