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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

Organophosphorus modified hollow bimetallic organic frameworks: Effective adsorption and catalytic charring of pyrolytic volatiles

Xiu Wang,Tong Wu,Jing Hong,Juguo Dai,Zhenwu Lu,Chunying Yang,Conghui Yuan,Lizong Dai

Up to now, hollow metal organic frameworks (MOFs) usually possess a single metal element, and the size and shape of hollow structure cannot be reasonably tuned. In this work, novel organophosphorus modified hollow bimetallic organic frameworks (W-Zr-MOF-DOPO) are successful synthesized. Briefly, zirconium-based MOFs octahedron is first prepared according to a modified method, then hollow bimetallic MOFs are obtained by etching with WO 4 2− under acidic condition, and organophosphorus is grafted onto it by the Kabachnik-Fields reaction. Inspiringly, the particle size of zirconium-based MOFs can be adjusted by the adding of acetic acid, thus acquiring hollow MOFs with controllable interior channels. The as obtained material is employed to reduce the fire risk of epoxy resin (EP), in which the hierarchical pores and metals can effectively facilitate the adsorption and catalytic charring of pyrolytic volatiles. Moreover, the P element of organophosphorus acts both in the condensed and gas phases, endowing EP with excellent thermal stability, fire retardancy and smoke suppression. The results indicate that the limiting oxygen index value of W-Zr-MOF-DOPO/EP composite increases from 24.6% (pure EP) to 32.2% and it can pass UL-94 V-0 rating when the additive amount is only 3 wt%. Especially, the total smoke production (14.5 m 2 ) and peak heat release rate (403 kW m −2 ) of W-Zr-MOF-DOPO/EP composite decrease by up to 36% and 58%, respectively, compared with pure EP. Therefore, this work draws novel inspirations for the rational design of polymer composites with high fire retardancy and smoke suppression performance.

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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

Facile access to highly flexible and mesoporous structured silica fibrous membranes for tetracyclines removal

Haoru Shan,Yang Si,Jianyong Yu,Bin Ding

Ceramic-based porous fibers, benefitting from their high specific surface area, and superior thermal stability as well as chemical durability, are highly desirable for efficient tetracyclines removal from wastewater. However, the current ceramic porous fibers are commonly fragile with poor recyclability during application. Here, facile access to mesoporous structured silica nanofibrous membranes (MPSNMs) with superior flexibility, high specific surface area, and large mesopore volume is provided, that is, using phase separation-driven electrospinning technique and subsequent calcination processing. The obtained single mesoporous silica nanofiber could be circularly folded into half without any fracturing, which is comparable to the bending behavior of flexible polymer-based material. The resultant MPSNMs exhibited superior adsorption capability towards tetracycline hydrochloride (TCH) and outstanding recyclability, and the capacity could reach 53.29 mg g −1 , which is more superior to most of the currently reported inorganic-based adsorbents. Furthermore, based on the calculated results of reduced density gradient (RDG) analysis and non-covalent interaction (NCI) isosurfaces, the adsorption mechanism could be the synergetic effects of hydrogen-bonding interactions and electrostatic attraction between TCH and MPSNMs. This work not only enlightens the preparation of flexible mesoporous inorganic nanofibrous membranes but also provides a reference for designing and developing new kinds of adsorbents for various fields.

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Sustainability · 2021 ·Vol. 13 ·期 5 ·2641 · IF 3.251

An Efficient Strategy for Enhancing the Adsorption Capabilities of Biochar via Sequential KMnO4-Promoted Oxidative Pyrolysis and H2O2 Oxidation

Siyao Bian,Shuang Xu,Zhibing Yin,Sen Liu,Jihui Li,Shuying Xu,Yucang Zhang

In this study, sequential KMnO4-promoted oxidative pyrolysis and H2O2oxidation were employed to upgrade the adsorption capacities of durian shell biochar for methylene blue (MB) and tetracycline (TC) in an aqueous solution. It was found that the KMnO4/H2O2co-modification was greatly influenced by pyrolysis temperature and the optimal temperature was 300 °C. Moreover, a low concentration of H2O2enabled the improvement of the adsorption capabilities greatly with the catalysis of pre-impregnated manganese oxides, addressing the shortcoming of single H2O2modification. The co-modified biochar exhibited high adsorption capabilities for MB and TC, remarkably surpassed KMnO4- and H2O2- modified biochars as well as pristine biochar. The increase of adsorption capabilities could be mainly contributed to the incorporation of MnOxand carboxyl by KMnO4-promoted oxidative decomposition and Mn-catalyzed H2O2oxidation. This would provide a novel and efficient method for preparing highly adsorptive biochar using sequential KMnO4-promoted oxidative pyrolysis and H2O2oxidation.Keywords:biochar;KMnO4/H2O2co-modification;methylene blue;tetracycline

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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

New insights into oxytetracycline (OTC) adsorption behavior on polylactic acid microplastics undergoing microbial adhesion and degradation

Ying Sun,Xuejiang Wang,Siqing Xia,Jianfu Zhao

Biodegradable plastics have been evaluated as promising alternatives for conventional polymers in various fields. Although microplastics (MPs) have been reported as vectors for pollutants in the environment ( e.g. antibiotics), knowledge about the chemicals carrying mechanisms of degradable MPs during the biodegradation process is limited. In this study, we investigated the adsorption behavior of oxytetracycline (OTC) on polylactic acid (PLA) MPs during its biodegradation process. Scanning electron microscopy (SEM) discovered the growth of scattered rod-shaped bacteria on the surface of PLA MPs. Two-dimensional correlation spectroscopy (2D-COS) combined with Fourier transform infrared spectroscopy (FTIR) identified the breakage of ester linkages and the generation of more oxygen-containing functional groups, indicating PLA biodegradation occurred. The presence of a biofilm coating increased the OTC adsorption capacity on MPs by 20.15%, mainly due to OTC complexing with chemical functional groups existing in biofilms ( e.g. N–H functional group). More oxygen-containing functional groups were exposed on the surface of PLA MPs after removing biofilms, which further increased the adsorption quantity of OTC by 39.01% through enhanced hydrogen bonding compared with biofilm coating MPs. The adsorption quantity of OTC adsorbed onto MPs first increased and then decreased with the pH ranging from 3.0 to 9.0, which was dominated by electrostatic interaction and hydrophobic interaction. In addition, the adsorption capacity of MPs was suppressed by the presence of fulvic acid (FA) due to that the adsorbed FA blocked further OTC adsorption and OTC showed higher affinity to free FA compared with MPs. These results unravel the OTC adsorption behavior of PLA MPs undergoing microbial adhesion and degradation, which could be useful for understanding the environmental sorption behavior of degradable MPs.

CAS / MDL: 75-05-8 144-62-7
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ENVIRONMENTAL POLLUTION · 2021 · IF 8.071

Impacts of bio-stimulants on pyrene degradation, prokaryotic community compositions, and functions

Manzoor Ahmad,Pandeng Wang,Jia-Ling Li,Renfei Wang,Li Duan,Xiaoqing Luo,Muhammad Irfan,Ziqi Peng,Lingzi Yin,Wen-Jun Li

Bio-stimulation of the indigenous microbial community is considered as an effective strategy for the bioremediation of polluted environments. This examination explored the near effects of various bio-stimulants on pyrene degradation, prokaryotic community compositions, and functions using 16S rRNA amplicon sequencing and qPCR. At first, the results displayed significant differences (p < 0.05) between the prokaryotic community structures of the control group, PYR (contains pyrene only), and bio-stimulants amended groups. Among the bio-stimulants, biochar, oxalic acid , salicylate , NPK, and ammonium sulfate augmented the pyrene degradation potential of microbial communities. Moreover, the higher abundance of genera, such as Flavobacterium, Hydrogenophaga, Mycobacterium, Rhodococcus, Flavihumibacter, Pseudomonas , Novosphingobium, etc., across the treatments indicated that these genera play a vital role in pyrene metabolism. Based on the higher abundance of GP-RHD and nidA genes, we speculated that Gram-positive prokaryotic communities are more competent in pyrene dissipation than Gram-negative. Furthermore, the marked abundance of nifH, and pqqC genes in the NPK and SA treatments, respectively, suggested that different bio-stimulants might enrich certain bacterial assemblages. Besides, the significant distinctions (p < 0.05) between the bacterial consortia of HA (humic acid) and SA (sodium acetate) groups from NPK, OX (oxalic acid), UR (urea), NH4, and SC (salicylate) groups also suggested that different bio-stimulants might induce distinct ecological impacts influencing the succession of prokaryotic communities in distinct directions. This work provides new insight into the bacterial degradation of pyrene using the bio-stimulation technique. It suggests that it is equally important to investigate the community structure and functions along with studying their impacts on degradation when devising a bio-stimulation technology .

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MATERIALS CHEMISTRY AND PHYSICS · 2021 · IF 4.094

Understanding photoelectrocatalytic degradation of tetracycline over three-dimensional coral-like ZnO/BiVO4 nanocomposite

Yaping Li,Xianglin Sun,Yiming Tang,Yun Hau Ng,Lintao Li,Feng Jiang,Jing Wang,Weirui Chen,Laisheng Li

The coral-like BiVO 4 was successfully constructed on ZnO nanorods grown on FTO substrates to reveal exceptional photoinduced charge migration kinetics as well as the underlying photoelectrocatalytic degradation process. The orderly ZnO nanorods array accelerated the separation of photogenerated carriers, while the three-dimensional coral structure of ZnO/BiVO 4 nanocomposite increased the efficiency of light absorption and mass transfer, thus improving the photoelectrochemical properties. Fine interfacial contact between ZnO and BiVO4 led to the optimized photoelectrochemical performance with a photocurrent density of 0.29 mA/cm2 at 0 V vs . Ag/AgCl under visible light illumination (λ ≧ 420 nm), which was 3.2 times, 1.6 times of that of pristine ZnO and BiVO4. Moreover, the photoelectrocatalytic degradation efficiency of tetracycline from the ZnO/BiVO4 nanocomposite on was c. a. 84.5% and the main degradation paths were analyzed by LC-MS. Radical scavengers were employed to evaluate the capability to produce •O 2 − and •OH active species upon visible light illumination. This study elucidated the reaction mechanisms of the ZnO/BiVO4 nanocomposite during the photoelectrocatalytic degradation process.

CAS / MDL: 144-62-7 7681-11-0
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Journal of Materials Chemistry C · 2021 ·Vol. 9 ·期 30 ·9492-9498 · IF 7.393

In situ growth of polyoxometalate in COF for trace monitoring of Ag+ and hepatocellular carcinoma biomarker via a dual responsive strategy

Jinmin Wang,Xin Xu,Limin Zhao,Bing Yan

Covalent organic frameworks (COFs) demonstrate a new trend in the field of chemical sensing mainly due to their potential for functional modification, defined pore environment and good chemical stability. Exploring functionalized-COF materials as chemosensors with low detection limits and high selectivity for biologically and environmentally important analytes is a campaign in this field. In this work, the incorporation of polyoxometalate (POM, Eu4W8) into the crystalline architecture a COF (EB-TFP) generates a functional composite material Eu4W8@EB-TFP. This material combines the merits of POM and COF together; it endows COF with outstanding luminescence properties and effectively broadens the sensing application of COF. It points out a new direction to employ POM-functionalized COF materials as efficient chemosensors to monitor trace amounts of Ag+ in environmental and CG (hepatocellular carcinoma biomarker) in biological systems. This work provides new insights into COF-based sensors and inspires the development of more versatile tools for analytical applications.

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ANALYTICAL CHEMISTRY · 2021 · IF 6.986

Identification, Quantification, and Imaging of the Biodistribution of Soot Particles by Mass Spectral Fingerprinting

Yue Lin,Xiu Huang,Yongchun Liu,Dong Cao,Dawei Lu,Zeming Feng,Qian Liu,Zhenyu Lin,Guibin Jiang

Soot is ubiquitous and has large detrimental effects on climate, air quality, and human health. However, identification of soot in carbonaceous media is very challenging due to its nanoscale carbon nature and complex sources. Due to the shortage in the methodology, until now, the fate and health effect of soot particles after inhalation are still poorly understood. Here, we report a new method for label-free identification, quantification, and imaging of soot particles in complex media based on laser desorption/ionization mass spectrometry fingerprinting. We found that soot particles from different origins and with different morphologies showed highly consistent mass spectral fingerprints deriving from peak ratios of small carbon cluster anions (C2––C10–), which enabled both accurate quantification of soot in fine particulate matter (PM2.5) samples and label-free imaging of soot particles in biological media. By using this technique, we tracked and imaged the suborgan distribution of soot particles in mice after exposure to PM2.5. The results showed that the lung is the main target organ for short-term inhalation exposure to soot particles. This study helps to better understand the inhalation toxicology of soot and also provides a practical novel methodological platform for identification, tracing, and toxicological studies of elemental carbon-based nanomaterials.

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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2021 · IF 8.128

Regeneration of porous Fe3O4 nanosheets from deep eutectic solvent for high-performance electrocatalytic nitrogen reduction

Hao Ying,Tingting Chen,Chenyun Zhang,Jiahui Bi,Zhonghao Li,Jingcheng Hao

The production of ammonia through electrocatalytic nitrogen reduction reaction (NRR) is environmentally friendly and energy-saving, but it still suffers from the low NH 3 yield rate and poor selectivity. Herein, enlightened by the unique solubility of Fe 3 O 4 in deep eutectic solvent (DES), we, for the first time, reported a DES-based regeneration strategy to fabricate porous Fe 3 O 4 nanosheets utilizing commercial Fe 3 O 4 powder as raw materials. The as-regenerated porous Fe 3 O 4 nanosheets exhibited satisfactory electrocatalytic performance toward NRR, affording a NH 3 yield rate of 12.09 μg h −1 mg −1 cat along with an outstanding Faradaic efficiency (FE) of 34.38% at −0.1 V versus reversible hydrogen electrode (RHE), in the 0.1 M Na 2 SO 4 electrolyte. The superior electrocatalytic activity of the as-regenerated Fe 3 O 4 nanosheets mainly resulted from their unique sheet-like morphology with large active surface area, high porosity, and abundant oxygen vacancies. Our proposed DES-based regeneration strategy opens a new avenue for the construction of high-performance electrocatalyst from commercial raw materials, holding great promise in NRR.

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INTERNATIONAL JOURNAL OF FOOD SCIENCE AND TECHNOLOGY · 2021 ·Vol. 56 ·期 10 ·5220-5229 · IF 3.713

Oxalic extraction of high methoxyl pectin and its application as a stabiliser

Ying-Xing Huang,Jun-Ru Qi,Jin-song Liao,Wen-Xin Jiang,Yong Cao,Jie Xiao,Xiao-Quan Yang

Summary The objective of this work was to extract high methoxyl (HM) pectin with oxalic acid, characterise its physicochemical properties and evaluate its dispersion stability in acidified milk drink (AMD). HPSEC–MALLS analysis revealed that the obtained HM pectin was high in molecular weight (522.4 kDa). The ζ-potential of the obtained HM pectin in aqueous solution at pH 4.0 was −31.5 mV. The AFM images proved that the obtained HM pectin contained several long linear molecules. The apparent diameter of AMD stabilised by the obtained HM pectin was 636 nm at the concentration of 3.0‰. The stability analysis of AMD and the microscopic observation with confocal laser scanning microscopy (CLSM) proved that the obtained HM pectin was a prominent stabiliser in AMD.

CAS / MDL: 144-62-7
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ENERGY & FUELS · 2021 · IF 3.605

Novel Deep Eutectic Solvents for Stabilizing Clay and Inhibiting Shale Hydration

Jingyuan Ma,Shaocong Pang,Wei Zhou,Boru Xia,Yuxiu An

The hydration and swelling of shale caused by water in water-based drilling fluids is one of the most important problems that causes wellbore instability. The development of high-performance shale inhibitors is an important prerequisite for ensuring the drilling of shale formations. In this study, four deep eutectic solvents (DESs) based on choline chloride (urea-DES, Gly-DES, Oxa-DES, and Cit-DES) were synthesized and introduced as promising shale inhibitors. Fourier transform infrared spectroscopy (FT-IR) and hydrogen nuclear magnetic resonance spectroscopy (1H NMR) were used to characterize the structural information on DESs. The inhibition ability of DESs was evaluated by a bentonite inhibition test, a linear swelling test, and a settlement test. Compared with the traditional inhibitors, such as potassium chloride (KCl) and polyether amine, the four DESs can effectively inhibit the hydration and swelling of shale. Five wt % DESs can maintain low rheological parameters when the content of sodium bentonite (Na-bent) was as high as 40 wt %. Among them, Gly-DES not only exhibited the most efficient inhibition capability but also had the advantage of not affecting the basic performance of the drilling fluid. Inhibitory mechanism analysis showed that the electrostatic interaction and hydrogen bonding between DESs and sodium bentonite (Na-bent) are the most important factors to inhibit clay hydration. Besides, the reduction of the surface tension of the liquid by DESs effectively weakened the driving force for water to penetrate the Na-bent layer. Finally, it is important to note that, although DESs exhibited strong inhibitory capabilities, some DESs, such as Oxa-DES and Cit-DES, are prone to adversely affect the basic performance of drilling fluids. Therefore, a careful selection is required.

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FOOD HYDROCOLLOIDS · 2021 · IF 9.147

Interactions between gut microbiota and soy hull polysaccharides regulate the air-liquid interfacial activity

Lina Yang,Jinghang Huang,Xinghui Wu,Li Li,Wenqi Cai,Lijie Zhu,Shengnan Wang,Hong Song,Danshi Zhu,Tao Ma,He Liu

The purpose of this study was to investigate the effects of interactions between gut microbiota and soy hull polysaccharides (SHPs) on the air-liquid interfacial activity. SHPs could be used as an energy source for gut microbiota metabolism, and within a certain concentration range, the acid production of gut microbiota had a SHP concentration dependence. In the process of interfacial adsorption, the polysaccharide concentration was negatively correlated with interfacial tension, and the simulated intestinal fluid viscosity and dilational modulus were positively correlated. The low concentration of SHPs had a greater impact on the diversity and structural composition of gut microbiota. 0.5% SHPs had a better effect on the proliferation of Lactobacillus . The gut microbiota degraded SHPs involved in the regulation of interfacial activity, which provided a new theoretical foundation for the utilization and absorption of polysaccharides in the intestine in vitro .

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