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APPLIED CATALYSIS B-ENVIRONMENTAL · 2023 · IF 22.1

Synergistic effect between Co single atoms and nanoparticles enables selective synthesis of bio-based benzimidazoles

Baoyu Wang,Mingrui Li,Songdang Zhang,Hongguo Wu,Yuhe Liao,Hu Li

Finite size effect is closely correlated with heterogeneous catalytic activity and selectivity as reducing the metal to a few nanometers, but may suffer from deficient active sites for cascade reactions. Here, a type of dual-size heterogeneous N-doped cobalt catalysts (Co SAs-NPs /NC(n)) with the coexistence of Co single-atoms (Co-SAs) and Co nanoparticles (Co-NPs) were prepared for efficient synthesis of benzimidazoles (up to 91% yield) from 2-nitroanilines and bio-based alcohols via cascade hydrogen transfer-dehydrogenative cyclization. Experimental results and density functional theory calculations suggested that the bio-alcohol dehydrogenation mainly occurs at Co-SAs sites, while Co-NPs sites remarkably facilitate the subsequent reduction of nitro species, indicating the synergistic effect between Co-SAs and Co-NPs in the coupled hydrogen transfer process. The Co SAs-NPs /NC(0.25) catalyst can be recycled and applied to a wide range of substrates (28 examples). This catalytic approach based on the metal size effect opens a new route for the direct upgrading of biomass feedstocks involving multiple reactions.

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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY · 2022 · IF 4.831

Effective and selective measurement of 2,4-dinitroaniline utilizing constructed fluorescent carbon dots sensor derived from vitamin B1

Shuangying Li,Qingxiang Zhou,Zhi Li,Menghua Liu,Yanhui Li,Chunmao Chen

2,4-Dinitroaniline is a multifunctional product and has been applicated in various fields. It has absorbed much concerns due to its large consumption and occurrence in many environmental matrices. It is urgent to explore reliable and sensitive measurement technology. Present study described an outstanding fluorescence sensor constructed with carbon dots (CDs) derived from vitamin B 1 . The CDs were fabricated by dealing with a facile hydrothermal process, and exhibited good water solubility, fluorescence stability and highly fluorescence quenching characteristics in presence of 2,4-dinitroaniline. The excitation and emission wavelengths of the obtained CDs were 305 and 378 nm, respectively. The sensor displayed good selectivity and sensitivity for 2,4-dinitroaniline. Good linearity can be achieved in two-stage of 0.2–3 μmol L −1 and 3–20 μmol L −1 . The sensor earned low detection limit for 2,4-dinitroaniline down to 0.05 μmol L −1 . The sensor has been commendably employed for analysis of 2,4-dinitroaniline in real aqueous samples with spiked recoveries in the range of 95.0–99.6%. The proposed sensor provided a promising alternative for analysis of environmental pollutants or other meaningful employment.

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JOURNAL OF HAZARDOUS MATERIALS · 2022 · IF 14.224

A paper-based microfluidic sensor array combining molecular imprinting technology and carbon quantum dots for the discrimination of nitrophenol isomers

Liang Zhu,Xuecui Mei,Zhengchun Peng,Jiao Yang,Yingchun Li

Paper-based microfluidic analytical devices (μPADs) have recently attracted attention as a rapid test kit owing to their low cost and nonrequirement for external driving pump. However, low accuracy and poor anti-interference ability of μPADs under complex detection condition limit their practical applications. Here, we present a facile way to prepare a novel fluorescence sensor-array μPAD for multi-analyte discrimination based on molecular imprinting technology , and its sensing behavior was studied by using three nitrophenol (NP) isomers (2-, 3-, and 4-NP) as the testing models. Carbon quantum dots (CQDs) emitting blue light were grafted on glass-fiber paper, followed by in-situ modification of three types of molecularly imprinted polymers (MIPs) with 2-, 3-, and 4-NP as template. Each sensing unit on the array showed differential yet cross-reactive binding affinity to NP isomers, resulting in distinct fluorescence quenching efficiency. Thus, precise distinguishment of the three NPs was realized with the MIPs/CQDs/paper-based sensor array. Furthermore, the discrimination ability of the platform was evaluated in mixtures of the NP isomers. Practicability of this apparatus was validated by identification of blind samples and 100% accuracy was achieved. The μPAD has proven to be highly sensitive and accurate, which will serve as an ideal analytical tool in the fields of environment monitoring, disease prognosis, food safety and so on.

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Analytical Methods · 2022 ·Vol. 14 ·期 10 ·1023-1030 · IF 3.532

Aggregation-induced emission monomer-based fluorescent molecularly imprinted poly(ionic liquid) synthesized by a one-pot method for sensitively detecting 4-nitrophenol

Hanxing Yang,Zhongguang Ji,Yanbo Zeng,Jian Zhang,Lifen Chen,Hailong Wang,Yiwen Yang,Longhua Guo,Lei Li

An aggregation-induced emission monomer-based fluorescent molecularly imprinted poly(ionic liquid) (AIE-FMIPIL) was synthesized for the first time with an AIE probe 4-(1,2,2-triphenylvinyl)phenyl acrylate (TPE), and an ionic liquid as dual functional monomers, and an ionic liquid as cross-linker. AIE-FMIPIL displayed a sphere-like shape and its average diameter was 410 nm. The absolute quantum yields of TPE and AIE-FMIPIL were 9.23% and 12.61%, respectively. The synergetic effect of TPE in the AIE-FMIPIL framework contributed to the higher quantum yield of AIE-FMIPIL. 4-Nitrophenol (4-NP) efficiently quenched AIE-FMIPIL with high fluorescence based on the Förster resonance energy transfer mechanism. The synthesized AIE-FMIPIL sensor was highly sensitive for 4-NP detection (linear range, 0.02–1.5 μM) in the optimal detection condition, with a low detection limit of 10 nM (S/N = 3). AIE-FMIPIL showed increased sensitivity and quenching efficiency compared with AIE-FMIP comprising a traditional monomer and cross-linker. AIE-FMIPIL exhibited selective binding to 4-NP because of the imprinted sites. AIE-FMIPIL was adopted to detect 4-NP in environmental samples.

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ANALYTICAL SCIENCES · 2022 ·Vol. 38 ·期 9 ·1181-1188 · IF 1.967

A label-free electrochemical sensor constructed with layer-by-layer assembly of GCE-AuNPs-Q[7]·HAuCl4 for detection of diphenylamine

Wang Cheng-Yan,Ge Qingmei,Jiang Nan,Cong Hang,Tao Zhu,Liu Mao,Fan Ying

Metal–organic frameworks (MOFs) including cucurbit[7]uril block (Q[7]·HAuCl 4 ) were employed to develop a diphenylamine (DPA) sensor in electrochemical method, the presence of HAuCl 4 improved the conductivity of the macrocyclic compound. To further enhance of the sensitivity, Au nanoparticles were inserted between the surface of glassy carbon electrode and Q[7]·HAuCl 4 MOFs (GCE-AuNPs-Q[7]·HAuCl 4 ). Cyclic voltammetry (CV), electrochemical impedance spectroscopy (EIS), and differential pulse voltammetry (DPV) were applied for evaluation on the electrochemical behavior. For the electrochemical inertness of DPA, a label-free electrochemical sensor in 5 mM K 3 [Fe(CN) 6 ] solution was achieved, to produce a limit of detection as low as 4.6 µM in a linear range of 5–1000 µM with good reproducibility, high stability and acceptable anti-interference ability. Application of the proposed electrode for the quantitative determination of DPA in tap water and apple juice confirms its real value. Graphical abstract

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JOURNAL OF MOLECULAR LIQUIDS · 2021 · IF 6.165

Crown ether and crown ether/K+ complex assisted DOSY NMR: A versatile tool for positional isomers identification in aqueous solution

Hui Ma,Dan Luo,Qi Zhao,Rui Liu,Zhenzhou Zhang,Xianglin Hou,Xiaohuan Sun,Yingxiong Wang

Diffusion-ordered spectroscopy (DOSY) is a powerful and efficient technique for the analysis of complex mixtures, relying on their differential in self-diffusion coefficient. However, DOSY is often struggled to separate signals pertaining to isomeric species, especially positional isomers. Here, for the first time, we describe the novel design of 18-crown ether-6 (18C6) and 18C6/K + complex as matrixes to discriminate and identify positional isomeric mixtures of phenylenediamine, nitroaniline, phthalic acid, dimethoxybenzoic acid, aminophthalic acid and even amino acids using 1 H DOSY spectrum. The superior performance of 18C6 and 18C6/K + complex as matrix depends on that they can interact with different components with varying binding energy as demonstrated by MMMF calculations and the DFT calculation. The methodology presented here is simple yet efficient. Moreover, the crown ether and crown ether/K + complex provide the dual mode discrimination for both amino and carboxylic substituted positional isomers.

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CHEMISTRY-A EUROPEAN JOURNAL · 2021 ·Vol. 27 ·期 41 ·10666-10676 · IF 5.236

Fabrication of Pd/Mg2P2O7 via a Struvite-Template Way from Wastewater and Application as Chemoselective Catalyst in Hydrogenation of Nitroarenes

Peng Zhang,Shaonan Xu,Yan Wang,Wei Zhang,Wenqing Li,Cundi Wei,Peiping Zhang,Shiding Miao

Graphical One man‘s trash is another man‘s treasure : A novel template strategy allows fibrous struvite—a composite Pd/Mg 2 P 2 O 7 with a mesoporous structure and an ultrahigh surface area—to be synthesized from wastewater. The prepared Pd/Mg 2 P 2 O 7 nanowires showed excellent performance in the selective hydrogenation of nitrobenzenes. This strategy provided a new pathway for synthesizing highly efficient catalysts as well as a solution for alleviate eutrophic pollution caused by N- and P-containing substances in wastewater. A highly efficient heterogeneous catalyst Pd/Mg 2 P 2 O 7 was fabricated by combining palladium nanoparticles (PdNPs) and mesoporous Mg 2 P 2 O 7 fibers/rods. Mg 2 P 2 O 7 fibers with ultra-high specific surface area were prepared from struvite as templates, which were synthesized from waste water containing N- and P-containing pollutants. This strategy provided a novel pathway for developing advanced catalysts from eutrophication-polluted water. The composite Pd/Mg 2 P 2 O 7 showed brilliant performance in selective hydrogenation of nitro aromatics to give anilines. As an example of nitrobenzene hydrogenation, the conversion to aniline and selectivity were found to reach almost 100 % at a temperature of T =90 °C and under a pressure of P =2.0 MPa. The superior performance was found to originate from PdNPs, which were boosted by electron transfer afforded by the nanofiber Mg 2 P 2 O 7 supports. The favorable adsorption of withdrawing groups (−NO 2 ) was realized by synergistic effects between Pd and oxygen vacancies provided by pyrolysis of struvite. The catalyst remained stable after cycles of reuse with little degradation in catalytic performance.

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FOOD CHEMISTRY · 2021 · IF 7.514

Rapid recognition of di-n-butyl phthalate in food samples with a near infrared fluorescence imprinted sensor based on zeolite imidazolate framework-67

Shan Chen,Jinli Fu,Shu Zhou,Pengfei Zhao,Xiaodan Wu,Sisi Tang,Zhaohui Zhang

Di- n -butyl phthalate (DBP) as a plasticizer is widely used in food and chemical industries. It is harm to human health when it appeared in food and water. A novel near-infrared (NIR) fluorescence molecularly imprinted sensor based on CdTe quantum dots and zeolite imidazolate framework-67 was developed with a sol–gel polymerization method for rapid and sensitive determination of DBP in foodstuff rapidly (only in 1.5 min). The fluorescence imprinted sensor provided a rapid detection method for DBP in the linear response concentration range of 0.05–18.0 μM with a low detection limit of 1.6 nM. Compared with previous fluorescence imprinted sensor, it behaved faster response speed and lower detection limit for determination of DBP. The fluorescence imprinted sensor was used to detect DBP in real samples successfully with satisfied recoveries of 97.2–106.4%, suggesting a potential application in food analysis.

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CARBON · 2021 · IF 9.594

Nanofiber based origami evaporator for multifunctional and omnidirectional solar steam generation

Huijie Liu,Ye Liu,Liming Wang,Xiaohong Qin,Jianyong Yu

Interfacial solar steam generation is considered as an effective and environment-friendly technology for clean water production. However, the preparation of an evaporator with omnidirectional light harvesting, high evaporation rate , catalytic and antibacterial properties simultaneously remains a great challenge. Herein, we report the Ag nanoparticles decorated MXene nanosheets/polyacrylonitrile (Ag@MXene/PAN) nanofiber based evaporators for high-efficiency, multifunctional and omnidirectional solar steam generation by solution electrospinning technology. The conjunction of Ag nanoparticles and MXene nanosheets not only enhances the broadband light absorption and heat production, but also contributes to the good catalytic and antibacterial performance. Furthermore, the flexibility and foldability of Ag@MXene/PAN nanofiber membranes enable the design of 3D fine-structure evaporator with increased evaporation surface area and optimized light absorption. As a proof of concept , Ag@MXene/PAN nanofiber based origami evaporator is constructed, which demonstrates relatively stable evaporation rates during a wide range of incident angle from 30° to 150°. The maximum evaporation rate reaches 2.08 kg m −2  h −1 under 1 sun illumination , far superior to the state-of-the-art solution-electrospun nanofiber based evaporators. Integration of structure flexibility, high performance and multi-functionality makes the designed nanofiber based evaporator promising for practical clean water production.

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APPLIED SURFACE SCIENCE · 2020 · IF 6.182

Exploring the enhanced catalytic performance on nitro dyes via a novel template of flake-network Ni-Ti LDH/GO in-situ deposited with Ag3PO4 NPs

Huizhen Deng,Juanjuan Yin,Jinming Ma,Jingxin Zhou,Lexin Zhang,Lili Gao,Tifeng Jiao

A novel catalyst composed of Ag 3 PO 4 bridged by Ni/Ti LDH-graphene heterojunction structure was successfully prepared by a simple in-situ deposition method, which has excellent catalytic performance for 4-NP and 2-NA. Various characterizations to the samples such as XRD, SEM, TEM, STEM-EDS, XPS, TG–DSC, and UV–vis DRS were adopted. Because the ternary structure is mixed with each other to form more heterojunctions and higher specific surface area, the ternary composite Ag 3 PO 4 /Ni-Ti LDH/GO has excellent catalytic and cycle performance. Compared to the precursors Ag 3 PO 4 /GO and Ni-Ti LDH/GO, the finally as-obtained nanocomposite Ag 3 PO 4 /Ni-Ti LDH/GO degraded 4-NP and 2-NA solutions represented more dominant degradation efficiency. In addition, the pseudo-first-order rate constants of the composite catalyst for 4-NP and 2-NA are 0.178 min −1 and 0.089 min −1 , respectively. The complex and irregular surfaces of Ni-Ti LDH/GO provided an ideal carrier with abundant active sites for in-situ depositing and stabilizing of Ag 3 PO 4 NPs, formed the Ag 3 PO 4 /Ni-Ti LDH/GO hybrid possessed an acceptable catalytic performance on the degradation of azo dyes, which could be applied in the efficient treatment of wastewater from industries.

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Journal of Materials Chemistry A · 2020 ·Vol. 8 ·期 17 ·8360-8375 · IF 11.301

Modulating charge migration in photoredox organic transformation via exquisite interface engineering

Shuai Xu,Ming-Hui Huang,Tao Li,Zhi-Quan Wei,Xin Lin,Xiao-Cheng Dai,Shuo Hou,Xiao-Yan Fu,Fang-Xing Xiao

Modulating photo-induced charge separation/transfer constitutes a central challenge in heterogeneous photocatalysis. Despite advancements in this area, finely tuning directional electron migration without involving conventional co-catalysts [e.g., metal nanocrystals and transition metal dichalcogenides (TMDs)] for boosted photoredox catalysis has not yet been explored. Herein, we report the exquisite design of a novel and general macromolecule-modulated photoredox selective organic transformation system, wherein an ultrathin macromolecular poly(diallyldimethylammonium chloride) (PDDA) layer was integrated at the interface of wide-band-gap (WBG) and narrow-band-gap (NBG) semiconductors to construct heterostructured photocatalysts. The ultra-thin PDDA interim layer expedites interfacial unidirectional electron transfer from the NBG to WBG semiconductor, resulting in a cascade electron transfer channel. The favorable energy level alignment among the building blocks, intimate interfacial integration and multilayered nanoarchitecture endow the WBG@PDDA@NBG heterostructures with substantially enhanced and versatile photoredox performance toward the selective oxidation of aromatic alcohols to aldehydes and the anaerobic reduction of nitroaromatics to amino compounds under visible light irradiation. This can be ascribed to the crucial role of the ultrathin intermediate PDDA layer as a highly efficient metal and TMD-free charge transfer mediator, relaying the electrons from the NBG to WBG semiconductor and slowing charge recombination. Our work could open up new frontiers to exploit diverse metal and TMD-free photocatalytic systems and provide a first insight into the fine tuning of charge transport utilizing non-conductive ionic polymers for solar energy conversion.

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Environmental Sciences Europe · 2020 ·Vol. 32 ·期 1 ·1-10 · IF 5.394

Mixture toxicity of zinc oxide nanoparticle and chemicals with different mode of action upon Vibrio fischeri

Chen Fen,Wu Ligui,Xiao Xiaoyu,Rong Lingling,Li Mi,Zou Xiaoming

Zinc oxide nanoparticle (nZnO) and chemicals with different mode of action (MOA, i.e., narcotic and reactive) were frequently detected in the Yangtze River. Organisms are typically exposed to mixtures of nZnO and other chemicals rather than individual nZnO. Toxicity of nZnO is caused by the dissolution of Zn2+, which has been proved in the field of single toxicity. However, it is still unclear whether the released Zn2+ plays a critical role in the nZnO toxicity of nZnO–chemicals mixtures. In the present study, the binary mixture toxicity of nZnO/Zn2+ and chemicals with different MOA was investigated in acute (15 min) and chronic (12 h) toxicity test upon Vibrio fischeri (V. fischeri). The joint effects of nZnO and tested chemicals were explored. Moreover, two classic models, concentration addition (CA) and independent action (IA) were applied to predict the toxicity of mixtures.The difference of toxicity unit (TU) values between the mixtures of Zn2+–chemicals with those of nZnO–chemicals was not significant (P > 0.05), not only in acute toxicity test but also in chronic toxicity test. The antagonistic or additive effects for nZnO-chemicals can be observed in most mixtures, with the TU values ranging from 0.75 to 1.77 and 0.47 to 2.45 in acute toxicity test and chronic test, respectively. We also observed that the prediction accuracy of CA and IA models was not very well in the mixtures where the difference between the toxicity ratios of the components was small (less than about 10), with the mean absolute percentage error (MAPE) values ranging from 0.14 to 0.67 for CA model and 0.17–0.51 for IA model, respectively.We found that the dissolved Zn2+ mainly accounted for the nZnO toxicity in the mixtures of nZnO–chemicals, and the joint effects of these mixtures were mostly antagonism and additivity. CA and IA models were unsuitable for predicting the mixture toxicity of nZnO–chemicals at their equitoxic ratios.

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