CHEMOSPHERE
·
2023
·
IF 8.8
Hao Li,Canyuan Lin,Ruhui Ma,Yuancai Chen
In this study, the selective adsorption of aromatic compounds on mesoporous MIL-53(Al) was investigated, and followed the order: Biphenyl (Biph) > Triclosan (TCS) > Bisphenol A (BPA) > Pyrogallol (Pyro) > Catechol (Cate) > Phenol (Phen), and exhibited high selectivity toward TCS in binary compounds. In addition to hydrophobicity and hydrogen bonding, π–π interaction/stacking predominated, and more evidently with double benzene rings. TCS-containing halogens could increase π interaction on the benzene rings via forming Cl–π stacking with MIL-53(Al). Moreover, site energy distribution confirmed that complementary adsorption mainly occurred in the Phen/TCS system, as evidenced by Δ Q pri (the decreased solid-phase TCS concentration of the primary adsorbate) < Q sec (the solid-phase concentrations of the competitor (Phen)) . In contrast , competitive sorption occurred in the BPA/TCS and Biph/TCS systems within 30 min due to Δ Q pri = Q sec , followed by substitution adsorption in the BPA/TCS system, but not for the Biph/TCS system, likely attributed to the magnitude of energy gaps (E g ) and bond energy of TCS (1.80 eV, 362 kJ/mol) fallen between BPA (1.74 eV, 332 kJ/mol) and Biph (1.99 eV, 518 kJ/mol) according to the density-functional theory of Gaussian models. Biph with a more stable electronic homeostasis than TCS lead to the occurrence of substitution adsorption in the TCS/BPA system, but not in the TCS/Biph system. This study provides insight into the mechanisms of different aromatic compounds on MIL-53(Al).
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Jingwei Li,Zhengyi Huang,Cong Wang,Lei Tian,Xiaoqing Yang,Rongfu Zhou,Mohamed Nawfal Ghazzal,Zhao-Qing Liu
Refining carrier transfer in bandgap-broken heterojunctions, which consist of two semiconductors with broken bandgaps, is crucial yet highly challenging for photocatalysis. Herein, we incorporated amorphous carbons (AC) into the bandgap-broken V 2 O 5 /GdCrO 3 heterojunctions, inducing a linkage effect to facilitate photoexcited carrier transfer. The created V-O-C and Cr-O-C bonds in V 2 O 5 -AC-GdCrO 3 interfaces show almost identical orbital energies to overcome the broken-gap energy barriers at interfaces. The holes at GdCrO 3 ’s valence band and electrons at V 2 O 5 ’s conduction band tent to migrating toward the carbon ring of amorphous carbon via Cr-O-C and V-O-C bonds, thereby enhancing carrier separation of bandgap-broken V 2 O 5 /AC/GdCrO 3 heterojunction. By controlling the relative amount of metal-O-C bonds in the interface, the modulation of charge transfer kinetics was also achieved on V 2 O 5 /AC/GdCrO 3 , resulting in ∼7 times higher of H 2 generation than V 2 O 5 /GdCrO 3 . The concept could be expanded to the other carbon allotropes, including graphene, carbon nanotube, and graphdiyne conjugated structures, demonstrating a universal strategy in reaching optimal charge transfer of broken-bandgap heterojunctions for photocatalytic H 2 production.
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EUROPEAN POLYMER JOURNAL
·
2023
·
IF 6
Zicheng Fan,Insub Noh,Changlong Zhuang,Qingqing Liu,Yanbin Wang,Hyung Do Kim,Meng Yue,Hideo Ohkita,Biaobing Wang
With the rapid development and application of 5G technology, design and fabrication of lightweight polymer materials with excellent flame retardancy, low dielectric constant, and high thermal insulation is a worthy but great challenge. In this study, a polar polyimide (PI) contain amide group was designed and incorporated into epoxy resin (EP) to fabricate multifunctional materials combing a small molecule named phenoxycycloposphazene (HPCTP). Due to the synergistic effect of PI and HPCTP in flame retardant, EP blend passed UL-94 V-0 rating only needing 3 wt% PI and 1 wt% HPCTP, meanwhile the limited oxygen index (LOI) obviously increased from 23.8% to 35.0%. More importantly, the dielectric constant obviously decreased at a wide range from 10 −1 to 10 7 Hz and the thermal conductivity also reduced by more than 45% from 0.236 to 0.127 W m −1 K −1 . Due to the good compatibility and reactivity between PI and EP, PI was uniformly dispersed and connected EP to construct intimate 3D interpenetrating polymer network, and thus the tensile and flexural properties were slightly enhanced. Moreover, combustion parameters, including peak heat release rate (PHRR), total heat release (THR), smoke produce rate (SPR) and total smoke production (TSP), all indicated that EP composites significantly reduced fire risk. Overall, this study offers a promising strategy to fabricate flame retardant EP composites with outstanding comprehensive performances.
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APPLIED ORGANOMETALLIC CHEMISTRY
·
2023
·Vol. 37
·期 10
·e7230
·
IF 3.9
Dingning Chen,Haojie Yu,Li Wang,Sergey Z. Vatsadze,Jinyi Liu,Yu Wang
Ferrocene-based compounds are promising burning rate catalysts due to their attractive catalytic activity, flammability, and non-toxic performance. Unfortunately, the high-migration issue of the ferrocene-based catalysts makes it challenging to store composite solid propellants for a long time. Therefore, a dendrimer containing ferrocene units with anti-migration ability was designed herein. The introduction of polar groups provides a large number of interaction sites for anti-migration, and no migration of the dendrimer in the propellant was observed after 4 weeks of the aging test. For catalytic performance, the results showed that the thermal decomposition temperature of ammonium perchlorate could be reduced from 404°C to 369°C by adding 3 wt% ferrocene-based dendrimer. Moreover, compared with the propellant mixed with Catocene, the propellant containing ferrocene-based dendrimer showed a lower pressure exponent (0.47) and a higher burning rate (2.03 mm·s −1 , at 0.1 MPa).
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CARBON
·
2023
·
IF 10.9
Yang Zhao,Biao Ma,Xiaomei Liu,Ning Li,Yang Li,Xiaobin Fan,Wenchao Peng
Recently, single atomic metals supported on carbon materials have attracted great interests because of their high catalytic activity and stability in peroxymonosulfate (PMS)-based Fenton-like process. Herein, we propose a convenient strategy to synthesize Co single atoms supported on nitrogen-doped carbon spheres (Co@MNC) via microwave treatment. The microwave irradiation can simultaneously induce the formation of carbon defects and immobilize the Co single atoms in N doped carbon support in a few minutes. The obtained Co@MNC can activate PMS for efficient catalytic oxidation of organic pollutants. The radical quenching tests and electron paramagnetic resonance (EPR) verify that Co (IV)-oxo species, 1 O 2 , and O 2 •− are responsible for the remediation of organic pollutants. Density functional theory (DFT) calculations confirm that unique and low coordinated Co–N 2 on void or edge defects are favorable for PMS adsorption. The electrons will then transfer from Co atoms to adsorbed PMS via the bonded N. Co (IV)-oxo species and other ROSs are therefore generated for pollutants degradation. This work provides a fast method for the synthesis of single atom catalysts for efficient Fenton-like reactions.
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ENVIRONMENTAL POLLUTION
·
2023
·
IF 8.9
Yingying Sun,Jie Chen,Wei Wang,Lizhong Zhu
Persistent organic pollutants (POPs) in agricultural soil often triggered metabolic alterations and phytotoxicity in plants, ultimately threatening crop quality. Unraveling the phytotoxic mechanisms of POPs in crops is critical for evaluating their environmental risks. Herein, the molecular mechanism of POP-induced phytotoxicity in rice ( Oryza sativa L.) was analyzed using metabolic profile, enzyme activity , and gene expression as linkages, including polycyclic aromatic hydrocarbons, polybrominated diphenyl ethers , polychlorinated biphenyls, and phthalate esters. Despite no observable changes in phenotypic traits (e.g., biomass and length of aboveground), the levels of reactive oxygen species (ROS) were promoted under stresses of the tested POPs, particularly 2,2′,4,4′-tetrabromodiphenyl ether (BDE-47), dibutyl phthalate (DBP), and di(2-ethylhexyl) phthalate (DEHP). Metabolomics analysis revealed that ROS contents positively correlated with metabolic perturbation levels ( r = 0.83), among which the galactose metabolism was significantly inhibited when exposed to DBP, DEHP, or BDE-47. The α-Galactosidase (α-Gal) involved in galactose metabolism was targeted as the key enzyme for the phytotoxicity of DBP, DEHP, and BDE-47, which was revealed by the inhibition of saccharide levels (45.5−82.1%), the catalytic activity of α-Gal (18.5−24.3%), and the gene expression (28.5−34.5%). Molecular docking simulation suggested that the three POPs occupied the active sites of α-Gal and formed a stable protein-ligand complex, thus inhibiting the catalytic activity of α-Gal. Partial least-squares regression analysis indicated that α-Gal activity was negatively associated with hydrogen bond acceptor, rotatable bond, and topological polar surface area of POPs. The results offered novel insights into the molecular mechanisms of phytotoxicity of POPs and provided important information for evaluating the environmental risk of POPs.
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NATURE
·
2023
·Vol. 621
·期 7979
·511-515
·
IF 64.8
Yang Guangxu,Gong Zhenggang,Luo Xiaolin,Chen Lihui,Shuai Li
Plywood is widely used in construction, such as for flooring and interior walls, as well as in the manufacture of household items such as furniture and cabinets. Such items are made of wood veneers that are bonded together with adhesives such as urea–formaldehyde and phenol–formaldehyde resins 1 , 2 . Researchers in academia and industry have long aimed to synthesize lignin–phenol–formaldehyde resin adhesives using biomass-derived lignin, a phenolic polymer that can be used to substitute the petroleum-derived phenol 3 , 4 , 5 , 6 . However, lignin–phenol–formaldehyde resin adhesives are less attractive to plywood manufacturers than urea–formaldehyde and phenol–formaldehyde resins owing to their appearance and cost. Here we report a simple and practical strategy for preparing lignin-based wood adhesives from lignocellulosic biomass. Our strategy involves separation of uncondensed or slightly condensed lignins from biomass followed by direct application of a suspension of the lignin and water as an adhesive on wood veneers. Plywood products with superior performances could be prepared with such lignin adhesives at a wide range of hot-pressing temperatures, enabling the use of these adhesives as promising alternatives to traditional wood adhesives in different market segments. Mechanistic studies indicate that the adhesion mechanism of such lignin adhesives may involve softening of lignin by water, filling of vessels with softened lignin and crosslinking of lignins in adhesives with those in the cell wall.
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Polymers
·
2023
·Vol. 15
·期 16
·3490
·
IF 5
Yujie Wang,Mengmeng Zhao,Yazhou Chen,Haifeng Bao,Chen Li
Dendrite growth and parasitic reactions with liquid electrolyte are the two key factors that restrict the practical application of the lithium metal anode. Herein, a bis(benzene sulfonyl)imide based single-ion polymer artificial layer for a lithium metal anode is successfully constructed, which is prepared via blending the as-prepared copolymer of lithiated 4, 4′-dicarboxyl bis(benzene sulfonyl)imide and 4,4′-diaminodiphenyl ether on the surface of lithium foil. This single-ion polymer artificial layer enables compact structure with unique continuous aggregated Li+clusters, thus reducing the direct contact between lithium metal and electrolyte simultaneously, ensuring Li+transport is fast and homogeneous. Based on which, the coulombic efficiency of the Li|Cu half-cell is effectively improved, and the cycle stability of the Li|Li symmetric cell can be prolonged from 160 h to 240 h. Surficial morphology and elemental valence analysis confirm that the bis(benzene sulfonyl)imide based single-ion polymer artificial layer effectively facilitates the Li+uniform deposition and suppresses parasitic reactions between lithium metal anode and liquid electrolyte in the LFP|Li full-cell. This strategy provides a new perspective to achieve a steady lithium metal anode, which can be a promising candidate in practical applications.
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ChemistrySelect
·
2023
·Vol. 8
·期 29
·e202300512
·
IF 2.1
Kangjing Wang,Xinyi Dong,Ting Li,Qian Wang,Zhongyang Ding,Weifu Dong
Graphical The contact angle of modified starch was changed from 12.2° to 71.5°, and the particle size was changed from ∼10 μm to ∼300 nm. In the subsequent enzyme catalyzed reaction, the immobilized enzyme is adsorbed at the water oil interface, thereby improving the lipase activity. As a natural macromolecular material, starch is an ideal carrier for enzyme immobilization because of its widely available source, easy regeneration and excellent biodegradability. However, the natural starch cannot be directly used for immobilization due to the large particle size and excessive hydrophilicity. In this paper, the epoxy groups were grafted onto esterified starch by bifunctional reagents. The grafting efficiency of epoxy groups was increased by starvation drop addition. The changes of contact angle and particle size are conducive to the adsorption of immobilized enzyme at the water oil interface in the subsequent enzyme catalytic reaction, hence improve of the lipase activity. The maximum amount of lipase mobilized on such modified starch was ∼143.7 mg/g, which was near 40 mg/g higher than that of those from direct crosslinking. The immobilized enzymes showed excellent resistance to organic solvents and good reusability. Immobilization of lipases on epoxy-functionalized starch nanoparticles can potentially improves the possibility of enzymes industrial application.
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INDUSTRIAL CROPS AND PRODUCTS
·
2022
·
IF 6.449
Jinsong Wang,Farzad Seidi,Yang Huang,Huining Xiao
Incorporating corrosion inhibitors in the formulation of coatings can yield active coatings which are able to provide a sustained release of the corrosion inhibitor in the case of emergence of microcrack in the structure of the coating. Herein, we developed bio-based polyurethane sublayer coatings with strong anticorrosion performances. First, lignin-corrosion inhibitor (LCI) conjugate was obtained through conjugation of nicotinic acid to lignin through hydrolytically cleavable ester linkage to afford the steady release of low concentrations of corrosion inhibitor in case of the emergence of microcracks. Subsequently, solution polyaddition of LCI with diisocyanates and polypropylene glycol and coating on the stainless steel surface afford the polyurethane coatings. Coating with a thickness of 16 µm increased the E corr from − 481 mV (for bare steel) to + 187 mV and reduced both I corr and corrosion rate more than 6700 times. As an added benefit, after creating artificial cracks on the surface of the coating, the release of corrosion inhibitors gradually increased the impedance value, indicating a thin barrier layer has formed within the cracks.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2022
·
IF 8.025
Lan Chen,Zhanming Liang,Xiaoxuan Zhang,Liming Zhang,Shuangfei Wang,Changzhou Chen,Ling Zeng,Douyong Min
Lignin is the most naturally abundant source of aromatics for phenolic chemicals, bioenergy sources, and functional materials. Recent works are devoted to the acid-catalyzed organosolv extraction for improving the lignin valorization. However, β –aryl ethers are mostly cleaved to form carbon–carbon bonds under the acidic condition. In this work, lignin isolated with methanolic hydrochloric acid (MHL) was compared with conventional milled wood lignin (MWL). The methanol incorporated into lignin as α –OCH 3 to prevent the cleavage of β –aryl ethers. As a result, the yield of MHL was over 12 times that of MWL. The MHL appeared a regular granular structure with an average diameter of 100 nm. Analysis of 13 C– 1 H HSQC NMR spectra showed that MHL contained 42.6 % β –O–4 linkages whereas 35.9 % for the MWL, as well as 6.5 % β –5 and 3.2 % β – β , which was less than MWL. Moreover, 13 C NMR spectroscopy confirmed that MHL was mainly isolated by the cleavage of the associated carbohydrates rather than the degradation of β –aryl ether bonds. Therefore, MHL can be utilized more as a native lignin representative than MWL for studying the physicochemical properties and the interior structures of the protolignin.
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CARBOHYDRATE RESEARCH
·
2022
·
IF 2.975
Huifang Ren,Xiao-Yang Yue,Wen-Sheng Dong
We propose a new approach for the synergistically catalytic conversion of cellulose to levulinic acid (LA) in water by SO 3 H-functionalized ionic liquid (SFIL) and lanthanide chloride (LnCl 3 ). Compared with using 1-methyl-3-(3-sulfopropyl)imidazolium chloride ([MIMPS]Cl) only, the LA yield using [MIMPS]Cl and ErCl 3 increased by 14.4% and 13.6% at 50 mol% of IL and 30 mol% of IL, respectively. Moreover, the combined [MIMPS]Cl and ErCl 3 system can tolerate high concentrations of substrates and maintain high activity at eleven runs. We also investigated the effects of the cation structure of ionic liquids (alkyl chain length, hydroxyl groups on the side chains, and aromatic properties) on LA production. The observations can provide useful information for designing efficient ionic liquid catalysts for biomass utilization.
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危险品化学品经营许可证（带存储）