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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

Controllable oxidative depolymerization of lignin to produce aromatic aldehydes and generate electricity under mild conditions with direct biomass fuel cells as flexible reactors

Daihong Gao,Denghao Ouyang,Xuebing Zhao

Lignin was oxidized and depolymerized by a direct biomass fuel cell (DBFC) for electricity generation and production of aromatic aldehydes. The yield of aromatic aldehydes could be easily controlled by changing the anodic catalyst, cathodic oxidants and external loading. Cobalt and (VO 2 ) 2 SO 4 were screened as the most suitable anodic catalyst and cathodic oxidant, respectively. A maximum power density of 199.8 mW/cm 2 was obtained under the optimized conditions for electricity generation; however, the yield of the aromatic aldehydes was greatly dependent on the type of lignin used, reaction conditions and the external loading (output voltage) of the DBFC. At a lignin concentration of 0.5 g/L, aromatic aldehydes yield of 7.8 % was obtained at an output voltage of 0.9 V. The formation of aromatic aldehydes was mainly caused by cleavage of β-O-4 linkage and oxidation of side chains by the hydroxyl radicals formed via oxidation of OH – by Co 3+ on the anode.

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SCIENCE OF THE TOTAL ENVIRONMENT · 2023 · IF 9.8

Imidacloprid-induced stress affects the growth of pepper plants by disrupting rhizosphere-plant microbial and metabolite composition

Dong Li,Chunran Zhou,Shuai Wang,Zhan Hu,Jia Xie,Canping Pan,Ranfeng Sun

Overusing imidacloprid (IMI) has been found to impede secondary metabolism and hinder plant growth. The impact of IMI stress on the interaction between metabolites, rhizosphere, and plant-microbe dispersion through various pathways in pepper plants has not been extensively studied. This study investigated the effects of IMI on plant signaling components, secondary metabolic pathways, and microbial communities in the rhizosphere and phyllosphere . Here, the distribution of IMI and its metabolites (6-chloronicotinic acid, IMI-desnitro, 5-hydroxy-IMI, IMI-urea, and IMI-olefin) was primarily observed in the pepper plant leaves. A rise in IMI concentration had a more significant inhibitive effect on the metabolism of pepper leaves than on pepper roots. The findings of non-target metabolomics indicated that IMI exposure primarily suppresses secondary metabolism in pepper plants, encompassing flavones, phenolic acids, and phytohormones. Notably, the IMI treatment disrupted the equilibrium between plants and microbes by decreasing the population of microorganisms such as Vicinamibacteria , Verrucomicrobiae , Gemmatimonadetes , and Gammaproteobacteria in the phyllosphere, as well as Vicinamibacteria , Gemmatimonadetes , Gammaproteobacteria , and Alphaproteobacteria in the rhizosphere of pepper plants. The study demonstrates that overexposure to IMI harms microbial composition and metabolite distribution in the rhizosphere soil and pepper seedlings, inhibiting plant growth.

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BIOCATALYSIS AND BIOTRANSFORMATION · 2022 · IF 2.325

A chlorogenic acid esterase from a metagenomic library with unique substrate specificity and its application in caffeic and ferulic acid production from agricultural byproducts

Jian Yao,Lun Gui,Qizhang Long

Soil microbes are an abundant source of enzymes with unique properties that may be useful for industrial applications. As most wild-type strains show low chlorogenic acid esterase expression and activity, and most microbes cannot be cultured in the laboratory, a metagenomic approach provides methods of identifying new enzymes. In this study, a gene encoding a chlorogenic acid esterase, named Tan410, was isolated from a soil metagenomic library and overexpressed in Escherichia coli BL21 (DE3). The recombinant enzyme, with a predicted molecular weight of 54.88 kDa, was purified to homogeneity. The Km and Vmax values for Tan410 were 1.26 mM and 0.33 mM min–1, respectively, with chlorogenic acid as the substrate. Its optimum temperature and pH for reaction were 30 °C and 7.5, respectively. The enzyme exhibited moderate thermostability and broad pH stability (3.0–10.0). Tan410 was also able to hydrolyse ethyl ferulate, methyl caffeate, propyl gallate, ethyl gallate, methyl vanillate, methyl benzoate, ethyl benzoate, methyl 2,5-dihydroxybenzoate, and methyl 3,5-dihydroxybenzoate, and it released caffeic and ferulic acids from agricultural byproducts (destarched wheat bran and coffee pulp). Tan140 has potential for industrial application in biomass valorization.

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JOURNAL OF CHROMATOGRAPHY B-ANALYTICAL TECHNOLOGIES IN THE BIOMEDICAL AND LIFE SCIENCES · 2022 · IF 3.318

Pseudo-mercaptoethyl pyridine functionalized polyhedral oligomeric silsesquioxane-graphene composite via thiol-ene click reaction for highly selective purification of antibody

Jiawei Liu,Xiangwei Liu,Yingying Liu,Quan Bai

In this work, we prepared a novel graphene-based composite by combination of mercapto-end capped polyhedral oligomeric silsesquioxane (POSS-SH) with graphene oxide (GO) through covalent bonding process. The composite was further conjugated with 4-vinyl pyridine (4-VP) through thiol-ene click reaction to fabricate pseudo-mercaptoethyl pyridine functionalized POSS-graphene composite (G-POSS-S-VP). The physicochemical properties were confirmed via FT-IR, TGA, XPS, and TEM characterizations and a high ligand density of ca. 87.3 μmol m −2 was obtained. G-POSS-S-VP composite displayed high selectivity toward antibody, i.e., immunoglobulin G (IgG) in this case based on the hydrophobic charge induced chromatography (HCIC) mechanism. A high adsorption efficiency of ca. 90% and large adsorption capacity of 500 mg g −1 were achieved for IgG at pH 7.4. At the same time, the non-specific adsorptions of co-existing proteins on graphene substrate were obviously hindered. The practical applicability of G-POSS-S-VP composite as adsorbent was verified by selective separation of IgG from human serum. SDS-PAGE assay and MALDI-TOF-MS analysis clearly demonstrated the successful isolation of IgG with high purity.

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TALANTA · 2022 · IF 6.556

MALDI-TOF MS method for differentiation of methicillin-sensitive and methicillin-resistant Staphylococcus aureus using (E)-Propyl α-cyano-4-Hydroxyl cinnamylate

Wenjing Gao,Bin Li,Ling Ling,Li Zhang,Shaoning Yu

Differentiating methicillin-sensitive and methicillin-resistant Staphylococcus aureus (MRSA and MSSA) is crucial for clinical diagnosis and anti-microbial treatment. Matrix-assisted laser desorption/ionization time of flight mass spectrometry (MALDI-TOF MS) is an efficient tool for identifying pathogenic microorganisms at the bacterial species level. Here, we found that MRSA and MSSA can be differentiated by MALDI-TOF MS by employing (E)-propylα-cyano-4-hydroxyl cinnamylate (CHCA-C3) as the matrix, which shows great performance for proteins/peptides, especially hydrophobic proteins. The results show that the mass spectra profile of standard MRSA (ATCC 43300) is significantly different from the profiles of standard MSSA strains (ATCC 25923 and 29213) when using CHCA-C3 as the matrix compared to traditional matrix. The mass profiles had great reproducibility and were scarcely influenced by the growth medium. Due to the enhanced discrimination ability of CHCA-C3, we collected the mass spectra of 62 clinical S. aureus strains and selected four representative peaks for principal component analysis, which showed great differentiation. Our results suggest that employing a suitable matrix could enhance the discrimination ability of antibiotic-resistant bacteria by MALDI-TOF MS.

CAS / MDL: 490-79-9 530-59-6
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SENSORS AND ACTUATORS B-CHEMICAL · 2022 · IF 9.221

One-step fabrication of high-density Si nanotips as SALDI-MS substrate for highly sensitive detection

Shuzhen Dou,Zhongshun Wang,Qiye Chen,Nan Lu

The high sensitivity of surface-assisted laser desorption/ionization mass spectrometry (SALDI-MS) analysis depends on the enhancement of the signal intensity and the reduction of the background. Here, high-density Si nanotips were prepared as SALDI-MS substrate by taking template-free reactive ion etching for sensitive detection . The high-density Si nanotips act as tiny antennas to concentrate the laser energy and generate photo-induced electrons on a small area, which promotes desorption and ionization of molecule, enhancing the signal intensity. Additionally, the high stability of Si nanotips under laser irradiation ensures low background interference. The applicability of the substrate was demonstrated by the detection of various small molecules, e.g., fatty acids, amino acids , environmental pollutants and drugs. In addition, this substrate can be successfully applied for detecting trace small molecules in complex sample, such as 10 −9 M verapamil in serum and 10 −12 M crystal violet in lake water. Moreover, the banned fungicides left on the fish skin was also detected. The substrate is compatible with imaging, and the endogenous and exogenous substances in fingerprint were visualized by MS imaging. These results demonstrate the easily prepared high-density Si nanotips SALDI-MS substrate is of high detection sensitivity and great value toward large-scale practical applications.

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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

Molecularly imprinted polymers embedded with double perovskite quantum dots: A ratiometric fluorescence sensor for visible and fluorescent determination of Rhein

Rongkun Zhu,Zengcheng Du,Mingfang Zhu,Huanru Liang,Shumei Wang,Qing Zhou,Rui Li,Yulan Li,Chaoying Zeng,Wenhao Liu,Qiqing Chen

A ratiometric fluorescence sensor based on molecularly imprinted polymers embedded with double perovskite quantum dots (green fluorescent CsPbBr 3 (GPQDs) and red fluorescent CsPbI 3 (RPQDs)) were prepared for the visible and fluorescent determination of Rhein. Double perovskite quantum dots were synthesized by a one-pot method with in-situ hydrolysis, and the fluorescent probes containing GPQDs and RPQDs with molecularly imprinted cavities (MIPs@RPQDs/GPQDs@SiO 2 ) were synthesized by sol gel method. And the synthesized MIPs@RPQDs/GPQDs@SiO 2 can emit two stable and independent fluorescence peaks at 520 nm with green fluorescence and at 695 nm with red fluorescence respectively. Since Rhein could specifically quench the red fluorescence without affecting the green fluorescence at 520 nm, a ratiomitric fluorescence sensor could be and was constructed with GPQDs as the internal standard signal and the RPQDs as the response signal. The sensor had a good linear relationship with the concentration of Rhein between 15 and 135 nM, and the detection limit was 1.90 nM (S/N = 3). Moreover, Rhein could be detected by observing the color transformation of the fluorescent probe directly with naked eyes. In addition, Rhein in the traditional Chinese medicine Rheum palmatum L. had been detected by the constructed ratiometric fluorescene probe with satisfactory.

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Foods · 2021 ·Vol. 10 ·期 11 ·2857 · IF 4.35

Effects of Different Pilot-Scale Milling Methods on Bioactive Components and End-Use Properties of Whole Wheat Flour

Wenfei Tian,Jingyang Tong,Xiaoyue Zhu,Philipp Fritschi Martin,Yonghui Li,Zhonghu He,Yan Zhang

The health benefits from consumption of whole wheat products are widely recognized. This study investigated the effects of different pilot-scale milling methods on physicochemical properties, bioactive components, Chinese steamed bread (CSB), and Chinese leavened pancakes (CLP) qualities of whole wheat flour (WWF). The results indicated that WWF-1 from the reconstitution of brans processed by a hammer mill had the best CSB and CLP quality overall. WWF from entire grain grinding by a jet mill (65 Hz) contained the highest concentration of bioactive components including dietary fibers (DF) and phenolic acids. A finer particle size did not necessarily result in a higher content of phenolic antioxidants in WWF. DF contents and damaged starch were negatively correlated with CSB and CLP quality. Compromised reduced quality observed in CLP made from WWF indicated its potentially higher acceptance as a whole-grain product.Keywords:milling methods;dietary fiber;phenolic acid;steamed bread;leavened pancake

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RENEWABLE ENERGY · 2021 · IF 8.001

Insight into the negative effects of lignin on enzymatic hydrolysis of cellulose for biofuel production via selective oxidative delignification and inhibitive actions of phenolic model compounds

Denghao Ouyang,Hongmei Chen,Nan Liu,Jingzhi Zhang,Xuebing Zhao

Oxidative pretreatment of wheat straw with sodium chloride has been used for selective delignification to obtain ideal samples to understand the negative effects of lignin on cellulose accessibility of lignocellulosic biomass . Strong interactive effects has been found between hemicellulose and lignin. To achieve a high enzymatic glucan conversion (EGC) (>80% with 20 FPU/g solid) in the case of high xylan content (25–30%), a moderate degree of delignification (56.3%) with relatively low lignin content (11.9%) is necessary; while in the case of low xylan content (2.6–3.9%), slight removal of lignin by oxidative treatment can well increase cellulose digestibility with a final EGC reaching 90% even that the residual lignin content is as high as 30.9%. Delignification greatly modifies substrate surface morphology with deformation, fracture of cell wall layers and even disappearance of middle lamella. Oxidation also modifies the functional groups and surface properties of lignin, leading to reduction in the inhibitive effects. Phenolic hydroxyl group (Ph-OH) in p -hydroxyphenyl unit has been found to show the strongest inhibition to filter paper activity of cellulase cocktail. Ph-OH exerts stronger inhibition to β -glucosidase than to the endo- and exo-glucanases. Hydrogen bonding and electrostatic interaction are primarily responsible for the inhibitive action of Ph-OH.

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CHINESE JOURNAL OF ANALYTICAL CHEMISTRY · 2021 · IF 1.134

A feasible processing-omics strategy for comprehensive evaluation of mechanisms of chemical transformation in processing Polygalae Radix

Ning-Ning ZHAO,Zhi-Qiang LIU,Mei-Ling FAN,Zi-Feng PI,Feng-Rui SONG,Shu LIU

Traditional processing methods have been used to relieve toxicity and enhance a calming effect of Polygalae Radix (PR). However, up to now, there is no comprehensive study on the changes of saponins , aromatic acids, and so on (from relatively big molecules to small molecules). Here, a novel processing-omics (PO) strategy was reported. It cleverly integrated the non-targeted and targeted chemomics technology, and the simulated processing method of compounds for mining original markers, to rapidly and comprehensively evaluate mechanisms of chemical transformation among PR, PR with refined honey (HP), and PR with licorice (LP). In this strategy, the advanced ultra-high performance liquid chromatography coupled with quadrupole time-of-flight data-independent mass spectrometry (UHPLC-Q-TOF-MS E ) and HPLC platform were employed to study and collect chemical composition data of PR processing. And the combination of QI and UNIFI TM software was designed to analyze relatively big molecules for PR, HP and LP sequentially, avoiding a waste of time for the identification of extra non-markers. A total of 57 relatively big markers were identified. Six small aromatic acids were quantified by targeted chemomics, as critical markers. Importantly, the hydrolysis mechanisms of saponins, isomerization of xanthones and glycolipids , and intact mechanisms of transformation, were reported by a combination of above chemomics and the simulated processing method. This study provided a rapid and comprehensive guidance to further study on processing procedures, chemical mechanisms, and construction of quality standards.

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AICHE JOURNAL · 2023 ·Vol. 70 ·期 4 ·e18342 · IF 3.7

Structural insights into variation of intramolecular acid site using phase transition experiments and computation

Dali Fu,Haodong Wang,Tan Wang,Chunming Xu,Yehua Han

Mass transfer from liquid to gas phase is a crucial process in chemical engineering. Due to the heterogeneity and dynamic nature of the phase transition process, monitoring the structural changes of compounds during this process is challenging. In this work, a combining of the mass spectrometry-based method and quantum chemistry calculations was used to study the structural changes during liquid-to-gas phase transitions. Electrospray is used to induce the transition of phenolic acid molecules from the liquid phase to the gas phase. The deprotonated structures were captured and separated using ion mobility mass spectrometry. Deprotonated structures helped to identify the most acidic functional group within the molecule. These deprotonated structures were confirmed by collision-induced dissociation and molecular collision cross-section measurements. Quantum chemistry calculations revealed the mechanisms about the variation of intramolecular acid site and “kinetic trapping.” Three liquid-to-gas phase transformation models were proposed, demonstrating that the variation in free energy among different deprotonated structures governs the thermodynamic/kinetic process of the liquid-to-gas phase conversion.

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TALANTA · 2017 · IF 4.162

An inorganic boronate affinity in-needle monolithic device for specific capture of cis-diol containing compounds

Shanxia Jin,Wei Zhang,Qin Yang,Lili Dai,Ping Zhou

In this work, inorganic boronate affinity monolith was prepared by in situ synthesis in 0.33   mm i.d. stainless steel needle through sol-gel process using tetraethoxysilane and tetrabutyl orthotitanate as the co-precursors. The morphology, structure and composition of the monolith were characterized. In contrast to conventional boronate affinity materials, inorganic boric acid was used as affinity ligand. Different compounds were used for the evaluation of the boronate affinity of this inorganic monolithic material. The monolith exhibited good selectivity towards cis-diol containing compounds. Recovery of greater than 90% was achieved for in-needle extraction of catechol under neutral conditions. Owing to the hydrophilic property of the monolith, the procedure of affinity chromatography could be performed in aqueous solution. This monolithic in-needle device will be useful for boronate affinity extraction of small-volume samples.

CAS / MDL: 76-05-1 530-59-6
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