CATALYSIS COMMUNICATIONS
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2023
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IF 3.7
Shengzhe Wang,Hongxia Lv,Chengyu Jin,Yu Wang,Huangzhao Wei,Chenglin Sun,Lian Yu,Lei Ma,Xiangnan Li,Xiaowei Liu
We synthesized a series of Ru-Ti-Ni/CNT electrodes to degrade levofloxacin in wastewater. The unique structure of Ni single-atom-kernelled Ru nanoparticles regulates the reaction process, producing a notable synergistic effect. The reaction kinetics constant of Ru-Ti-Ni/CNT with a Ru: Ti ratio of 10:0 outperforms Ni/CNT by 3.7 times and CNT alone by 16.4 times. Comprehensive characterizations revealed its morphology and structure nature. Ru nanoparticles can shield Ni, while Ni single-atom facilitates electron transfer in Ru nanoparticles, generating abundant reactive oxygen radicals (ROS) that degrade pollutants.
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CATALYSIS COMMUNICATIONS
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2023
·
IF 3.7
Zhao Yang,Yan Xiong,Ting Li,Zhiqing Yang,Bing Hui Chen
Carbon supported Ru-Sn bimetallic catalyst shows excellent performance in room-temperature hydrogenation of acetone, 100% acetone conversion with 100% product selectivity to isopropyl alcohol can be achieved within a short reaction time. Catalyst structure-function relationship reveals a synergetic behavior between Ru and Sn sites, demonstrating the essential correlation between Sn/Ru atomic ratio and the resultant variation in catalytic performance. Room temperature hydrogenation of 4-heptanone was also studied, verifying the consistency of the established structure-function relationship in ketones hydrogenation reactions.
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Nanoscale
·
2023
·Vol. 15
·期 28
·12064-12070
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IF 6.7
Hai Liu,Zhuang Zhang,Mengxuan Li,Yaping Li,Yun Kuang,Xiaoming Sun
Developing highly efficient hydrogen oxidation reaction (HOR) electrocatalysts in alkaline media is of great significance for anion exchange membrane fuel cells (AEMFCs). Herein, we report an efficient Ru-doped hexagonal tungsten trioxide (Ru-WO3) HOR electrocatalyst through a hydrothermal strategy. The prepared Ru-WO3 electrocatalyst exhibits enhanced HOR performance with a 6.1 times higher exchange current density and better durability than commercial Pt/C. Structural characterizations and theoretical calculations reveal that the uniformly distributed Ru was modulated by oxygen defects and the electron transfer from O to Ru modulated the H* adsorption of Ru sites. In addition, plenty of W sites can serve as hydroxyl adsorption sites to accelerate the HOR kinetics. This work not only provides an efficient HOR catalyst in alkaline media, but also promotes the fundamental understanding of the effect of modulation on the adsorption of H* and *OH in tungsten oxides with a relatively low oxidation state by Ru doping, broadening the range of HOR catalysts to Ru-doped metal oxides.
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Materials Chemistry Frontiers
·
2023
·Vol. 7
·期 11
·2266-2276
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IF 7
Qizhi Hu,Hongzhong Xu,Yue Wu,Shi Jiang,Jun Wang,Yu Zhou
The development of an efficient heterogeneous system for the selective synthesis of primary amines via reductive amination of carbonyl compounds has long been an important goal of chemical research. Here, we show that ionic polyamide stabilized Ru nanoparticles act as a broadly effective reductive amination catalyst, showing a high yield, large turnover frequency, stable recycling performance, and extendable substrate compatibility to a diverse set of alkane and aromatic primary amines. The ionic polyamide support provided a strong affinity towards the Ru species, enabling facile adjusting of the surface chemical state and dispersion. Metallic Ru0 species with high dispersion were achieved with a moderate loading amount, allowing a suitable hydrogenation ability that accelerated the rate-determining step in the reductive amination of a carboxyl compound, the ammonolysis of a Schiff base intermediate, and avoided side reactions such as direct hydrogenation to generate alcohols. The ionic moieties were found to be crucial for the stabilization of the Ru species that account for the stable recyclability.
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JOURNAL OF POWER SOURCES
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2018
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IF 6.945
Shidong Song,Limei Yu,Yanli Ruan,Jian Sun,Butian Chen,Wu Xu,Ji-Guang Zhang
Irreversible parasitic reactions and the resulting accumulation of insulating side products are main barriers for practical application of rechargeable lithium–oxygen (Li O 2 ) batteries . Therefore, it is critical to develop multifunctional oxygen electrodes suitable for oxygen reduction reaction , oxygen evolution reaction , and decomposition of side reaction products. Here we report the application of ultrafine ruthenium on boron carbide (Ru/B 4 C) with highly efficient multifunctional activities as carbon-free oxygen electrodes for Li O 2 batteries. Li 2 CO 3 and LiOH can be completely decomposed by Ru/B 4 C at 4.0 V and 4.1 V, respectively, within the stability window of the electrolyte. A Li O 2 battery using the Ru/B 4 C oxygen electrode achieves low overpotentials for Li O 2 reactions, and excellent cycling performance under the capacities of 300 and 500 mAh g −1 Ru/B4C . In-situ gas chromatography analysis reveals that O 2 is the major gas product during charging. Only a negligible amount of CO 2 is observed in the first charging process. Therefore, Ru/B 4 C can be a very promising oxygen-electrode material for Li O 2 batteries and Li–air batteries operated in ambient air.
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SENSORS AND ACTUATORS B-CHEMICAL
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2018
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IF 5.667
Yan Li,Zhongqiu Hua,Yi Wu,Yan Zeng,Zhilei Qiu,Xuemin Tian,Mengjun Wang,Erping Li
In this paper, WO 3 nanoparticles in a lamellar-structured were fabricated via an acidification method and the surface of nanoparticles were catalytically modified by Ru through a modified impregnation method based on an electronic adsorption mechanism. Gas sensors based on neat and Ru-loaded WO 3 nanoparticles were fabricated based on screen printing and sensor responses of acetone were evaluated under a dry and humid ambient, respectively. Experimental results clearly indicated that most of Ru was removed from the WO 3 during the washing process, however, a strong sensitization effect of Ru was achieved with a very few loading amount. Accordingly, the basic sensitization mechanism of Ru was investigated based on TPR results and oxygen adsorption behaviors. It is revealed that Ru is loaded on the surface with an oxidized state contributing to an electronic sensitization effect. In addition, Ru on the surface of WO 3 as a catalyst significantly enhanced the activity of surface lattice oxygens. As a consequence, surface lattice oxygens could also react with acetone and reduce sensor resistance leading to a sensitization effect. However, we do not expect that reactions of lattice oxygens dominate the sensing process.
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Journal of the American Chemical Society
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2022
·
IF 16.383
Xiaodong Yang,Bo Ouyang,Peiqi Shen,Yiqiang Sun,Yisong Yang,Yanan Gao,Erjun Kan,Cuncheng Li,Kun Xu,Yi Xie
Developing efficient hydrogen oxidation reaction (HOR) electrocatalysts in alkaline media is of great significance for anion exchange membrane fuel cells. Herein, we report the synthesis of hollow colloidosomes composed of Ru nanocrystals based on a novel gas/liquid interface self-assembly strategy. Structural characterizations reveal that much defects are present in the building block (Ru nanocrystals) of Ru colloidosomes. Theoretical calculations suggest that the defects in the Ru structure can optimize the adsorption binding energy of reaction intermediates for the HOR. Benefiting from the assembled colloidosome and optimized electronic structure, the Ru colloidosomes exhibit remarkable HOR catalytic performance in alkaline media with a mass activity higher than that of benchmark Pt/C. Our work may shed new light on the rational design of advanced electrocatalysts with an assembled structure for energy-related applications.
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JOURNAL OF CATALYSIS
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2021
·
IF 7.92
Wenfeng Han,Bing Liu,Yanjun Chen,Zhongsheng Jia,Xiaoli Wei,Weiyu Song
The design and synthesis of highly dispersed metal catalyst have attracted increasing attention, and it is still challenging to generate stable metal clusters with high metal loadings. Support plays a crucial role in determining particle morphology and dispersion. Herein, we demonstrate a strategy for synthesizing an amorphous alumina with 62% Al 3+ penta sites (penta-coordinated Al 3+ ) via solution combustion synthesis. It provides sufficient oxygen defects to anchor Ru species. For benzene hydrogenation reaction, the catalyst displays the high TOF (18833 h −1 ), which is about 2 times higher than that of catalysts supported on commercial alumina. The DFT calculations also confirm that the high catalytic performance is closely correlated with the special configuration of Ru active sites over coordinatively unsaturated alumina. The penta-coordinated Al 3+ was also applied to prepare Pd catalyst with high dispersion. This work provides a superior support which possesses abundant Al 3+ penta sites and affords a possibility for the generation of high and stable dispersion for the preparation of supported metal catalysts.
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ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Caihong Fang,Xiaomin Jiang,Jinwu Hu,Jiaojiao Song,Na Sun,Deliang Zhang,Long Kuai
Ruthenium nanocrystals with small size and special morphology are of great interest in various catalytic reactions due to their high activities. However, it is still a great challenge to downsize these nanocatalysts to a sub-nano scale (<2 nm). Herein, we reported a synthesis of ultrasmall size and uniform Ru nanoparticles through a rapid one-pot method. The prepared Ru nanocrystal shows a wormlike shape, in which the diameter is as thin as 1.6 ± 0.3 nm and the length is 13.6 ± 4.4 nm. These Ru nanoworms (NWs) are quite steady during the synthetic process even though the reaction time was further prolonged. We also examined their catalytic activity toward CO oxidation by loading Ru NWs on TiO2 to form Ru NWs/TiO2 catalysts. These catalysts exhibit a high activity of 100% CO conversion at 150 °C, which is much lower than the normal Ru NPs/TiO2 nanostructures. Based on our detailed investigations, we proposed that the small size, special morphology, and TiO2 support are the keys for their significantly improved catalytic activity. We believed that these reasonable discoveries provide a methodology and opportunity to get highly active catalysts for CO oxidation by a detailed increase in their active sites.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
·
IF 24.319
Jing Wang,Bingxin Guo,Junting Sun,Yingshuang Zhou,Chengfei Zhao,Zhongzhe Wei,Junjie Guo
The design and construction of electrocatalysts with multiple components to modulate the intrinsic catalytic activity is a compelling strategy to achieve Pt-like activity for hydrogen generation. Challenging on the inert Cu-based electrocatalysts for water reduction, herein, a novel and fruitful CuRu-based electrocatalysts (RuCuO x /NC) is established by combining dual-templates assembling and pyrolysis protocol with a subsequent hot-alkali corrosion. Benefitting from the synergetic effect of Cu 2+1 O (with copper excess defects) and Ru, the as-prepared RuCuO x /NC affords brilliant activity and stability under alkaline condition. In 1 M KOH, the RuCuO x /NC provides Pt-like activity with overpotential of ∼29 mV to reach 10 mA cm −2 . Theoretical calculations certified that H 2 O dissociation was accelerated and hydrogen adsorption free energy was optimized by the cooperation of Cu 2+1 O and Ru. This work proposes a promising methodology to construct multi-components electrocatalysts, which may lend perspective for the design of advanced electrocatalysts for renewable energy systems.
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Nanoscale
·
2022
·Vol. 14
·期 20
·7596-7606
·
IF 8.307
Yiming Jiang,Jiawei Zhu,Li Li,Yahui Gao,Juncai Leng,Jiai Yan,Shuoming Liu,Feng Zhang,Han Liu,Chenlu Zhu,Lichun Guo,Haijiao Xie,Wei Zhao
Although the application of nanoscale artificial enzymes in various industries is an attractive way to circumvent the intrinsic drawbacks of natural enzymes, their catalytic constant (Kcat) as a critical reaction parameter is far from satisfactory. Presented here is the rational design and fabrication of a unique peroxidase mimic catalyst based upon Pd@PtxRu4−x (1 ≤ x ≤ 3) prepared by coating PtRu alloy as conformal, ultrathin shells on Pd nanocrystals. Benefiting from an optimal Pt/Ru ratio and well-defined {100} facets, together with confining the Pt–Ru alloy to a shell of averagely 3.3-atomic-layer thick (i.e. Pd@Pt–Ru3.3L), the nanocrystals exhibit the highest catalytic activity and kinetics (1.2 × 106 s−1), resulting in a significant increase of catalytic activity compared with the classical PtRu nanozyme (3.6 × 103 s−1) and horseradish peroxidase (4.0 × 103 s−1), respectively. The following density functional theory calculations demonstrate that the origin of the superior catalytic performance could be attributed to the modulation of the adsorption behavior of the key reaction intermediates on the surface. As a proof of concept, its peroxidase mimicking ability is adopted for sensing glucose and glutathione molecules in human serum, with a long linear range and high selectivity. This work opens new horizons for the future development of advanced catalysts based upon alloy nanocrystals for various applications.
研究领域:
纳米材料科学
·
生物医学工程
·
催化化学
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ELECTROCHIMICA ACTA
·
2014
·
IF 4.086
Daifang Wang,Longhua Guo,Rong Huang,Bin Qiu,Zhenyu Lin,Guonan Chen
Electrochemiluminescence (ECL) of Ru(bpy) 3 2+ has been widely used in analytical chemistry . Herein, we present a new approach to enhance the ECL of Ru(bpy) 3 2+ by the localized surface plasmon resonance (LSPR) of gold nanorods (AuNR). Our investigations reveal that the ECL intensity could be greatly enhanced by controlling the distance between Ru(bpy) 3 2+ and the surface of AuNRs. We call this kind of surface plasmon induced ECL enhancement as surface-enhanced electrochemiluminescence (SEECL). This kind of SEECL phenomenon is utilized to fabricate a biosensor for ultrasensitive Hg 2+ detection. The SEECL biosensor is fabricated by self-assembling AuNRs and T-rich ssDNA probes on gold electrode surface. With the presence of Hg 2+ , the conformation of ssDNA probes changed to be hairpin-like structure via formation of T-Hg 2+ -T structure. And Ru(bpy) 3 2+ could insert into the grooves of the hairpin structured DNA probes to generate ECL emission, which could be enhanced by the LSPR of AuNR. The ECL intensity of the sensor increased with the concentration of Hg 2+ , and a detection limit of 10 fM Hg 2+ in aqueous solution was achieved. The effect of different LSPR peak location of AuNR on the sensitivity of biosensor has been investigated. The results show that a good overlap between the LSPR absorption spectrum and the ECL emission spectrum of Ru(bpy) 3 2+ could achieve the best ECL signal enhancement.
研究领域:
分析化学
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生物传感
·
纳米技术
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