SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2022
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IF 4.831
Kun Ge,Qiyue Wu,Yonghui Li,Ying Gu
In this work, a hexagonal boron nitride (h-BN)/AuAg nanoalloy hybrids (NAHs) was synthesized to fabricate h-BN/Au 1 Ag 3 membrane as a solid surface-enhanced Raman spectroscopy (SERS) substrate for sensitive SERS detection of melamine. The AuAg nanoalloys were in situ grown on h-BN by chemical reduction method, and the Au/Ag molar ratio was tuned to achieve optimal SERS performance. After the SERS performance of h-BN/AuAg NAHs with different Au/Ag ratios was analyzed, h-BN/Au 1 Ag 3 NAHs were chosen for SERS analysis. The h-BN/Au 1 Ag 3 membrane can be obtained through simple filtration of h-BN/Au 1 Ag 3 NAHs on chromatographic paper. As expected, the solid SERS substrates of h-BN/Au 1 Ag 3 membrane were uniform and demonstrated good selectivity, repeatability and reproducibility for SERS detection of melamine. The results demonstrate that h-BN/Au 1 Ag 3 membrane exhibited high SERS activity for 4-mercaptobenzoic acid (4-MBA) with limit of detection (LOD) at 1.0 ng L −1 , and its analytical enhancement factor (AEF) reached 3.6 × 10 8 . The possible enhancement mechanism, including electromagnetic mechanisms (EM) and chemical mechanisms (CM) were illustrated by finite-difference time-domain (FDTD) and density functional theory (DFT) simulations in detail, respectively. The concentration of melamine in the 0.05–5.0 mg L −1 range showed good linear relationship ( R 2 = 0.9940) with SERS intensity with LOD of 0.01 mg L −1 . Finally, the recoveries of melamine in liquid milk samples are 87.7–105.7% with relative standard deviations (RSDs) in range of 0.6–2.6%, providing precise safety evaluation of melamine in milk samples.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2021
·
IF 6.953
Xiaoyu Xia,Xiaoyi Tan,Chao Wu,Yao Li,Guanghua Zhao,Ming Du
The aggregation-induced emission (AIE) material has been widely used in biological detection due to their unique property of fluorescing in aggregation state. However, the poor dispersion and biocompatibility limit its application in in vivo real-time imaging. Here, a novel strategy is designed to obtain pH-responsive AIE nanomaterials, working through 4-Undecoxy Tetraphenyl Ethylene Methacrylate (PM1) block, with excellent features (dispersion, biocompatibility, self-reconstruction and cancer specific recognition). The recombinant human H-ferritin (rHuHF) was used to prepare rHuHF-PM1 nanocomposites which effectively supported the dispersion and transfer of PM1 in the biological environment, even making it target tumor cells due to the overexpression of ferritin receptors on tumor cells. To simulate the changes of rHuHF in intracellular lysosomes, particle size and fluorescence of rHuHF-PM1 were analyzed, which reflected the loose structural changes of rHuHF nanocages in weak acid system that facilitated the degradation of macromolecular rHuHF in intracellular lysosomes and following release of PM1. The released PM1 molecules aggregated and emitted brilliant blue fluorescence. Several cell lines, Hela, HT-29, HepG2, L-O2 and HUVEC have all been sensitively detected and distinguished. Accordingly, this nanocage has a potential to be applied to disease diagnosis and provides a novel sensing platform for the identification of cancer.
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JOURNAL OF MEMBRANE SCIENCE
·
2023
·
IF 9.5
Shiwei Tian,Yaqi Zhang,Qiankun Sha,Tian Yang,Yan Huang,Xingxiang Zhang,Wei Wang,Na Han
Highly efficient treatment of oil-water emulsions in severe environments (organic solvents, strong acids) is recognized as a challenging subject. Polyphenylene sulfide (PPS) is an ideal membrane material with superior thermal stability as well as chemical resistance that is expected to settle this challenge. However, the hydrophobicity of PPS (h-PPS) membrane inherently prevents its efficient treatment of oil-in-water (O/W) emulsions. In this study, superhydrophilic modification of PPS substrates was achieved by in situ electrostatic self-assembly of hydrophilic Zr-MOFs to obtain UiO-66-NH 2 @h-PPS membranes. The introduction of UiO-66-NH 2 crystals constructed the micro/nanoscale hierarchical structure for the substrate, which transforms the PPS substrate from a hydrophobic to a superhydrophilic state (water droplets require only 0.6 s to be completely immersed in the membrane). Meanwhile, the UiO-66-NH 2 @h-PPS membranes gain under-water superhydrophobicity (the under-water oil contact angle exceeds 150° for toluene, hexane , dichloromethane , and carbon tetrachloride , of which toluene reaches 163.1°), thereby improving wettability selectivity and decreasing oil adhesion, permitting the fabricated UiO-66-NH 2 @h-PPS membranes to effectively separate different types of O/W emulsions. The UiO-66-NH 2 @h-PPS membranes acquire excellent permeate fluxes (for the surfactant-free toluene-in-water emulsion, it reaches up to 7638.1 L m −2 h −1 ) and separation accuracy (99.1% oil rejection). Moreover, the UiO-66-NH 2 @h-PPS membrane exhibited outstanding harsh environment resistance. Interestingly, the combination of UiO-66-NH 2 and h-PPS substrate was applicable to degrade the organic compound in water, and the degradation efficiency of the methylene blue achieved 85.7% under visible light within 120 min. In summary, loading Zr-MOFs onto h-PPS substrates provides a novel strategy for the efficient treatment of wastewater under complex conditions with great potential for practical applications.
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Journal of Environmental Chemical Engineering
·
2023
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IF 7.7
Junyong He,Ya Yang,Peidong Hong,Yulian Li,Chao Xie,Zijian Wu,Minqiang Li,Lingtao Kong
The use of peroxymonosulfate (PMS) activation to eliminate organic contaminants is a promising technology to purify water owing to its strong reactivity. However, because of the existed rate limiting step, the performance of PMS activation was restrained and required external energy consumption. Therefore, a new strategy was proposed to solve this problem by preparing catalysts with abundant electron-rich sites and electron traps to accelerate PMS activation. In this research, a novel MnCeO x -H catalyst with rich surface oxygen vacancies was firstly synthesized to accelerate the transfer of electrons among the catalysts, oxidant and pollutants. The contaminants were rapidly eliminated in the MnCeO x -H/PMS system, while the reaction rate constant of MnCeO x -H/PMS system was 30 times higher than that of CeO 2 /PMS system. The surface oxygen vacancies were able to adsorb and trap PMS, then the free electrons of oxygen vacancies would reduce PMS and produced HO•, 1 O 2 and SO 4 •- , while 1 O 2 played a major role. The contaminants which acted as electron-donors in this system were adsorbed at Mn, Ce sites, achieving effective conversion recycling of Ce(IV)/Ce(III), Mn(III)/Mn(II) and Mn(IV)/Mn(III). This discovery is believed to inaugurate a novel way for designing powerful electron-rich sites and electron traps to accelerate PMS activation for contaminants degradation.
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MACROMOLECULAR CHEMISTRY AND PHYSICS
·
2023
·Vol. 224
·期 23
·2300304
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IF 2.5
Mingzhao Li,Jia Wang,Anjun Qin,Ben Zhong Tang
Hyperbranched polymers have been widely applied in various fields because of their good solubility, high reactive end groups, and low viscosity, etc. Therefore, it is of great importance to develop new strategies to build multifunctional hyperbranched polymers with novel architectures. In this work, a C(sp 3 )─H activation-based polymerization of internal alkynes and bifunctional secondary amines is successfully established, and multifunctional hyperbranched polyamines (hb-PAs) with 100% E -isomers and high molecular weights ( M w up to 76 500) are prepared in good yields (up to 82%). The hb-PAs containing tetraphenylethylene moiety show unique aggregation-enhanced emission properties and can be used for explosive detection with a low limit of detection (9.14 × 10 −8 m ). Notably, the hb-PAs display high refractive indices (up to 1.7607) that can be further modulated to 1.7825 by the coordination of its peripheral ethynyl group with metallic cobalt. Moreover, the hyperbranched structure endows the hb-PAs with much better properties than their linear counterparts, such as higher photoluminescence quantum yields and refractive indices. In addition, the hb-PAs can be modified by a C(sp 3 )─H activation reaction of internal alkynes and alcohols. This work not only prepares a series of functional nitrogen-containing hyperbranched polymers but also promotes the application of C(sp 3 )─H activation in polymer chemistry.
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Materials
·
2021
·Vol. 14
·期 11
·2741
·
IF 3.623
Pengcheng Lv,Ruihong Meng,Zhongyang Mao,Min Deng
In this study, the hydrated sodium aluminosilicate material was synthesized by one-step hydrothermal alkaline desilication using fly ash (FA) as raw material. The synthesized materials were characterized by XRD, XRF, FT-IR and SEM. The characterization results showed that the alkali-soluble desilication successfully had synthesized the sodium aluminosilicate crystalline (N-A-S-H) phase of sodalite-type (SOD), and the modified material had good ionic affinity and adsorption capacity. In order to figure out the suitability of SOD as an adsorbent for the removal of ammonium and phosphorus from wastewater, the effects of material dosing, contact time, ambient pH and initial solute concentration on the simultaneous removal of ammonium and phosphorus are investigated by intermittent adsorption tests. Under the optimal adsorption conditions, the removal rate of ammonium was 73.3%, the removal rate of phosphate was 85.8% and the unit adsorption capacity reached 9.15 mg/L and 2.14 mg/L, respectively. Adsorption kinetic studies showed that the adsorption of ammonium and phosphorus by SOD was consistent with a quasi-secondary kinetic model. The adsorption isotherm analysis showed that the equilibrium data were in good agreement with the Langmuir and Freundlich model. According to thermodynamic calculations, the adsorption of ammonium and phosphorus was found to be a heat-absorbing and spontaneous process. Therefore, the preparation of SOD by modified FA has good adsorption properties as adsorbent and has excellent potential for application in the removal of contaminants from wastewater.Keywords:N-A-S-H;sodalite;simultaneous removal;ammonium;phosphorus
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Journal of the American Chemical Society
·
2015
·
IF 12.113
Xiao-Li Pei,Yang Yang,Zhen Lei,Shan-Shan Chang,Zong-Jie Guan,Xian-Kai Wan,Ting-Bin Wen,Quan-Ming Wang
The activation of C(sp3)–H bonds is challenging, due to their high bond dissociation energy, low proton acidity, and highly nonpolar character. Herein we report a unique gold(I)–silver(I) oxo cluster protected by hemilabile phosphine ligands [OAu3Ag3(PPhpy2)3](BF4)4 (1), which can activate C(sp3)–H bonds under mild conditions for a broad scope of methyl ketones (RCOCH3, R = methyl, phenyl, 2-methylphenyl, 2-aminophenyl, 2-hydroxylphenyl, 2-pyridyl, 2-thiazolyl, tert-butyl, ethyl, isopropyl). Activation happens via triple deprotonation of the methyl group, leading to formation of heterometallic Au(I)–Ag(I) clusters with formula RCOCAu4Ag4(PPhpy2)4(BF4)5 (PPhpy2 = bis(2-pyridyl)phenylphosphine). Cluster 1 can be generated in situ via the reaction of [OAu3Ag(PPhpy2)3](BF4)2 with 2 equiv of AgBF4. The oxo ion and the metal centers are found to be essential in the cleavage of sp3 C–H bonds of methyl ketones. Interestingly, cluster 1 selectively activates the C–H bonds in −CH3 rather than the N–H bonds in −NH2 or the O–H bond in −OH which is traditionally thought to be more reactive than C–H bonds. Control experiments with butanone, 3-methylbutanone, and cyclopentanone as substrates show that the auration of the C–H bond of the terminal methyl group is preferred over secondary or tertiary sp3 C–H bonds; in other words, the C–H bond activation is influenced by steric effect. This work highlights the powerful reactivity of metal clusters toward C–H activation and sheds new light on gold(I)-mediated catalysis.
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Soft Matter
·
2013
·Vol. 9
·期 48
·11585-11597
·
IF 3.909
Wenlong Li,Peiyi Wu
The dynamic thermally reversible phase transition behaviour of poly(ethylene oxide) (PEO) in 1-ethyl-3-methylimidazolium tetrafluoroborate ([EMIM][BF4]) has been investigated by calorimetric measurements (DSC) and FT-IR, in combination with perturbation correlation moving window (PCMW) and two-dimensional correlation spectroscopy (2DCOS) for the first time. A relatively high lower critical solution temperature (LCST) was observed which is different from that of conventional thermo-sensitive polymers in aqueous solution. Four types of hydrogen bonds were found in this system, among which the type I (the hydrogen bonds between the unsaturated C–H on the imidazole ring and the oxygen atoms of PEO) and type II (the hydrogen bonds between the saturated C–H on the PEO backbone and the fluorine atoms of the IL anions) ones have a more predominant influence on the phase transition. Moreover, type I plays the predominant role in both the heating and cooling process. DSC revealed that the phase transition temperature of PEO–[EMIM][BF4] solutions decreases with the increasing concentration of PEO, as well as with a decreasing scanning rate. Through PCMW, the LCST was determined to be ca. 137 °C during heating and ca. 131 °C during cooling. Finally, 2DCOS was employed to elucidate the dynamic mechanism of PEO in [EMIM][BF4], which revealed hydrogen bond disruption, chain aggregation and exclusion of IL molecules. Solutions with a low PEO concentration tend to form loosely aggregated globules, compared to the more densely aggregated globules in samples with a high PEO concentration. Additionally, it is worth mentioning that several unusual and peculiar phenomena were also observed, such as opposite frequency shifts in C–H groups, a “tail-raising” phenomenon, critical PEO concentration for the phase transition temperature, and intersection of the frequency shift curves for samples with high concentrations of PEO during cooling.
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ANALYTICAL BIOCHEMISTRY
·
2016
·
IF 2.243
Wei Zhang,Min Zhu,Feng Wang,Danhui Cao,Jennifer Jin Ruan,Weike Su,Benfang Helen Ruan
Glutamate dehydrogenase (GDH) catalyzes the oxidative deamination of L-glutamate and is important for several biological processes . For GDH inhibitor screening, we developed a novel mono-sulfonated tetrazolium salt (EZMTT), which can be synthesized using H 2 O 2 oxidation and purified easily on silica gel in large quantities. The EZMTT detection method showed linear dose responses to NAD(P)H, dehydrogenase concentration and cell numbers. In E. coli GDH assay, the EZMTT method showed excellent assay reproducibility with a Z factor of 0.9 and caused no false positives in the presence of antioxidants (such as BME). Using the EZMTT-formazan-NAD(P)H system, we showed that EGCG is a potent E. coli GDH inhibitor (IC 50 45 nM) and identified that Ebselen , a multifunctional thioredoxin reductase inhibitor, inactivated E. coli GDH (IC 50 213 nM). In cell-based assays at 0.5 mM tetrazolium concentration, EZMTT showed essentially no toxicity after a 3-day incubation, whereas 40% of inhibition was observed for WST-8. In conclusion, EZMTT is a novel tetrazolium salt which provides improved features that are suitable for dehydrogenases and real-time cell-based high-throughput screening (HTS).
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TETRAHEDRON
·
2016
·
IF 2.645
Weijian Li,Guanghui Lv,Xu Cheng,Rui Sang,Xiaojun Ma,Yong Zhang,Ruifang Nie,Jie Li,Mei Guan,Yong Wu
A moisture- and air-stable palladium(II)-Schiff base complex supported on h-BN was simply prepared by using commercially available reagents. This nanomaterial was applied as an excellent and recyclable heterogeneous catalyst for the Suzuki and Heck cross-coupling reactions. And it has been characterized by FT-IR, XRD, SEM, XPS , TG and ICP-AES techniques. High yields, ligand-free, low reaction time, water as solvent, non-toxicity and recyclability of the catalyst are the main merits of these protocols. In addition, a series of pharmacologically relevant products were successfully synthesized using this catalyst. Above all, this work opens up an interesting and attractive avenue for the use of h-BN as an efficient support for heterogeneous catalysts.
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Materials Today Communications
·
2024
·
IF 3.7
Yufei An,Yiping Su,Gang Li,Shuoyang Liang,Yingying Cai,Ruiheng Zhang,Xuehua Shen,Feng Yan,Zuotai Zhang
CO 2 capture through mineral carbonation extends the applicability of carbon sequestration by enabling storage in various cementitious materials derived from solid wastes. Calcium-containing cementitious materials receive extensive attention due to their potential for carbon capture, however, the underlying mechanisms both decalcification and carbonation during composition-structure evolution remain to be fully elucidated. Herein, a mineral carbonation strategy was reported to enhance carbon uptake performance, depending on the evolution stage of calcium (alumino) silicate hydrates (C-(A-)S-H) gel induced by alkali activation. Sequential dynamic monitoring and experimental characterizations confirmed that the decalcification and carbonation processes are closely linked to Ca-bonding states within the C-(A-)S-H structure. The results indicate that the short chains of alumino-silicate and the majority of the weakly bonded Ca phases are more prone to carbonation. Estimation of carbonation capacities also revealed that samples with 3h-activation exhibit the highest carbonation capacities (80.5 %), showing the higher carbonate potential with free Ca and weakly bound Ca (e.g. Ca(OH) 2 and interlay Ca in tobermorite-like structure) than samples with more intralayer Ca. Our work can provide new insights into the understanding of alkali activation induced decalcification and the improvement on carbonation capacities in early-formed C-(A-)S-H analogues.
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ACS Applied Energy Materials
·
2024
·
IF 5.4
Cuicui Li,Tongtong Gao,Wanzhen Wu,Xinpu Zhou,Shuyu Zhang,Guangpeng Ma,Xianfeng Guan,Shuang Wang
A series of composite membranes (sPBIp3-CAUX) are prepared by using modified sulfonated polybenzimidazole with an optimal side link grafting degree of 30% as a polymer matrix and then doping with CAU-10-H. The hydrophobic alkyl side chains and hydrophilic sulfonic acid groups easily form microphase separated structures due to the polarity difference, which is conducive to the enhancement of proton conductivity. The introduction of CAU-10-H into the polymer effectively prevents the passage of vanadium ions because the vanadium ion transport path becomes more tortuous. The sPBIp3-CAU2 membrane has low vanadium permeability (3.1 × 10–9 cm2 min–1) and excellent ion selectivity (9.16 × 106 S min cm–3). In addition, the sPBIp3-CAU2 membrane shows good cell performance at 60 mA cm–2 with CE of 93.32% and EE of 83.03% compared with those of Nafion 117.
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