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.
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高影响因子
Small Methods
·
2021
·Vol. 5
·期 7
·2100505
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IF 14.188
Yong-Ya Zhang,Nan Zhang,Peng Peng,Rui Wang,Yan Jin,Ya-Kun Lv,Xin Wang,Wei Wei,Shuang-Quan Zang
Design and development of cost-effective electrocatalysts with high efficiency and stability for scalable and sustainable hydrogen production through water splitting is still challenging. Herein, with the aid of divinyl functionalized ionic liquids, uniformly distributed Ru nanoparticles (NPs) on nitrogen-doped carbon frameworks are obtained via an in situ confined polymerization strategy. Attributed to the unique lamellar structure and confinement effect of carbon supports, the optimized homo-PIL-Ru/C-600 (with Ru 10 wt%) catalyst exhibits superior catalytic efficiency for the hydrogen evolution reaction with the overpotential of only 16 mV at a current density of 10 mA cm −2 and the corresponding Tafel slope of only 42 mV dec −1 . Moreover, the performance can be well reserved even after 10 000 cycles, demonstrating excellent stability and promising potentials for industrial application. This work not only provides a facile approach for the preparation of highly efficient Ru-based catalysts, but also guides the synthesis of other highly dispersed metallic NPs for special applications.
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Inorganic Chemistry Frontiers
·
2021
·Vol. 8
·期 21
·4712-4719
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IF 6.569
Tianxing Wu,Hanqi Meng,Rui Dang
Electrocatalytic hydrogenation is a competing reaction for hydrogen evolution that occurs in the presence of organic compounds containing unsaturated chemical bonds using water as the hydrogen donor. Here, we propose a simple method to synthesize amorphous Ta2O5 loaded amorphous Ru with poor crystallinity. The amorphous composite (Ta2O5/Ru-4.0-400) with an ultra-low Ru loading amount (2.16 wt%) exhibits 69.8% conversion of cinnamaldehyde with 29.1% FE and 100% selective formation of half-hydrogenated hydrocinnamaldehyde under a constant potential of −1.1 V vs. RHE for 5 h. Detailed experimental studies revealed that the amorphous structure with poor crystallinity offers structural flexibility and rich defects for electrochemical hydrogenation reactions, and the Ta2O5 substrate serves as a bridge to effectively facilitate electron transfer from Ru to CAL molecules. This work presents a new strategy for designing highly efficient electrocatalysts with an amorphous structure for the hydrogenation of organic compounds containing unsaturated chemical bonds.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
·
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.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2019
·
IF 14.229
Meijiao Qu,Yimin Jiang,Miao Yang,Shu Liu,Qifei Guo,Wei Shen,Ming Li,Rongxing He
Highly active and stable catalysts toward hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) is extremely important but challenging for overall water splitting. Herein, a strategy by modulating surface electron densities is adopted to design new catalyst: the Ru-NiFe-P nanosheets on 3D self-supported nickel foam was developed by doping a small quantity of Ru into transition metals phosphates. The designed catalyst displays excellent electrocatalytic performance in 1.0 M KOH, with low overpotentials of 44 mV at 10 mA cm −2 for HER and 242 mV at 100 mA cm −2 for OER. Particularly, it only needs 1.47 V to yield 10 mA cm −2 for overall water splitting. Density functional theory calculations reveal that Ru-incorporated NiFe-P can generate new active sites on Ru atoms and increase the catalytic activity of original P sites leading to an optimal Gibbs free-energy on catalysts surface. This work offers a new perspective for designing admirable electrocatalysts.
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ChemCatChem
·
2019
·Vol. 11
·期 5
·1518-1525
·
IF 4.495
Fengli Yu,Lihua Xie,Fangzhu Wu,Bing Yuan,Congxia Xie,Shitao Yu,Xien Liu,Lei Wang,Dan Wang
Graphical Take core ! Highly dispersed and stable Ru nanoparticle catalysts loaded on boron-doped amphiphilic, core-shell, mesoporous molecular sieves are successfully prepared and used to catalyze the hydrogenation of α-pinene to cis -pinane with an excellent catalytic activity, high selectivity, and good recyclability, in mild experimental conditions given that every nanocomposite is equivalent to a microreactor. Highly dispersed and stable catalysts comprising Ru nanoparticles supported on boron-doped amphiphilic core-shell mesoporous molecular sieves (MMS−C@MMS−NH 2 /B/Ru) with alkyl-modified hydrophobic silica core and NH 2 -functionalized hydrophilic silica shell are successfully prepared for use in hydrogenation of α-pinene for the first time. Dodecyl-modified MMS−C 12 @MMS−NH 2 /B/Ru exhibits the best catalytic activity under mild hydrogenation conditions. The abundant −NH 2 functional groups on the molecular sieve surface and their amphipathy allow the sieves to facilitate attachment of more Ru nanoparticles, and to simplify their dispersion in the water-organic reaction medium. Moreover, B-doped molecular sieves may adjust their acidity to meet the needs of α-pinene hydrogenation. Under mild reaction conditions (25 °C, 1 MPa H 2 , and 1 h), α-pinene can be completely converted with 99 % selectivity to cis -pinane, because every nanocomposite is equivalent to a microreactor. The catalytic activity does not change much over 5 cycles, indicating that Ru nanoparticles are stably loaded on the molecular sieves.
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APPLIED CATALYSIS A-GENERAL
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2018
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IF 4.521
Zhenzhen Lin,Mengting Luo,Yindi Zhang,Xiaoxue Wu,Yanghe Fu,Fumin Zhang,Weidong Zhu
Heterogeneous catalytic conversion of biomass-derived methyl levulinate (ML) to γ-valerolactone (GVL) is highly attractive as a sustainable route to mitigating the dependence on nonrenewable fossil resources. However, this route is limited by its low selectivity toward GVL and severe reaction conditions. Here, we present a synergistic catalytic process that offers exclusive GVL selectivity with complete ML conversion under mild conditions (80 °C, 0.5 MPa of H 2 pressure). This is achieved over a dual-functionalized catalyst of Ru nanoparticles (Ru-NPs) and Brønsted acid SO 3 H groups in a Cr-based metal-organic framework (MIL-101). The Ru-NPs served as metal sites for the hydrogenation of ML to methyl-3-hydroxyvalerate (MHV) and the acidic SO 3 H moieties promoted the cyclization of MHV to generate GVL via lactonization. In contrast, GVL production was significantly suppressed over the physically mixed congener (2.0 wt% Ru/MIL-101 + MIL-101-SO 3 H). This result demonstrates an unrivalled advantage of the dual integration of metal/acid sites in a single MOF crystal, and the relative amount of sulfonic acid groups in the catalyst can exert significant influence on the overall catalytic performances. The activation energies for the hydrogenation and lactonization steps with the developed catalyst were 29.5 and 42.1 kJ/mol, respectively, which are much lower than those observed with the traditional 5.0 wt% Ru/AC catalyst.
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SENSORS AND ACTUATORS B-CHEMICAL
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2015
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IF 4.097
Amin Zhang,Chongchong Miao,Hongyuan Shi,Hongkun Xiang,Chusen Huang,Nengqin Jia
Recent years have witnessed the great development of electrochemiluminescence (ECL) as a platform for the analytical processes in many fields, which includes pharmaceutical analysis, immunoassay, DNA analysis as well as clinical analysis. Herein, a novel electrochemiluminescence (ECL) sensor was fabricated for ultrasensitive detection of atropine based on Ru(bpy) 3 2+ /carbon nanospheres/Nafion composite film. The carbon nanospheres (CNPs) in composite film were obtained through a hydrothermal method. Then, electrochemical and ECL behaviors of the proposed sensor were investigated. Under the optimal conditions, the constructed atropine sensor showed a wide linear range from 0.5 to 250 μM with a detection limit of 0.17 μM (at signal-to-noise ratio of 3). Moreover, the results indicated that the CNPs-based ECL sensor exhibited excellent sensitivity and favorable stability, which might be ascribed to the high surface area and the good electrical conductivity of CNPs. Furthermore, the ECL sensor was applied for the determination of atropine in atropine sulfate injection samples and displayed a desirable result. The proposed ECL sensor could be easily obtained and be promising used for drug assay.
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GREEN CHEMISTRY
·
2017
·Vol. 19
·期 9
·2201-2211
·
IF 9.125
Wenxiu Cao,Wenhao Luo,Hongguang Ge,Yang Su,Aiqin Wang,Tao Zhang
The hydrogenation of levulinic acid (LA) to γ-valerolactone (GVL) is a crucial reaction included in many biorefinery schemes for the production of renewable chemicals and fuels. The development of highly stable supported Ru-based catalysts in the polar protic liquid phase under hydrothermal conditions is still a major challenge. Here, we prepared a 0.85 wt% Ru/ZrO2@C catalyst using a new stabilization strategy based on the UiO-66 (Zr-MOF) material. The catalytic performance of this Ru/ZrO2@C in LA-to-GVL was tested and compared with commercial 5 wt% Ru/C at 10 bar H2, 413 K in water and also in high protic aqueous solution (pH = 1). The full conversion of LA and quantitative yield of GVL were achieved with both catalysts. However, the 5 wt% Ru/C showed poor resistance to deactivation already after the first run. ICP, XPS, HRTEM, AC-STEM, TPR and physisorption data showed that quick deactivation of Ru/C was mainly caused by the leaching of ruthenium in addition to the loss of surface area via carbonaceous deposition in micro-pores. In contrast, the self-prepared Ru/ZrO2@C catalyst showed no apparent drop in catalytic performance either in water or in high protic aqueous solution upon multiple recycling, and no leaching of ruthenium was found even under harsh conditions (pH = 1). Remarkably, in the Ru/ZrO2@C catalyst, Ru (probable single-atom) was highly dispersed on nanotetragonal ZrO2 (3.3 nm), embedded in the amorphous carbon, and no apparent Ru nanoclusters were observed even after reactions. TPR results indicated that this excellent stability might be attributed to strong metal–support interaction between Ru and nanotetragonal ZrO2.
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Small
·
2024
·
IF 13
Hongjie Yu,Lijun Zhang,Shaojian Jiang,Wenke Liu,Kai Deng,Ziqiang Wang,You Xu,Hongjing Wang,Liang Wang
Water splitting for hydrogen production is limited by high cell voltage and low energy conversion efficiencies due to the slow kinetic process of the oxygen evolution reaction (OER). Here, an electrolytic system is constructed in which the cathode and anode co-release H 2 at ultra-low input voltage using formaldehyde oxidation reaction (FOR) instead of OER. The prepared RuCe co-doped Cu 2 O nanotubes on copper foam (RuCe-Cu 2 O/CF) are used as electrode materials for the HER-FOR system. A current density of 0.8 A cm −2 is achieved at 0.55 V, and a stable hydrogen production process is realized at both the cathode and anode. Density functional theory (DFT) studies show that the synergistic effect of Ru and Ce drives: i) the d -band center of RuCe-Cu 2 O/CF away from the Fermi energy level; ii) the energy barrier for the C─H cracking of the H 2 C(OH)O * intermediate in FOR is lowered, which promotes the formation of H 2 from H * , and iii) ΔG H* tends to 0 (−0.1 eV), optimizing the reaction kinetics of HER. This work provides a new design for an efficient catalyst for dual hydrogen production systems from water splitting.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Ruyi Cui,Yong Zhou,Xingyi Xu,Hengxin Fang,Wenlong Wang,Sanmei Wang,Pengbo Lyu,Lizhong Sun,Biao Wang,Changqing Sun
Ammonia borane (AB) is a highly promising hydrogen carrier with significant potential for safe and efficient hydrogen storage and transportation. However, its high chemical stability poses considerable challenges for hydrogen release, emphasizing the importance of highly efficient catalysts. In this study, we present Ru nanocatalysts supported on UiO-66-NH 2 -derived carbon nitride (Ru/CN) as high-performance catalysts for AB hydrolysis. A facile pyrolysis-impregnation method was employed to synthesize highly dispersed Ru nanoparticles with tunable sizes, while retaining the octahedral morphology of the MOF-derived support. Detailed characterizations revealed tunable Ru nanoparticle sizes achieved by simply adjusting the Ru loading. Among the catalysts, the 2.5Ru/CN, featuring Ru nanoparticles with an average size of 2.2 nm, achieved an impressive turnover frequency of 493 mol H 2 (mol Ru −1 ·min −1 ) at 30 °C, demonstrating exceptional catalytic activity. Density functional theory (DFT) calculations confirmed that the optimized Ru cluster size enhances key catalytic steps, including H 2 O dissociation, AB activation, and H 2 desorption. This study highlights the critical role of fine-tuning nanoparticle sizes and provides valuable insights into the rational design of advanced catalysts for more efficient hydrogen production.
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Journal of Energy Chemistry
·
2025
·
IF 14.9
Chenggong Niu,Yi Liu,Shuqing Zhou,Heyang Liu,Linyu Chen,Jingya Guo,Tayirjan Taylor Isimjan,Xiulin Yang
Triggering structural asymmetry can induce charge redistribution and modify electronic structures, which is of great significance for the design of high-performance hydrogen oxidation reaction (HOR) electrocatalysts. Herein, we propose a dual anion-induced strategy to create an innovative RuS 2 -RuO 2 heterostructure featuring abundant S-Ru-O interfaces (RuS 2 -RuO 2 @C). This RuS 2 -RuO 2 @C demonstrates an impressive mass activity of 2.61 mA μ g R u - 1 and an exchange current density of 2.96 mA cm −2 , surpassing Pt/C and other comparative samples by over 20 times. Durability assessments confirm the superior stability of RuS 2 -RuO 2 @C, with only minimal performance loss during operation. Density functional theory (DFT) calculations indicate that the asymmetric S-Ru-O configuration optimizes the interfacial electronic structure and shifts the d -band center closer to the Fermi level, effectively reducing the energy barrier of the rate-determining step (RDS) in the alkaline HOR process. Moreover, in situ attenuated total reflection surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) characteristics disclose the formation of a substantial hydrogen bond network at the S-Ru-O interface, which aids in the desorption of H 2 O ad and facilitates the vital Volmer step in the HOR pathway.
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