Applied Sciences-Basel
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2018
·Vol. 8
·期 12
·2530
·
IF 1.689
Nan Fang Nie,Xin Xing Zhang,Chu Shan Fang,Qiu Yan Zhu,Jiao Yang Lu,Fu Rui Zhang,Qing Feng Yao,Wei Tao Huang,Xue Zhi Ding,Li Qiu Xia
Game theory—the scientific study of interactive, rational decision making—describes the interaction of two or more players from macroscopic organisms to microscopic cellular and subcellular levels. Life based on molecules is the highest and most complex expression of molecular interactions. However, using simple molecules to expand game theory for molecular decision-making remains challenging. Herein, we demonstrate a proof-of-concept molecular game-theoretical system (molecular prisoner’s dilemma) that relies on formation of the thymine–Hg2+–thymine hairpin structure specifically induced by Hg2+and fluorescence quenching and molecular adsorption capacities of cobalt oxyhydroxide (CoOOH) nanosheets, resulting in fluorescence intensity and distribution change of polythymine oligonucleotide 33-repeat thymines (T33). The “bait” molecule, T33, interacted with two molecular players, CoOOH and Hg2+, in different states (absence = silence and presence = betrayal), regarded as strategies. We created conflicts (sharing or self-interest) of fluorescence distribution of T33, quantifiable in a 2 × 2 payoff matrix. In addition, the molecular game-theoretical-system based on T33 and CoOOH was used for sensing Hg2+over the range of 20 to 600 nM with the detection limit of 7.94 nM (3σ) and for determination of Hg2+in pond water. Inspired by the proof-of-concept for molecular game theory, various molecular decision-making systems could be developed, which would help promote molecular information processing and generating novel molecular intelligent decision systems for environmental monitoring and molecular diagnosis and therapy.Keywords:cobalt oxyhydroxide nanosheets;fluorescent sensing;game theory;Hg2+;thymine–Hg2+–thymine
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2018
·
IF 3.141
Anyao Ma,Jiakang Zhang,Na Wang,Liangjiu Bai,Hou Chen,Wenxiang Wang,Huawei Yang,Lixia Yang,Yuzhong Niu,Donglei Wei
Robust and self-healable nanocomposite hydrogels were realized by the encapsulation of components of photoinduced electron transfer–atom transfer radical polymerization (PET–ATRP) into surface-modified silica nanoparticles (SiO2). The prepared SiO2@P4VP was in the form of self-healing nanocomposite hydrogels, where 4-vinylpyridine (4VP) was polymerized through PET–ATRP with organic photocatalyst Rhodamine B. The modified nanoparticles were characterized by X-ray photoelectron spectroscopy (XPS), thermogravimetric analysis (TGA), transmission electron microscopy (TEM), and Fourier transform infrared (FT-IR) spectroscopy. The nanocomposite hydrogels can be healed rapidly and autonomously without any stimulation at ambient temperature. Specifically, the nanocomposite hydrogels have a tensile strength of about 2.90 MPa, which recovered to 77.0% after 12 h, and an elongation at break of about 730%. These self-healing hydrogels with cheap raw material, possessing better strength and self-healing performance, will have broad prospects.
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CHEMICAL ENGINEERING JOURNAL
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2018
·
IF 6.735
Huawei Yang,Liangjiu Bai,Donglei Wei,Lixia Yang,Wenxiang Wang,Hou Chen,Yuzhong Niu,Zhongxin Xue
In this work, poly(ionic liquid)-based porous hybrid materials were facilely prepared through ionic self-assembly method and proposed as adsorbents for removal and separation of ionic dyes. PIL, namely poly-[ N , N -dimethyl-dodecyl-(4-vinylbenzyl)ammonium chloride], was synthesized by simple radical polymerization and directly assembled with the multi-charged anionic cluster of polyoxometalate (POM) to yield PIL/POM hybrid materials without involving any toxic organic solvents and tedious modification processes. The obtained hybrid materials were characterized by various techniques and utilized as adsorbents for removal of a variety of ionic dyes from water. By adjusting the proportion of PIL and POM in the hybrid materials, the adsorption capability and selectivity towards cationic and anionic dyes could be effectively regulated. The preferred adsorbent showed fast adsorption rate and large adsorption capacity, and was able to selectively remove anionic dyes from cationic/anionic mixed dyes aqueous solutions. Furthermore, the used adsorbent can be easily collected and regenerated. All the results demonstrate that the PIL/POM hybrid material is an efficient, durable and sustainable adsorbent in water purification treatment.
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POLYMER
·
2014
·
IF 3.766
Xin Zhou,Yongyue Chen,Jin Han,Xuedong Wu,Gang Wang,Daoyi Jiang
Betaine ester-shell functionalized hyperbranched polyethylenimines (BEHPEI) were synthesized by Menschutkin reaction between per-N-methylated polyethylenimine (MeHPEI) and alkyl bromoacetate. BEHPEI could play dual antimicrobial roles that were, the betaine ester-shell acted as contact-based antibacterial polycations and the drug-loaded BEHPEI could controllably release the drugs due to the cleavage of the betaine ester groups under weak alkaline condition. The BEHPEI exhibited high transport capacities that per gram of BEHPEI could encapsulate 0.24–2.67 g of dyes or drugs. The model drug release experiment employing methyl orange (MO) showed that the drug release of MO-loaded BEHPEI complex occurred slowly in weak alkaline solutions and the release rate was controlled by varying pH, while the complex kept very stable under weak acid condition (pH = 3.0–7.0). BEHPEI generated from long chain alkyl bromoacetate was compatible with organic resins implying the possible usage in antimicrobial fibers and coatings. Another BEHPEI obtained from short-chain alkyl bromoacetate was water soluble and maybe used in lotion formula. The hydrolysis of BEHPEI afforded zwitterionic shell.
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ANALYTICA CHIMICA ACTA
·
2014
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IF 4.517
Xia Hao,Jing Lei Lei,Nian Bing Li,Hong Qun Luo
A simple and effective method for the detection of electrochemically inactive sodium dodecyl sulfate (SDS) has been designed, based on different binding affinity of polyethyleneimine (PEI) toward electrochemically active eosin Y and electrochemically inactive SDS. The stronger binding affinity of the PEI toward SDS than eosin Y results in the decrease of the redox peak current of surface confined eosin Y and provides a quantitative readout for the SDS. The difference in value of the cathodic peak current showed a linear relationship with SDS concentration in a concentration range from 1 to 40 μg mL −1 , and a detection limit of 0.9 μg mL −1 for SDS was obtained. Furthermore, the method has been successfully applied to the detection of SDS in real samples. The developed approach provided a simple and reliable detection for SDS and might have potential applications in electrochemical methods for inactive molecules.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2015
·
IF 2.353
Jiaman Liang,Xiaoyan Deng,Kejun Tan
In this paper, a novel sensing method with a higher sensitivity of perfluorooctane sulfonate (PFOS) than perfluorooctanoic acid (PFOA) has been proposed detection of PFOS in aqueous solution replying on the “off–on” switch of eosin Y/polyethyleneimine (PEI)/PFOS fluorescence system due to the higher affinity of PEI to PFOS than eosin Y. In pH 7.0 Britton–Robinson buffer solution, eosin Y reacts with protonated PEI to form complex by electrostatic attraction, which leads to a strong fluorescence quenching of the eosin Y. When PFOS presents, the fluorescence of eosin Y is recover due to the electrostatic and hydrophobic interactions between PFOS and PEI. The recovered fluorescence intensity is proportional to the concentration of PFOS in the ranging from 0 to 2.0 × 10 −6 mol/L with the limit of detection (LOD, 3 σ ) being 1.5 × 10 −8 mol/L without preconcentration. In this study, the optimum reaction conditions and the interferences of foreign substances were investigated. In addition, the effects of PFOA, the analog of PFOS, on the fluorescence recovery of the system were also studied. The presented approach has been successfully used to detect PFOS in real samples with RSD ⩽2.9%.
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CATALYSIS COMMUNICATIONS
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2015
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IF 3.699
Weiming Wu,Teng Teng,Xiao-Yuan Wu,Xuejing Dui,Lei Zhang,Jinhua Xiong,Ling Wu,Can-Zhong Lu
A cobalt-based polyoxometalate, Na 7 H 10 [Co 6 (H 2 O) 2 (PW 9 O 34 ) 2 (PW 6 O 26 )]·30H 2 O, was synthesized by a simple aqueous solution method. It showed catalytic activity for the visible-light-driven H 2 evolution from water splitting with eosin Y as the photosensitizer and triethanolamine as the electron donor. The initial rate of the H 2 evolution was 141 μmol h − 1 , which was higher than that of Co 2 + cations (55 μmol h − 1 ). The efficient catalytic activity was attributed to that the [B-PW 9 O 34 ] 9 − units in the sample act as electron transmitters to accelerate charge transfer. Moreover, a possible mechanism was proposed to explain the H 2 evolution from water splitting in the present system.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2015
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IF 3.368
Jianwei Fu,Qianqian Xin,Xuechen Wu,Zhonghui Chen,Ya Yan,Shujun Liu,Minghuan Wang,Qun Xu
Polydopamine (PDA) microspheres, synthesized by a facile oxidation polymerization route, were evaluated as a potential adsorbent for selective adsorption and separation of organic dyes. The adsorption processes towards nine water-soluble dyes (anionic dyes: methyl orange (MO), eosin-Y (EY), eosin-B (EB), acid chrome blue K (ACBK), neutral dye: neutral red (NR), and cationic dyes: rhodamine B (RhB), malachite green (MG), methylene blue (MB), safranine T (ST)) were thoroughly investigated. The adsorption selectivity of organic dyes onto PDA microspheres was successfully applied for the separation of dyes mixtures. Various influential factors such as solution pH, temperature, and contact time were employed to ascertain the optimal condition for adsorption of representative organic dyes including MB, MG and NR. The pseudo-first-order and pseudo-second-order kinetics models were used to fit the adsorption kinetics process. Five isothermal adsorption models (Langmuir, Dubnin–Radushkevich, Temkin, Freundlich and Harkins–Jura) were used to investigate the adsorption thermodynamics properties. The results showed that the PDA microspheres owned good selective adsorption ability towards cationic dyes. The adsorption kinetics process conformed to the pseudo-second-order kinetics model and the Langmuir isotherm model was more appropriate for tracing the adsorption behavior than other isotherm models. Thus, we can conclude PDA microspheres may be a high-efficiency selective adsorbent towards some cationic dyes.
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ACS Applied Materials & Interfaces
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2015
·
IF 6.723
Lin-Feng Gao,Ting Wen,Jing-Yin Xu,Xin-Ping Zhai,Min Zhao,Guo-Wen Hu,Peng Chen,Qiang Wang,Hao-Li Zhang
Graphitic carbon nitrides have appeared as a new type of photocatalyst for water splitting, but their broader and more practical applications are oftentimes hindered by the insolubility or difficult dispersion of the material in solvents. We herein prepared novel two-dimensional (2D) carbon nitride-type polymers doped by iron under a mild one-pot method through preorganizing formamide and citric acid precursors into supramolecular structures, which eventually polycondensed into a homogeneous organocatalyst for highly efficient visible light-driven hydrogen evolution with a rate of ∼16.2 mmol g–1 h–1 and a quantum efficiency of 0.8%. Laser photolysis and electrochemical impedance spectroscopic measurements suggested that iron-doping enabled strong electron coupling between the metal and the carbon nitride and formed unique electronic structures favoring electron mobilization along the 2D nanomaterial plane, which might facilitate the electron transfer process in the photocatalytic system and lead to efficient H2 evolution. In combination with electrochemical measurements, the electron transfer dynamics during water reduction were depicted, and the earth-abundant Fe-based catalyst may open a sustainable strategy for conversion of sunlight into hydrogen energy and cope with current challenging energy issues worldwide.
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CARBON
·
2017
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IF 6.337
Jianliang Xiao,Jifei Zhang,Weiyang Lv,Yihu Song,Qiang Zheng
Comprehensive treatment of multifarious contaminations in waterbody demands multifunctional adsorbents with easy reusability , high efficiency, and broad-spectrum adsorption performance. Herein hydrothermally reduced graphene oxide/poly (vinyl alcohol) (TRGO/PVA) aerogels fulfilling these requirements were developed via a facile and green in situ hydrothermal reduction followed by direct sol-aerogel transformation strategy. The interfacial interaction between TRGO sheets and PVA macromolecules as proved by various methods could effectively prevent TRGO from aggregation, which improves mechanical and adsorption performances and assures reusability of aerogels. The aerogels demonstrate an attractive broad-spectrum universality in adsorbing diverse cationic, anionic and nonionic dyes, surpassing most adsorbents that could only remove either positively or negatively charged dyes. The aerogels demonstrate a promising synergetic effect for adsorption two oppositely charged dyes, exhibiting the highest total adsorption amount (>900 mg/g) among known absorbents for removing mixed dyes. Besides, the aerogels after hydrophobic modification are able to effectively adsorb common oils and organic solvents spilling on water. Furthermore, the aerogels are compressible, dimension stable and solvent resistive and can be easily regenerated, bringing a great superiority in the comprehensive treatment of multiple contaminations in waterbody.
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CHEMISTRY-A EUROPEAN JOURNAL
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2017
·Vol. 23
·期 55
·13696-13703
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IF 5.317
Rui Zhang,Zhenchuan Yu,Lei Wang,Qizhe Shen,Xiaoyan Hou,Xuhong Guo,Junwei Wang,Xuedong Zhu,Yuan Yao
Graphical Rationally designed spherical polyelectrolyte brushes with cationic charges were adopted as the absorbent, and compressed carbon dioxide as the anti-solvent to separate anionic dye from a solution of mixed dyes. The combined dye and polymer brush could be easily separated by adding NaCl aqueous solution through ion exchange. The recovered PS-PAEMH still kept high adsorption capacity even after ten times of regeneration. Dye-containing wastewater has caused serious environmental pollution. Herein, rationally designed spherical polyelectrolyte brushes (SPBs) with cationic charges, polystyrene–poly(2-aminoethylmethacrylate hydrochloride) (PS-PAEMH) as the absorbent, and compressed carbon dioxide as the antisolvent are proposed for the separation of the anionic dye eosin Y (EY) from a solution of mixed dyes. The adsorption behavior of EY onto PS-PAEMH was highly dependent on CO 2 pressure, contact time, and initial concentration. The maximum adsorption capacity of PS-PAEMH was 335.20 mg g −1 . FTIR and UV/Vis measurements proved that the electrostatic interactions between EY and PS-PAEMH played an important role in the absorbance process. The adsorption process fitted the pseudo-second-order kinetic model and Freundlich isotherm model very well. The combined dye and polymer brush could be easily separated through ion exchange by adding an aqueous solution of NaCl. Recovered PS-PAEMH retained a high adsorption capacity even after ten cycles of regeneration. This method provides a simple and effective way to separate ionic materials for environmental engineering.
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ANALYTICAL AND BIOANALYTICAL CHEMISTRY
·
2016
·Vol. 408
·期 22
·6223-6233
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IF 3.125
He Xiao-Mei,Ding Jun,Yu Lei,Hussain Dilshad,Feng Yu-Qi
Quantitative analysis of small molecules by matrix-assisted laser desorption/ionization time-of-flight mass spectrometry (MALDI-TOF MS) has been a challenging task due to matrix-derived interferences in low m/z region and poor reproducibility of MS signal response. In this study, we developed an approach by applying black phosphorus (BP) as a matrix-assisted laser desorption ionization (MALDI) matrix for the quantitative analysis of small molecules for the first time. Black phosphorus-assisted laser desorption/ionization mass spectrometry (BP/ALDI-MS) showed clear background and exhibited superior detection sensitivity toward quaternary ammonium compounds compared to carbon-based materials. By combining stable isotope labeling (SIL) strategy with BP/ALDI-MS (SIL-BP/ALDI-MS), a variety of analytes labeled with quaternary ammonium group were sensitively detected. Moreover, the isotope-labeled forms of analytes also served as internal standards, which broadened the analyte coverage of BP/ALDI-MS and improved the reproducibility of MS signals. Based on these advantages, a reliable method for quantitative analysis of aldehydes from complex biological samples (saliva, urine, and serum) was successfully established. Good linearities were obtained for five aldehydes in the range of 0.1–20.0 μM with correlation coefficients ( R
2 ) larger than 0.9928. The LODs were found to be 20 to 100 nM. Reproducibility of the method was obtained with intra-day and inter-day relative standard deviations (RSDs) less than 10.4 %, and the recoveries in saliva samples ranged from 91.4 to 117.1 %. Taken together, the proposed SIL-BP/ALDI-MS strategy has proved to be a reliable tool for quantitative analysis of aldehydes from complex samples.
An approach for the determination of small molecules was developed by using black phosphorus (BP) as a matrix-assisted laser desorption ionization (MALDI) matrix
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