CATALYSIS LETTERS
·
2022
·Vol. 152
·期 10
·3046-3057
·
IF 2.936
Yu Pei,Jiang Junxiang,Chen Can,Wang Zhong,Wang Da,Li Guangci,Li Xuebing
Catalytic selective hydrogenation of esterified malic acid to produce 1,2,4-butanetriol (1,2,4-BT) using H 2 as the reducing reagent suffers from the low 1,2,4-BT selectivity. Here, Ru/SiO 2 catalyst was employed for selective hydrogenation of dimethyl malate (DM) to produce 1,2,4-BT, which gave abnormal high DM conversion (100%) and 1,2,4-BT selectivity (92.4%) in aqueous solvent at 363 K, especially, the 1,2,4-BT yield even is higher than the optimal catalyst reported (Ru-Re, 79.8%). The reaction pathways for the DM hydrogenation on Ru/SiO 2 were also proposed, suggesting that extremely high 1,2,4-BT selectivity require for the much high hydrogenation rates at low temperatures, where side-reaction transesterification rates are relatively low. The extremely high hydrogenation activity and 1,2,4-BT selectivity on Ru/SiO 2 in aqueous solvent at low temperatures arise from that H 2 O may coordinate to Ru 2+ and prevent the reduction of Ru 2+ to Ru under high H 2 pressure. Ru/SiO 2 surface presents abundant Ru 2+ in aqueous solvent, can activate H 2 through heterolytic cleavage mode to form hydride, which can significantly increase hydrogenation rates of C = O groups at low temperatures. In addition, the activity and 1,2,4-BT selectivity on Ru/SiO 2 catalyst only reduced by 2.3% and 2.6%, respectively over a period of 550 h. Graphical Abstract
研究领域:
催化
·
化学工程
·
有机化学
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DOI
高影响因子
MOLECULES
·
2023
·Vol. 28
·期 12
·4830
·
IF 4.6
Xiaorui Yang,Xiaotong Li,Jing Zhao,Jinhua Liang,Jianliang Zhu
Sorbitol, a product primarily derived from glucose hydrogenation, has extensive applications in the pharmaceutical, chemical and other industries. Amino styrene-co-maleic anhydride polymer encapsulated on activated carbon (Ru/ASMA@AC) catalysts were developed for efficient glucose hydrogenation and were prepared and confined Ru by coordination with styrene-co-maleic anhydride polymer (ASMA). Through single-factor experiments, optimal conditions were determined to be 2.5 wt.% ruthenium loading and a catalyst usage of 1.5 g, 20% glucose solution at 130 °C, reaction pressure of 4.0 MPa, and a stirring speed of 600 rpm for 3 h. These conditions achieved a high glucose conversion rate of 99.68% and a sorbitol selectivity of 93.04%. Reaction kinetics testing proved that the hydrogenation of glucose catalyzed by Ru/ASMA@AC was a first-order reaction, with a reaction activation energy of 73.04 kJ/mol. Furthermore, the catalytic performance of the Ru/ASMA@AC and Ru/AC catalysts for glucose hydrogenation were compared and characterized by various detection methods. The Ru/ASMA@AC catalyst exhibited excellent stability after five cycles, whereas the traditional Ru/AC catalyst suffered from a 10% decrease in sorbitol yield after three cycles. These results suggest that the Ru/ASMA@AC catalyst is a more promising candidate for high-concentration glucose hydrogenation due to its high catalytic performance and superior stability.Keywords:Ru/ASMA@AC catalyst;coordination;glucose conversion;sorbitol yield;confine
研究领域:
化学工程
·
催化科学
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DOI
PubMed
高影响因子
ENERGY & FUELS
·
2024
·
IF 5.2
Jia-yuan Tian,Jun Hu,Feng Lin,Yu-long Ma,Yong-gang Sun,Ying-bo Zhu,Jin-peng Wei,Yi-ting Lei,Jing-jing Wu
The catalytic selective hydrodeoxygenation of guaiacol to value-added cyclohexane is one of the sustainable biomass utilization pathways for which the Ru/HZSM-5 support catalyst has been considered as promising. However, the effect of the catalyst morphology on the catalytic properties must be further investigated. Four Ru catalysts with different support morphologies, two-dimensional nanosheets (Ru/HZSM-5-P), brick-shaped (Ru/HZSM-5-G), cross-shaped (Ru/HZSM-5-J), and irregular particles (Ru/HZSM-5-D), were prepared by the impregnation method to investigate the effects of catalyst morphology and acidity on the conversion efficiency of lignin-derived guaiacol to cyclohexane. The catalytic activity data showed that Ru/HZSM-5-P exhibited the best catalytic performance among the four catalysts with a conversion rate of 99.9% for guaiacol and a yield of 99.9% for cyclohexane. The characterization results showed significant differences among the four catalysts in terms of accessibility (thickness and pore volume), acidity, metal particle size, and reduction temperature. The Ru/HZSM-5-P catalyst with a two-dimensional nanosheet structure showed the best accessibility, smaller metal particle size, reasonable metal–support interaction, and appropriate B/L. The relatively strong acid centers facilitate the activation of C–C and C–O bonds. Besides, the reduced Ru species on the Ru/ZSM-5 catalyst exhibited high H2 adsorption activity, which was beneficial for the adsorption of guaiacol. This indicates that the difference in catalyst morphology could greatly affect its catalytic activity, thereby altering the conversion rate of reactants and selectivity of the products.
研究领域:
化学工程
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催化科学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Di Wang,Wen Liu,Haining Wang,Shanfu Lu,Yunqi Li,Liang Luo,Linfeng Yu,Yan Xiang
The rational design of high-performance electrodes for hydrogen evolution reaction (HER) is crucial for water splitting in industrial applications. Herein, dual regulation of both mass transfer and intrinsic activity for in situ grown integrated electrodes was achieved via 3D electrode design and interfacial regulation. An innovative ruthenium (Ru)-based integrated electrode was constructed through a gravity-guided chemical vapor deposition (CVD) technique, featuring a three-dimensional carbon nanotube (CNT) network structure with embedded Ru clusters. This interlaced CNT structural configuration with high porosity and superhydrophilicity improved bubble transfer efficiency by reducing bubble coverage, bubble departure time, and bubble diameter at the reaction interface. Subsequently, the introduction of appropriate covalent Ru-O bonds on the interface of the integrated electrode boosted its intrinsic HER activity. Furthermore, DFT and AIMD calculations elucidated that the formation of covalent Ru-O bonds could reduce the adsorption and desorption of H*/OH* species, strengthen the hydrogen-bond network, and optimize the orientation of water molecules in the double electric layer (EDL). Consequently, the RuOCNT integrated electrode demonstrated a remarkably low overpotential of 41 mV at 10 mA cm −2 in a 1.0 M KOH solution and the high durability indicated by a degradation rate of only 140 μV h −1 at 100 mA cm −2 after 100 h. In addition, an in-depth analysis was carried out to distinguish the contribution of covalent Ru-O sites and electrode’s 3D structure to the boosted HER activity. This study highlighted a new approach to fabricating and understanding an efficient electrode by combining electrode engineering and active site modification to enhance HER efficiency in a mutually reinforcing manner.
研究领域:
材料科学
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电化学
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DOI
高影响因子
MICROCHIMICA ACTA
·
2025
·Vol. 192
·期 5
·1-11
·
IF 5.3
Tian Li,Li Huiling,Han Pengfei,Ma Guangping,Wang Wenzhuo,Jiang Hanyue,Lu Juan
An electrochemiluminescence (ECL) sensor was constructed based on Ru(bpy) 3 2+ @Au and GO@CdS for the detection of tartrazine (TTZ). In the presence of the co-reactant TPrA, Ru(bpy) 3 2+ and CdS quantum dots (QDs) were used as dual luminophores to synergistically amplify the ECL signal of the sensor. Gold nanoparticles (Au NPs) enhanced the electron transport capability of the system and thereby amplified the ECL intensity. Graphene oxide (GO), as a carrier, has a special wrinkle-like structure that not only adsorbed a substantial amount of CdS QDs but also prevented their agglomeration. Additionally, a more sensitive detection method was established based on the quenching of the ECL signal, which occurred due to the interaction between Ru(bpy) 3 2+ and TTZ. A low detection limit (1.3 × 10 –13 mol·L −1 , S/N = 3) was obtained for TTZ concentrations ranging from 4.0 × 10 –13 to 4.0 × 10 –8 mol·L −1 . Finally, actual measurement results from three beverage samples demonstrated that the prepared sensors possess excellent practical capabilities for TTZ detection. Graphical
研究领域:
分析化学
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食品科学
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DOI
PubMed
高影响因子
Green Energy & Environment
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2024
·
IF 10.7
Junming Zeng,Yongbin Yao,Fang Wang,Jiajian Gao,Lili Zhang,Guangwen Xu,Ziyi Zhong,Fabing Su
Nickle-based catalysts are commonly used for CO 2 methanation. However, there is still potential to improve their catalytic performance under mild conditions. In this study, we synthesized a series of Ru-Ni-Al catalysts from Ru-doped NiAl-hydrotalcite using a hydrothermal method. The Ru-Ni-Al catalyst demonstrated much higher activity for CO 2 methanation than the Ni-Al catalyst that did not have Ru doping. Both experimental results and theoretical calculations indicate that the enhanced performance of the Ru-Ni-Al catalyst is related to electronic interactions between nickel (Ni) and ruthenium (Ru). The Ru sites transfer electrons to the Ni sites, increasing the local electron density of Ni, which enhances the adsorption and activation of H 2 . Furthermore, the Ru-Ni metal interface sites improve the adsorption and activation of CO 2 . In situ Diffuse Reflectance Infrared Fourier Transform Spectroscopy (DRIFTS) analysis indicates that adjusting the electronic structure of Ni sites can accelerate the production of intermediates HCOO*, while Ru-Ni intermetallic interface sites can directly dissociate CO 2 into CO*. In addition, CO 2 methanation on the Ru-Ni-Al catalyst follows HCOO*- and CO*-mediated pathways. This study underscores the potential for enhancing CO 2 methanation performance by modulating the electronic structure of Ni sites.
研究领域:
催化化学
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材料科学
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环境科学
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DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2017
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IF 5.951
Wei Lv,Zhan Si,Zhipeng Tian,Chenguang Wang,Qi Zhang,Ying Xu,Tiejun Wang,Longlong Ma
An EtOAc/H2O biphasic solvent–Ru/C coupling biorefinery process was developed to selectively produce aromatics from cornstalk hydrolysis residue (CHR). In this process, CHR was depolymerized in an ethyl acetate (EtOAc)/H2O biphasic solvent system over Ru/C catalyst, which produced aromatics and carbohydrates instantly separated by EtOAc and H2O. Most lignin in CHR was converted to aromatics and nonvolatile fractions, accompanied with partial degradation of cellulose. Optimized results showed that more than 42.7% of aromatics can be obtained under 260 °C for 5 h without external hydrogen pressure. Monophasic and biphasic parallel experimental results show that the strong lignin dissolving ability of the biphasic dissolution/separation system is helpful for aromatics production and separation, which promoted CHR depolymerization over Ru/C. Furthermore, CHR, products, depolymeirzation residue solid (DRS), and catalysts were carefully characterized by gas chromatography (GC-MS), Fourier transform infrared (FT-IR), gel permeation chromatrography (GPC), high-performance liquid chromatrography mass spectrometry (HPLC-MS), nuclear magnetic resonance (NMR), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM), and inductively coupled plasma atomic emission spectroscopy (ICP-AES) analysis. Results demonstrated that the biphasic solvent–Ru/C coupling process can significantly alleviate repolymerization reactions. Based on these analysis results, the catalytic process in biphasic EtOAc/H2O was discussed. This work demonstrates that such a green biphasic catalytic/separation coupling system highlights a promising route for efficient biomass degradation and product separation at mild conditions without external hydrogen pressure.
研究领域:
生物化学
·
可再生能源
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DOI
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2016
·Vol. 163
·期 7
·B280
·
IF 3.014
F. Shang,Y. Liu,S. Wang
A simple, economic, highly sensitive and highly selective electrochemiluminescence (ECL) sensor for the detection of tetrodotoxin (TTX) has been developed at Nafion-graphene-Ru(bpy)32+ composite modified glassy carbon electrode (GCE). Nafion can be used as a modified electrode material to achieve the one-step immobilization of graphene and Ru(bpy)32+ due to its good electrochemical stability and high ion selectivity. The modified glassy carbon electrode not only can be acted as a solid phase microextraction tool to perform the enrichment of TTX, but also can provide good stability of the ECL sensor. Under optimal conditions, the ECL intensity of the sensor increased proportionally to the logarithmic concentrations of TTX in the range of 0.5–5000 ng·mL−1 with a detection limit of 0.1 ng·mL−1. This one-step ECL sensor showed good performance in stability, reproducibility and precision.
研究领域:
分析化学
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毒理学
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生物传感技术
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DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
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IF 9.7
Da Yue,Zhicheng Zhu,Liyuan Chen,Haizhu Sun,Bai Yang
Developing high-performance hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) electrocatalysts to accelerate water splitting kinetics is essential for advancing electrolytic hydrogen production. Herein, a Ru-RuO 2 heterostructure catalyst with stabilized active interfaces is developed by utilizing carbonized polymer dots (CPDs) as electron-modulating mediators. Specifically, CPDs serve as electron reservoir that dynamically regulate the valence state of Ru through coupling with Ru sites during the reduction-oxidation process, driving the oriented formation of small-sized, high-density Ru-RuO 2 nano-heterojunction structure. Simultaneously, CPDs' nanoscale template effect synergistically induces abundant nanoporous structures with Ru-RuO 2 species. The dual modification of geometric and electronic properties not only achieves efficient charge separation but also optimizes bifunctional active sites and significantly improves mass transfer performance. The resultant Ru-RuO 2 /CPDs catalyst successfully integrates the advantages of HER and OER active components, achieving highly efficient and stable bifunctional catalytic activity. In overall water splitting devices, the Ru-RuO 2 /CPDs catalyst exhibits cell voltages of merely 1.51 V in H 2 SO 4 and 1.44 V in 1.0 M KOH to achieve 10 mA cm −2 , with both systems demonstrating stability exceeding 220 h. This work provides a facile strategy for designing efficient and stable catalysts for water splitting across a broad pH range.
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Xiaoting Li,Cheng Qian,Yonghui Tian,Naizhi Yao,Yixiang Duan,Zhijun Huang
In this work, Pt-Ru bimetallic nanoclusters (Pt-Ru NCs) were prepared by a simple one-pot hydrothermal method. The as-prepared Pt-Ru NCs has extremely high peroxidase-like activity, showing a specific activity of 115.36 U/mg far superior to Pt NCs and many reported single-atom nanozymes. This can be attributed to the various microstructures effective for catalysis and unique electron transfer characteristics leading to active hydroxyl radicals ( OH) activation as revealed by density functional theory. By using the Pt-Ru NCs as a substitute for natural horseradish peroxidaseand when cross-linking with antibody as a catalytic label, the colorimetric enhanced lateral flow immunoassay (LFIA) for D-dimer detection was established. As a result, with only 20 s of additional coloration, the visual sensitivity can be improved by about 100 times to 1 ng/mL, while maintaining good specificity and anti-interference. In general, the excellent performance indicates that the Pt-Ru NCs have great potential in colorimetric detection, which is worthy of further promotion.
研究领域:
生物化学
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医学诊断
·
纳米材料
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DOI
高影响因子
CATALYSIS TODAY
·
2014
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IF 3.309
Senlin Wang,Wei Wei,Yu Zhao,Hexing Li,Hui Li
In this paper, highly ordered mesoporous silica nanospheres externally covered by methyl groups ( CH 3 ) but internally grafted by aminopropyl groups ( NH 2 ) were used as host matrix for loading Ru–B amorphous alloy nanoparticles (NPs). The NH 2 and the CH 3 groups served synergistically as effective functionalities for highly dispersing Ru–B NPs within the pore channels of the mesoporous host. Such catalyst was used in the liquid-phase d -glucose hydrogenation and delivered much higher activity than industrial Raney Ni and the commercial Ru/C catalysts. Meanwhile, it could be used repetitively for more than 9 times, showing a good potential in practical applications. This work demonstrated that the surface properties of mesoporous materials can be modified through region-selective immobilization of diverse organic groups, which is essential to optimize the catalysis for some reactions.
研究领域:
材料科学
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催化化学
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DOI
高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Yuntao Qi,Bin Zhang,Dengrong Xue,Hui Zhang,Xiaoning Liu,Zhi Liu,Shichao Zhao,Zhuo Li,Fanchun Meng,Yong Qin
The catalytic conversion of CO2 to CO through hydrogenation has emerged as a promising strategy for CO2 utilization, given that CO serves as a valuable C1 platform compound for synthesizing liquid fuels and chemicals. However, the predominant formation of CH4 via deep hydrogenation over Ru-based catalysts poses challenges in achieving selective CO production. High reaction temperatures often lead to catalyst deactivation and changes in selectivity due to dynamic metal evolution or agglomeration, even with a classic strong metal–support interaction. Herein, we have developed a FeOx/Ru/Rutile multilayer epitaxial structure by depositing a FeOx layer onto the epitaxially grown RuO2 nanolayers on the surface of rutile nanoparticles. This multilayer epitaxial structure transformed into a structure in which Ru nanoparticles were decorated with FeOx layers with ultrastable strong metal-support interaction (SMSI). Subsequently, the FeOx decoration on Ru nanoparticles effectively shifted the dominant product from CH4 to 95% CO during CO2 hydrogenation. Remarkably, this catalyst exhibits exceptional stability and can be operated stably at 550 °C for a long time without apparent deactivation. Compared with the dynamic changes observed in supported Ru nanoparticles, the interaction between Ru and FeOx maintains their electronic states at different reaction temperatures. Furthermore, this Ru–FeOx interaction inhibits H2 activation capability, CO adsorption, and subsequent hydrogenation of CO. The transformation strategy employed here, which utilizes initial multilayer epitaxial structures, can be applied to construct SMSI to enhance metal catalysts’ catalytic performance.
研究领域:
催化
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材料科学
·
化学工程
·
环境科学
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产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）