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FOOD CHEMISTRY · 2021 · IF 7.514

Selective uptake determines the variation in degradation of organophosphorus pesticides by Lactobacillus plantarum

Shaofeng Yuan,Changjian Li,Hang Yu,Yunfei Xie,Yahui Guo,Weirong Yao

Organophosphorus pesticides (OPPs) are widely used worldwide, leading to varying degrees of residues in food. Lactic acid bacteria (LAB) can degrade OPPs by producing phosphatase. This study explored the reasons for the variation in the degradation of different OPPs by Lactobacillus plantarum . The results showed that the degradation effects of OPPs by L. plantarum (intact cells) varied greatly, the degradation rate constant of phoxim was 1.65-fold higher than that of dichlorvos. However, the phosphatase extracted from L. plantarum had no degradation selectivity for OPPs in vitro . It was speculated that the selective uptake of cells determines this degradation selectivity. The results of molecular docking supported this hypothesis because there was no difference in the binding energies between phosphatase and OPPs, while the binding energies between phosphate-binding protein and pesticides were different, and they were negatively correlated with the degradation rate constants of the eight OPPs by L. plantarum .

研究领域: 微生物学 · 食品安全 · 环境科学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2023 · IF 8.6

Pillar-layered metal-organic frameworks with benchmark C2H2/C2H4 and C2H6/C2H4 selectivity for one-step C2H4 production

Hua Shuai,Junhui Liu,Yesong Teng,Xing Liu,Lingmin Wang,Hanting Xiong,Pengxiang Wang,Jingwen Chen,Shixia Chen,Zhenyu Zhou,Shuguang Deng,Jun Wang

Energy-efficient adsorptive separation shows great potential for the one-step production of high-purity ethylene (C 2 H 4 ) from ternary C 2 hydrocarbons. However, it remains a formidable challenge to fabricate high-performance adsorbents that exhibit simultaneous high selectivity (>2) towards acetylene/ethylene (C 2 H 2 /C 2 H 4 ) and ethane/ethylene (C 2 H 6 /C 2 H 4 ). Herein, we report a pillar-layered metal–organic framework, Ni(sdba)(dabco) 0.5 (H 2 sdba = 4,4′-sulfonyldibenzoic acid; dabco = 1,4-diazabicyclo [2.2.2] octane), for preferential trapping of C 2 H 6 and C 2 H 2 over C 2 H 4 . The abundant accessible binding sites endow Ni(sdba)(dabco) 0.5 with outstanding C 2 H 2 /C 2 H 4 (2.28) and C 2 H 6 /C 2 H 4 (2.47) selectivity with high C 2 H 6 (3.15 mmol g −1 ) and C 2 H 2 (4.41 mmol g −1 ) uptake among porous materials reported for one-step C 2 H 4 purification. Dynamic breakthrough experiments demonstrated the feasibility of producing high-purity C 2 H 4 (>99.9%) from C 2 H 2 /C 2 H 6 /C 2 H 4 gas-mixtures (1/1/1 and 1/9/90, v/v/v ) in a single step. Computational simulations reveal that the aromatic-rich pore spaces, which decorated with accessible interlayer uncoordinated oxygen atoms of sulfonyl groups and alkyl functionalities, can provide multiple C-H···O, C-H···π, and C-H···H interactions for selectively recognizing C 2 H 6 and C 2 H 2 over C 2 H 4 .

研究领域: 材料科学 · 化学工程
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ChemPlusChem · 2023 ·Vol. 88 ·期 6 ·e202300138 · IF 3.4

Near-IR Fluorescent Recognition of Arginine: High Chemoselectivity and Enantioselectivity Promoted by La3+

Hongyu Guo,Jiaqiao Yang,Jian Zeng,Xiaoqi Yu,Shanshan Yu,Lin Pu

Graphical The first near IR fluorescent probe for the chemoselective and enantioselective recognition of arginine in aqueous solution is reported in this work. This probe also allows visual discrimination of the arginine enantiomers because of its fast and distinct color change upon interaction with the substrate. The first near IR fluorescent probe for the chemoselective and enantioselective recognition of arginine in aqueous solution is reported in this work. This probe, made of a 1,1’-binaphthyl-based chiral aldehyde unit and a rhodamine-based near IR chromophore, in combination with La 3+ exhibits highly chemoselective as well as enantioselective fluorescent enhancement with arginine at λ=764 nm upon excitation at λ=690 nm. Little or no fluorescent response is observed toward the chirality miss-matched arginine enantiomer or other common amino acids and their enantiomers. This probe also allows visual discrimination of the arginine enantiomers because of its fast and distinct color change upon interaction with the substrate.

研究领域: 生物化学 · 分析化学
✓ 已验证 DOI PubMed 高影响因子
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JOURNAL OF MEMBRANE SCIENCE · 2019 · IF 7.015

Zwitterion structure membrane provides high monovalent/divalent cation electrodialysis selectivity: Investigating the effect of functional groups and operating parameters

Muhammad Irfan,Tingting Xu,Liang Ge,Yaoming Wang,Tongwen Xu

Monovalent cation perm-selective membranes (MCPMs) with enhanced monovalent flux and the capability to reject multivalent cations are critical; however, their realization remains challenging in various industrial applications, such as seawater desalination and wastewater purification. To achieve this criterion, we designed and synthesized a series of MCPMs with a zwitterion structure comprising three quaternary ammonium groups, two carboxylic acids, and one sulfonic acid group. These functional groups act to balance the cation flux and perm-selectivity of the MCPM. The cation fluxes and perm-selectivity of the fabricated MCPMs were investigated for Na + /Mg 2+ and Li + /Mg 2+ systems. High perm-selectivities of 58.4 and 16.5 were obtained for ( P M g 2 + N a + ) and ( P M g 2 + L i + ) systems, respectively, using a QPO/DAN-SA-5 membrane. The performance of the MCPMs was compared with the state-of-art commercial monovalent cation selective membrane Neosepta TM CIMS. The influence of feed concentration and current density on the cation fluxes and perm-selectivity was examined, and the pH was measured to investigate the effect of concentration polarization and water splitting on electrodialysis . Moreover, the presence of various functional groups in the membrane matrix provided additional insights into electrostatic repulsive and interaction effects. The zwitterion structure of the MCPM was capable of tuning the cation flux and perm-selectivity. Our study provides an effective strategy for developing MCPMs with high cation flux and ion perm-selectivity.

研究领域: 材料科学 · 环境工程 · 化学工程
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JOURNAL OF MEMBRANE SCIENCE · 2019 · IF 7.015

Nanostructured switchable pH-responsive membranes prepared via spherical polyelectrolyte brushes

Rui Zhang,Tianxu Zhou,Hongwei Peng,Min Li,Xuedong Zhu,Yuan Yao

A nano-porous and switchable pH-responsive polymeric membrane was fabricated through filtration technique with the assist of metal hydroxide nanostrands as template. A common used spherical polyelectrolyte brush (SPB), PAA@PS (poly (acrylic acid)) brushes grafted on polystyrene nanospheres , employed in this work as polymeric membrane. It features tunable pore size on line by shrinkage or stretching of PAA brushes under different pH value or ionic strength . Furthermore, both the length of PAA chains and the dimension of PS cores could tailor the pore size of the membrane effectively. These properties of PAA@PS membrane could separate nanoparticles within 10 nm with precise size-selective permeation. Meanwhile, since the membrane was endowed negative charge by PAA brushes, the membrane could adsorb and separate positive charge nanoparticles including dyes though the mixture solution effectively. Herein, this stimuli-responsive membrane is promising in the separation of ultrafine nanoparticles with precise size and charge selectivity.

研究领域: 材料科学 · 化学工程 · 生物分离技术
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HIGH PERFORMANCE POLYMERS · 2025 · IF 1.6

Bifunctionalized NH2-UiO-66-CF3 mixed matrix membranes for gas separation

Zhiqing Liang,Zhongying Liu,Xiuyuan Wei,Hui Wu,Chanjuan Liu,Xiaohua Huang

Bifunctionalized NH2-UiO-66-CF3 nanofillers were successfully prepared by grafting - CF3 on NH2-UiO-66 via aldehyde-amine condensation reaction and applied to the preparation of 6FDA-ODA/NH2-UiO-66-CF3 mixed matrix membranes (MMMs). The successful introduction of -NH2 and -CF3 groups was verified by FT-IR, XRD, and XPS characterization, and the integrity of the crystal structure was ensured. Due to the presence of hydrogen bonding, NH2-UiO-66-CF3 showed good interfacial compatibility with the polymer matrix. Due to the introduction of the - CF3 group, the MMMs exhibited excellent thermal stability (T10% > 500°C, Tg = 300°C–305°C), hydrophobicity (contact angle of 92.96–97.71), and mechanical properties (tensile strength of 74–85 MPa). The gas separation performance tests showed that the MMMs exhibited significantly improved gas permeability and selectivity compared to the pure 6FDA-ODA membranes, which was attributed to the fact that the -NH2 and -CF3 groups provided more adsorption sites for gases. In particular, the PI/NUF(10) MMMs showed the best performance, with permeabilities of 42.71, 9.22, and 92.79 Barrer for CO2, O2, and He, respectively, which were 248%, 213%, and 173% higher than those of the pure membranes. Meanwhile, the selectivities of CO2/N2, O2/N2 and He/N2 were improved by 37%, 24%, and 8%, respectively. Close to the Robeson upper limit, demonstrating excellent gas separation potential.

研究领域: 材料科学 · 化学工程 · 膜技术 · 气体分离 · 纳米技术
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DESALINATION · 2025 · IF 9.8

Piperazine concentration-driven effect fabricated NF membrane with ambidextrous selectivity for SO42−/cl− and Mg2+/Na+: Mechanism and efficient water purification

Hailin Chang,Shilei Fu,Ziao Zhang,Yating Hu,Zijian Cui,Jun Ma,Kexin Hou,Xiaobin Tang,Guibai Li,Heng Liang

Nanofiltration (NF) membranes with efficient selectivity are critical for addressing water source pollution from toxic heavy metals and emerging micropollutants. Herein, we engineered a polyamide (PA) NF membrane with ambidextrous selectivity by leveraging the concentration-driven effect of piperazine (PIP) during interfacial polymerization (IP). This PIP concentration-driven effect was verified by modulating the PIP concentration gradient from low to high, which enhanced IP efficiency via both an intensified alkaline reaction environment and concentration-driven diffusion. The optimized NF membrane features an ultrafine pore size distribution and reduced electronegativity, exhibiting a remarkable shift from sole SO 4 2− /Cl − selectivity to impressive ambidextrous selectivity, encompassing both SO 4 2− /Cl − (α ≈ 48, 98.3 % for Na 2 SO 4 ) and Mg 2+ /Na + (α ≈ 37, 98.2 % for MgCl 2 ). Moreover, it membrane also achieved exceptional removal efficiencies of 94.8–98.9 % for heavy metals and 77.6–99.3 % for antibiotics, while maintaining a water permeability of 19.3 L/m 2  h bar and mitigating the perm-selectivity trade-off. When purifying surface water containing heavy metals and antibiotics, the optimized NF membrane exhibited superior multi-pollutant removal and improved water production quality compared to the NF270 and NF90 membranes, and especially with its water permeance increased by ~27 % to 179 %. Our work uncovers a fundamental correlation between the PIP concentration, IP reaction, PA nanostructures and NF performance, providing valuable insights into customizing high-performance NF membranes to address complex water pollution challenges.

研究领域: 环境工程 · 膜科学 · 水处理 · 高分子化学 · 纳米技术
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CATALYSIS TODAY · 2022 · IF 6.562

Improved olefin selectivity during CO hydrogenation on hydrophilic Fe/HAP catalysts

Xinyu Guo,Bo Liu,Xinhua Gao,Fugui He,Qingxiang Ma,Subing Fan,Tian-sheng Zhao,Jumei Tian,Prasert Reubroycharoen,Jianli Zhang

The hydrophilic/hydrophobic properties of catalysts greatly influence product distribution by tuning the secondary reactions during Fischer–Tropsch synthesis. Studies have confirmed that hydrophilic modification can inhibit secondary reactions. Herein, hydroxyapatite (HAP)-supported Fe catalysts (Fe/HAP) were prepared using an impregnation method. The effect of the catalyst surface properties on the product distribution in CO hydrogenation was studied. The surface hydroxyl groups on Fe/HAP promoted the growth of carbon chains and improved olefin selectivity. The addition of Na as a promoter to Fe/HAP suppressed the formation of undesirable CH 4 , further improving the selectivity for light olefins and C 5 + hydrocarbons. Compared with Fe 2 O 3 , Fe/HAP showed lower CH 4 selectivity (15%) and higher C 5 + selectivity (45%). Meanwhile, the Fe/HAP -Na catalysts with a higher selectivity of light olefins (with an O/P ratio reaching 4.51).

研究领域: 催化 · 化学工程 · 材料科学
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CATALYSIS TODAY · 2022 · IF 6.562

Promoting hydroisomerization selectivity using channel axis reduced ZSM-48 fabricated by a combined bead-milling and porogen-assisted recrystallization method

Yifan Zheng,Hongxin Ding,Enhui Xing,Jinghua Zhou,Yibin Luo,Jichang Liu,Kake Zhu

ZSM-48 is a unidimensional zeolite that is frequently used as acid component of bi-functional hydroisomerization catalyst. As selectivity towards unwanted cracking products increases with retention time of isomerized products inside micropores, shortening their retention time inside the micropores by reducing channel length offers an effective way to improve isomerization selectivity. Direct synthesis of unidimensional zeolitic crystals with reduced channel axis is particularly difficult, since they habitually grow into rod-like shape along their channel direction. Post-synthetic bead-milling is a cost effective, mechanochemical method to decrease crystal size of zeolites from micro meter to nano meter scale, but suffers from amorphization or partial destruction of zeolitic crystals. Consequently, a post-milling recrystallization process is often entailed to remedy the destructed domains, which, nonetheless, readily causes secondary crystal growth and formation of bulky crystals that compromises the effect of bead-milling. Here, we show that porogen-assisted recrystallization can overcome the problem to fabricate channel axis reduced ZSM-48 nanocrystals. The Si/Al ratio is tunable between 30 and 200 and the acidity is largely preserved after recrystallization. The catalytic advantages of the obtained material are demonstrated in catalytic n -heptane hydroisomerization. The obtained ZSM-48 nanocrystal with Si/Al ratio of 100 outperforms the rest samples and shows enhanced isomerization yield (72% vs 62%) with respect to the parent sample. By combined diagnoses of the impact of diffusion length on product selectivity (product shape selectivity) and kinetic studies , selectivities to monomethyl branched isomers (2-methyl hexane and 3-methyl hexane) and small bulky dimethyl branched isomers (2,3- and 2,4-dimethyl pentane) are attributed to product shape selectivity, whereas the formation to bulky dimethyl branched isomers (2,2- and 3,3-dimethyl pentane) is hindered mainly by transition-state shape selectivity. The combined destructive-constructive synthetic protocol and the revelation of the origin of shape-selectivity in n -heptane hydroisomerization are useful for hydroisomerization catalyst design.

研究领域: 催化材料 · 化学工程
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APPLIED CATALYSIS A-GENERAL · 2022 · IF 5.723

Modulating multi-active sites in CeO2-modified MnOx/ZSM-5 catalyst for selective catalytic oxidation of diethylamine

Lin-Cong He,Xu-Fang Wang,Chu-Feng Liu,Bei Li,Meng-Fei Luo,Jian Chen

An efficient MnO x /CeO 2 /ZSM-5 catalyst was developed for selective oxidation of diethylamine (DEA) with high N 2 selectivity in a wide temperature window ( Δ T = 140 °C), owing to the existence of oxidation and selective catalytic reduction (SCR) active sites. MnO x species prefer to locate on the surface of CeO 2 compared to ZSM-5, and the presence of CeO 2 is beneficial to form more Mn 4+ species, the active sites for oxidation reaction. The mechanistic investigation suggests that internal SCR of NO x generated from the over-oxidized DEA is the crucial pathway for N 2 generation. The high SCR activity of the MnO x /CeO 2 /ZSM-5 catalyst in oxidation conditions is mainly attributed to the synergistic catalysis of Mn 4+ species and acid sites of ZSM-5, the active sites for SCR reaction. Thus, it has been clearly clarified that addition of CeO 2 and its addition sequence could modulate the surface active sites of MnO x /ZSM-5 catalyst for the selective catalytic oxidation of DEA.

研究领域: 环境科学 · 催化化学
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AICHE JOURNAL · 2020 ·Vol. 66 ·期 5 ·e16917 · IF 3.519

Selective steam reforming of n-dodecane over stable subnanometric NiPt clusters encapsulated in Silicalite-1 zeolite

Bofeng Zhang,Yajie Tian,Dali Chen,Ling Li,Guozhu Li,Li Wang,Xiangwen Zhang,Guozhu Liu

Multimetallic nanocatalysts have attracted increasing attention for steam reforming owing to highly exposed active sites, but often suffering from severe sintering. Herein, we design subnanometric Ni-Pt bimetal clusters (ca. 1.7 nm) encapsulated in Silicalite-1 zeolite (2Ni0.5Pt@S-1) through ligand-stabilized method to prevent sintering by fixing the metal into microporous channels. In the steam reforming of n -dodecane test, 2Ni0.5Pt@S-1 gave an excellent activity and stability with a decrease of conversion only 4% at 600°C for 4 hr, which was about a quarter that of 2Ni0.5Pt/S-1 synthesized by co-impregnation method, ascribing to superior sinter-resistance of encapsulation structure. Moreover, 2Ni0.5Pt@S-1 exhibited a higher H 2 selectivity up to 69.9% than that of 2Ni0.5Pt/S-1 (64.4%), owing to suppressed methanation reaction based on subnanometric clusters. Shape-selective steam reforming of n -dodecane and ofm -xylene was also observed, because of m -xylene could hardly diffuse into the zeolite channels due to its bulky molecular size, further preventing potential deactivation by tars in reforming process.

研究领域: 催化化学 · 材料科学 · 能源化学
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Journal of Materials Chemistry A · 2019 ·Vol. 7 ·期 5 ·2385-2391 · IF 10.733

An ultrathin and highly porous silica nanochannel membrane: toward highly efficient salinity energy conversion

Fei Yan,Lina Yao,Kenxin Chen,Qian Yang,Bin Su

Artificial solid-state nanochannels are capable of regulating unipolar ion transport in their confined space and thus converting the Gibbs free energy stored in the salinity gradients to electricity. In order to achieve a large conversion efficiency, highly ion-selective and permeable nanochannel membranes are inevitably desired. In this work we report the salinity energy conversion using an ultrathin silica isoporous membrane (SIM, ∼90 nm in thickness) that consists of straight, uniform and close packed nanochannels (diameter, 2–3 nm; pore density, ∼4 × 1012 cm−2, corresponding to a porosity of 16.7%). Thanks to its unique structure and negatively charged surface, the SIM displayed excellent cation selectivity and meanwhile preserved a high ionic flux, and was capable of harnessing the osmotic energy efficiently upon mixing artificial seawater and river water. We rationalized the ion distribution inside the nanochannels in the presence of salinity gradients and the effect of the channel length on the energy conversion efficiency by finite element simulations. The simulated results suggest that short nanochannels with an ultrasmall dimeter of ∼2.3 nm and a length of ∼100 nm possess excellent cation selectivity. Both experimental and theoretical results suggest that the SIM is a highly potential material in salinity energy conversion.

研究领域: 材料科学 · 能源科学
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