Catalysis Science & Technology
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2022
·Vol. 12
·期 8
·2578-2588
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IF 6.177
Leilei Zhou,Weiwei Lin,Xinchao Wang,Zhuangqing Wang,Yinze Yang,Liyan Zhang,Haiyang Cheng,Masahiko Arai,Fengyu Zhao
The production of biofuels (hydrocarbons) from renewable biomass resources has attracted much attention in the fields of green energy and sustainable chemistry. Herein, catalytic hydrodeoxygenation of methyl laurate (n-C11H23COOCH3) to produce hydrocarbons n-C12H26 and n-C11H24 has been investigated over Ru dispersed on acidic supports H-ZSM-5, Al2O3 and SiO2, and the reaction rate and the product distribution were discussed and correlated with surface Brønsted and Lewis acid sites and active Ru species in detail. The reaction rate at the initial stage increased with the amount of the total acid sites, and the ratio of n-C12H26/n-C11H24 and the selectivity to n-C12H26 were positively correlated with the amount of Brønsted acid sites. The Ru active species presented to be more electron-deficient on the catalysts with a larger amount of Brønsted acid sites on which an η1-(O) adsorption configuration of 1-C11H23CHO was confirmed, which favoured the formation of n-C12H26, thus varying the product distribution. Besides, Brønsted acid sites could provide protons to promote the hydrogenolysis of n-C11H23COOCH3 and the following dehydration to produce n-C12H26.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Weidong He,Jianpo Chen,Qianyu Zhang,Hao Cui,Chengxin Wang
Reasonable structure design and fine electronic modulation are the keys to achieving the platinum-like hydrogen evolution reaction (HER) performance on Ru-based catalyst, but also challenges. Here, the integration of uniformly dispersed ultra-fine Ru nanoparticles with β-hexagonal ammonium tungsten bronze (β-HATB) nanowires is reported as an efficient acidic electrocatalyst. Due to the strong metal-support interaction, the surface charge state of Ru is effectively regulated, forming a mixed valence state composed of zero valence and offset state. The prepared Ru@β-HATB/CC exhibits a Pt-like catalytic activity with a small overpotential of 25 mV and a very low Tafel slope of 27.6 mV dec −1 . In-situ Raman spectroscopy and electrochemical analysis reveal that β-HATB does not directly participate in HER reaction and hydrogen spillover effect (H ads from β-HATB to Ru NPs) is not the main reason for the hydrogen evolution activity, but β-HATB can optimize the kinetics of hydrogen adsorption/desorption behavior on Ru surface and provide a stable and fast charge transfer channel, thus improving HER activity.
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LUMINESCENCE
·
2022
·Vol. 37
·期 6
·980-986
·
IF 2.613
Weiwei Luo,Zhuoxin Ye,Daqian Song,Pinyi Ma
In this work, an electrochemiluminescence (ECL) sensor chip for sensitive detection of thrombin (TB) was prepared using a screen-printed electrode (SPE) as a working electrode and an aptamer as a specific recognition moiety. To produce an ECL sensor chip, a layer of p L -Cys was immobilized on the surface of the SPE using the cyclic voltammetry scanning method. A layer of gold nanoparticles (AuNPs) was assembled through an Au–S bond and hairpin DNA was further immobilized on the electrode surface. Ru(bpy) 2 (mcpbpy) 2+ , as a luminescent reagent, was covalently bound to single-stranded DNA (ssDNA) to prepare a luminescence probe ssDNA-Ru. The probe was hybridized with TB aptamer to form a capture probe. In the presence of TB, the TB aptamer in the capture probe bound to TB, causing the release of ssDNA-Ru that could bind to hairpin DNA on the electrode surface. The Ru(II) complex as a luminescent reagent was assembled onto the electrode, and p L -Cys was used as a co-reactant to enhance the ECL efficiency. The ECL signal of the sensor chip generated based on the above principles had a linear relationship with log TB concentration at the range 10 fM to1 nM, and the detection limit was 0.2 fM. Finally, TB detection using this method was verified using real blood samples. This work provides a new method using an aptamer as a foundation and SPE as a material for the detection of biological substances.
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MATERIALS SCIENCE IN SEMICONDUCTOR PROCESSING
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2022
·
IF 4.644
Zhun Zhou,Xiaozhong Li,Jinjun Li,Zhixiong You
In the present study, CO 2 methanation with Ru nanoparticles loaded onto three TiO 2 nanocrystal supports (TiO 2 anatase with both exposed (001) facets and oxygen vacancies , TiO 2 anatase with exposed (001) facets and general TiO 2 anatase) was demonstrated. The three samples were denoted as Ar700-R, 700-R and Ana-R, respectively. XRD results confirmed that Ar700-R and 700-R sample exposed (001) facets, XPS and EPR results demonstrated the presence of oxygen vacancies on the surface of Ar700-R. In tests of CO 2 methanation activity, Ar700-R showed the highest CO 2 conversion efficiency of 75% and CH 4 formation rate of 18.84 μmol•g −1 •s −1 (GHSV = was 21600 ml•h −1 •g −1 ) at 400 °C. The enhanced CO 2 methanation activity of Ar700-R was attributed to the co-activity achieved by exposing (001) facets and oxygen vacancies on the surfaces of TiO 2 nanocrystal supports.
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Journal of CO2 Utilization
·
2022
·
IF 8.321
Xiaowei Hu,Maowei Luo,Mooeez ur Rehman,Junhao Sun,Hamzah A.S.M. Yaseen,Faisal Irshad,Yujun Zhao,Shengping Wang,Xinbin Ma
The electron-donating effect of supports on active metals has been reported to be beneficial to improve catalytic activity of heterogenized molecule catalysts for CO 2 hydrogenation to formic acid . However, this effect has not been discussed in depth from the perspective of reaction mechanism, especially for CO 2 activation with the combination of theoretical calculations. Herein, we report a catalyst prepared via anchoring RuCl 3 on a post-synthetic modified (PSM) zeolitic imidazolate framework-8 (ZIF-8) in which linkers 3-methyl-1,2,4-triazole (Mtz) with a surplus of uncoordinated N sites have been incorporated. X-ray photoelectron spectroscopy (XPS) and density functional theory (DFT) calculations reveal that uncoordinated N sites in linkers donate additional electron-density to Ru, resulting in the decrease of energy barrier of CO 2 activation. And the RuCl 3 @ZIF-8-Mtz(0.29) catalyst containing the most Mtz ligands displayed the highest catalytic performance for the CO 2 hydrogenation to formic acid as compared to RuCl 3 @ZIF-8-Mtz(0.15) and RuCl 3 @ZIF-8.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Dong Zhang,Wenqiang Yang,Zhenbin Wang,Cong Ren,Yao Wang,Mingyue Ding,Tong Liu
Electrochemical carbon dioxide reduction reaction (CO 2 RR) via a solid oxide CO 2 electrolyzer has been attracting increasing attention because it can effectively convert CO 2 into high value-added chemical products and efficiently store the excessive electricity. However, the lack of efficient electrodes to catalyze this reaction process severely limits their practical applications. Herein, we report Ru promoted perovskite type Pr 0.4 Sr 0.6 Fe 0.9 Mo 0.1 O 3-δ with a general formula of Pr 0.4 Sr 0.6 Fe 0.8 Ru 0.1 Mo 0.1 O 3-δ (Ru-PSFM) cathode to overcome the constraints of low current density, low Faradaic efficiency, and high overpotential of CO 2 RR. The cathode electrolysis current density of CO 2 RR at 800 °C and 2.0 V is considerably improved from 0.707 to 1.480 A cm −2 with an enhancement rate of 109%, while its corresponding electrode polarization resistance at 1.4 V is significantly lowered from 2.228 to 0.319 Ω cm −2 . Furthermore, the solid oxide CO 2 electrolyzer exhibits superior stability during the operation. Distribution of relaxation times analysis results reveal that the rate-determining process, involving CO 2 adsorption, dissociation, and activation on the cathode surface, is significantly activated and dramatically accelerated after Ru doping. Density function theory calculations demonstrate that the in-situ exsolved Fe-Ru alloy nanocatalyst is a more favorable site for the activation of CO 2 dissociation. This work provides valuable insights into the rational design of efficient cathodes for CO 2 RR.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
·
IF 24.319
Rong Shang,Qizhao Zhang,Peng Lin,Bang Gu,Qinghu Tang,Qiue Cao,Wenhao Fang
Direct oxidative coupling of alcohols and amines is an environmental-benign and atomic-economy approach for imine synthesis. We disclosed that UiO-66 framework successfully confined Ru to single-atom scale with assistance of oxophilic Zn 2+ promoter. This RuZn@UiO-66 catalyst showed a highest TOF of 78 h -1 among all Ru catalysts in literature and attained > 99% yield to benzylideneaniline in the model reaction in an O 2 atmosphere at a low temperature without alkaline additives. In addition, this catalyst demonstrated satisfying gram-scale imine synthesis, wide substrate scope and stable reusability. Kinetic investigations and in situ characterizations allowed getting insights to active sites, amphoteric carrier and reaction mechanism. Dynamic interactions between Ru and Zn based on their ratios induced electron-deficient Ru 0 active sites promoted by oxophilic Zn 2+ species. Hence, primary alcohols can be efficiently converted to the corresponding aldehydes using molecular O 2 , i.e. , the rate-determining step. Besides, Zr 4+ -O 2- pairs on UiO-66 provided adequate acidic-basic sites for the tandem catalysis.
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ACS Sustainable Chemistry & Engineering
·
2022
·
IF 9.224
Zhuo Li,Yaqian He,Chunhui Li,Yuchu He,Xuwu Zhang,Song Ni,Desong Wang,Dawei Gao
The high interstitial fluid pressure at the tumor tissue is a key factor that hinders the deep penetration of nanomedicines into the tumor and affects the therapeutic effect. Herein, we designed a CaO2-based Ru nanozyme to efficiently consume the tumor interstitial fluid and enhance deep tumor penetration as well as treatment. CaO2/Ru-PDA-HA (CRPH) reached tumors via hyaluronic acid (HA)-mediated tumor targeting. Under 808 nm laser irradiation, CRPH pyrolyzed and released CaO2 and Ru, and then CaO2 would consume H2O to produce O2 and H2O2 for reducing the tumor interstitial fluid volume to promote the tumor penetration of medicines. Meanwhile, Ru nanoparticles with good peroxidase activity can decompose H2O2 to generate cytotoxic •OH. Therefore, photothermal and ROS synergistic therapy damaged deep tumor stem cells. The results showed that the relative tumor interstitial pressure was reduced to 56.34%, and the tumor inhibition rate was 99.67%. The design provides a synergetic hydrodynamic therapy strategy for enhancing the deep penetration of nanomedicines and boosting the antitumor effect.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Qiyan Wang,Sara Santos,César A. Urbina-Blanco,Wenjuan Zhou,Yong Yang,Maya Marinova,Svetlana Heyte,Thuriot-Roukos Joelle,Ovidiu Ersen,Walid Baaziz,Olga V. Safonova,Mark Saeys,Vitaly V. Ordomsky
Catalytic processes in water have a lower environmental impact, cost, and toxicity than in organic solvents. Considering the high content of water in biomass, it would be natural to use aqueous phase catalytic technology for the production of valuable products. However, in the aqueous phase, most metal-based catalysts suffer from low activity, low selectivity and deactivation due to metal oxidation and leaching. In this paper, we propose a solid micellar Ru catalyst (Ru(III)@MCM) based on single-site Ru (III) species stabilized by cetyltrimethylammonium (CTA + ) surfactant and immobilized in the walls of MCM-41 for the selective aqueous phase hydrogenation of carbonyl groups. This catalyst demonstrates exceptional selectivity, activity, and stability in comparison with conventional metallic catalysts. DFT modeling suggests that the reaction proceeds via heterolytic dissociation of hydrogen, forming a Ru-Hydride species, and subsequent hydride transfer to the carbonyl group. Water plays a key role in avoiding product inhibition.
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Inorganic Chemistry Frontiers
·
2021
·Vol. 8
·期 21
·4712-4719
·
IF 6.569
Tianxing Wu,Hanqi Meng,Rui Dang
Electrocatalytic hydrogenation is a competing reaction for hydrogen evolution that occurs in the presence of organic compounds containing unsaturated chemical bonds using water as the hydrogen donor. Here, we propose a simple method to synthesize amorphous Ta2O5 loaded amorphous Ru with poor crystallinity. The amorphous composite (Ta2O5/Ru-4.0-400) with an ultra-low Ru loading amount (2.16 wt%) exhibits 69.8% conversion of cinnamaldehyde with 29.1% FE and 100% selective formation of half-hydrogenated hydrocinnamaldehyde under a constant potential of −1.1 V vs. RHE for 5 h. Detailed experimental studies revealed that the amorphous structure with poor crystallinity offers structural flexibility and rich defects for electrochemical hydrogenation reactions, and the Ta2O5 substrate serves as a bridge to effectively facilitate electron transfer from Ru to CAL molecules. This work presents a new strategy for designing highly efficient electrocatalysts with an amorphous structure for the hydrogenation of organic compounds containing unsaturated chemical bonds.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2021
·
IF 7.46
Jinjie Hou,Pei Jia,Kairong Yang,Tong Bu,Xinyu Sun,Li Wang
In the last decades, nanozymes have drawn significant attention because of their higher stability and lower preparation cost than natural enzymes. In this report, the novel Ru@V 2 O 4 nanocomposite with multi-enzyme-like activities has been synthesized via one-step hydrothermal method and simple stirring. It was proved that the prepared Ru@V 2 O 4 nanowires presented magnificent tetra-enzyme-like activities, comprising oxidase-like (OD-like), peroxidase-like (POD-like), catalase-like (CAT-like) and superoxide dismutase-like (SOD-like) activity. Firstly, the kinetic investigation validated the OD and POD-mimics behaviors of Ru@V 2 O 4 nanowires, which were in conformity with the Michaelis-Menten kinetics. Then a bifunctional colorimetric sensing platform was constructed for the sensitive detection of H 2 O 2 and cysteine (Cys) on the basis of POD-like and OD-like enzyme activities of Ru@V 2 O 4 nanowires. H 2 O 2 could be detected by Ru@V 2 O 4 nanowires over a range of 1–500 μM and the response limit was 0.788 μM. Under optimal conditions, the degree of discoloration was linearly proportional to the concentration of Cys in the range of 3–50 μM with a low detect limit of 0.139 μM. Besides, Ru@V 2 O 4 nanowires can detect H 2 O 2 in water samples and Cys in serum samples. Therefore, this research significantly expands the application of the tetra-enzyme mimetic Ru@V 2 O 4 nanowires in the fields of biosensing, biocatalysis, environmental monitoring and medical diagnosis.
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Small Methods
·
2021
·Vol. 5
·期 7
·2100505
·
IF 14.188
Yong-Ya Zhang,Nan Zhang,Peng Peng,Rui Wang,Yan Jin,Ya-Kun Lv,Xin Wang,Wei Wei,Shuang-Quan Zang
Design and development of cost-effective electrocatalysts with high efficiency and stability for scalable and sustainable hydrogen production through water splitting is still challenging. Herein, with the aid of divinyl functionalized ionic liquids, uniformly distributed Ru nanoparticles (NPs) on nitrogen-doped carbon frameworks are obtained via an in situ confined polymerization strategy. Attributed to the unique lamellar structure and confinement effect of carbon supports, the optimized homo-PIL-Ru/C-600 (with Ru 10 wt%) catalyst exhibits superior catalytic efficiency for the hydrogen evolution reaction with the overpotential of only 16 mV at a current density of 10 mA cm −2 and the corresponding Tafel slope of only 42 mV dec −1 . Moreover, the performance can be well reserved even after 10 000 cycles, demonstrating excellent stability and promising potentials for industrial application. This work not only provides a facile approach for the preparation of highly efficient Ru-based catalysts, but also guides the synthesis of other highly dispersed metallic NPs for special applications.
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