Batteries & Supercaps
·
2022
·Vol. 6
·期 3
·e202200434
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IF 6.043
Han Wang,Wentao Zou,Chao Liu,Yi Sun,Yi Xu,Weiwei Sun,Yong Wang
Graphical Coordination strategy has been adopted to fabricate the Co ion intercalated two-dimensional COF composite, which delivers improved lithium-storage performances and mechanism as the anode for lithium-organic batteries. As a new kind of crystalline porous polymers, covalent organic frameworks (COFs) exhibit great potential as electrode materials for rechargeable metal-ion batteries due to their stable and adjustable structure, high porosity and abundant electrochemical active centers. In this paper, facile one-step synthesis process is proposed to obtain the cobalt ion intercalated two-dimensional β -ketoenamine-linked COF (Co−DAAQ−TFP-COF, denoted as Co-COF). The intercalation of Co ion in adjacent two layered structure of COF via coordination effects can activate the Li + storage ability of aromatic ring in the original COF, greatly improve the utilization of redox active sites, shorten the migration length of electrons and ions, and promote fast lithium reaction kinetics. Adopted as the anode for lithium-ion batteries, substantial improvement on the reversible capacity and cycling performance can be achieved for the obtained Co intercalated COF electrode (780 mAh g −1 after 200 cycles at 100 mA g −1 ) compared to original COF electrode (120 mAh g −1 under the same condition). The two-dimensional COF materials with morphology justification and/or performance improvement via metal ion intercalation would promote the application of COF related electrodes for other energy-storage fields.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Yichuan Wang,Xiaojin Zhang,Yu Dai,Fan Xia
Organometallic nanozymes, organometallics of which mimic the cofactor of natural enzymes, have the advantages of tunable catalytic activity, high stability, and material variety. By assembling organometallics (catalytic site) on inorganic nanoparticles (support), organometallic nanozymes have been rationally designed, but modulating their assembly and activity remains a tough challenge. Here, we construct a photo-modulated organometallic nanozyme by anchoring azobenzene-modified triethylenetetramine (Azo-N4) to the surface of β-cyclodextrin-capped gold nanoparticles (AuNP@CDs) through host–guest interaction, followed by Zn(II) coordination to form organometallics. The catalytic site derives from the outer organometallic layer. The nanozyme catalyzes the hydrolysis of 4-nitrophenyl acetate to 4-nitrophenol and the catalytic signal is used to detect Zn(II). Due to the photoisomerization of azobenzene, the supramolecular assembly of host–guest interaction is modulated by light. The disassembly leads to cascade catalysis of AuNP@CDs-Azo-N4-Zn and the recovery of AuNP@CDs. Our study provides a new idea and reference for the rational design and activity modulation of organometallic nanozymes.
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METALLURGICAL AND MATERIALS TRANSACTIONS B-PROCESS METALLURGY AND MATERIALS PROCESSING SCIENCE
·
2023
·Vol. 54
·期 2
·712-733
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IF 3
Zhang Xi,Na Hao,Liu Pengyao,Wang Yajun,Li Junguo,Meng Qian,Li Guopeng
Regulating the phase transformation of γ → β in dicalcium silicate (C 2 S) can effectively improve the hydration activity and recycling rate of AOD slag; however, the evolution law for γ → β in C 2 S has not been extensively investigated. In this study, a novel “two-step” γ → α ′ L → β phase transformation method in C 2 S was designed based on the study of the pure C 2 S phase at a nonequilibrium state in the low- and middle-temperature ranges. The “two-step” method can be used to realize the transformation from needle-like nanostructured γ -C 2 S grains to lamellar-structured β -C 2 S grains, exhibiting the trend of interlaminar peeling accompanied by expansion of the particle volume and leading to the appearance of macroscopic lamellar cracking in β -C 2 S particles. In addition, the β -C 2 S mass fraction in AOD slag treated by water cooling at 680 °C reaches a maximum value of 47.5 wt pct, while the treated AOD slag presents abundant holes and defects, which can effectively enlarge the hydration contact area.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Shaokun Ling,Xiaoyan Qin,Chang chen,Kai Meng,Yifeng Yan,Junyun Ming,Sen Liao,Yingheng Huang,Lei Hou
Despite long-term development of LEDs, problems urgent to resolve is still existing. The most outstanding problem to tackle is luminescent stability at high temperature working situation. In this study, a novel type of β-NaYF 4 based phosphor incorporated with Eu 3+ and Tb 3+ is reported. A series of β-NaYF 4 :0.065Eu 3+ , x Tb 3+ ( x = 0.001, 0.002, 0.003, 0.004, 0.005) phosphors were synthesized by hydrothermal method . The sample β-NaYF 4 :0.065Eu 3+ ,0.002Tb 3+ possesses optimal luminescent property at room temperature. The mechanism of energy transfer from Tb 3+ to Eu 3+ ion is quadrupole-quadrupole interactions. The sample β-NaYF 4 :0.065Eu 3+ ,0.002Tb 3+ demonstrates zero thermal quenching (ZTQ) property at 303 K to 383 K. According to XRD and XPS characterizations, nonequivalent replacement between intrinsic ion Na + and Y 3+ were discovered, which finally leads to production of crystal defects. According to electron paramagnetic resonance (EPR) characterization and density functional theory (DFT) calculation, the type of crystal defect of β-NaYF 4 :0.065Eu 3+ ,0.002Tb 3+ is confirmed to be V Y vacancies which are the predominant defect of crystal. The depths and densities of defects were calculated according to data of thermoluminescence spectra (TL spectra). Crystal defects play the role of electrons traps that could store electrons. Electrons stored in traps will be excited to excitation state of Eu 3+ under the thermal stimulation to offset undesirable impact of thermal quenching (TQ), which leads to ZTQ property of the sample β-NaYF 4 :0.065Eu 3+ ,0.002Tb 3+ . The CRI and CCT of fabricated WLED are 3830 K and 84.1, respectively.
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APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Huijing Wang,Xi Quan,Qinyi Xiong,Linlin Yin,Yu Tian,Jun Zhang
In recently year, cuprous oxide(Cu 2 O) has been proved to be an important photocatalyst for fast removal of contaminants. However, as we known that the single Cu 2 O cannot get the satisfactory degradation efficiency. Herein, a new photocatalyst was prepared by coating β-cyclodextrin on Cu 2 O(CuCD) under mild hydrothermal conditions, reducing the particle size of cuprous oxide from 200 nm to 40 nm. The as-prepared CuCD exhibit excellent photocatalytic activity , which degradation rate of tetracycline(TC), methylene orange(MO) and congo red(CR) increased by 2.0, 1.7 and 2.1 times, respectively, compared to pristine Cu 2 O in reaction system. This design confirms the synergistic effect of adsorption and photocatalysis due to the introduction of β-cyclodextrin on Cu 2 O, which can provide mass and electron transfer channels to accelerate the separation and migration of photogenerated electrons. Overall, this work provides an important step in developing Cu 2 O-based hybrids for wastewater treatment.
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WATER RESEARCH
·
2023
·
IF 12.8
Yuanping Fang,Congli Chen,Bin Cui,Dandan Zhou
Storing reclaimed water via managed aquifer recharge (MAR) is an effective strategy for alleviating groundwater overdraft and achieving water resource recycling simultaneously. However, β-lactam antibiotics in the reclaimed water can induce stress on aquifer system, reshape microbial community, and affect the emergence and prevalence of antibiotic resistance genes (ARGs). In this study, three sandy soil columns (H 1.5 m, ID 14 cm) were employed to simulate MAR, and synthetic reclaimed water containing either amoxicillin (AMO), ampicillin (AMP) or oxacillin (OXA) was continuously recharged for 120 d The temporal and spatial attenuation of β-lactams and nitrogen was studied, and microbial collaboration and the resistance mechanism were elaborated. Biodegradation is the main pathway for β-lactams elimination, AMO and AMP were eliminated when migrating 30 cm, while the attenuation of OXA experienced in the whole column with final removal efficiency of 82%. Moreover, refractory OXA induced more ARGs production, and approximately 10% and 13% higher than that of AMO and AMP columns. Efflux pump and antibiotics inactivation were the two major resistance mechanisms. NO 3 − -N gradually decreased (by 26%, 38%, and 49% for AMO, AMP, and OXA, respectively) along the recharge direction. Microbial co-occurrence network revealed that nitrogen-cycling bacteria were the keystone species in aquifer community, and ammonation provided NH 4 + -N for the nitrification process of ammonia-oxidizing archaea (AOA), promoting the further denitrification for nitrogen removal in MAR process. Nitrogen-cycling bacteria were the key and active ARG hosts, which could keep nitrogen transformation activity under antibiotics stress. In sum, nitrogen-cycling bacteria exhibited intimate collaboration and elastic resistance in response to the malnutrition environment and β-lactams exposure during MAR.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Rui Jiao,Yanming Wang,Yuxia Pang,Dongjie Yang,Zhixian Li,Hongming Lou,Xueqing Qiu
Metal–organic frameworks (MOFs) have become promising accommodation for enzyme immobilization in recent years. However, the microporous nature of MOFs affects the accessibility of large molecules, resulting in a significant decline in biocatalysis efficiency. Herein, a novel strategy is reported to construct macroporous MOFs by metal competitive coordination and oxidation with induced defect structure using a transition metal (Fe2+) as a functional site. The feasibility of in situ encapsulating β-glucosidase (β-G) within the developed macroporous MOFs endows an enzyme complex (β-G@MOF-Fe) with remarkably enhanced synergistic catalysis ability. The 24 h hydrolysis rate of β-G@MOF-Fe (with respect to cellobiose) is as high as approximately 99.8%, almost 32.2 times that of free β-G (3.1%). Especially, the macromolecular cellulose conversion rate of β-G@MOF-Fe reached 90% at 64 h, while that of β-G@MOFs (most micropores) was only 50%. This improvement resulting from the expansion of pores (significantly increased at 50–100 nm) can provide enough space for the hosted biomacromolecules and accelerate the diffusion rate of reactants. Furthermore, unexpectedly, the constructed β-G@MOF-Fe showed a superior heat resistance of up to 120 °C, attributing to the new strong coordination bond (Fe2+–N) formation through the metal competitive coordination. Therefore, this study offers new insights to solve the problem of the high-temperature macromolecular substrate encountered in the actual reaction.
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Polymers
·
2023
·Vol. 15
·期 4
·839
·
IF 5
Yin Tang,Tang Zhu,Huichao Liu,Zheng Tang,Xingwen Kuang,Yongna Qiao,Hao Zhang,Caizhen Zhu
Hydrogel coatings that can endow various substrates with superior properties (e.g., biocompatibility, hydrophilicity, and lubricity) have wide applications in the fields of oil/water separation, antifouling, anti-bioadhesion, etc. Currently, the engineering of multifunctional hydrogel-coated materials with superwettability and water purification property using a simple and sustainable strategy is still largely uninvestigated but has a beneficial effect on the world. Herein, we successfully prepared poly(2-acrylamido-2-methyl-1-propanesulfonic acid) hydrogel/β-FeOOH-coated poly(vinylidene fluoride) (PVDF/PAMPS/β-FeOOH) membrane through free-radical polymerization and the in situ mineralization process. In this work, owing to the combination of hydrophilic PAMPS hydrogel coating and β-FeOOH nanorods anchored onto PVDF membrane, the resultant PVDF/PAMPS/β-FeOOH membrane achieved outstanding superhydrophilicity/underwater superoleophobicity. Moreover, the membrane not only effectively separated surfactant-stabilized oil/water emulsions, but also possessed a long-term use capacity. In addition, excellent photocatalytic activity against organic pollutants was demonstrated so that the PVDF/PAMPS/β-FeOOH membrane could be utilized to deal with wastewater. It is envisioned that these hydrogel/β-FeOOH-coated PVDF membranes have versatile applications in the fields of oil/water separation and wastewater purification.Keywords:hydrogel coating;photo-fenton catalysis;PVDF membrane;oil/water separation;water purification
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2023
·
IF 8.2
Zhen Zhang,Shanlin Cui,Ruixue Ma,Qiuyang Ye,Jiahui Sun,Yaming Wang,Chuntai Liu,Zhen Wang
High-toughness biodegradable poly(lactic acid) (PLA) has always been intensively pursued on the way of replacing traditional petroleum-based plastics. Regulating microstructures to achieve self-toughening holds great promise due to avoidance of incorporating other heterogeneous components. Herein, we propose a straightforward and effective way to tailor microstructures and properties of PLA through melt-stretching and quenching of slightly crosslinked samples. The melt stretching drives chains orientation and crystallization at high temperature, while the quenching followed can freeze the crystallization process to any stage. For the first time, we prepare a type of transparent and low-crystalline PLA filled with rod-like β-form shish, which displays an outstanding tensile toughness, almost 17 times that of the conventional technique-processed one. This mechanical superiority is enabled by an integration of high ductility due to oriented chain network, and high tensile stress endowed by nanofibrous filler's role of β-form shish. Furthermore, the mechanically toughened PLA is demonstrated to generate the richest micro-cracks and shear bands under loading, which can effectively dissipate the deformational energy and underlie the high toughness. This work opens a new prospect for the bottom-up design of high-performance bio-based PLA materials that are tough, ductile and transparent by precise microstructural regulation through scalable melt processing route.
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JOURNAL OF PHARMACY AND PHARMACOLOGY
·
2022
·Vol. 75
·期 1
·129-138
·
IF 4.81
Li Shi-ying,Shi Chuan-jian,Fu Wei-ming,Zhang Jin-fang
BackgroundBerberine, a non-prescription medicine clinically applied for diarrhoea and gastroenteritis. Recent studies have demonstrated that it possesses anti-tumour properties in colorectal cancer, but the exact molecular mechanism remains obscure.ObjectivesTo elucidate the underly molecular mechanisms of berberine in colorectal cancer from a perspective of epigenetics, and tried to explore the role of lincROR-Wnt/β-catenin molecular axis in the berberine induced the anti-tumour activity in colorectal cancer.MethodsThe effects of berberine on cell growth, cell cycle and apoptosis were examined in CRC cells. The in vivo effect of berberine on tumour growth was investigated using a xenograft mice model. Moreover, lincROR and Wnt/β-catenin signalling were detected by luciferase activity, qRT-PCR and western blotting assays.Key findingsBerberine suppressed cell growth in vitro via inducing cell cycle arrest and apoptosis in CRC cell, and inhibited tumourigenesis in vivo. LincROR was significantly down-regulated by berberine, inducing the inactivation of the canonical Wnt/β-catenin signalling, meanwhile, the overexpression of lincROR partially reversed the suppressive effects on tumour growth and Wnt/β-catenin signalling induced by berberine.ConclusionsBerberine inhibits tumour growth partially via regulating the lincROR-Wnt/β-catenin regulatory axis, which provides a strategy for the design of anti-tumour drugs for CRC patients after our advanced validation.
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Frontiers in Microbiology
·
2022
·
IF 6.064
Xiaowei Gong,Fan Li,Yupeng Liang,Xiulin Han,Mengliang Wen
Biosynthesis of β -ionone by microbial cell factories has become a promising way to obtain natural β -ionone. The catalytic activity of carotenoid cleavage dioxygenase 1 (CCD1) in cleavage of β -carotene to β -ionone severely limits its biosynthesis. In this study, NtCCD1-3 from Nicotiana tabacum with high ability to cleave β -carotene was screened. Multiple strategies for improving the β -ionone yield in Saccharomyces cerevisiae were performed. The results showed that NtCCD1-3 could cleave a variety of caroteniods at the 9,10 (9',10') double bonds and lycopene at the 5,6 (5',6') positions. The insertion site delta for NtCCD1-3 gene was more suitable for enhancing the yield of β -ionone, showing 19.1-fold increase compared with the rox1 site. More importantly, mutant K38A of NtCCD1-3 in membrane-bonding domains could greatly promote β -ionone production by more than 3-fold. We also found that overexpression of the NADH kinase Pos5 could improve β -ionone yield up to 1.5 times. These results may provide valuable references for biosynthesis of β -ionone.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
·
2022
·
IF 4.831
Kun Ge,Yihong Huang,Hanqiang Zhang
In this paper, we report a novel surface-enhanced Raman spectroscopy (SERS) substrate based on hierarchical β-Bi 2 O 3 /Au 2 Ag 2 microspheres for rapid, sensitive and selective detection of environment pollutants including o -dianisidine ( o -diASD) and Hg 2+ in environmental samples. The sheet-like β-Bi 2 O 3 not only provides large specific surface areas for adsorption of molecules and AuAg, but also emerges as semiconductor matrix with chemical enhancement combined with AuAg with electromagnetic enhancement, making promising SERS activity. Particularly, the β-Bi 2 O 3 /Au 2 Ag 2 shows high SERS performance for 4-mercaptobenzoic acid and TMB with minimum detectable concentration of 0.1 μg/L with enhancement factor of 3.1 × 10 7 and 6.3 × 10 7 , respectively. The density functional theory simulations were further adopted to explain the high SERS activity and selectivity for o -diASD and TMB. Finally, the β-Bi 2 O 3 /Au 2 Ag 2 was applied to direct detection of o -diASD, and indirect detection of Hg 2+ by TMB marking in environmental samples. The linearity range of 0.5–200.0 and 0.2–500.0 μg/L with limit of detection of 0.2 and 0.07 μg/L for o -diASD and Hg 2+ ions can be achieved, respectively. This method provides a novel strategy in designing and fabricating SERS substrates with high performance for rapid, sensitive and accurate analysis of environmental pollutants.
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