ADVANCED FUNCTIONAL MATERIALS
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2015
·Vol. 25
·期 18
·2754-2762
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IF 11.805
Yujing Zuo,Jinfeng Cao,Shengyu Feng
The increasing pursuit of biocontained elastic materials led the investigation of the potential use of the monoterpene limonene in film synthesis via thiol–ene reaction. Poly[(mercaptopropyl)methylsiloxane] (PMMS) is first synthesized. By controlling the molar ratio of PMMS and functional monomers, such as polyethylene glycol allyl methyl ether or rhodamine-B, PMMS is partially functionalized while leaving spare mercapto groups that could be further used as cross-linking sites. On the basis of the functionalized PMMS, novel transparent silicone luminescent films with hydrophilic tunable properties are prepared by natural-sunlight-triggered thiol–ene “click” chemistry by using d -limonene as a cross-linker. Their structures and properties are thoroughly characterized. Transparent luminescent films are coated on commercially available UV-light emitting diode (LED) cell from solution medium followed by an in situ cross-linking step; a colorful LED cell is obtained through this facile and efficient method. The UV-LED coated by films show very intense photoluminescence under normal visible light or the light is on, and has very high coloric purity.
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JOURNAL OF BIOTECHNOLOGY
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2024
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IF 4.1
Yufeng Zhou,Xiaolong Sun,Jiahuan Hu,Yingjie Miao,Xiangyu Zi,Xi Luo,Yongqian Fu
Serving as a vital medical intermediate and an environmentally-friendly preservative, D-PLA exhibits substantial potential across various industries. In this report, the urgent need for efficient production motivated us to achieve the rational design of lactate dehydrogenase and enhance catalytic efficiency . Surprisingly, the enzymatic properties revealed that a mutant enzyme , Lr LDH T247I/D249A/F306W/A214Y ( Lr LDH-M 1 ), had a viable catalytic advantage. It demonstrated a 3.3-fold increase in specific enzyme activity and approximately a 2.08-fold improvement of K cat . Correspondingly, molecular docking analysis provided a supporting explanation for the lower K m and higher K cat /K m of the mutant enzyme. Thermostability analysis exhibited increased half-lives and the deactivation rate constants decreased at different temperatures (1.47–2.26-fold). In addition, the mutant showed excellent resistance abilities in harsh environments, particularly under acidic conditions. Then, a two-bacterium ( E. coli /pET28a- lrldh -M 1 and E. coli /pET28a- ladd ) coupled catalytic system was developed and realized a significant conversion rate (77.7%) of D-phenyllactic acid, using 10 g/L L-phenylalanine as the substrate in a two-step cascade reaction.
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JOURNAL OF MEMBRANE SCIENCE
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2024
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IF 8.4
Nan Sun,Huan Wang,Huazhang Zhao,Fangqin Cheng,Jianfeng Li
Low flux and membrane fouling are major challenges in membrane distillation (MD) for treating concentrated wastewater. This study compared the performance of GO composite membranes with different interlayer distances , by covalently bonding the terminal amine groups of ethylenediamine (EDA) and 1,12-diaminododecane (DADD) with the carboxyl groups present on the GO sheets. The results indicated that the GO-DADD/PTFE membrane, with longer carbon chain cross-linking, achieved the highest flux and antifouling properties. At 70 °C, the pure water flux reached 68.5 kg/m 2 ·h, and the fluxes for treating NaCl, HA containing NaCl, and BSA containing NaCl were 29.8 %, 37.1 %, and 38.5 % higher than the uncrosslinked GO/PTFE, and 95.7 %, 121.2 %, and 146.9 % higher than the PTFE membrane, respectively. Through mathematical models for mass and heat transfer, the study identified the key to this enhancement as the increased d-spacing within the GO layer due to cross-linking, which weakened the Kelvin effect and enhanced the vapor partial pressure on the hot side. The unique surface structure and electrostatic interactions induced by long-chain cross-linking further boosted the antifouling effect. These modifications not only overcome the typical trade-off between retention rates and flux but also offer a scalable and efficient solution for advanced membrane distillation applications.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Yahui Zhu,Xiaohua Ma,Wenjie Lai,Zengxiang Tang,Weiming Xiao,Rong Zeng,Shunmin Ding,Chao Chen
D-π conjugated coordination polymers (CCPs) are often widely used in photocatalysis and electrocatalysis due to their unique electronic conductivity and structural flexibility. However, it remains a challenge to overcome the self-degradation of d-π CCPs in thermal catalysis and to effectively utilize their excellent electron transfer properties. Here, we present a series of d-π CCPs derivative after calcination treatment. The derivatives were optimized for overall electron cloud density by constructing two-dimensional pyridinic-nitrogen (N) doped carbon carriers, which exhibited the inherent π-electron delocalization and charge transfer properties of d-π CCPs. The presence of electron transfer was confirmed by X-ray Photoelectron Spectroscopy (XPS), Raman and kinetic analysis, demonstrating that this d-π CCPs derivative possesses excellent electron conduction ability and low activation energies for the reaction. Density-functional theory (DFT) calculations further confirmed the modulation of the nickel nanoparticles (Ni NPs) electronic state by the carriers, which resulted in strong Ni NPs interactions with the high-electron-density π-bonds of the C C bond. This property significantly enhances the target adsorption and activation of the C C bond, leading to a substantial enhancement of the reaction performance. This strategy provides a new development direction for the application of d-π CCPs in thermal catalysis.
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Foods
·
2024
·Vol. 13
·期 11
·1727
·
IF 4.7
Chengyu Lu,Ziwei Chen,Yuvaraj Ravikumar,Guoyan Zhang,Xinrui Tang,Yufei Zhang,Mei Zhao,Wenjing Sun,Xianghui Qi
L-Arabinose isomerase (L-AI) has been commonly used as an efficient biocatalyst to produce D-tagatose via the isomerization of D-galactose. However, it remains a significant challenge to efficiently synthesize D-tagatose using the native (wild type) L-AI at an industrial scale. Hence, it is extremely urgent to redesign L-AI to improve its catalytic efficiency towards D-galactose, and herein a structure-based molecular modification ofLactobacillus plantarumCY6 L-AI (LpAI) was performed. Among the engineered LpAI, both F118M and F279I mutants showed an increased D-galactose isomerization activity. Particularly, the specific activity of double mutant F118M/F279I towards D-galactose was increased by 210.1% compared to that of the wild type LpAI (WT). Besides the catalytic activity, the substrate preference of F118M/F279I was also largely changed from L-arabinose to D-galactose. In the enzymatic production of D-tagatose, the yield and conversion ratio of F118M/F279I were increased by 81.2% and 79.6%, respectively, compared to that of WT. Furthermore, the D-tagatose production of whole cells expressing F118M/F279I displayed about 2-fold higher than that of WT cell. These results revealed that the designed site-directed mutagenesis is useful for improving the catalytic efficiency of LpAI towards D-galactose.
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JOURNAL OF ETHNOPHARMACOLOGY
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2024
·
IF 4.8
Hongxin Cai,Yu Zhang,Jingyu Wang,Yufeng Deng,Jiangyuan Liu,Zhiguo Wu,Dejian Cao,Zhiying Song,Lele Wang,Baogang Xie
Ethnopharmacological relevance Liuwei dihuang pills is a famous Traditional Chinese Medicine with various anti-cancer properties. Over 50 pharmaceutical manufacturers produce Liuwei dihuang pills in China and an estimated millions of people around the world orally take it every day. D-glucaro-1,4-lactone (1,4-GL) was quantified to be about 12.0 mg/g in Liuwei dihuang pills and a primary bioactive component of it inhibiting the activity of β-glucuronidase in vivo. 1,4-GL can prevent and effectively inhibit various types of cancer. However, its exact mechanism of action remains unknown. The study would justify the traditional usage of Liuwei dihuang pills against cancers. Aim of the study 1,4-GL, a bioactive ingredient derived from Liuwei dihuang pills, a famous Traditional Chinese Medicine, could delay the progression of diethylnitrosamine (DEN)-induced hepatocellular carcinoma (HCC) in rats. The mechanism underpinning the effect, however, remains poorly understood. Materials and methods Healthy and HCC rats were treated with or without 1,4-GL (40.0 mg/kg) and 1 HNMR-based metabonomic analysis was employed. 10 metabolites in uric acid pathway were quantitatively determined by UPLC-MS/MS. The expression of xanthine dehydrogenase (XDH), SLC2A9 mRNA, and SLC2A9 protein was determined using RT-qPCR and Western Blot. The effect of 1,4-GL on HCC-LM3 cells was verified in vitro. The alterations of ROS activity, SLC2A9 and XDH gene levels were observed in NCTC-1469 cells induced by lipopolysaccharide (LPS) after 1,4-GL treatment. Results After the intervention of 1,4-GL, improved pathological morphology, liver lesions in HCC rats was observed with restored serum levels of AFP, AST, ALP, γ-GGT and Fisher's ratio. Hepatic metabonomics revealed that puring metabolism were significantly regulated by 1,4-GL in HCC rats. Uric acid, xanthine and hypoxanthine levels were quantified by UPLC-MS/MS and found to be nearly restored to control levels after 1,4-GL treatment in HCC rats. Changes in xanthine oxidase activity, XDH mRNA expression, and SLC2A9 mRNA and protein expression were also reversed. 1,4-GL treatment in LM3 HCC cells were consistent with the results in vivo. Furthermore, oxidative stress indicators such as T-SOD, GSH, CAT and MDA in serum and liver were improved after HCC rats treated with 1,4-GL. In vitro, 1,4-GL was observed to reduce lipopolysaccharide-induced ROS levels in NCTC-1469 cells with enhanced mRNA and protein expression of SLC2A9 and decreased mRNA level of XDH. Conclusion The protective effects of 1,4-GL against DEN-induced HCC by reducing uric acid and ROS levels due to down-regulation of uric acid production and up-regulation of SLC2A9 expressions. 1,4-GL may represent a novel treatment that improves recovery from HCC by targeting uric acid-ROS pathway.
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MICROCHEMICAL JOURNAL
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2024
·
IF 4.9
Jun-Xi Zhou,Ting Wu,Qing-Yin Ni,Bo-Yi Yuan,Shu-Chang Zhao,Yun-Yun Sun,Jing Huang,Min-Lin Zou,Rui-Lin Liu
No reports disclosed that whether the plastic centrifuge tube with intrinsic photoenzyme activity can be used for the specific sensing of pharmaceuticals and biomarkers in biofluids so far. We herein report the plastic eppendorf (EP) tube as both reaction vessel and sunlight-activated plastic mimic enzyme for colorimetric/smartphone dual-mode detection of D-penicillamine (D-PA) and iron (Ⅲ) ions in goat and rabbit serums accordingly. The photooxidation of 3,3′,5,5′-tetramethylbenzidine (TMB) combined with simulated sunlight-activated EP tube was selectively inhibited by adding D-PA, and the absorbance at 652 nm of oxidized TMB decreased. Good linearity between the absorbance variation (or R/(R + G + B)) and D-PA level ranging from 10 to 300 µM was obtained, and the limits of detection (LOD) were determined as 8.50 μM (colorimetric) and 6.92 μM (smartphone). Furthermore, the polyvinyl alcohol hydrogel encapsulated TMB in EP tube as a smartphone biosensor had been triumphantly used to monitor D-PA level in goat serum. Interestingly, the adsorption band of photo-oxidized EP tube-TMB system inhibited by D-PA gradually increased as the enhancement of iron (Ⅲ) ions concentration. Based on the “on–off-on” effect, a sensitive and selective method was further used for selectively sensing iron (Ⅲ) in rabbit serum. Notably, the dual-mode sensing platforms exhibited outstanding detection performance, with LOD values as low as 0.50 µM and 0.65 µM respectively. In short, this work not only excavated a photoactivated-plastic mimics, but also developed a robust, low-cost, simple and sensitive biosensor for simultaneous detection of D-PA and Fe (Ⅲ) ions in biofluids. The current photoactivated sensor does not requires the introduction of exogenous catalyst except for simulated sunlight, plastic tube and chromogenic substrate.
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Computational and Structural Biotechnology Journal
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2024
·
IF 4.4
Li Luo,Tao Yan,Le Yang,Minggao Zhao
Alzheimer’s disease (AD) is an age-related neurodegenerative disorder. Transgenic and pharmacological AD models are extensively studied to understand AD mechanisms and drug discovery. However, they are time-consuming and relatively costly, which hinders the discovery of potential anti-AD therapeutics. Here, we established a new model of AD in larval zebrafish by co-treatment with aluminum chloride (AlCl 3 ) and D-galactose (D-gal) for 72 h. In particular, exposure to 150 μM AlCl 3 + 40 mg/mL D-gal, 200 μM AlCl 3 + 30 mg/mL D-gal, or 200 μM AlCl 3 + 40 mg/mL D-gal successfully induced AD-like symptoms and aging features. Co-treatment with AlCl 3 and D-gal caused significant learning and memory deficits, as well as impaired response ability and locomotor capacity in the plus-maze and light/dark test. Moreover, increased acetylcholinesterase and β-galactosidase activities, β-amyloid 1–42 deposition, reduced telomerase activity, elevated interleukin 1 beta mRNA expression, and enhanced reactive oxygen species production were also observed. In conclusion, our zebrafish model is simple, rapid, effective and affordable, incorporating key features of AD and aging, thus may become a unique and powerful tool for high-throughput screening of anti-AD compounds in vivo.
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CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Ting Zhang,Wantong Zhao,Shiyan Li,Wenguang Cui,Baojun Wang,Yuefeng Liu,Riguang Zhang,Zhongkui Zhao
Selective transfer hydrogenation coupling of nitroarenes with benzyl alcohol is one of the most reliable strategies to access functionalized imines, but challenges remain, such as the multiple and complicated operate process, low reactivity, poor selectivity results from deep hydrogenation. Constructing highly efficient catalyst is critical for this organic transformation process. Herein, we propose a unique single-atom Co-N 4 sites on N-doped carbon, with significantly upshifted d -band center, fabricated by a one-pot solid-phase carbonization strategy, which generates an excellent catalyst for one-pot selective transfer hydrogenation coupling of nitroarenes with benzyl alcohol to various functionalized imines. Experimental and theoretical investigations demonstrate the clear linear correlation among the nitrobenzene turnover number ( TON ) and d -band center over the as-prepared Co based samples, indicating the vital effect of electronic structure of Co sites on catalytic performances. Furthermore, owing to the upshifted d -band center of Co-N 4 sites, thedesorption of aniline and N -benzylideneaniline is promoted, which accelerates the spontaneous condensation coupling of aniline with benzaldehyde and inhibits the deep hydrogenation of N -benzylideneaniline. Consequently, an outstanding catalytic performance with high activity and selectivity in transfer hydrogenation coupling for imine synthesis has been realized. This work not only presents a highly efficient non-precious metal catalyst for functionalized imines production, but also illustrates the critical effect of electron structure of metallic active site on catalytic properties and opens a new avenue for fabricating diverse single-atom catalysts for selective hydrogenation reactions.
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Molecular Catalysis
·
2025
·
IF 4.9
Sixia Liu,Xiaobo Zhang,Nidu Wang,Nagimovich Karimov,Yujie Wang,Zihan Gao,Dongguang Wang,Baikang Zhu,Shuying Gao,Fu Yang
The electrochemical nitrogen reduction reaction (e-NRR) is a promising energy-efficient and low-emission alternative to the traditional Haber–Bosch process, but the sluggish kinetic and difficult activation of nitrogen impede the reaction activity. In particular, addressing the weak interaction of nitrogen with catalysts is very challenging in this field. Here, a surface oxygen vacancies tailored method was proposed to shift the d -band center of iron-based electrocatalysts to Femi energy level, by leveraging molecule self-assembly strategy to obtain Fe-base gels followed by ultrafast calcined process. The optimal electrocatalysts (Fe 3 O 4 -xGO) possess a hierarchical porous architecture (coral-like morphology), thereby endowed with outstanding structural properties (329.1 cm 2 g⁻ 1 ). Meanwhile, interfacial oxygen vacancies could be constructed during the ultrafast heat-pyrolysis process, and their concentration could be tailored with the assistance of graphene oxide (GO). Benefiting from these structure characters, the d -band center of Fe in coral-like iron oxide can be shifted to a higher energy level, which is conducive to trapping and activating the intermediate in the e-NRR process. The results of the electrocatalytic NRR test, as anticipated, indicated that Fe 3 O 4 –10GO achieved a high Faradaic efficiency of 28 % and an NH 3 production rate of 30.45 μg h⁻¹ mg cat ⁻¹ at −0.3 V vs. RHE in a 0.1 M Na 2 SO 4 , positioning it comparably to most iron-based electrocatalytic materials used in e-NRR applications. This work could provide new insight for moldering the d band center of the electrocatalyst.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Cui Zhang,Saiyu Dong,Zhaoli Liu,Nairu Liu,Xi Zhang,Jie Dong,Xueping Zhou,Yirong Guo,Jianxiang Wu
Immunochromatographic test strip (ITS) has been widely employed for point-of-care diagnoses. However, how to significantly enhance the analytical sensitivity of device-free ITS remains a challenge. Here, we synthesized a Cu single-atom anchored Co 3 O 4 (CuSA/Co 3 O 4 ) nanozyme that possesses ultrahigh peroxidase-mimicking catalytic activity owing to d -band center upshift mediated by Cu single-atom. Molecular orbital analysis demonstrated that d orbitals in CuSA/Co 3 O 4 have stronger orbital hybridization affinity than Co 3 O 4 to H 2 O 2 ′s π* orbitals. This reinforces hydroxyl radical ( OH) production and provides a stronger catalytic colorimetric signal, which is beneficial for improving the sensitivity of ITS. Moreover, we applied the CuSA/Co 3 O 4 to ITS as a signal reporter for monitoring Xanthomonas oryzae pv. oryzicola (Xoc) , the pathogen of rice bacterial leaf streak. The visual limit of detection (LOD) of the developed CuSA/Co 3 O 4 -based ITS was as low as 6.4 × 10 2 CFU mL −1 , which is 25-fold more sensitive than the traditional Au nanoparticles (AuNP)-based ITS. Taken together, this work demonstrates the great potential of CuSA/Co 3 O 4 nanocomposite as a signal reporter to improve the sensitivity of ITS for on-site Xoc detection.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Zhiliang Jin,Cheng Yang
The research in the field of photocatalysis has progressed, with the development of heterojunctions being recognized as an effective method to improve carrier separation efficiency in light-induced processes. In this particular study, CuCo 2 S 4 particles were attached to a new cubic CdS surface to create an S-scheme heterojunction, thus successfully addressing this issue. Specifically, owing to the higher conduction band and Fermi level of CuCo 2 S 4 compared to CdS, they serve as the foundation and driving force for the formation of an S-scheme heterojunction. Through in-situ X-ray photoelectron spectroscopy and electron paramagnetic resonance analysis, the direction of charge transfer in the composite photocatalyst under light exposure was determined, confirming the charge transfer mechanism of the S-scheme heterojunction. By effectively constructing the S-scheme heterojunction, the d-band center of the composite photocatalyst was adjusted, reducing the energy needed for electron filling in the anti-bonding energy band, promoting the transfer of photogenerated carriers, and ultimately enhancing the photocatalytic hydrogen production . performance. After optimization, the hydrogen evolution activity of the composite photocatalyst CdS-C/CuCo 2 S 4 -3 reached 5818.9 μmol g −1 h −1 , which is 2.6 times higher than that of cubic CdS (2272.3 μmol g −1 h −1 ) and 327.4 times higher than that of CuCo 2 S 4 (17.8 μmol g −1 h −1 ), showcasing exceptional photocatalytic activity. Electron paramagnetic resonance and in situ X-ray photoelectron spectroscopy have established a theoretical basis for designing and constructing S-scheme heterojunctions, offering a viable method for adjusting the D-band center to enhance the performance of photocatalytic hydrogen evolution.
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