JOURNAL OF HAZARDOUS MATERIALS
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2023
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IF 13.6
Jia Zhao,Heng Zhang,Yang Shi,Mengfan Luo,Hongyu Zhou,Zhenjun Xie,Ye Du,Peng Zhou,Chuanshu He,Gang Yao,Bo Lai
Ferrate (Fe(VI)) has aroused great research interest in recent years due to its environmental benignancy and lower potential in disinfection by-product generation. However, the inevitable self-decomposition and lower reactivity under alkaline conditions severely restrict the utilization and decontamination efficiency of Fe(VI). Here, we discovered that Ru(III), a representative transition metal, could effectively activate Fe(VI) to degrade organic micropollutants, and its performance on Fe(VI) activation exceeded that of previously reported metal activators. The high-valent metal species (i.e., Fe(IV)/Fe(V) and high-valent Ru species) made a major contribution to SMX removal by Fe(VI)−Ru(III). Density functional theory calculations indicated the function of Ru(III) as a two-electron reductant, leading to the production of Ru(V) and Fe(IV) as the predominant active species. The characterization analyses proved that Ru species was deposited on ferric (hydr)oxides as Ru(III), indicating the possibility of Ru(III) as an electron shuttle with the rapid valence circulation between Ru(V) and Ru(III). This study not only develops an efficient way to activate Fe(VI) but also offers a thorough understanding of Fe(VI) activation induced by transition metals.
研究领域:
环境科学
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化学
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水处理
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DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
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IF 19.503
Qiyan Wang,Sara Santos,César A. Urbina-Blanco,Wenjuan Zhou,Yong Yang,Maya Marinova,Svetlana Heyte,Thuriot-Roukos Joelle,Ovidiu Ersen,Walid Baaziz,Olga V. Safonova,Mark Saeys,Vitaly V. Ordomsky
Catalytic processes in water have a lower environmental impact, cost, and toxicity than in organic solvents. Considering the high content of water in biomass, it would be natural to use aqueous phase catalytic technology for the production of valuable products. However, in the aqueous phase, most metal-based catalysts suffer from low activity, low selectivity and deactivation due to metal oxidation and leaching. In this paper, we propose a solid micellar Ru catalyst (Ru(III)@MCM) based on single-site Ru (III) species stabilized by cetyltrimethylammonium (CTA + ) surfactant and immobilized in the walls of MCM-41 for the selective aqueous phase hydrogenation of carbonyl groups. This catalyst demonstrates exceptional selectivity, activity, and stability in comparison with conventional metallic catalysts. DFT modeling suggests that the reaction proceeds via heterolytic dissociation of hydrogen, forming a Ru-Hydride species, and subsequent hydride transfer to the carbonyl group. Water plays a key role in avoiding product inhibition.
研究领域:
催化
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绿色化学
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材料科学
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化学工程
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DOI
高影响因子
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
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2025
·Vol. 26
·期 2
·677
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IF 4.9
Yuhan Zhang,Guilong Peng,Yuting Yan,Xukun Meng,Wenwen Gong
The design of efficient advanced oxidation processes (AOPs) in the presence of bicarbonate has long attracted considerable attention in the field of environmental catalysis. In this study, sodium bicarbonate (NaHCO3) as one of the most abundant substances in actual water, was introduced to a NaClO/Ru(III) system to enhance the removal of acid orange 7(AO7). NaHCO3could significantly improve the removal efficiency of the Ru(III)/NaClO process in HCO3−at a pH range of 6.9–10.0. Ru(V)=O was identified as a dominant reactive species involved in the degradation of pollutants in the NaHCO3/NaClO/Ru(III) system. HCO3−interacts with Ru(III) to generate Ru(III)-HCO3−, which enhances the activation performance of Ru(III) under neutral or alkaline conditions. The removal of AO7 was significantly enhanced with increasing NaHCO3concentration, and the rate constant increased more than 2-fold to 4-fold as NaHCO3concentrations increased from 0 to 100 mM at pH 6.9 and 8.5. This study proposed a novel strategy to enhance the Ru(III)/NaClO process with environmentally friendly inorganic ligands and highlights its potential applications in the removal of pollutants.
研究领域:
环境催化
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化学工程
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水处理技术
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DOI
PubMed
高影响因子
Materials
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2020
·Vol. 13
·期 18
·4026
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IF 3.057
Shasha Zhang,Wenxin Ji,Ning Feng,Liping Lan,Yuanyuan Li,Yulong Ma
In this study, a Rh(I)/Ru(III) catalyst with a bimetallic space structure was designed and synthesized. The interaction between the metals of the bimetallic catalyst and the structure of the bridged dimer can effectively reduce the steric hindrance effect and help speed up the reaction rate while ensuring the stability of the catalyst. X-ray photoelectron spectroscopy (XPS) results show that rhodium accepts electrons from chlorine, thereby increasing the electron-rich nature of rhodium and improving the catalytic activity. This promotes the nucleophilic reaction of the catalyst with methyl iodide and reduces the reaction energy barrier. The methanol carbonylation performance of the Rh/Ru catalyst was evaluated, and the results show that the conversion rate of methyl acetate and the yield of acetic acid are 96.0% under certain conditions. Furthermore, during the catalysis, no precipitate is formed and the amount of water is greatly reduced. It can be seen that the catalyst has good stability and activity.Keywords:carbonylation;acetic acid;bimetallic catalyst
研究领域:
化学工程
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催化化学
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2016
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IF 5.31
Hong Zhang,Xiaoyu Yang,Zhaohui Liu,Yanzhao Yang
An arisen and environment-friendly method of cloud point extraction (CPE) which involved Octylphenoxypolyethoxyethanol (TX-114) as surfactant and 2-Mercaptobenzothiazole-functionalized ionic liquid as extractant was carried out to separate Ru(III) from aqueous phase to bottom surfactant phase for the first time. A host of variable ( e.g. , the extractant concentration, hydrochloric acid concentration, nitric acid concentration, TX-114 mass fraction, TX-114 volume and sodium chloride concentration) were evaluated and optimized to investigate the extraction behavior. At optimized experimental conditions, the extraction percentage of Ru(III) was found to be 82%, together with the enrichment factor of 40. A special complexation extraction mechanism of Ru(III) in CPE process was studied systemically and confirmed via job method, UV–vis spectrum and FT-IR spectrum in detail. Taking together, the rational-designed functional ionic liquid as a novel extractant exhibited superior extractability for Ru(III) in CPE system.
研究领域:
化学
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环境科学
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DOI
高影响因子
ACS Applied Polymer Materials
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2024
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IF 4.4
Wan Xu,Bingqian Wang,Yuan Sun,Xiaojian Ou,Yuanjun Sun,Peng Zhang,Zhenbin Chen
Ruthenium, one of the platinum group elements, plays a crucial role in industrial development, and it is important to develop a material to separate and purify ruthenium with high efficiency to ensure its supply. Herein, a thermoresponsive Ru(III)-imprinted polymer (Ru(III)-TIIP) was prepared by combining thermoresponsive technology, Pickering emulsion technology, and imprinted technology. The Ru(III)-TIIP could regulate its structure by controlling the external temperature and maintained good adsorption and separation performance. The structure and performances of Ru(III)-TIIP were tested and evaluated by Fourier transform infrared, scanning electron microscopy, energy-dispersive spectrometry, transmission electron microscopy, specific surface area, porosity analysis, zeta potential, X-ray photoelectron spectroscopy, thermogravimetric analysis, and inductively coupled plasma-atomic emission spectrometry. The results showed that the maximum adsorption capacity (Q) of Ru(III)-TIIP was 0.2203 mmol/g under 33 °C. The maximum desorption rate (D %) was 78.1%, which was reached at 25 °C. When Fe(III) was used as the interfering ion, the separation degree (R) of Ru(III)-TIIP was 3.2. Meanwhile, the study of the adsorption process of Ru(III)-TIIP to Ru(III) was more suitable to be expressed by pseudo-first-order kinetics and the Langmuir model. When Ru(III)-TIIP was applied to the platinum group catalyst leach solution, the content of platinum group elements ranged from 53.72 to 82.09% after one adsorption/desorption cycle. In addition, Ru(III)-TIIP had maintained 66.14 and 81.25% of the original capacity for Q and R after 11 adsorption/desorption cycles.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
Applied Materials Today
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2020
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IF 8.352
Fangman Chen,Fan Zhang,Dan Shao,Weibin Zhang,Liqin Zheng,Wei Wang,Wendi Yang,Zheng Wang,Jianxin Chen,Wen-fei Dong,Fangnan Xiao,Yunkun Wu
Ruthenium-based agents are promising in cancer chemotherapy but lack specific targeting and controlled release properties. Herein, a new class of bioreducible mer-[Ru(III)Cl 3 (dmso)(L)] prodrugs with highly DNA binding affinity were designed and synthesized for nucleus-targeted chemotherapy and selective activation in response to the tumor microenvironment. In this regard, ruthenium(III) prodrugs were reduced into highly active ruthenium(II) drugs in response to high intracellular glutathione levels, resulting in tumor apoptosis through synergistic intercalation that blocked DNA replication and coordination that cleaved nuclear DNA. In light of this, a multifunctional nanodrug (Ru-MSN-PLip) was constructed by integrating RuDPNI prodrug-loaded mesoporous silica nanoparticles (Ru-MSN) with a fusion protein-incorporated liposome (PLip) to achieve multiple targeting and eGFP-based fluorescence imaging of nonsmall cell lung cancer. Due to fusion protein-based cancer cell recognition and Ru(III) prodrug-mediated nuclear DNA targeting, Ru-MSN-PLip achieved sequential delivery and greater antitumor activity. In addition, Ru-MSN-PLip exhibited long-term blood circulation and selective accumulation in tumors, leading to significantly limited tumor growth in vivo without notable toxicity. Our findings indicated the potential applications of these types of bioreducible and traceable nanoprodrugs for efficient and safe nonsmall cell lung cancer therapy.
研究领域:
癌症研究
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纳米技术
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药学
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分子生物学
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产品关联
DOI
高影响因子
JOURNAL OF PHARMACEUTICAL AND BIOMEDICAL ANALYSIS
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2021
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IF 3.935
Ying Cheng,Jing Tang,Xue Chen,Fang Wang,Zilin Chen
Ten-eleven translocation protein 1 (TET1) is one member of TET proteins family which plays a key role in dynamic DNA methylation-demethylation process. Herein, a novel biosensor was constructed for TET1 detection and its inhibitors screening utilizing restriction digestion of endonuclease enzyme MspI. Half-methylated oligonucleotide (5mC DNA) was used as target and Ru(NH 3 ) 6 3+ as electrochemical signal probe. After the treatment by TET1 and T4 β-glucosyltransferase (T4 β-GT), target oligonucleotide would not be recognized and digested. If there was no TET1, the target would be digested and the response of biosensor decreased greatly. The current difference of biosensor with and without the incubation with TET1 was therefore dependent on the concentration of TET1. To increase sensitivity of the biosensor, nanostructured film at electrode surface and nanoparticles modified oligonucleotides were employed as signal amplification elements for Ru(NH 3 ) 6 3+ recycling. Finally, this biosensor showed high performance with a wide linear range of TET1 concentration from 3.5–21 ng/μL and a low detection limit of 0.33 ng/μL, which is superior to other existing methods. The inhibition effects of Bobcat339 on TET1 was successfully proved by our biosensor with an IC 50 of 38 μM. Not only that, but the feasibility of the biosensor for inhibitors screening was evaluated and further confirmed by other compounds including two anticancer drugs and three active ingredients of traditional Chinese medicine.
研究领域:
生物化学
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分子生物学
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分析化学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF PHARMACEUTICAL AND BIOMEDICAL ANALYSIS
·
2021
·
IF 3.935
Li Hou,Xuanhan Zhang,Yuxiu Huang,Min Wang,Xiaoyu Chen,Tianran Lin,Yanhui Tan,Shulin Zhao
A sensitive and ratiometric electrochemical biosensor was developed for the determination of dimethoate via alkaline phosphatase (ALP) mediated dissolution of nano-MnO 2 and [Ru(NH 3 ) 6 ] 3+ (Ru(III)) redox recycling. The electroactive probe Ru(III) was adsorbed on the nano-MnO 2 with the high specific surface area through electrostatic interaction to form the MnO 2 -Ru(III) nanocomposite, which was then fixed on the surface of the glassy carbon electrode. When the dimethoate inhibited the catalytic activity of ALP in a homogeneous system, the hydrolysate L -ascorbic acid (AA) produced by ALP hydrolysis of L -ascorbic acid-trisodium 2-phosphate (AAP) decreased. The solution was then incubated with a glassy carbon electrode modified by MnO 2 -Ru(III). At this time, only a small amount of MnO 2 -Ru(III) was decomposed and Ru(III) was rapidly electroreduced to Ru(II) on the surface of the electrode. The in-situ produced Ru(II) was chemically oxidized back to Ru(III) by Fe(III). The redox recycling of Ru(III) was completed and the Ru(III) reduction current signal was amplified. The process consumed part of Fe(III) to reduce the reduction current signal of Fe(III), and the ratio of the two reduction currents (I Ru(III) /I Fe(III) ) increased significantly. The I Ru(III) /I Fe(III) value increased with the increase of dimethoate concentration in the linear range of 0.01–300 ng mL −1 , and the detection limit was 6.3 pg mL −1 . It has been successfully applied to the determination of dimethoate in oilseed rape and lettuce with a satisfactory result.
研究领域:
分析化学
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电化学
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生物传感器
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环境监测
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DOI
PubMed
高影响因子
ANALYTICAL CHEMISTRY
·
2016
·
IF 5.886
Hui Zhang,Huilei Dong,Guoqing Yang,Hongfei Chen,Chenxin Cai
Effective detection of DNA methyltransferase (DNMT) activity is significant for cancer research. Herein, we developed a sensitive electroanalytical method to detect human DNA (cytosine-5)–methyltransferase 1 (DNMT1) from crude lysates of cancer cells. In this assay, capture DNA having a preferred DNMT1 methylation site was immobilized on a gold electrode and then hybridized with gold nanoparticle (Au NP)–DNA complexes. The modified electrodes were equilibrated with the lysate and then incubated with methylation-sensitive restriction enzyme. If the lysate was negative for DNMT1 activity, the Au NP–DNA complexes would be cut by the restriction enzyme and released from the electrode. Conversely, restriction enzyme cleavage would be blocked by the fully methylated duplexes, and the Au NP–DNA complexes would remain on the electrode. Electroactive Ru(NH3)63+ was used as the signal reporter, because of its electrostatic attraction to DNA, resulting in an electrochemical signal. Since the electrochemical signal reflects the amount of Ru(III) redox and the amount of Ru(III) redox is correlated with the activity of DNMT1, the activity of DNMT1 is proportional to the electrochemical signal. The signal could be amplified by the numerous DNAs on the Au NPs and further amplified by Ru(III) redox recycling. With this method, a detection limit down to 0.3 U/mL for pure DNMT1 and 8 MCF-7 cells was achieved. DNMT1 activities of different cell lines were also successfully evaluated.
研究领域:
生物化学
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分析化学
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分子生物学
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产品关联
DOI
PubMed
高影响因子
SEPARATION SCIENCE AND TECHNOLOGY
·
2018
·
IF 1.2
Yan Yan,Qi Wang,Zeyang Xiang,Yanzhao Yang
A reasonable project was presented for the extraction and separation of Pt(IV), Pd(II), Ru(III), and Rh(III) from the mixed imidazolium-based ionic liquids (ILs) [C6mim]Cl, [C6mim][NTf2], and [C6mim][DDTC]. Pt(IV) was first separated from other three platinum group metals with a mixture of [C6mim]Cl and [C6mim][NTf2]. Then, separation of Pd(II) and Ru(III) from Rh(III) was realized by changing the concentration of [C6mim][DDTC]. Back-extraction of Pt(IV), Pd(II), and Ru(III) from loaded hydrophobic phase and the recovery of Rh(III) in aqueous phase were also investigated. Mechanisms between Pd(II)/Ru(III) and [C6mim][DDTC] were further explored using ultraviolet spectrophotometry (UV-Vis), infrared spectrophotometry (FTIR), the method of continuous variations, ab initio quantum chemical studies, and X-ray crystallographic analysis. The results afford more directions for extracting and separating metals by introducing devisable functionalized group into ILs.
研究领域:
化学工程
·
分析化学
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产品关联
DOI
高影响因子
REACTIVE & FUNCTIONAL POLYMERS
·
2017
·
IF 3.151
Jianxian Zeng,Zhe Zhang,Zhihui Dong,Panfeng Ren,Yuan Li,Xiao Liu
An ion-imprinted blend membrane (Ru(III)-IIM) for selectively adsorbing ruthenium(III) from aqueous solutions was fabricated by blending poly(methyl methacrylate- co -2-hydroxyethyl methacrylate) P(MMA-HEMA) with polyvinylidene fluoride (PVDF). Firstly, P(MMA-HEMA) was successfully synthesized and characterized. Subsequently, combining with the ion-imprinting technology, a series of Ru(III)-IIMs were fabricated via the non-solvent induced phase inversion method. The results indicated that increasing the polymer concentration and extending the evaporation time led to transform the cross-section of membranes from macrovoid structure to a finger-like or tear-like even sponge structure, and also decreased the water flux. The contact angle tests showed the hydrophilicity of Ru(III)-IIMs were effectively improved by blending with P(MMA-HEMA), compared with the PVDF membrane. The adsorption experiments showed that the adsorption capacity of ruthenium(III) onto the Ru(III)-IIM was pH-dependent, and the maximum adsorption capacity reached 42.31 mg g − 1 at pH 2.0. The adsorption process was well described by the pseudo-second-order kinetic model and the Langmuir isotherm model. The selective adsorption was studied by using Ni(II) as an interfering ion. Compared with the non-imprinted membrane, the Ru(III)-IIM showed a higher selectivity for Ru(III), with a selectivity coefficient of 6.0 for Ru(III)/Ni(II). In addition, the Ru(III)-IIM had a high reusability and still maintained about 95% of its initial adsorption capacity for Ru(III) after eight cycles.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
危险品化学品经营许可证（带存储）