ChemElectroChem
·
2020
·Vol. 7
·期 20
·4239-4244
·
IF 4.154
Fan Yuan,Mohamed Ibrahim Halawa,Xiangui Ma,Abubakar Abdussalam,Baohua Lou,Guobao Xu
Graphical Shine and detect : Oxamic hydrazide (OHA) can dramatically increase the electrochemiluminescence (ECL) intensity of Ru(bpy) 3 2+ on glassy carbon electrode (GCE). 4-Nitrobenzaldehyde (4-NBA) can react with OHA to form a hydrazone product through nucleophilic addition, inducing a significant quenching on the ECL intensity of the developed Ru(bpy) 3 2+ /OHA system. Based on this, a sensing platform of 4-NBA was constructed. Oxamic hydrazide (OHA) was utilized as an efficient coreactant of Ru(bpy) 3 2+ for the first time, which can dramatically increase the electrochemiluminescence (ECL) intensity of Ru(bpy) 3 2+ on glassy carbon electrode (GCE). 4-nitrobenzaldehyde (4-NBA), a nitroaromatic compound, has mutagenic and carcinogenic toxicity on humans′ genome and causes a serious impact on the environment. Hence, the detection of its level in biological and environmental samples is of great significance. Interestingly, 4-NBA was found to induce a dramatic quenching for the ECL intensity of the developed Ru(bpy) 3 2+ /OHA system owing to the formation of hydrazone product through the nucleophilic addition reaction with OHA. Under optimal conditions, the ECL decreasing value of Ru(bpy) 3 2+ /OHA in the presence of 4-NBA is linear in the range of 20 μM to 800 μM with a limit of detection (LOD) of 1.09 μM (signal-to-noise 3 : 1). Finally, this strategy enabled the detection of 4-NBA in tap water with satisfactory recoveries from 97.84 % to 103.56 %.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2020
·
IF 7.1
Pei Zhang,Yao Zhang,Xin Xiong,Yao Lu,Nengqin Jia
A sensitive electrochemiluminescence (ECL) immunosensor was successfully fabricated utilizing Ru(bpy) 3 2+ -doped mesoporous polydopamine (MPDA) for subtle exploration of the diabetes biomarker glycosylated hemoglobin (HbA1c). In this protocol, with the advantages of relatively large specific surface area and good biocompatibility, MPDA nanoparticles are capable of loading more Ru(bpy) 3 2+ to greatly amplify the ECL efficiency during the existence of trinpropylamine (TPA) as common coreactant. The acquired Ru(bpy) 3 2+ @MPDA nanoparticles are used as a beneficial substrate for immobilizing aptamer, thereby specifically recognizing the targeting substance HbA1c as much as possible with high selectivity. It could be noted from the experimental results that the ECL intensity was evidently reduced as the proposed Ru(bpy) 3 2+ @MPDA ECL immunosensor captured HbA1c, which showed the principle of the ECL quenching determination. Under optimal experimental conditions, the prepared Ru(bpy) 3 2+ @MPDA ECL immunosensor exhibited wide linear range from 0.1% to 18.5% with the low detection limit (LOD) of 0.015% (S/N = 3) and the correlation coefficient (R 2 ) of 0.994. Moreover, the Ru(bpy) 3 2+ @MPDA immunosensor displayed high sensitivity and selectivity for detecting HbA1c. Therefore, the as-obtained Ru(bpy) 3 2+ @MPDA ECL immunosensor will open up a new promising platform for highly sensitive bioassay of HbA1c.
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EUROPEAN JOURNAL OF MEDICINAL CHEMISTRY
·
2020
·
IF 5.573
Jincan Chen,Jie Wang,Yuanyuan Deng,Baojun Li,Chengpeng Li,Yuxue Lin,Dongbin Yang,Huanyun Zhang,Lanmei Chen,Tao Wang
Two novel cyclometalated Ru(II) complexes containing isoquinoline ligand, [Ru(bpy) 2 (1-Ph-IQ)](PF 6 ), (bpy = 2,2′-bipyridine; 1-Ph-IQ = 1-phenylisoquinoline; RuIQ-1 ) and [Ru(phen) 2 (1-Ph-IQ)](PF 6 ) (phen = 1,10-phenanthroline; RuIQ-2 ) were found to show high cytotoxic activity against NCI–H460, A549, HeLa and MCF-7 cell lines. Notably, both of them exhibited IC 50 values that were an order of magnitude lower than those of clinical cisplatin and two structurally similar Ru(II)-isoquinoline complexes [Ru(bpy) 2 (1-Py-IQ)](PF 6 ) 2 ( Ru3 ) and [Ru(phen) 2 (1-Py-IQ)](PF 6 ) 2 ( Ru4 ) (1-Py-IQ = 1-pyridine-2-yl). The cellular uptake and intracellular localization displayed that the two cyclometalated Ru(II) complexes entered NCI–H460 cancer cells dominantly via endocytosis pathway, and preferentially distributed in the nucleus. Further investigations on the apoptosis-inducing mechanisms of RuIQ-1 and RuIQ-2 revealed that the two complexes could cause S, G2/M double-cycle arrest by regulating cell cycle related proteins. The two complexes also could reduce the mitochondrial membrane potential (MMP), promote the generation of intracellular ROS and trigger DNA damage, and then lead to apoptosis-mediated cell death . More importantly, RuIQ-2 exhibits low toxicity both towards normal HBE cells in vitro and zebrafish embryos in vivo . Accordingly, the developed complexes hold great potential to be developed as novel therapeutics for effective and low-toxic cancer treatment.
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PubMed
高影响因子
JOURNAL OF NANOPARTICLE RESEARCH
·
2020
·Vol. 22
·期 5
·1-13
·
IF 2.132
Maimaiti Halidan,Wang Shixin,Awati Abuduheiremu,Xu Bo
Graphene oxide/silica (GO/SiO 2 ) containing various inorganic particles is obtained by using the Xinjiang Wucaiwan coal as carbon source and silicon source. The ruthenium/graphene oxide/silica (Ru/GO/SiO 2 ) composite was prepared by loading Ru nanoparticles on the surface of GO/SiO 2 . Then, the photocatalytic ammonia synthesis performance was investigated while characterizing the structure of Ru/GO/SiO 2 . On the one hand, the Ru can be sufficiently dispersed to make the surface plasmon resonance (SPR) effect enhance significantly. On the other hand, the quantum confinement effect of the defect structure on the Ru/GO/SiO 2 can effectively separate electron and hole, and it can participate in the reducing/oxidizing reaction of photocatalytic ammonia synthesis.
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KOREAN JOURNAL OF CHEMICAL ENGINEERING
·
2020
·Vol. 37
·期 2
·224-230
·
IF 2.69
Si Zhihao,Zhang Xin,Zuo Miao,Wang Tao,Sun Yong,Tang Xing,Zeng Xianhai,Lin Lu
2, 5-furandicarboxylic acid (FDCA) is a one of the most promising biomass-derived chemicals to substitute the non-renewable terephthalic acid as the monomer for producing polyethyleneterephthalate. At present, the oxidation of HMF is regarded as a prevalent way to prepare FDCA. Nevertheless, the isolation and storage of HMF is still a challenge. Herein, based on the higher stability of 5-formyloxymethylfurfural (FMF) than 5-hydroxymethylfurfural (HMF), we present an effective preparation route to prepare FDCA by substituting HMF with FMF as feedstock. A complete conversion of FMF and a 93.55% selectivity of FDCA were obtained in the mixed solvent of water and 1, 2-dioxane using Ru/C as catalyst and O 2 as oxidant. An improved process was developed for preparing FDCA using FMF as feedstock. The investigation of conversion pathway showed that FMF and HMF were simultaneously oxidized to 2, 5-diformylfuran (DFF) in a case of the existence of the reversible equilibrium between FMF and HMF. Then DFF was oxidized to 5-formyl-2-furancarboxylic acid (FFCA). Subsequently, FFCA was oxidized to FDCA. In this process, the oxidation of FFCA to FDCA was determined as the rate-determining step. Furthermore, appropriate alkalinity favored the selectivity of FDCA and the conversion of FMF.
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RSC Advances
·
2020
·Vol. 10
·期 28
·16515-16525
·
IF 3.119
Junya Cao,Fenggang Han,Liguo Wang,Xiaoyu Huang,Yan Cao,Peng He,Huanhuan Yang,Jiaqiang Chen,Huiquan Li
A series of Ru/g-C3N4 materials with highly dispersed Ru were firstly prepared by an ultrasonic impregnation method using carbon nitride as a support. The catalysts were characterized by various techniques including BET and elemental analysis, ICP-AES, XPS, XRD, CO2-TPD and TEM. The results demonstrated that Ru/g-C3N4 materials with a mesoporous structure and highly dispersed Ru were successfully prepared. The chemo-selective hydrogenation of p-phenylenediamine (PPDA) to 1,4-cyclohexanediamine (CHDA) over Ru/g-C3N4 as a model reaction was investigated in detail. PPDA conversion of 100% with a CHDA selectivity of more than 86% could be achieved under mild conditions. It can be inferred that the carbon nitride support possessed abundant basic sites and the Ru/g-C3N4-T catalysts provided suitable basicity for the aromatic ring hydrogenation. Compared to the N-free Ru/C catalyst, the involvement of nitrogen species in Ru/g-C3N4 remarkably improved the catalytic performance. In addition, the recyclability of the catalyst demonstrated that the aggregation of Ru nanoparticles was responsible for the decrease of the catalytic activity. Furthermore, this strategy also could be expanded to the selective hydrogenation of other aromatic diamines to alicyclic diamines.
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PubMed
高影响因子
Biomass Conversion and Biorefinery
·
2021
·Vol. 13
·期 12
·10701-10710
·
IF 4.987
Zeng Qin,Du Zhenyu,Luo Ligang
In this study, different bimetallic (Ru, Pd, and Pt) catalysts over a variety of supports (activity carbon, γ-Al 2 O 3 , TiO 2 , HZSM-5) were employed to improve the kraft lignin depolymerization process using isopropanol as in situ hydrogen source. The effect of catalysts was firstly investigated, which suggested that 1wt%Ru-1wt% Pd/HZSM-5 promoted the hydrogenolysis and hydrodeoxygenation effect on conversion of kraft lignin (95.86 wt%) and the selectivity of aliphatic alcohol (26.92 wt%) and hydrocarbon monomers (35.73 wt%), respectively. The effect of temperature and reaction time were also discussed, which indicated that the high temperature (250 to 310 °C) promoted the hydrogenolysis process; while the temperature is higher than 310 °C, the repolymerization process was appeared, leading to the decreasing yield of total monomers. For the influence of reaction time, it was noted that the optimal reaction time to acquired high yield and selectivity of aliphatic alcohol and hydrocarbon monomer was 120 min. It was also conducted FTIR and 2D HSQC NMR analysis to understand the effective depolymerization of the major linkages with attacked by the Ru-Pd/HZSM-5 catalyst, which was corresponding with the results with GC–MS. Graphical abstract
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JOURNAL OF THE ENERGY INSTITUTE
·
2021
·
IF 6.186
Riyang Shu,Zhuojie Zhong,Hongyun You,Zhipeng Tian,Ying Chen,Longlong Ma
Hydrodeoxygenation (HDO) is an important pathway for lignin-oil upgradation to produce high quality liquid fuels, in which the high-active catalyst is the key point to achieve a high HDO efficiency. In this study, Ru/TiO 2 , Ru/CeO 2 and Ru/TiO 2 –CeO 2 catalysts were synthesized by a novel photochemical method with a high Ru dispersion and used for the HDO of lignin-derived phenolic compounds. Among these three catalysts, Ru/TiO 2 –CeO 2 showed a better performance than Ru/TiO 2 and Ru/CeO 2 . And guaiacol was transformed into cyclohexane with conversion and product selectivity close to 100 % at 230 °C under 1 MPa hydrogen atmosphere. Ru/TiO 2 –CeO 2 took the advantages of Ru/TiO 2 and Ru/CeO 2 , namely high Ru metal dispersion, plenty of medium strength acid sites and abundance of oxygen vacancy , which promoted the guaiacol adsorption and the HDO catalytic activity . Moreover, Ru/TiO 2 –CeO 2 catalyst showed an effective upgrading of other lignin-derived phenolic compounds. And the lignin-oil also enabled to be upgraded efficiently, producing a high content of hydrocarbons and alkylphenols.
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高影响因子
FUEL
·
2021
·
IF 6.609
Zier Jin,Hong Xia,Wenxin Yang,Mingen Liu,Xiaoyu Liu,Jiao Xiang,Abdul Qayum,Liangsheng Hu,Lianfeng Duan,Wenhua Gao,Zhi Liu,Fushen Lu
Ammonia borane (NH 3 BH 3 , AB) has been considered as one of the most attractive candidates for chemical hydrogen-storage materials. Development of low-cost and high-performance catalysts for hydrogen generation from AB is highly desirable, which is still a huge challenge. Herein, Ru-Ni bimetallic nanoparticles were fabricated on (3-aminopropyl) triethoxysilane-functionalized reduced graphene oxide nanosheet (APTS-rGO) by a facile one-step in situ co-reduction strategy. The newly developed Ru 1 Ni 4 /APTS-rGO catalyst with hydrophilic interface and narrow particle size-distribution presented a remarkably enhanced catalytic activity for hydrolytic H 2 generation from AB, affording an ultra-high TOF value of 1559 min −1 . The APTS-rGO support was effective to minimize the aggregation of Ru-Ni nanoparticles, achieving the immobilization of ultrasmall Ru-Ni nanoparticles (2.0 nm) on support surface. The change in local charge density of catalyst surface caused by Ru-Ni synergistic effect and metals-support interaction improved the catalytic performance of Ru 1 Ni 4 /APTS-rGO. Hydrophilic NH 2 -containing interface ensured high dispersibility of catalysts in reaction solution, increasing the contact opportunities between active sites and AB molecules. These factors contributed together to the exceptional catalytic performance of Ru 1 Ni 4 /APTS-rGO. This catalytic system has potential applications in various catalytic fields due to its obvious advantages of the facile preparation method, good hydrophilicity, and the outstanding catalytic performance.
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GREEN CHEMISTRY
·
2020
·Vol. 22
·期 3
·850-859
·
IF 9.48
Yang Qian,Ze-Jun Li,Xian-Long Du,Qi Zhang,Yi Zhao,Yong-Mei Liu,Yong Cao
Development of a highly efficient and robust catalyst with reduced usage of noble metals is extremely desirable for selective hydrogenations of furan-containing bio-based feedstocks, which represents an attractive and sustainable alternative to petrochemical resources. Herein, we describe a new type of well-dispersed Ru subnanoclusters (ca. 0.50 wt%) supported on commercial P25 TiO2 material obtained from a facile and effective amino acid-assisted deposition–precipitation strategy. The as-synthesized catalyst exhibits superior catalytic activity and selectivity for direct hydrogenation of industrially important furfural as well as a range of structurally diverse bio-based furanic compounds to their corresponding fully hydrogenated derivatives. An average turnover frequency (ATOF) value as high as 367 h−1 at 80 °C and 4 MPa H2 is obtained, which is the highest reported value. This catalyst also shows stable furfural total hydrogenation in 5 reaction cycles conducted at 80 °C (52 mmol-scale, turnover number up to 12 500). In terms of the kinetic and structural characterizations, the key performances of the ultrasmall Ru clusters are proposed to mainly originate from an enhanced number of unsaturated surface Ru atoms and change in local coordination environment. Our work highlights the importance of the subnanometric size of Ru clusters in the advancement of efficient and affordable approaches towards bio-based chemical production.
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Journal of Materials Chemistry A
·
2019
·Vol. 7
·期 6
·2780-2786
·
IF 10.733
Zhen Zhang,Ping Li,Qi Wang,Qi Feng,Youkun Tao,Jiaoyan Xu,Cheng Jiang,Xiner Lu,Jiantao Fan,Meng Gu,Hui Li,Haijiang Wang
As a cheaper Pt-group metal, ruthenium (Ru) is a highly competitive alternative to Pt for commercialization towards the hydrogen evolution reaction (HER). Herein, we report the modulation effect on the Gibbs free energy (ΔGH*) of hexagonal-close-packed (hcp) Ru resulting from heteroatom Mo doping. In particular, for the first time the hcp MoRu3 crystal structure is theoretically predicted with pretty high intrinsic HER activity. Meanwhile, the Mo hetero-dopant could act as a new active site with Pt-like ΔGH*. Motivated by the prediction, we report a novel metal organic framework (MOF)-assisted synthetic strategy to prepare a Mo-doped hcp Ru electrocatalyst. Accordingly, the hcp MoRu3 catalyst exhibits an ultralow overpotential of 30.5 mV at 10 mA cm−2, ensuring excellent Pt-like intrinsic HER activity. More importantly, the excellent electrochemical performance measured with a proton exchange membrane (PEM) electrolyzer further highlights the promising potential of the hcp MoRu3 catalyst for hydrogen production.
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高影响因子
GREEN CHEMISTRY
·
2019
·Vol. 21
·期 10
·2739-2751
·
IF 9.405
Naseeb Ullah,Atheer Hameid Odda,Kuang Liang,Miza Ali Kombo,Shafaq Sahar,Liu-Bo Ma,Xiao-Xiang Fang,An-Wu Xu
The catalytic fractionation of lignin in a native lignocellulose matrix is crucial to the comprehensive achievement of sustainable and green chemicals. Herein, we prepared a novel metal–acid bifunctional nanocomposite of finely scattered metallic Ru nanoclusters (NCs) sustained on porous hafnium phosphate nanoplates (α-HfP NPs) to effectively depolymerise lignocellulosic biomass. A native lignin fraction of pine lignocellulose was promptly depolymerised into 19.86 wt% yield (lignin based) of valuable phenolic monomers (with dihydroeugenol as the main compound with high selectivity) and few cyclic ketones through one-pot catalytic reductive fractionation under mild conditions (190 °C, 3.5 MPa H2). Detailed scanning and transmission electron microscopy, X-ray photoelectron spectroscopy, and temperature-programmed desorption ammonia investigation correlated with the obtained results revealed that the metal–acid synergistic influence and the presence of Brønsted acid sites in the support for dehydration and the well-dispersed metallic role of Ru NCs for hydrodeoxygenation were responsible for the cleavage of lignin–carbohydrate (ester and ether linkages) bonds. Moreover, treating commercial lignin as a substrate in an organic solvent generated 4-hydroxy-3-methoxybenzaldehyde (vanillin) in high yield, as well as other functionalised phenolic monomers up to 85% selectivity, illustrating the high susceptibility of Ru/α-HfP NPs towards C–O bond cleavage through reductive fractionation. Multiple recycling tests of the catalyst were performed without any apparent loss of activity. Overall, this report highlighted the potential of the synthesis strategy of the metal–acid supported catalyst to immediately depolymerise untreated biomass and can thus encourage the green, cost-efficient, large-scale production of intermediate chemicals.
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