APPLIED CATALYSIS A-GENERAL
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2020
·
IF 5.006
Sishi Zhang,Jie Xu,Hongmei Cheng,Cuicui Zang,Bin Sun,Heyan Jiang,Fengxia Bian
Atomic economy, non-toxicity, harmlessness and multidirectional selectivity advocated by green chemistry have increasingly become a hot and difficult research topic. Herein, we present a highly efficient, one-pot tandem and easy-to-operate method through which we could directly produce a broad range of multi-directional selective hydrogenated amines or N-alkyl aliphatic amines using aromatic nitro compounds as raw materials. Ru/LDH with characteristics of layered mesoporous structure, well dispersed small Ru nanoparticles and LDH stabilization to the Ru NPs was employed as the catalyst. It is remarkable that multi-directional superb chemoselectivity to aromatic amines, alicyclic amines as well as N-alkyl aliphatic amines could be achieved with excellent catalytic activity and recyclability by tuning reaction conditions over 5wt%Ru/LDH-2. Additionally, this catalytic system also exhibited attractive activity and multi-directional chemoselectivity in the hydrogenation of quinoline and its derivatives with solvents of different polarity. Chemoselectivity to 5,6,7,8-tetrahydroquinoline derivatives could reach as high as 95.6 %.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2020
·
IF 7.1
Dandan Fang,Huizhu Ren,Yitian Huang,Hong Dai,Defu Huang,Yanyu Lin
Herein, an ultrasensitive electrochemiluminescence (ECL) immunosensor based on a high performance probe of Nb 2 CTx MXene immobilized ZnO quantum dots (QDs) was constructed for Thyroglobulin (Tg) detection. ZnO QDs with good biocompatibility and catalytic property was for the first time utilized as coreaction accelerator in Ru(bpy) 3 2+ /S 2 O 8 2− system and enhanced ECL signal. Specifically, ZnO QDs can facilitate S 2 O 8 2− reduction to generate more SO 4 − , and then reacted with cathodic radical of Ru(bpy) 3 2+ , realizing 2-fold enhancement in ECL intensity. Additionally, Nb 2 CTx MXene possesses excellent properties and was used as prominent supporter, improving the loading capacity of Ru(bpy) 3 2+ and ZnO QDs, and accelerating the electron transfer, resulting in ECL signal enhancement. Furthermore, Nb 2 CTx MXene acted as temperature controller and increased the electrode surface temperature by converting laser energy into heat, further amplified ECL signal. Because of the high sensitivity, good specificity and favorable stability, the proposed immunosensor realized sensitive detection of Thyroglobulin and had a great application prospect in bioanalysis and clinical diagnosis.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2020
·
IF 4.65
Siqi Zhang,Ying Wang,Dan Li,Ziye Kang,Feilong Dong,Haiming Xie,Jia Liu
The synergistic effect between noble metal and spinel-type compounds is beneficial for enhancing the electrochemical performance in a Li–O 2 battery. Herein, Ru-impregnated needle-like NCO embedded in porous carbon textiles (CTs) (x wt% Ru@NCO/CTs (x = 0, 0.5, 1, 2, and 5)) is applied as a flexible and binder-free O 2 electrode for Li–O 2 batteries. The NCO structure can benefit to the Li + migration, O 2 diffusion, and Li 2 O 2 accommodation. The Ru nanoparticles can promote OER and ORR reaction kinetics and lower the overpotential. A flexible Li–O 2 cell with 1 wt% Ru@NCO/CTs exhibits a good cyclic stability of 360 cycles with an overpotential of 0.78 V at a constant current density of 200 mA/g, a considerable rate performance, a high reversibility with the Li 2 O 2 formation and its reverse decomposition, and a good flexibility stability under bending and twisting at the different conditions. This work can contribute to the development of electrode material and its architecture design for portable and wearable devices .
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Nano Energy
·
2019
·
IF 15.548
Shenghua Ye,Feiyan Luo,Tingting Xu,Pingyu Zhang,Hongdong Shi,Shiqi Qin,Jiaping Wu,Chuanxin He,Xiaoping Ouyang,Qianling Zhang,Jianhong Liu,Xueliang Sun
The development of the hydrogen evolution reaction (HER) in alkaline electrolyte is highly desirable but is hindered by sluggish water dissociation and the high cost of Pt–based catalysts. In this study, a facile pyrolyzation method is proposed for synthesizing the Ru nanoclusters (NCs) anchored on B/N–doped graphene (BNG) (denoted as Ru NCs/BNG). During the pyrolyzation, boron was doped into graphene and facilitated the formation of ultra−small Ru NCs with a diameter of 0.5–1 nm. The electronic interaction between B and Ru NCs accelerated the cleavage of H–OH, altering the HER mechanism and lowering the activation energy of H 2 formation, endowing Ru NCs/BNG with excellent alkaline HER activity, even surpassing that of Pt/C. This study reveals the importance of water dissociation barriers for alkaline HER activity and provides a new strategy for improving the HER catalytic activity .
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Russian Journal of Physical Chemistry A
·
2019
·Vol. 93
·期 9
·1754-1761
·
IF 0.581
Yin Hu,Chen Wei,Ba Mingwei,Xie Xin,Song Weiguo
Abstract Ru/TiO 2 nanocomposite was prepared via loading the active ruthenium species on anatase TiO 2 by a simple hydrothermal approach combined with a sol–gel method. The optimal catalyst with 5.0% of Ru species showed excellent catalytic performance in the solvent-free selective hydrogenation of α-pinene with the conversion of α-pinene and selectivity to cis -pinane of 100.0 and 97.1%, respectively. It has been verified that the superior performance depends on the large amounts of acidic sites induced by HF acid and the SMSI effect between the reducible TiO 2 support and Ru species on its surface. The partial loss of its activity after five hydrogenation cycles should be due to the agglomeration of the catalyst particles and the carbon deposition on the surface. The possible hydrogenation mechanism was also discussed. This work provides an effective approach to develop a highly efficient and recyclable catalyst for the solvent-free selective hydrogenation of α-pinene.
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Applied Materials Today
·
2020
·
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.
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Journal of Materials Chemistry B
·
2019
·Vol. 7
·期 40
·6210-6223
·
IF 5.047
Yanan Liu,Yayu Wen,Xu Chen,Xufeng Zhu,Qianqian Yu,Youcong Gong,Guanglong Yuan,Jie Liu,Xiuying Qin
Due to the complexity and heterogeneity of solid tumors, traditional clinical treatments often only achieve limited therapeutic effects. Tumor-associated macrophages (TAMs) play a key role in the development of solid tumors, and the elimination of solid tumors based on the tumor microenvironment has proven to be an effective therapeutic strategy. Here, we successfully developed Ru-based nanoparticles, Ru@ICG–BLZ NPs, with inflammation-responsive release ability, which could repolarize TAMs into M1 macrophages (with an antitumor role) and further produce hyperthermia and ROS to eliminate cancer cells. In vitro experiments showed that Ru@ICG–BLZ NPs had superior drug (ICG and BLZ-945) loading capacity and sensitive inflammation-responsive drug release behavior, which enhanced CT26 cell uptake and penetration ability. Furthermore, in vivo experiments showed that Ru@ICG–BLZ NPs could effectively up-regulate the expression of M1 markers (iNOS, and IL-12) and exert phototherapy to ablate solid tumor, without causing obvious damage to the surrounding tissues of the tumor. The lower toxicity and excellent antitumor ability of Ru@ICG–BLZ NPs could provide new ideas for the clinical transformation of nanomedicine.
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PubMed
高影响因子
FOOD CHEMISTRY
·
2019
·
IF 5.399
Lijun Luo,Shuai Ma,Libo Li,Xiaohong Liu,Jiayi Zhang,Xia Li,Dong Liu,Tianyan You
Accurate and early diagnosis of mycotoxin is particularly significant to the food and agricultural product safety. In the present work, a sensitive and effective monitoring method for zearalenone (ZEN) was exploited based on a novel self-enhanced electrochemiluminescence (ECL) aptasensor. The self-enhanced lumonophore was compounded by electrostatically combining amine-functionalized Ru(bpy) 3 2+ -doped silica nanoparticles (NH 2 [email protected] 2 NPs) and nitrogen doped graphene quantum dots (NGQDs) together. Since the emitter and co-reactant simultaneously existed in the same nanoparticle, shortened electron-transfer distance and decreased energy loss was obtained. Therefore, self-enhanced ECL aptasensor based on the novel complex expressed the widest linear range of 10 fg mL −1 –10 ng mL −1 and the lowest detection limit of 1 fg mL −1 for ZEN detection. More importantly, ZEN produced during the mildew process of corn flour was monitored by the developed aptasensor, which exhibited superior determination and potential application in real samples.
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PubMed
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SENSORS AND ACTUATORS B-CHEMICAL
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2019
·
IF 6.393
Li Tian,Xuerong Wang,Kexin Wu,Yue Hu,Yue Wang,Juan Lu
A ultrasensitive electrochemiluminescence (ECL) biosensor was designed for the detection of dopamine using ZnSe quantum dots and Ru(bpy) 3 2+ as the signal probes, and graphite oxide and multi-walled carbon nanotube as the supporting matrix. The biosensor exhibits efficient and stable anodic ECL signal (at 1.10 V vs. Ag/AgCl) in phosphate buffer solution (pH 9.0) containing Tripropyl amine. The ECL emission decreases with adding dopamine, which can be attributed to the quenching effect from interaction between ZnSe and dopamine. The possible reaction mechanism of the ECL system is studied, and a method for the determination of dopamine is proposed. Under the optimal experimental conditions, the ECL emission decreases linearly with the logarithm of dopamine concentration in a wide linear range from1 × 10 −9 to 1 × 10 -5 mol L −1 with a detection limit of 6 × 10 -10 mol L -1 (S/N = 3). The biosensor is also successfully applied to detect dopamine in human blood serum samples.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2019
·
IF 14.229
Xiaoqing Gao,Shanhui Zhu,Mei Dong,Jianguo Wang,Weibin Fan
Highly efficient synthesis of valuable γ-valerolactone (GVL) by levulinic acid (LA) hydrogenation is still a challenge for Ru-based catalysts under mild condition. In this work, we have reported that ultrathin TiO 2 nanosheets supported Ru nanoparticles showed extraordinarily high catalytic activity, GVL yield (99.1%) and reusability owing to the formation of Ru O Ti interfacial structure. The turnover frequency (TOF) reached as high as 19,045 h −1 at 100 °C, much higher than those of Ru/SiO 2 , Ru/GO, Ru/MoS 2 , and commercial Ru/C. DFT calculation elucidates that the dominant reaction pathway of LA hydrogenation to GVL is preferentially hydrogenated to CH 3 CHOCH 2 CH 2 COOH*, followed by cyclization to CH 3 (OH)C 4 OH 4 OH* (GVL − OH) and final dehydroxylation, irrespective of surface structure. Compared to Ru (0 0 2) facet, Ru/TiO 2 interfacial structure changes the rate-determining step from initial hydrogenation to cyclization, which greatly declines the activation barrier from 0.81 eV to 0.48 eV.
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APPLIED SURFACE SCIENCE
·
2018
·
IF 4.439
Fengyi Zhong,Qi Wang,Caili Xu,Yingchun Yang,Yi Wang,Yun Zhang,Daojiang Gao,Jian Bi,Guangyin Fan
Ultrafine monodisperse Ru nanoparticles were synthesized by a facile strategy with nitrogen-doped porous hierarchically porous carbon material (HPCM) as support. The as-synthesized Ru nanoparticles with an average particle size of 1.41 nm were dispersed uniformly on the HPCM surface (Ru/HPCM). The Ru/HPCM catalyst exhibited a high turnover frequency of 440 min −1 and could be reused for eight times in hydrogen generation from ammonia borane hydrolysis. The enhanced catalytic activity of Ru/HPCM could be attributed to the numerous active surface areas provided by ultrafine monodisperse Ru nanoparticles for the reaction. The confinement space of the support and the abundant surface functional groups increased the stability and reusability of the Ru/HPCM catalyst. This facile strategy for synthesis of ultrafine monodisperse metal nanoparticles with high catalytic activity and reusability shows potential for practical applications.
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Catalysis Science & Technology
·
2014
·Vol. 4
·期 5
·1286-1292
·
IF 4.76
Bing Liu,Ting Huang,Zehui Zhang,Zheng Wang,Yuhua Zhang,Jinlin Li
The present study reported the results on the water–gas shift (WGS) reaction over a series of Ru/C catalysts. It was found that the reduction method showed a remarkable effect on the catalytic activity of Ru/C catalysts over WGS reaction, which increased in an order of the reduction by NaBH4, ethylene glycol, H2. It has been shown that alkali additives with K2CO3 significantly improved the activity of the Ru/C catalysts. XPS results indicated that Ru species were further oxidized by the addition of K2CO3, which indicated an electron transfer from the alkali metal to the substrate, resulting in stronger bonding of the adsorbed gas. FTIR results showed that the absorption peak intensity of H2O and hydroxyl group increased with the increase of K2CO3 content, due to the strong hygroscopic ability of K2CO3. Through the addition of K2CO3 to the Ru/C catalyst, much more water was adsorbed around the catalytic active sites, reducing the strong adsorption of CO on the active sites. Thus the addition of K2CO3 balanced the concentration of water and CO on the active sites, which was considered to be the key step for low temperature WGS reaction over Ru supported on irreducible activated carbon.
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