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SCIENCE OF THE TOTAL ENVIRONMENT · 2022 · IF 10.753

Rapid As(III) oxidation mediated by activated carbons: Reactive species vs. direct oxidation

Changyin Zhu,Chenyan Xue,Mingquan Huang,Fengxiao Zhu,Guodong Fang,Dixiang Wang,Shaochong Liu,Ning Chen,Song Wu,Dongmei Zhou

Activated carbon (AC) is widely used in pollutant removal , due to its adsorption capacity, conductivity and catalytic performance. However, few studies focus on the redox activity of AC and its role in pollutant transformation. In this study, we found that AC could efficiently mediate the oxidation of As(III) and the process of As(III) oxidation was pH and oxygen concentration dependent. In general, the presence of O 2 promoted As(III) oxidation at pH 3.0–9.5. Acidic and alkaline conditions favored As(III) oxidation regardless of whether there was oxygen, but the mechanisms involved were quite different when there was oxygen. At pH 3.0, reactive species (H 2 O 2 and ·OH) were generated and accounted for As(III) oxidation; at pH 9.5, As(III) was directly oxidized by O 2 (electron transfer from As(III) to O 2 mediated by carbon matrix) under aerobic conditions . Pre-oxidation and cyclic experiments results indicated the ability of AC to oxidize As(III) at pH 9.5 was sustainable and recyclable. This study provided a new insight in pollutant oxidation by AC in the environment.

CAS / MDL: 9001-05-2 9003-99-0
研究领域: 环境科学 · 化学
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ANALYTICAL CHEMISTRY · 2024 · IF 6.7

Electrochemiluminescence Detecting and Imaging of Yeast Metabolism Indicated by Endogenetic Co-reactant

Jiancong Ni,Shengxiu Huang,Weiqiang Yang,Qiaoling Chen,Zhenyu Lin

Glycolysis, a pivotal step in yeast metabolism, plays an indispensable role as a carbohydrate utilization process crucial for cellular survival. Developing advanced technologies to elucidate this fundamental physiological process holds significant scientific implications. Electrochemiluminescence (ECL) imaging exhibits the advantage of negligible background interference and facilitates straightforward visualization, thereby conferring significant value in biomolecular observation. In this study, we present an ECL imaging method for investigating yeast metabolism by utilizing the endogenetic NADH as an efficient coreactant for ECL generation. The yeast glycolysis process drives the conversion of NAD+ to NADH, resulting in enhanced ECL response as well as the increased brightness of ECL images that can be used for quantification of yeast activity. There was a linear correlation between the reciprocal of both the gray value of ECL image and yeast concentration within the range of 6.25 × 106 – 6.25 × 108 CFU/mL. Due to the highly efficient coreactant behavior of NADH, our method demonstrated excellent selectivity with minimal interference. Furthermore, we employed this approach to investigate some toxic inhibitors on yeast metabolism, yielding reliable results. This ECL imaging method not only avoids the use of additional coreactants but also provides a sensitive and intuitive approach for monitoring yeast metabolism, demonstrating great potential in revealing various complex biological processes.

研究领域: 生物化学 · 分析化学
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH · 2018 · IF 3.141

Reversible Reaction-Assisted Intensification Process for Separating the Azeotropic Mixture of Ethanediol and 1,2-Butanediol: Reactants Screening

Xingang Li,Rui Wang,Jian Na,Hong Li,Xin Gao

The feasibility of employing reversible reactions to convert the separation of ethanediol (EG) and 1,2-butanediol (1,2-BDO) azeotropic system was analyzed in our previous work. This article aims at systematically screening the feasible reactants for the reaction-assisted separation process. A screening principle was brought up and applied. Through preliminary screening, acetic acid, acrylic acid, acetaldehyde, propionaldehyde, propanol, and butanone were obtained as potential reactants. Propionaldehyde was chosen as the proper one after fully comparing the reaction selectivity difference and conversion of EG and 1,2-BDO in the reaction process, the separation efficiency in the purification process, and final EG yield. The separation efficiency was predicted based on the relative volatility of EG, 1,2-BDO, and their corresponding products and was verified by distillation experiments. The stratification appeared in the reaction was found beneficial to the coupling of reaction and separation.

CAS / MDL: 123-38-6
研究领域: 化学工程 · 分离技术
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ANALYTICAL CHEMISTRY · 2021 · IF 6.986

Self-Photocatalysis Boosted Electrochemiluminescence Signal Amplification via In Situ Generation of the Coreactant

Xinke Kong,Cui Wang,Li Pu,Panpan Gai,Feng Li

The classic luminol-based electrochemiluminescence (ECL) platform generally suffers from self-decomposition of the coreactant (i.e., H2O2) during the reaction process, seriously hampering the luminous signal stability, as well as its practical application. To address this issue, apart from the introduction of complex exogenous species, preoxidation of the luminophore, and electrocatalysis for ECL signal amplification, we proposed a novel ECL model to realize the signal enhancement via in situ self-photocatalytic generation of the coreactant H2O2. Interestingly, the luminescence of luminol was simultaneously utilized as the light source to promote the conversation of O2 to H2O2 with the assistance of the photocatalyst resorcinol-formaldehyde resin, which could further improve the luminescence of luminol in turn. In comparison with the traditional case, this new ECL model not only exhibited obvious signal amplification but also efficiently boosted its stability of signal output. To sum up, an exogenous coreactant-free, highly stable ECL platform was obtained via simply integrating the photocatalyst RF and the luminol-based system. This work will not only inspire the design of a new integrated ECL system with a coreactant translator but also provide an ingenious insight for the construction of a new generation of ECL models.

研究领域: 分析化学 · 材料科学 · 生物传感
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CHEMISTRY-A EUROPEAN JOURNAL · 2024 · IF 3.9

Dual-Coreactants Enhanced Electrochemiluminescence

Jialian Ding,Bin Su

Graphical One plus one is greater than two: A remarkable electrochemiluminescence (ECL) enhancement of Ru(bpy) 3 2+ /TPrA is observed by introducing another coreactant, TEOA, with a 10.8-fold increase of ECL intensity and 1.7-fold extension of ECL layer. The enhancement was interpreted by a chemical oxidation route, in which TEOA + ⋅ acts as an enhancer to produce more TPrA + ⋅ and meanwhile allow the remote formation of TPrA + ⋅. This dual-coreactants strategy works not only in solution with freely diffusive Ru(bpy) 3 2+ but also on Ru(bpy) 3 2+ -functionalized microbeads, showing promise in ECL-based bioassay and microscopy. The electrochemiluminescence (ECL) of ruthenium(II) tris(2,2′-bipyridyl) (Ru(bpy) 3 2+ ) with tri- n -propylamine (TPrA) as the good coreactant can be unexpectedly enhanced by a weak coreactant, such as triethanolamine (TEOA). First, the intensity of ECL emitted by Ru(bpy) 3 2+ /TPrA can be remarkably amplified by 10.8-fold after adding some amount of TEOA. Moreover, the ECL layer thickness, measured by self-interference spectroscopy, is also doubled. The enhancement far exceeding the superposition of respective contribution of TPrA and TEOA was elucidated by a “chemical oxidation mechanism”, in which TEOA + ⋅ acts as a chemical enhancer to oxidize TPrA in solution and to accelerate significantly the ECL reaction kinetics. This mechanism was proved by single-photon counting experiment and finite element simulations. In addition, the dual-coreactants strategy works well not only in solution with freely diffusive Ru(bpy) 3 2+ , but also on Ru(bpy) 3 2+ -functionalized microbeads, suggesting that ethanolamines could act as cheap, easily available and low-background enhancers for ECL-based bioanalysis and microscopy.

研究领域: 分析化学 · 生物分析 · 显微技术
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JOURNAL OF POLYMER SCIENCE PART A-POLYMER CHEMISTRY · 2011 ·Vol. 49 ·期 12 ·2755-2760 · IF 3.894

Functionalization of polymeric surfaces by simple photoactivation of C?H bonds

Jing Xu,Yuhong Ma,Jingyi Xie,F.J. Xu,Wantai Yang

A universal photoassisted pathway to functionalize polymeric surfaces is presented by transferring the inert surface sp 3 C  H bonds into reactive groups, such as  SO 3 H,  NH 2 ,  SH, and  COOH. The proposed method uses acetone as photoinitiator and different phenols with a para substituent XR as the reactants. Acetone excited by UV irradiation acts as a pair of scissors cutting both the surface C  H bonds of the polymer substrate and the O  H bonds of phenol, leading to the formation of carbon-centered surface chain free radicals and oxygen-centered phenoxy free radicals. By coupling of these two radicals, a variety of functional X groups with an R spacer from XR species of different phenol reactants were readily bonded to the polymeric surfaces, where phenol reactants included 4-hydroxylbenzene sulfonic acid for  SO 3 H, p -aminophenol and tyramine for  NH 2 , 4-hydroxythiophenol for  SH, and tyrosine for  COOH. © 2011 Wiley Periodicals, Inc. J Polym Sci Part A: Polym Chem, 2011

研究领域: 材料科学 · 化学工程
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES · 2024 · IF 7.7

Enhanced activity of enzymes encapsulated in spheres metal azolate framework-7 with defects

Cai Cheng,Xiaoliang Guo,Yu Feng,Jie Yu,Shi Huang,Liexiong Zhang,Yu Wu,Linna Shao,Xuehan Xu,Lingling Feng

Developing metal-organic frameworks (MOFs) with specific structures is critical for improving the activity of embedded enzymes, and defects may be one of the effective methods. Several methods have been demonstrated to be effective in creating defects in MOFs, including post-synthetic treatments, the use of acid as a modulator, and the use of ordinary or thermally sensitive linkers. However, these methods necessitate the utilization of additional substances. Metal azolate framework-7 (MAF-7) is a kind of MOF that was formed by the coordination of Zn 2+ with 3-methyl-1,2,4-triazole (Hmtz). This paper presents a method for the preparation of defect MAF-7 by changing the sequence of reactants without the introduction of additional substances. The defects were characterized by a range of techniques, including scanning electron microscopy, transmission electron microscopy, Brunauer-Emmett-Teller, X-ray photoelectron spectroscopy, and powder X-ray diffraction. The activity of microcystinase A (MlrA) encapsulated in defective MAF-7 (CMlrA@DMAF-7) was found to be significantly increased in comparison to non-porous MAF-7 (NMAF-7), and was largely unaffected by alterations in synthesis conditions. It is also noteworthy that lysozyme (LZ) and horseradish peroxidase (HRP), which are commonly used in industry, also demonstrated enhanced activity when encapsulated in DMAF-7. It was therefore anticipated that modifying the sequence of reactant addition would be a straightforward and simple method of introducing defects into MAF-7, thereby improving enzyme utilization.

CAS / MDL: 868-77-9
研究领域: 生物化学 · 材料科学
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BIOSENSORS & BIOELECTRONICS · 2022 · IF 12.545

In situ coordination interactions between metal-organic framework nanoemitters and coreactants for enhanced electrochemiluminescence in biosensing

Haomin Fu,Zhiyuan Xu,Tianrui Liu,Jianping Lei

Coreactant electrochemiluminescence (ECL) is one of the most popular pathways in commercial analysis, which can provide simplicity and convenience for getting intense ECL emission. However, the low efficiency of intermolecular electron transfer could weaken ECL intensity. In this work, we developed an enhanced ECL strategy through in situ coordination interactions between metal-organic framework emitters and coreactants. First, a metal-organic framework (MOF) emitter was synthesized with 1,1,2,2-tetrakis(4-(pyridin-4-yl)phenyl)ethane (TPPE) as aggregation-induced emission linkers and Zn as nodes. Interestingly, compared to TPPE ligand, the resulted MOF nanoemitters demonstrated 49.5 folds enhancement of ECL emission in the presence of 1,4-diazabicyclo[2.2.2]octane (DABCO) as the coreactant. More significantly, different from the constant ECL intensity using TPrA coreactant, DABCO exhibited time-dependent ECL intensity due to the intrareticular electron transfer through coordination interaction between DABCO and Zn 2+ , which was confirmed by X-ray photoelectron spectroscopy and Fourier transform infrared spectral experiments. The enhanced ECL was then applied to construct a sensitive ECL method to detect dopamine in serum samples. The coordination interaction between emitters and coreactants not only provides a universal way to enhance ECL, but also expands the applications of coreactant ECL system in convenience route.

CAS / MDL: 127-18-4 7646-85-7
研究领域: 分析化学 · 生物传感 · 材料科学
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APPLIED CATALYSIS A-GENERAL · 2017 · IF 4.339

Integrated study on the role of solvent, catalyst and reactant in the hydrodeoxygenation of eugenol over nickel-based catalysts

Jingbo Qi,Xianyong Sun,Si-Fu Tang,Yuanyuan Sun,Chen Xu,Xiaoyu Li,Xuebing Li

The hydrodeoxygenation (HDO) of phenols to hydrocarbons is a very promising technique process for the lignin valorization. To reveal the role of reactant, solvent and catalyst, the HDO experiments of eugenol to hydrocarbons were carried out at 523   K under 3   MPa H 2 over Ni catalysts supported on activated carbon (AC) and MFI-type zeolites in polar water and nonpolar n-hexane, respectively. It was found that Ni/AC was more efficient for the HDO of eugenol in water than in n-hexane, but Ni/HZSM-5 was just the opposite. The respective roles of Brønsted acid sites and Lewis acid sites on supports were also investigated by employing NaZSM-5, HZSM-5 and silicalite-1 as supports. It was revealed that Brønsted acid showed superior advantages (TOF: 37.9   h −1 to 11.1   h −1 ) over Lewis acid in the dehydration of 4-propyl-cyclohexanol. Oxygen-containing functional groups could be removed from the aromatic ring completely over Ni/HZSM-5 in n-hexane.

研究领域: 化学工程 · 催化科学
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JOURNAL OF SOLID STATE CHEMISTRY · 2021 · IF 3.498

Development of a novel cathodic deposition method for thin-film metal azolate frameworks toward Cd2+ adsorption

Jie Ding,Xiaoxuan Yuan,Jinfeng Wang,Wenfeng Mao,Jianzhong Huo,Jingbo Zhang

Metal-Organic Frameworks (MOFs) have attracted much attention due to its large specific surface, flexible porosity and unsaturated coordination bonds. Cathodic deposition is a unique in-situ potential-driven synthesis method for the deposition of thin film MOFs; however, the gradually consumption of reactants during cathodic deposition might lead to unstable and uncontrollable reaction during thin-film MOF deposition. Herein, oxygen is selected as the initial reactant for the formation of OH − , which can result in gradually and successive formation of thin-film MAF-66 (Metal azolate framework-66), and the particle size and film thickness of the MAF-66 film can be easily tuned by the deposition time. Furthermore, the cathodic deposited thin-film MAF-66 show good adsorption property for heavy metal ions , with Cd 2+ as a representative species. The adsorption capacity can reach 32.3 ​mg/g (removal ratio: 69%) and the deposited MAF-66 film can achieve a satisfactory recovery degree with structural and morphological stability. In this way, a novel, environmental-friendly, and controllable cathode deposition method is developed for preparation of thin-film MAF-66, which also show great promise as a candidate for heavy metal ions adsorbent.

研究领域: 材料科学 · 环境科学 · 化学工程
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MICROCHEMICAL JOURNAL · 2025 · IF 5.1

Electrochemiluminescent solid-droplet via coordination inhibition in high transparency hydrogel for convenient analysis of heavy metal ions

Sheng-Han Tang,Ying Zhang,Ling Qin,Wei-Guo Yang,Wen-Bin Liang,Jun Yang,Yan Li,Shan-Shan Hu

Despite the significant advantages of electrochemiluminescence (ECL) technology in ultrasensitive analysis of various molecules, the traditional three-electrode ECL system utilizes solution phase as the reaction medium often requires laborious preparations of the solution, leading to a relative complex and potential contamination. In this study, an organic ECL hydrogel based on poly(vinyl alcohol)/sodium alginate/glycerol (PVA/SA/Gly) hydrogel with luminophore tris (2,2′-bipyridine) ruthenium (Ⅱ) hexafluorophosphate ( R u ( b p y ) 3 2 + ) and co-reactant N, N’-bis (salicylidene)-1, 2-propanediamine (PropH) was explored for the construction of a novel solid-phase portable ECL sensing platform to detect heavy metal ions. To be specific, the unique Schiff base cavity structure of PropH specifically coordinated with Co 2+ , altering that its own nitrogen atoms’ electron cloud distributes to hinder co-reaction and reduce the hydrogel’s ECL emission. Notably, this novel ECL system utilized an organic ECL hydrogel as the reaction vessel, streamlining detection procedures and reducing detection time. Furthermore, the organic ECL hydrogel exhibited excellent stability and prolonged storage capability while maintaining strong ECL emission even after extended periods at room temperature. The proposed solid-phase portable ECL sensing platform demonstrates an excellent linear range from 1 nM to 10 mM and low detection limit of 0.31 nM for Co 2+ , providing new strategies for practical application capabilities in the field of food safety detection and environmental monitoring.

CAS / MDL: 9002-89-5
研究领域: 分析化学 · 环境科学 · 食品安全
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ACS Applied Energy Materials · 2021 · IF 6.024

Reactant Concentration and Aging-Time-Regulated Potassium Manganese Hexacyanoferrate as a Superior Cathode for Sodium-Ion Batteries

Ying Li,Kwok Ho Lam,Xianhua Hou

In this study, the sodium citrate assisted coprecipitation method was adopted to prepare high-quality potassium manganese hexacyanoferrate (KMHCF) by adjusting the reactant concentration and aging time. The influences of reactant concentration and aging time on the microstructures and electrochemical performance were investigated systematically. With the variations in preparation conditions, the as-prepared samples showed similar monoclinic crystal structure but different morphologies as well as electrochemical behaviors. The results proved that the lower reactant concentration is more beneficial to the formation of large particles with fewer defects of Fe(CN)6 vacancies and interstitial and coordinated water in the crystal structure. As a result, better cycling stability was obtained for the KMHCF1 samples prepared with a lower reactant concentration when compared to the KMHCF3 samples prepared with a higher reactant concentration. However, the small particles (KMHCF3) benefited the electrochemical kinetics, resulting in a larger specific capacity when compared with the large particles (KMHCF1). Similarly, the aging time also exhibited significant impacts on the microstructure and electrochemical performance of the as-prepared samples. The 24 h was confirmed to be the optimal aging time for the KMHCF samples. Among all samples, the KMHCF2_24h exhibited the best electrochemical performance with a large initial specific capacity of 140.3 mA h g–1 and a high capacity retention of 80.61% after 100 cycles at 20 mA g–1. A very high capacity retention of 85.02% after 500 cycles was achieved even at a high current density of 200 mA g–1. This should be ascribed to the regular cubic morphology of particles with the optimal size (1 μm) and less defects resulted from the optimal reactant concentration and aging time. This study provides a valuable and practical guidance for the synthesis of high-performance Prussian blue analogue cathode materials for sodium-ion batteries.

研究领域: 材料科学 · 电化学
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