FOOD CHEMISTRY
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2023
·
IF 8.8
Ying Yu,Xiaodan Wang,Mingyang Li,Dengyong Liu
5′-Guanosine monophosphate (5′-GMP) is one main source of freshness in broths. Herein, an electrochemical platform based on a novel ternary nanocomposite glassy carbon electrode modified with advantageously-united gold nanoparticles, 2,2′-bipyridine hydrated ruthenium (Ru(bpy) 2 Cl 2 ) and sulfonated multi-walled carbon nanotubes (SMWCNTs)was prepared and used to detect 5′-GMP. After conditions optimization, the best performance of the electrochemical sensor was found in acidic media, including high specificity, sensitivity and selectivity. The electrochemical sensor exhibited a wide linear range under the optimal conditions. The enhanced sensitivity of this sensor was attributed to the Ru(bpy) 2 Cl 2 and functionalized SMWCNTs that provided high electrical conductivity and electrocatalytic properties during electrochemical reaction . Precise analysis of 5′-GMP in actual broth samples showed satisfactory recovery. Thus, the sensor can be used in the market and food enterprises.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Lulu Zhang,Rui Li,Luyao Cui,Zijun Sun,Lijun Guo,Xiaochao Zhang,Yunfang Wang,Yawen Wang,Zhuobin Yu,Tao Lei,Xuan Jian,Xiaoming Gao,Caimei Fan,Jianxin Liu
Synergistic water activation and nitrogen reduction process is significant to the photocatalytic ammonia synthesis reaction, in which the obtainment of active hydrogen (H*) from H 2 O dissociation and then transfer to N 2 activation site is essential. Herein, the oxygen vacancies (OVs) enhanced hydrogen spillover is used to increase the H* transfer between the H 2 O activation site (Ru) and the N 2 activation site (OVs-rich W 18 O 49 ). Results shown that the OVs-rich Ru/W 18 O 49 achieves high activity for NH 3 production with a yield of 222.75 µmol‧g −1 ‧h −1 , which is 5.60 folds of the OVs-deficient Ru/W 18 O 49 . Control experiments, characterization, and theoretical calculation made it clear that OVs played crucial roles in enhancing the hydrogen spillover by modifying the support's Gibbs free energy for hydrogen adsorption and lowering the barrier of H* migration. Finally, the detail mechanism was explained from a new perspective. This strategy may provide new insights for other hydrogenation reactions under mild conditions.
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ACS Applied Materials & Interfaces
·
2023
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IF 9.5
Wentao Wang,Qizhu Qian,Yapeng Li,Yin Zhu,Yafei Feng,Mingyu Cheng,Huaikun Zhang,Yangyang Zhang,Genqiang Zhang
Hydrazine oxidation-assisted water electrolysis provides a promising way for the energy-efficient electrochemical hydrogen (H2) and synchronous decomposition of hydrazine-rich wastewater, but the development of highly active catalysts still remains a great challenge. Here, we demonstrate the robust and highly active Ru nanoparticles supported on the hollow N-doped carbon microtube (denoted as Ru NPs/H-NCMT) composite structure as HER and HzOR bifunctional electrocatalysts. Thanks to such unique hierarchical architectures, the as-synthesized Ru NPs/H-NCMTs exhibit prominent electrocatalytic activity in the alkaline condition, which needs a low overpotential of 29 mV at 10 mA cm–2 for HER and an ultrasmall working potential of −0.06 V (vs RHE) to attain the same current density for HzOR. In addition, assembling a two-electrode hybrid electrolyzer using as-prepared Ru NPs/H-NCMT catalysts shows a small cell voltage of mere 0.108 V at 100 mA cm–2, as well as the remarkable long-term stability. Density functional theory calculations further reveal that the Ru NPs serve as the active sites for both the HER and HzOR in the nanocomposite, which facilitates the adsorption of H atoms and hydrazine dehydrogenation kinetics, thus enhancing the performances of HER and HzOR. This work paves a novel avenue to develop efficient and stable electrocatalysts toward HER and HzOR that promises energy-saving hybrid water electrolysis electrochemical H2 production.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Ziyi Xu,Meiling Fan,Shifeng Tan,Rui Wang,Wenmao Tu,Xiege Huang,Hongfei Pan,Haining Zhang,Haolin Tang
The development of efficient and stable electrocatalysts for hydrogen evolution reaction (HER) is impending for the advancement of water-splitting. In this study, we developed a novel electrocatalyst consisting of highly dispersed Ru nanoclusters ameliorated by cobalt single atoms and N, S co-doped reduced graphene oxide (Co SA Ru NC @NSG). Benefitted from the optimized electronic structure of the Ru nanoclusters induced by the adjacent single atomic Co and N, S co-doped RGO support, the electrocatalyst exhibits exceptional HER performance with overpotentials of 15 mV and 74 mV for achieving a current density of 10 mA cm −2 in alkaline and acidic water. The catalyst outperforms most noble metal-based HER electrocatalysts . Furthermore, the electrolyzer assembled with Co SA Ru NC @NSG and RuO 2 demonstrated an overall voltage of 1.56 V at 10 mA cm −2 and an excellent operational stability for over 25 h with almost no attenuation. Theoretical calculations also deduce its high HER activity demonstrated by the smaller reaction energy barrier due to the optimized electronic structure of Ru nanoclusters . This strategy involving the regulation of metal nanoparticles activity through flexible single atom and GO support could provide valuable insights into the design of high-performance and low-cost HER catalysts.
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高影响因子
NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 31
·14819-14827
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IF 3.3
Zijian Wang,Yuyao Wang,Zhengyu Pan,Guoquan Zhou,Lele Yan,Lina Zhu,Zheng Fang,Tongyang Song,Xianlang Chen,Rongrong Li
The selective hydrogenation of benzoic acid (BA) under mild conditions has great significance in industrial applications. In this study, Ru catalysts supported on P and N-doped mesoporous carbons (PPNCs) were prepared and tested for the selective hydrogenation of BA. Among all the catalysts, Ru/PPNC-2 exhibited superior conversion (99.46%) and selectivity (99.95%), maintaining a high yield and good stability even after seven repeated tests. The experimental results show that the introduction of an appropriate amount of P into the catalyst forms an enhanced synergistic effect with N, so that the ruthenium nanoparticles (Ru NPs) are uniformly dispersed on the support and have a strong interactive force with the support to obtain more active sites, thereby promoting the catalyst activity and stability. This study provides an idea for the study of BA catalytic hydrogenation catalysts.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2023
·
IF 7.2
Jiayao Chen,Yuan Gao,Wenwen Yang,Zhiwei Li,Kun Xiong
Designing highly active and durable catalysts is considered to be crucial for enhancing hydrogen evolution reaction (HER) from water electrolysis . Although some studies indicate that anatase TiO 2 is a promising candidate for electrolytic hydrogen evolution reaction, the influence of different crystalline phases of TiO 2 on the supported Ru catalysts for electrocatalytic HER performance is rarely systematically explored. Herein, a series of Ru/TiO 2 -X (X = R (Rutile), A (Anatase), and P25) catalysts were prepared to investigate the influence of the rutile and anatase phases of TiO 2 on the catalytic activity of Ru catalysts in HER. The findings demonstrate that the HER activity is much affected by the variation of the titania structure, when other factors are kept constant. The 15Ru/TiO 2 -R-H 2 has superior HER performance with a small overpotential of 63 mV to achieve a current density of 10 mA cm −2 in acidic electrolyte and 99 mV in alkaline electrolyte compared to 15Ru/TiO 2 -A-H 2 and 15Ru/TiO 2 -P25-H 2 . This might be attributed to the faster electron transfer and lower Fermi level caused by the oxygen vacancy (V O ) and strong metal-support interaction (SMSI), along with the exposure of active sites afforded by the highly dispersed ruthenium nanoparticles on the rutile TiO 2 . Our results indicate that the presence of rutile TiO 2 support alone is adequate to maintain Ru in its most active form and make it a more performing catalyst, compared to anatase titania and P25.
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FUEL
·
2022
·
IF 8.035
Zhi Yang,Bowen Luo,Riyang Shu,Zhuojie Zhong,Zhipeng Tian,Chao Wang,Ying Chen
Hydrodeoxygenation (HDO) is an indispensable reaction in the field of fuel and chemical production, and the synergistic effect of metal–acid sites in the catalyst makes great influence to it. Herein, a bifunctional catalyst of Ru/C combined with phosphotungstic acid (HPW) was employed for the hydrodeoxygenation (HDO) of lignin-derived compounds to make full use of the synergistic effect of active metal–acid sites. HPW possessed a temperature-controlled phase-transfer behavior, which made it dispersed well on the surface of Ru/C catalyst and resulted in a close integration of acid site with metal site. Ru/C-HPW catalyst also owned the advantage of high reaction rate and good recyclability, which exhibited no obvious catalytic activity loss after 5 runs. Lignin-derived phenolic compounds including monomers and dimers enabled to obtain an efficient transformation to cycloalkanes at the temperature of 200 °C. Moreover, a high HDO reaction efficiency of raw lignin-oil was also observed in this study, with the increasing hydrocarbon content from 5.5% to 78.9%. This novel catalytic system can achieve a high HDO efficiency under mild conditions.
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MICROCHEMICAL JOURNAL
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2022
·
IF 5.304
Xueyuan Li,Xuezhong Du
Surface enhanced electrochemiluminescence (SEECL) emission of the Ru(bpy) 3 2+ (bpy = 2,2′-bipyridyl)/tripropylamine (TPA) system by [email protected] 2 core/shell nanoparticles (NPs) was achieved owing to the electromagnetic field enhancement induced by localized surface plasmon resonance (LSPR) of internal Au cores. The Ru(bpy) 3 2+ /TPA system in electrolyte solution showed a maximum ECL enhancement when a glassy carbon electrode (GCE) was modified with [email protected] 2 NPs ( [email protected] 2 /GCE; Au core, ca. 68 nm; silica shell, 12 nm). The ECL emission of the system in the case of [email protected] 2 /GCE was 29 fold stronger than the ECL emission in the case of bare GCE, ca. 39 fold stronger than the ECL emission in the case of hollow silica NP-modified GCE, and 100 fold stronger than the ECL emission in the case of AuNP-modified GCE. To the best of our knowledge, the respective folds of ECL enhancement in the Ru(bpy) 3 2+ /TPA system by the LSPR-induced electromagnetic field of AuNPs are the largest reported to date. The ECL emission of TPA •+ radical cations was detected for the first time taking the advantage of the electromagnetic field enhancement. A SEECL platform based on the [email protected] 2 /GCE in the Ru(bpy) 3 2+ /TPA system was constructed for the detection of dopamine (DA). This is the first example that the AuNP-enhanced ECL emission was quenched by DA for the selective detection of DA, and a wide linear range of 0.01–600 μM directly relevant to DA concentration was obtained with a low detection limit of 0.004 μM and high sensitivity and accuracy. The mechanism that the ECL emission of the Ru(bpy) 3 2+ /TPA system was quenched by DA for the detection of DA was clearly elaborated. The level of DA in human serum was determined using the SEECL platform.
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GREEN CHEMISTRY
·
2021
·Vol. 24
·期 3
·1152-1164
·
IF 10.182
Jiahui Zhan,Rui Hu,Xi Luo,Cheng Zhang,Gang Luo,Jiajun Fan,James H. Clark,Shicheng Zhang
Cyclohexanol is an essential intermediate in the chemical industry for the synthesis of nylon and other materials, but the direct hydrogenation of phenol to produce cyclohexanol is problematic owing to excessive energy consumption associated with the harsh reaction conditions. In this regard, novel composite catalysts (Ru/Nb2O5-nC18PA) coated with octadecylphosphonic acid (C18PA) were prepared via an impregnation method to be applied for the efficient hydrogenation of phenol to produce cyclohexanol in a biphasic system consisting of water and decalin solvent. Under a hydrogen pressure of 12 bar and 80 °C, nearly 100% conversion of phenol and 93% yield of cyclohexanol were achieved within 4 hours. With the introduction of more Lewis acid sites the aromatic ring is activated, which promotes the HYD (hydrogenation) path of phenol, thereby giving improved selectivity to cyclohexanol. A mechanism-exploration experiment was carried out and showed that the strong binding effect between the surface of the Ru/Nb2O5-nC18PA catalysts and the benzene ring allows the aromatic ring in phenol to be hydrogenated, increasing the selectivity to cyclohexanol. This biphasic catalytic system enhances the potential value of lignin via the catalytic hydrogenation of lignin-derived phenols.
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BIOORGANIC CHEMISTRY
·
2021
·
IF 5.275
Lanmei Chen,Jie Wang,Xianhong Cai,Suxiang Chen,Jingjing Zhang,Baojun Li,Weigang Chen,Xinhua Guo,Hui Luo,Jincan Chen
Both ruthenium (Ru) and isoquinoline (IQ) compounds are regarded as potential anticancer drug candidates. Here, we report the synthesis and characterization of three novel cyclometalated Ru(II)-isoquinoline complexes: RuIQ-3 , RuIQ-4 , and RuIQ-5, and evaluation of their in vitro cytotoxicities against a panel of cell lines including A549/DDP, a cisplatin-resistant human lung cancer cell line. A549/DDP 3D multicellular tumor spheroids (MCTSs) were also used to detect the drug resistance reversal effect of Ru(II)-IQ complexes. Our results indicated that the cytotoxic activities against cancer cells of Ru(II)-IQ complexes, especially RuIQ-5 , were superior compared with cisplatin. In addition, RuIQ-5 exhibited low toxicity towards both normal HBE cells in vitro and zebrafish embryos in vivo . Further investigation on cellular mechanism of action indicated that after absorption by A549/DDP cells, RuIQ-5 was mainly distributed in the nucleus, which is different from cisplatin. Besides, RuIQ-5 could induce apoptosis through mitochondrial dysfunction, reactive oxygen species (ROS) accumulation, ROS-mediated DNA damage, and cycle arrest at both S and G2/M phases. Moreover, RuIQ-5 could inhibit the overexpression of Nrf2 through regulation of Akt/GSK-3β/Fyn signaling pathway and hindering the nuclear translocation of Nrf2. Based on these findings, we firmly believe that the studied Ru(II)-IQ complexes hold great promise as anticancer therapeutics with high effectiveness and low toxicity.
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ENVIRONMENTAL RESEARCH
·
2023
·
IF 8.3
Zhengquan Yan,Xuemei Zhou,Lingmin Kong,Wenjing Xu,Junkai Hao,Shuo Sun,Jing Feng,Huitian Zhi,Xiao Zhu,Lei Hu
To effectively differentiate toxic aminophenol isomers, a kind of spindle-shaped Cu-Ru bimetal mesoporous nanozyme (Cu-Ru MPNZ) with high specific surface was developed by one-pot homogeneous reduction method, directed by hexadecyl trimethyl ammonium bromide (CTAB) in this work. By virtue of the distinctive microstructure, Cu-Ru MPNZ expressed superior bi-functional oxidase- and peroxidase-mimic activity to catalyze the oxidation of 3,3′,5,5,’-tetramethylbenzidine (TMB) and 2,2′-azinobis (3-ethylbenzothiazoline-6- sulfonic acid) ammonium salt (ABTS) with low Michaelis-Menten constants and quick reaction rates. Especially, toxic aminophenol isomers could exclusively react with the oxydates of TMB or ABTS to express differentiable signals in color. Under the optimal conditions, Cu-Ru MPNZ was successfully applied for visual differentiation of toxic aminophenol isomers in real aqueous, juices and medicinal samples with low detection limits (1.60 × 10 −8 mol/L for o -aminophenol and 3.25 × 10 −8 mol/L for m -aminophenol) and satisfactory recoveries (96.6–103.5%). The different recognition mechanisms of Cu-Ru MPNZ to toxic o - and m -aminophenol isomers were proposed for the first time as far as we known. This work will provide a potential way to monitor different organic isomer pollution in future.
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FUEL
·
2021
·
IF 6.609
Ya-Qi Shan,Lin-Xin Yin,Oraléou Sangué Djandja,Zhi-Cong Wang,Pei-Gao Duan
Ru supported on activated carbon (C), Al 2 O 3 , CeO 2 , MgO, TiO 2 , and ZrO 2 were prepared and employed to boost supercritical water gasification (SCWG) of microalgae hydrothermal liquefaction (HTL) downstream water at 600 °C for 1 h. Effects of catalysts, water density, and Ru/C loading on total organic carbon (TOC) reduction, carbon gasification efficiency (CGE), and gas yield were examined. All the Ru catalysts showed a positive effect on TOC reduction and converted organics in the HTL downstream water to fuel gas, with H 2 and CH 4 as the two most abundant component. With the addition of Ru/C, almost complete removal of TOC, the highest CGE, and H 2 yield were achieved due to its largest metal dispersion. With the addition of Ru/C, increasing water density and catalyst loading favored TOC reduction and CGE increase as well as the total gas yield. The highest H 2 content of 50% and yield of 2.62 mmol/g (aq.) were obtained at the highest catalyst loading of 12.0 mg (Ru/C) /mL (aq.) . This study suggested that SCWG with the addition of Ru/C was a promising strategy to produce fuel gas rich in H 2 , from the organics in the microalgae HTL downstream water.
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