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ANALYTICA CHIMICA ACTA · 2021 · IF 6.558

Dual-functionalized magnetic bimetallic metal-organic framework composite for highly specific enrichments of phosphopeptides and glycopeptides

Yini Pan,Chenhui Zhang,Ruili Xiao,Lingyi Zhang,Weibing Zhang

In this work, a dual-functionalized magnetic bimetallic metal-organic framework composite denoted as Fe 3 O 4 @SiO 2 @(Zr–Ti-MOF) 10 -NH 2 was ingeniously designed and fabricated by a facial layer-by-layer assembly technique. The composite not only exhibited strong affinity for phosphopeptide due to the coexistence of Zr–O clusters and Ti–O clusters, but also owned great hydrophilicity for glycopeptides relying on abundant hydrophilic NH 2 groups, meeting the demand for simultaneously enrichment and sequential elution of phosphopeptides and glycopeptides. As expected, the synthesized composite showed great selectivity (1:2000 M ratio of β-casein:BSA; 1:50 M ratio of IgG:BSA), good sensitivity (1 fmol μL −1 for both α-casein and IgG), and good capacity (80 mg g −1 for α-casein and 200 mg g −1 for IgG). By using sequential elution strategy, 29 phosphopeptides and 24 glycopeptides from α-casein and IgG digests mixture could be simultaneously enriched and respectively detected through a single-step enrichment and sequential elution method. Furthermore, the composite was successfully applied to the analysis of intricate biological samples. 4 endogenous phosphopeptides and 20 phosphopeptides were trapped from human serum and non-fat milk tryptic digest respectively. From 0.5 mg of tryptic digest of rat brain, 141  N -linked glycopeptides corresponding to 127 glycoproteins and 918 phosphopeptides corresponding to 397 phosphoproteins were enriched simultaneously and identified respectively, proving the Fe 3 O 4 @SiO 2 @(Zr–Ti-MOF) 10 -NH 2 to be a dependable candidate for the simultaneously enrichment of trace phosphopeptides and glycopeptides in intricate biological samples.

研究领域: 分析化学 · 蛋白质组学
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TALANTA · 2025 · IF 6.1

Bioinspired hydrophilic material with parallel ordered channels for simultaneously selective enrichment and rapid separation of glycopeptides and phosphopeptides

Jie Li,Junlong Wang,Jiajun Cui,Fei Gao,Hongying Guo,Jiyou Yang,Mengren Li,Zhan Ma,Zijun Wang,Liuping Zhang,Weiwei Huan

Natural plants with fascinating structures give inspirations to fabricate advanced affinity chromatography materials for glycoproteome and phosphoproteome analyses. In this study, inspired by the long-range ordered structure and rapid water transportation capability of lotus stem, a biomimetic hydrophilic material (PE/HAVP-Ti 4+ ) with parallel ordered channels is developed and applied to selectively enrich low-abundant glycopeptides and phosphopeptides in biological samples. The biomimetic PE/HAVP-Ti 4+ has honeycomb porous structure, robust mechanical property, excellent hydrophilicity, and abundant affinity sites. It demonstrates the excellent selectivity (molar ratio human IgG: BSA=1:1000, β-casein: BSA=1:2500), high sensitivity (0.2 fmol μL –1 for glycopeptides, 0.01 fmol μL –1 for phosphopeptides), satisfactory recovery rate (90.7 % for glycopeptides, 91.1 % for phosphopeptides), and good recyclability (at least 10 cycles). Moreover, after enrichment treatment by PE/HAVP-Ti 4+ , a total of 411 N - glycopeptides assigned to 212 N-glycoproteins and 63 phosphopeptides associated with 41 phosphoproteins in human serum are identified by mass spectrometry. The PE/HAVP-Ti 4+ has significant potential in applications of glycopeptide and phosphopeptide enrichment of real complex biological samples for the simultaneous study of glycoproteome and phosphoproteome.

研究领域: 生物化学 · 分析化学 · 蛋白质组学
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Analytical Methods · 2020 ·Vol. 12 ·期 38 ·4657-4664 · IF 2.596

Facile preparation of polymer-grafted ZIF-8-modified magnetic nanospheres for effective identification and capture of phosphorylated and glycosylated peptides

Linhua Yi,Yinghua Yan,Keqi Tang,Chuan-Fan Ding

As a member of MOFs, Zn-MOFs (ZIF-8) are seldom used in phosphopeptide enrichment because ZIF-8 is soluble in acid solutions. Therefore, properly designing a novel strategy to overcome the defect of ZIF-8 is necessary. In this study, a novel multifunctional nanoprobe was designed by uniting magnetic core, titania shell and hydrophilic metal–organic frameworks (named as Fe3O4@PDA@mTiO2@PEI-g-ZIF-8). Integrating the strategies of hydrophilic interaction affinity chromatography (HILIC), immobilized metal ion affinity chromatography (IMAC) and metal oxide affinity chromatography (MOAC), the Fe3O4@PDA@mTiO2@PEI-g-ZIF-8 mesoporous microspheres can enrich phosphorylated peptides and glycosylated peptides simultaneously. Fe3O4@PDA@mTiO2@PEI-g-ZIF-8 has high selectivity (maximum molar ratio β-casein/HRP : BSA = 1 : 1000), low detection limit (2 fmol) towards phosphopeptides and glycopeptides. Besides, the Fe3O4@PDA@mTiO2@PEI-g-ZIF-8 also exhibited a fine performance in the actual sample detection. In the experiment, taking saliva as a sample, 16 phosphorylated peptides were identified, and from a human serum sample, 4 phosphorylated peptides were selectively identified. All in all, the materials show great potential in the future study of phosphoproteomics and glycoproteomics.

研究领域: 分析化学 · 蛋白质组学 · 生物化学
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Foods · 2023 ·Vol. 12 ·期 14 ·2712 · IF 5.2

Arsenic Contents, Speciation and Toxicity in Germinated Rice Alleviated by Selenium

Xin Zheng,Jing Hong,Jingyi Zhang,Yulong Gao,Peng Li,Jian Yuan,Guanglei Li,Changrui Xing

Rice can accumulate more organic and inorganic arsenic (iAs) than other crop plants. In this study, the localization of As in rice grains was investigated using High Performance Liquid Chromatography-Inductively Coupled Plasma Mass Spectrometry (HPLC-ICP-MS) based on 26 rice varieties collected from two provinces. In all the samples, the total As contents in polished rice were 0.03–0.37 mg/kg, with average values of 0.28 and 0.21 mg/kg for two sample sets. The results of the determination of arsenic speciation in different components of rice grain showed that in the polished and brown rice the mean value of arsenite (As(III)) was nearly twice than that of arsenate (As(V)). The regional difference was observed in both total As contents and As speciation. The reason may be that As(III) is more mobile than As(V) in a dissociated form and because of soil properties, rice varieties, and the growing environment. The proportion of iAs and the total As in rice bran was higher than that in polished rice, and this is because As tends accumulate between the husk and the endosperm. In our study, selenium could alleviate the risk of arsenic toxicity at the primary stage of rice growth. Co-exposure to As and Se in germinated rice indicated that the reduction in As accumulation in polished rice reached 73.8%, 76.8%, and 78.3% for total As, As(III), and As(V) when compared with rice treated with As alone. The addition of Se (0.3 mg/kg) along with As significantly reduced the As amount in different parts of germinated rice. Our results indicated that Se biofortification could alleviate the As accumulation and toxicity in rice crops.

CAS / MDL: 188860-26-6 80-62-6
研究领域: 植物学 · 环境科学 · 食品科学
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ANALYTICAL CHEMISTRY · 2018 · IF 6.042

Hydrophilic Phytic Acid-Coated Magnetic Graphene for Titanium(IV) Immobilization as a Novel Hydrophilic Interaction Liquid Chromatography–Immobilized Metal Affinity Chromatography Platform for Glyco- and Phosphopeptide Enrichment with Controllable Selectivity

Yayun Hong,Hongli Zhao,Chenlu Pu,Qiliang Zhan,Qianying Sheng,Minbo Lan

In this work, multifunctional Ti4+-immobilized phytic acid-modified magnetic graphene (denoted as MagG@PEI@PA-Ti4+) nanocomposites were fabricated through a facile route for simultaneous/respective enrichment of N-glyco- and phosphopeptides. Phytic acid (PA), with six phosphate groups, possesses excellent hydrophilicity and metal ion coordination ability, which endowed the MagG@PEI@PA-Ti4+ with combined properties of immobilized metal ion affinity chromatography (IMAC)- and hydrophilic interaction liquid chromatography (HILIC)-based materials. On the basis of the different binding ability of N-glyco- and phosphopeptides on MagG@PEI@PA-Ti4+, the MagG@PEI@PA-Ti4+ nanocomposites could enrich N-glyco- and phosphopeptides simultaneously or respectively by using different enrichment conditions, achieving controllable selective enrichment of N-glyco- and phosphopeptides. The proposed nanocomposites demonstrated an outstanding performance for selective enrichment of N-glycopeptides (selectivity, 1:1000 molar ratios of IgG/BSA; sensitivity, 0.5 fmol/μL IgG; loading capacity, 300 mg g–1; recovery, >90%) and phosphopeptides (selectivity, 1:5000 molar ratios of α-casein/BSA; sensitivity, 0.1 fmol/μL α-casein; loading capacity, 100 mg g–1; recovery, >90%). Taking advantage of these merits, a total of 393 N-glycopeptides derived from 259 glycoproteins and 574 phosphopeptides derived from 341 phosphoproteins were identified from 200 μg of HeLa cell extracts through a single-step enrichment using MagG@PEI@PA-Ti4+.

研究领域: 分析化学 · 蛋白质组学 · 生物医学
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TALANTA · 2021 · IF 6.057

Flexible and hierarchical metal-organic framework composite as solid-phase media for facile affinity-tip fabrication to selectively enrich glycopeptides and phosphopeptides

Muhammad Mujahid Ali,Zhiyuan Zhu,Dilshad Hussain,Zhengchao Shen,Yutian He,Zhenxia Du

Micro-tip-based solid-phase microextraction is considered as one of the green and powerful analytical sample preparation techniques, but its efficiency is severely hampered by some basic issues such as tedious fabrication, instability of sorbent bed, and blocking of the tip, especially for biological samples due to low permeability. These issues are tackled by introducing a flexible and hierarchical substrate in the microtip, having good mechanical strength and specific functionality to capture the desired biomolecules. Considering the well-ordered and flexible structure of melamine foam, it was used as a substrate and for hydrophilic interaction chromatography (HILIC). Metal-organic framework, due to its excellent characteristics, was grafted on its surface anchored by self-assembling polydopamine. The resulting material was characterized and packed in the tip by just pressing the material in the conical structure of the tip. This affinity tip established good and tunable permeability and was used to selectively enrich glycopeptides as well as phosphopeptides. The affinity tip demonstrated excellent performance to enrich glycopeptides and phosphopeptides with a low limit of detection up to 0.5 fmol μL −1 from tryptic digests of horseradish peroxidase and β-Casein, respectively, and was stable up to 5 rounds of enrichment. Moreover, this affinity-tip also exhibited high selectivity up to up to 1:1000 (HRP digest to BSA digest) for glycopeptides and 1:200 (β-Casein digest to BSA digest) for phosphopeptides and demonstrated several other fascinating characteristics such as; excellent size exclusion effect for the omission of large-sized proteins, modest backpressure, reproducibility, reusability, smooth enrichment, and successfully applied to a human saliva sample.

研究领域: 分析化学 · 蛋白质组学
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Journal of Proteomics · 2023 · IF 3.3

Negative enrichment strategy combined with site-specific derivatization for the C-terminomics

Yuanyuan Zhang,Yutong Han,Wenjie Zhu,Jing Yuan,Xin Liu

Protein C-termini containing valuable biological information plays a vital role in various physiological processes , such as protein localization, protein recognition, and signal transduction in organisms. However, C-terminal peptide identification is still challenging due to their low abundance and similar physicochemical properties to other digested peptides. Herein, we developed a simple and mild strategy for the enrichment of C-terminal peptides that incorporates selectively 2-pyridinecarbaldehyde (2-PCA) derivatization of α-amine with negative enrichment by NHS resin. Two synthesized peptides were utilized to evaluate the efficiency of 2-PCA derivatization and optimize the coupling conditions of NHS resin. The feasibility of the method was further validated by enriching the C-terminus of the bovine serum albumin (BSA). Finally, this method was successfully applied to the C-terminus analysis of mouse brain tissue, identifying 404 protein C-termini with physicochemical properties unbiasedly. Additionally, the GO and KEGG analyses revealed that these identified proteins are crucial for proper brain function. In summary, our proposed method is effective and has the potential to facilitate comprehensive C-terminal analysis of proteins . Significance Effective enrichment methods are essential for the identification of the proteins C-terminus. In this study, a mild and simple method for negative C-terminal enrichment combined with site-specific derivatization was developed. The enrichment process was simplified and minimized sample loss simultaneously, using 2-PCA derivatization which has high α-amino specificity. Up to 346C-terminal proteins were identified in mouse brain tissue unbiasedly and reliably. This approach has the potential to facilitate comprehensive analysis of protein C-termini in a variety of biological contexts.

CAS / MDL: 540-69-2 9048-46-8
研究领域: 生物化学 · 蛋白质组学 · 系统生物学
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MINERALS ENGINEERING · 2018 · IF 2.707

A novel approach for pre-concentrating vanadium from stone coal ore

Baijun Yan,Daya Wang,Liushun Wu,Yuanchi Dong

Stone coal, a kind of important vanadium-bearing resources in China, accounts for about 87% of the domestic reserves of vanadium. But the currently developed techniques to extract vanadium from stone coal are all confronted with environmental problems. For example, large quantities of caustic or greenhouse gases discharged in the oxidizing roast process, enormous consumptions of acid or alkali in the leaching step and massive tailings containing toxic V 5+ ions. With a view to solve those problems, an innovative process for pre-concentration of vanadium from stone coal was designed and confirmed on a laboratory scale. The distinct features of this design are as follows. Firstly, the environment-friendly Fe 2 O 3 is selected as a capturer of vanadium. Secondly, the natural reducing property of stone coal is utilized to promote the formation of magnetic V-rich phase, Fe 2 VO 4 . Thirdly, a high-grade vanadium concentrate is obtained by magnetic separation method. The practicability of this design was confirmed using industrial stone coal on a laboratory scale. When 10 mass% Fe 2 O 3 relative to stone coal was added and roasted at 1200 °C for 3 h, a high-grade concentrate containing vanadium higher than 14 mass% was obtained, and more than 91% of the total vanadium in stone coal was recovered.

CAS / MDL: 7440-44-0
研究领域: 冶金学 · 环境科学
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ACS Sustainable Chemistry & Engineering · 2019 · IF 6.97

Boronic Acid-Functionalized Magnetic Metal–Organic Frameworks via a Dual-Ligand Strategy for Highly Efficient Enrichment of Phosphopeptides and Glycopeptides

Bin Luo,Qiang Chen,Jia He,Zhiyu Li,Lingzhu Yu,Fang Lan,Yao Wu

To date, abundant strategies and affinity materials are proposed to enrich phosphopeptides and glycopeptides from biological systems. However, few affinity materials can meet the demand for enriching both phosphopeptides and glycopeptides with an integrated single material. In this work, a novel magnetic metal–organic framework nanocomposite with Zr4+ ions as metal unit as well as terephthalic acid (PTA) and 1,4-phenylenebisboronic acid (denoted as PBA) as dual organic ligands was designed and fabricated for highly efficient enrichment of both phosphopeptides and glycopeptides. It is worth mentioning that Zr4+ ions and PBA were well assembled into the MOF coating via the dual-ligand strategy to achieve both phosphopeptide and glycopeptide enrichment by the Zr–O clusters based on metal oxide affinity chromatography (MOAC) and abundant boronic acid groups based on boronic acid affinity chromatography (BAAC) methods. The quick magnetic response performance and high surface area endowed the affinity material outstanding ability for phosphopeptide and glycopeptide enrichment in the model protein mixtures (β-casein, human IgG, and bovine serum albumin). Furthermore, the nanocomposites exhibited specific enrichment capacity in complex biological samples (rat brain and rat liver), revealing the great potential for the identification and analysis of trace phosphopeptides and glycopeptides in biological samples.

研究领域: 分析化学 · 蛋白质组学 · 生物医学
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WATER SCIENCE AND TECHNOLOGY · 2024 ·Vol. 89 ·期 4 ·873-886 · IF 2.5

Preparation of PDMS and PDMS-UiO-66 oxygen-rich membranes and modules for membrane-aerated biofilm reactors

Tao Haiyan,Cao Xiaochang,Song Rujie,Zhou Zebin,Cheng Fang

A membrane-aerated biofilm reactor (MABR) combines membrane technology with biofilm processes and has unique advantages in the treatment of organic wastewater and volatile wastewater. The common membranes for MABR systems usually have relatively uneven pore structures and low bubble point pressure, resulting in unsatisfactory O 2 utilization and wastewater treatment efficiency. In this work, polydimethylsiloxane (PDMS) and UiO-66 (a Zr-based metal organic framework) were coated on the surface of a commercial polypropylene (PP) hollow fiber membrane to prepare oxygen-rich MABR membranes and modules, which showed an attractive O 2 utilization rate and wastewater treatment efficiency. The bubble points of the PDMS and PDMS-UiO-66 membranes were significantly higher than those of the PP membranes, and the PDMS-UiO-66 membranes had better oxygen enrichment capacity and biological affinity. The optimal PDMS-UiO-66 membrane modules had an O 2 permeance of 31.65 GPU (1 GPU = 3.35 × 10 −10 mol m −2 s −1 Pa −1 ), with O 2 /N 2 selectivity of 2.21. The membrane hanging effect and processing capacity for domestic sewage were greatly improved. This study may provide insights and guidelines to fabricate porous mixed matrix membranes and modules in the industry for MABR. The developed products are expected to be applied in the actual separation process. PDMS and PDMS-UiO-66 were coated on the PP support to prepare O 2 -rich MABR membranes and modules. With UiO-66 loading, the module has a higher O 2 /N 2 separation performance, a rougher and more hydrophilic membrane surface. The PDMS-UiO-66 membrane module exhibits a good biofilm hanging effect and high NH 4 + -N removal performance.

研究领域: 环境科学 · 材料科学 · 生物技术
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JOURNAL OF THE AMERICAN OIL CHEMISTS SOCIETY · 2023 · IF 2

Enrichment of EPA and DHA by enzymatic ethanolysis: Effects of lipases from Thermomyces lanuginosus, Rhizomucor miehei, Rhizopus oryzae and Candida antarctica

Miao Qiao,Xin Hua,Yongjun Yuan,Xi Cao

This work attempts to achieve the enrichment of eicosapentaenoic acid (EPA) and docosahexaenoic acid (DHA) in acylglycerols as well as biodiesel production by investigating the performance of various lipases in ethanolysis. The ethanolysis activities of five immobilized lipases in decreasing order were as follows: Lipozyme TL IM, Novozym 40086/Lipozyme RM IM, Novozym 435 and Rhizopus oryzae lipase immobilized on polypropylene (RO PP). EPA could be enriched to a certain content by Lipozyme TL IM, Novozym 40086, Lipozyme RM IM, and RO PP. The enrichment of DHA was achieved well by those four sn -1,3 regioselective lipases, and DHA contents in acylglycerols were the highest when Lipozyme TL IM and Novozym 40086 were used, reaching 2.87-fold and 2.81-fold of the initial content. However, Novozym 435 could not enrich EPA and DHA effectively. Fatty acid ethyl esters produced in this work contained abundant palmitic acid and palmitoleic acid, which could be ideal biodiesel considering their chain length. The competitive factors of five lipases towards DHA were all significantly higher than those towards EPA. When Lipozyme TL IM and Novozym 40086 achieved the maximum DHA contents, their DHA recoveries in acylglycerols reached 91.87% and 89.00%, respectively. The DHA recoveries were all significantly higher than the corresponding EPA recoveries in the reactions catalyzed by five lipases. Moreover, Lipozyme TL IM could be a potential lipase for the separation of EPA and DHA. This study may promote the full use of fish oil and broaden the application of lipases.

研究领域: 生物化学 · 食品科学 · 酶工程
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FUEL · 2021 · IF 6.609

The transformation and enrichment of Cd in fine particulate matter during coal combustion: The key roles of Ti-bearing components

Yong Wei,Guijian Liu,Biao Fu,Yuan Liu,Xuan Xue

Fine particulate matter (PM) emitted from coal-fired power plants (CFPPs) has aroused widespread environmental and human health concerns. Cadmium (Cd), as one of the prime toxic air pollutants, which exists in fine PM intensifies its toxicity. In this research, three particle sizes of PM (PM 1 , PM 2.5 , and PM 10 ) at the outlet of electrostatic precipitator (ESP), along with feed coal, bottom ash, and ESP ash, were collected from a 300-MW pulverized CFPP. Results showed that Cd was more enriched in the fly ash than in bottom ash. With the PM diameter decreasing, the relative enrichment index (REI) value of Cd increases from 2.30 to 7.84. The concentration of Cd was found to be intimately related to Ti in the PM. Abundant Ti-rich particles were identified in the PM 1 , having quite different chemical compositions as compared to particles larger than 2.5 μm. The major processes governing the formation of Ti-rich particles included melting of silicate-bound Ti and heterogeneous condensation of gaseous Ti from the decomposition of organic-associated Ti in coal. The transformation behavior of Cd to PM in a coal combustion process was discussed based on its occurrence mode in coal, thermodynamic property, and the possible interactions with ash particle compositions. The retention of Cd (g) by Ti-rich particle were probably dominated by chemisorption at high temperature; at lower temperature, physical adsorption or condensation may be the primary mechanisms for capturing CdCl 2 (g).

研究领域: 环境科学 · 化学
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