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APPLIED CATALYSIS A-GENERAL · 2021 · IF 5.706

Synthesis of hydrophobic nanosized hierarchical titanosilicate-1 zeolites by an alkali-etching protocol and their enhanced performance in catalytic oxidative desulphurization of fuels

Linghao Li,Wei Wang,Jian Huang,Rongmin Dun,Rui Yu,Yiwei Liu,Zile Hua

Nanosized hierarchical titanosilicate-1 zeolites ( nano TS-1_D) with variable Ti doping content were synthesized by a simple and sequent two-step procedure consisting of microporous TS-1 nanocrystal synthesis through steam-assisted dry-gel conversion and post alkali-etching treatment for mesopore formation. Comprehensive characterizations, e.g. XRD, N 2 sorption isotherms, DLS, UV-Vis, SEM, TEM and water-droplet contact angle, indicated that the resultant nano TS-1_D materials not only possess abundant intracrystal mesopores and high surface area, but importantly maintain the intrinsic surface hydrophobicity as those of microporous TS-1 zeolites. Consequently, they showed the expected superior catalytic performance in both bulky cyclohexene/cyclooctene epoxidation and phenol hydroxylation probe reactions, contrast to the microporous TS-1 and amorphous Ti-MCM-41 mesoporous counterparts. In the oxidative desulfurization of fuels, they exhibited 100% removal ability for thiophene and its bulky derivatives and excellent recyclability. In addition, a new Ti-dopant directed alkali-etching mechanism has been proposed to illustrate the synthesis of high-specific-surface-area nano TS-1_D.

CAS / MDL: 108-95-2
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Aggregate · 2021 ·Vol. 3 ·期 2 ·e147 · IF 0

Color-tunable and bright nonconjugated fluorescent polymer dots and fast photodegradation of dyes under visible light

Bingyan Han,Qifang Yan,Ze Xin,Qingdong Liu,Dan Li,Jiao Wang,Gaohong He

Nonconjugated polymer dots (PDs) without largely conjugated structures entitle their advantages such as environment friendliness, nontoxicity, and intrinsic fluorescence. However, color-tunable PDs remain a challenge. Herein, polyvinyl pyrrolidone (PVP) and ascorbic acid (AA) are used to synthesize nonconjugated PDs, namely, PA PDs with intensive blue emission. The introduction of a third component, m-phenylenediamine (MPD), redshifted the emission to green. The as-prepared color-tunable blue to green emissive PDs exhibit excellent properties, whether in solution or in solid state, originated from the mechanism of clustering-triggered emission (CTE) induced by the overlap of electron-rich atoms, the strong inter/intrachain interaction. The quantum yields of blue and green PDs reached up to 15.07% and 28.22%, respectively. Furthermore, PA PDs were successfully applied to the highly efficient photocatalytic degradation for dyes: methylene blue (MB) and methyl orange (MO) were degraded by 89.9% and 93.8% within 20 min under visible light, respectively.

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Journal of Environmental Chemical Engineering · 2021 · IF 5.909

Dual modification of BiOIO3 via doping iodine and fabricating heterojunction with basic bismuth salt: Facile synthesis, superior performance for degradation of multiple refractory organics

Xia Zhang,Xitong Yang,Bing Liu,Guifen Zhu,Jing Fan

An approach of simultaneous iodine doping and heterojunction fabricating with basic bismuth salt was proposed, Based on this, a novel I/BiOIO 3 /[Bi 6 O 6 (OH) 3 ](NO 3 ) 3 ∙1.5H 2 O (I/BiOIO 3 /BHN) photocatalyst was prepared. The photocatalytic activity was evaluated by the degradation of multiple refractory pollutants (rhodamine B, methyl orange, phenol , bisphenol A, bisphenol B, bisphenol Z) in water under solar light irradiation. Compared with single photocatalyst, the optimized sample displayed the reaction rate constant of 0.1606 min −1 , which was 69.8, 11.4 and 2.2 times of individual [Bi 6 O 6 (OH) 3 ](NO 3 ) 3 ∙1.5H 2 O, BiOI and BiOIO 3 , respectively. The performance improvement was attributed to the inhibition of charge carrier recombination by type II heterojunction formation and the expanded solar capture range caused by the springboard effect of iodine impurity level. The photocatalytic mechanism of I/BiOIO 3 /BHN was hole oxidation , followed by·OH oxidation. Besides, the I/BiOIO 3 /BHN photocatalyst in bulk structure with micrometer size and high-density could be easily separated and recovered by simple sedimentation, confirming its good application prospect in the wastewater treatment .

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Vietnam Journal of Chemistry · 2021 ·Vol. 59 ·期 6 ·813-822 · IF 0

Decomposition of glyphosate in water by peroxymonosulfate activated with CuCoFe-LDH material

Nguyen Trung Dung,Vu Dinh Thao,Nguyen Nhat Huy

In this study, the CuCoFe-layered double hydroxide was employed for the degradation of glyphosate in water via peroxymonosulfate (PMS) activation. Scanning electron microscopy, X-ray powder diffraction, energy-dispersive X-ray spectroscopy, Fourier-transform infrared spectroscopy, and Brunauer-Emmett-Teller analyses were used to characterize the material. The effects of the catalytic system, initial solution pH, and catalyst and PMS dose on the degradation efficiency of glyphosate were investigated. The results indicated that after 6 min the CuCoFe-LDH/PMS system can degrade 99.54 % of glyphosate (100 mg/L) using 100 mg/L of CuCoFe-LDH, 200 mg/L of PMS, and pH 11. In addition, radical quenching experiments prove that the reactive oxygen species (e.g., SO 4 ●- , HO ● , O 2 ●– , and 1 O 2 ) are formed and SO 4 ●- plays a decisive role in glyphosate degradation. Moreover, the CuCoFe-LDH catalyst is reusable and stable with a glyphosate removal efficiency of 90.34 % after five continuous degradation cycles.

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SEPARATION AND PURIFICATION TECHNOLOGY · 2021 · IF 7.312

Singlet oxygen-dominated activation of peroxymonosulfate by CuO/MXene nanocomposites for efficient decontamination of carbamazepine under high salinity conditions: Performance and singlet oxygen evolution mechanism

Peizhen Yang,Songrong Li,Liang Xiaofu,An Xiaojing,Dongfang Liu,Wenli Huang

The degradation of organic contaminants via traditional radical-dominated advanced oxidation processes (AOPs) under high salinity conditions was limited due to side reactions between coexisting inorganic anions and radicals. Herein, a nonradical oxidation process via peroxymonosulfate (PMS) activation by CuO/MXene for treating high-salinity organic wastewater was developed. Rapid removal efficiency of target pollutant carbamazepine (CBZ) was significantly enhanced to 95.88% within 20 min by CuO/MXene under high salinity conditions (NaCl, 200 mM), compared to the efficiency of 4.30% exhibited by PMS alone. Besides, CBZ maintained a higher removal efficiency of > 81.04% in complex highly saline wastewater composed of eight common inorganic anions. Radical quenching experiments and electron paramagnetic resonance (EPR) analysis confirmed that radical and nonradical oxidation processes were involved in the catalytic process. However, singlet oxygen ( 1 O 2 ) was identified as the primary reactive species, and its contribution rate to CBZ degradation was > 73.58% in a wide pH range (3.0-9.0). The oxygenated functional groups and the interaction between CuO/MXene and PMS facilitated the production of 1 O 2 . The degradation pathway was proposed based on the detection of intermediates. This work provided a new inspiration for the decontamination of organic contaminants under high salinity conditions via a nonradical oxidation process.

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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

Photo-assisted generation of versatile zwitterionic carboxybetaine-based hypercrosslinked polymers for separation science

Lingjue Sun,Dongsheng Xu,Yuan Shen,Jacques Crommen,Qiqin Wang,Zhengjin Jiang

Zwitterionic super-hydrophilic polymeric monoliths showed fascinating attributes because of their excellent biocompatibility, hydrophilicity, and antifouling properties. However, their commercial developments are limited by their tedious preparation process and unsatisfactory performance. 1-Carboxy- N -methyl- N -di(2-methacryloyloxyethyl)methanaminium inner salt (CBMAX), an important zwitterionic functional monomer , which exhibits excellent hydrophilicity and extremely low protein adsorption from undiluted serum. However, no carboxybetaine based monolith has been reported to date. In this study, a rapid photo-assisted generation strategy based on a sole-monomer system (CBMAX being simultaneously used as monomer and crosslinker) was proposed for preparing versatile hyper-crosslinked zwitterionic carboxybetaine polymers in capillaries within only 5 min. It is significantly faster than the conventional sole-monomer (1 h) and multi-monomer system (over 12 h) via thermally-initiated polymerization approach. Moreover, a high column efficiency of 82,000 plates/m, abundant electrostatic and hydrophilic interactions were achieved on the novel monolith due to the unique advantages of carboxybetaine. These excellent features were beneficial for the high-performance separation of various bioactive compounds (including nucleotide bases, phenols, benzoic acid and its derivatives, urea and allantoin) on this monolith. It is worth noting that this zwitterionic monolith exhibited good anti-protein adsorption ability as well as excellent enrichment capacity for N -glycopeptides from hIgG tryptic digest. In summary, the proposed photo-assisted generation strategy based on sole-monomer CBMAX is very successful and opens up a promising solution for the commercial development of zwitterionic super-hydrophilic polymeric monoliths.

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ACS ES&T Water · 2021 · IF 0

Removal of Typical Volatile Organic Compounds in Condensed Freshwater by Activated Persulfate during Interfacial Solar Distillation

Yangyi Xiao,Chenxing Li,Xiaojiao Zhou,Ningyao Tao,Miaomiao Ye

Recently, seawater desalination based on interfacial solar heating has attracted attention because of its environmental protection and high photothermal conversion efficiency. However, the high air–water interface temperature may cause freshwater quality safety risks because the volatile organic compounds (VOCs) in seawater are more likely to evaporate and condense into freshwater. In this work, typical VOCs (phenol) were prevented from entering into the condensed freshwater by using activated persulfate to take full advantage of interfacial solar distillation. The results showed that the addition of both peroxodisulfate (PDS) and peroxymonosulfate (PMS) could effectively reduce the concentration of phenol in condensed freshwater. The phenol’s distillation concentration rate (RD) was reduced from 74.4% to 14.3% with PMS and 20.5% with PDS. The Cl– was the main factor for activation of PMS, while carbon black, light, and heat were the main factors for activation of PDS. Meanwhile, PMS is better suited for removing VOCs due to its lower oxidant dosage and chlorinated disinfection byproducts compared with PDS. Finally, when real seawater samples were used as the source water for solar distillation, the water quality of typical indicators was lower than the limits set by Drinking Water Quality in China, US EPA, and WHO.

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CHINESE JOURNAL OF POLYMER SCIENCE · 2021 ·Vol. 40 ·期 1 ·56-66 · IF 3.603

Reversible CO2-, Photo- and Thermo- Triple Responsive Supramolecular Chirality of Azo-containing Block Copolymer Assemblies Prepared by Polymerization-induced Chiral Self-assembly

Sun Ya-Jing,Cheng Xiao-Xiao,Miao Teng-Fei,Ma Hao-Tian,Zhang Wei,Zhu Xiu-Lin

Polymerization-induced chiral self-assembly (PICSA) is an efficient strategy that not only allows the construction of the supramolecular chiral assemblies in a controlled manner but also can regulate the morphology in situ. Herein, a series of azobenzene-containing block copolymer (Azo-BCP) assemblies with tunable morphologies and supramolecular chirality were obtained through the PICSA strategy. The supramolecular chirality of Azo-BCP assemblies could be regulated by carbon dioxide (CO 2 ) stimulus, and completely recovered by bubbling with Ar. A reversible morphology transformation and chiroptical switching process could also be achieved by the alternative 365 nm UV light irradiation and heating-cooling treatment. Moreover, the supramolecular chirality is thermo-responsive and a reversible chiral-achiral switching was successfully realized, which can be reversibly repeated for at least five times. This work provides a feasible strategy for constructing triple stimuli-responsive supramolecular chiral nano-objects in situ .

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ACS Applied Nano Materials · 2021 · IF 5.097

Pd Nanoparticles Loaded on CoAlCe Layered Double Oxide Nanosheets for Phenol Hydrogenation

Haiping Li,Xue Wang,Yanan Liu,Yufei He,Junting Feng,Dianqing Li

The catalytic upgrading of phenolic derivatives is vital for the efficient utilization of biomass resources. Herein, we construct a reductive layered double oxide material (CoAlCe-LDO) with the Ce–Co interface and abundant oxygen vacancy (VO) via heat-treating layered double hydroxide (LDH) precursors. The support spontaneous in situ redox method is employed to prepare the supported catalyst using CoAlCe-LDO as a support and reductant. Interestingly, highly dispersed Pd nanoparticles prefer to distribute at the contact edge of the Ce–Co interface. Pd2+ is successfully reduced to Pd0 by the reductive Co/Ce sites. Due to the redox reaction between the support and Pd species, a strong metal–support interaction is introduced. The Pd/CoAlCe-LDO catalyst shows high activity for phenol hydrogenation under mild conditions and a low molar ratio of Pd to phenol. The kinetic study suggests that the highly dispersed Pd sites could preferably activate H2 molecules, thereby boosting the rapid phenol hydrogenation.

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Materials Today Chemistry · 2021 · IF 8.301

Cellulose-based fluorescent macromolecular sensors and their ability in 2, 4, 6-trinitrophenol detection

X. Jiao,H. Li,X. Cheng

This article deals with three cellulose-based fluorescent macromolecular sensors by introducing 1,8-naphthalimide fluorophore to cellulose . First, through the etherification reaction of cellulose with BrCH 2 CH 2 NH 2 , –NH 2 group–bearing cellulose CS 1 was obtained. Then, the –NH 2 group reacts with 4-bromo-1,8-naphthalic anhydride to synthesize a naphthalimide cellulose derivative ( CS 2 ). Finally, the recognition group was introduced by substituting Br atoms, and three cellulose fluorescent probes ( CS 3 , CS 4 , and CS 5 ) were obtained eventually. Structure and fluorescence properties of the macromolecular sensors were characterized and confirmed. Fluorescence detection measurements show that these probes can be used as selective and sensitive fluorescent sensors to 2,4,6-trinitrophenol (TNP). The detection limits are 0.52 μM, 0.76 μM, and 0.81 μM, indicating good detection performance. This work provides a new method for the selective detection of TNP and also a method to enlarge the application scope of cellulose.

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JOURNAL OF POROUS MATERIALS · 2021 ·Vol. 29 ·期 2 ·331-340 · IF 2.496

Gas exfoliation mechanisms of graphitic carbon nitride into few-layered nanosheets

Zheng Tao,Li Meisheng,Zhou Shouyong,Zhao Yijiang,Zhong Zhaoxiang,Chen Chenglung

Two-dimensional (2D) graphitic carbon nitride (g-C 3 N 4 ) nanosheets are widely used in photocatalysis, energy storage and membrane separation owing to their high specific surface area, rapid photogenic carrier migration rate and numerous active sites. In this study, high performance g-C 3 N 4 nanosheets with a particle size of about 290 nm were prepared by gas exfoliation. It was observed that the structure and properties of g-C 3 N 4 nanosheets prepared at 500 °C were superior as compared to 300 °C and 400 °C. The state of g-C 3 N 4 layers at different temperatures was also studied by molecular dynamics simulation. It was revealed that the liquid nitrogen (L-N 2 ) molecules could only penetrate the edge space between g-C 3 N 4 layers at 500 °C, however, no penetration took place in the layers. The traditional gas exfoliation mechanisms were observed to be incapable in explaining this phenomenon. Combining the experimental studies and molecular dynamics simulations, a novel gas exfoliation mechanism was proposed in this study so as to prepare few-layered g-C 3 N 4 nanosheets. Based on this, the L-N 2 molecules entered the edge space in g-C 3 N 4 layers and subsequently pushed deeper to exfoliate the nanosheets.

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ANALYST · 2021 ·Vol. 146 ·期 24 ·7593-7600 · IF 4.616

Simultaneous detection of 4-chlorophenol and 4-nitrophenol using a Ti3C2Tx MXene based electrochemical sensor

Ling Lei,Caoling Li,Wensheng Huang,Kangbing Wu

Developing a sensitive and rapid detection method for 4-chlorophenol (4-CP) and 4-nitrophenol (4-NP) is very important due to their high toxicity. In this work, bulk Ti3AlC2 powder was etched to Ti3C2Tx for the first time through a hydrothermal reaction in NaF/HCl solution. After ultrasonication in N-methylpyrrolidone (NMP), Ti3C2Tx powder was successfully exfoliated into multilayered Ti3C2Tx nanosheets (i.e. Ti3C2Tx MXene). The prepared Ti3C2Tx MXene not only has a large electrochemical surface area for the oxidation of 4-CP and 4-NP, but also lowers their electron transfer resistance. As a result, the oxidation signals of 4-CP and 4-NP are significantly improved on the surface of the Ti3C2Tx MXene. Based on the remarkable signal amplification of the Ti3C2Tx MXene, a sensitive and rapid method was developed for the simultaneous detection of 4-CP and 4-NP. The linear range is from 0.1 to 20.0 μM for 4-CP, and from 0.5 to 25.0 μM for 4-NP, with detection limits of 0.062 μM (4-CP) and 0.11 μM (4-NP). This method was used in wastewater samples, and the accuracy was confirmed to be good by high-performance liquid chromatography.

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