INORGANIC CHEMISTRY
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2023
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IF 4.6
Encheng Liu,Zhenzhen Wang,Zhonghua Sun,Zhihui Zhang,Mingyang He,Qun Chen,Junfeng Qian
The chemical microenvironment modulation of active sites holds promise for facilitating their catalytic performance. Herein, single-atom Ru anchored by ZrSBA-15 modified with diverse organic amine groups has been fabricated and enabled CO2 hydrogenation to produce formic acid (FA) under mild conditions. However, the reaction cannot be achieved without the modification of organic amines. The functional groups as the microenvironment around Ru active sites effectively regulated the activity, in which Ru encapsulated in ZrSBA-15 bearing –NH2 groups exhibited the highest activity, with turnover number (TON) and turnover frequency (TOF) values of 505 and 64 h–1, respectively. Both characterization and experimental results validated that the functional group manipulated the adsorption capacity of the reactant, the electronic state of Ru and hydrophilicity/hydrophobicity of the materials, and thus the catalytic performance.
研究领域:
催化化学
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材料科学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2024
·
IF 11.2
Mengyao Xu,Fei Liu,Shike Liu,Jun Ma,Mengqin Yao,Xiaodan Wang,Jianxin Cao
Metal-based catalysts are prevalent in the CO 2 hydrogenation to methanol owing to their remarkable catalytic activity. Herein, Ru/In 2 O 3 catalysts with different morphologies obtained by doping Ru into In 2 O 3 with irregular, rod-like, and flower-like morphologies are used for catalytic CO 2 hydrogenation to methanol. Results indicate that the flower-like Ru/In 2 O 3 (Ru/In 2 O 3 -F) exhibits higher catalytic performance than Ru/In 2 O 3 with other morphologies, achieving a 12.9% CO 2 conversion, 74.02% methanol selectivity, and 671.36 mg MeOH ·h −1 ·g cat −1 methanol spatiotemporal yield. Furthermore, Ru/In 2 O 3 -F maintains its catalytic stability over 200 h at 5 MPa and 290 °C. The promotional effect mainly stems from the fact that electronic structure of Ru can be effectively adjusted by modulating the morphology of In 2 O 3 . The strong interaction between atomically dispersed Ru and In 2 O 3 -F enhances the structural stability of Ru, inhibiting the agglomeration of the catalyst during the reaction process. Furthermore, density-functional theory calculations reveal that highly dispersed Ru atoms not only perform efficient and rapid electronic gain and loss processes, facilitating the catalytic activation of H 2 into H intermediates. It also enables the generated reactive H to rapidly overflow to the surrounding In sites to participate in CO 2 reduction. These findings provide a theoretical basis for the development of high-performance catalysts for CO 2 hydrogenation.
研究领域:
催化
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材料科学
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化学工程
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理论化学
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产品关联
DOI
高影响因子
ChemCatChem
·
2020
·Vol. 12
·期 20
·5149-5155
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IF 4.853
Suli Liu,Xueqin Mu,Pengxia Ji,Yun Lv,Lei Wang,Quan Zhou,Changyun Chen,Shichun Mu
Graphical Decorating nanorods : We demonstrate the first metal-phosphides-metal system consisting of Ru and FeCoP, which forms unique CoFeP@Ru nanorod using a simple one-pot synthetic method. Due to its optimal dual cation decorating effects, improved conductivity and rod-like morphology, this catalyst shows superior electro-catalytic HER and OER performances, which are superior to those of some recently reported phosphides and close to that of commercial catalysts. Interfacial engineering and defect modulation can provide abundant active sites for catalysts to further boost the catalysis process. In this work, we develop a strategy to grow multi-heterogeneous cobalt phosphide (CoP) nanorods with rich interfaces and defects along the one-dimensional (1D) nanostructure by dual incorporation of Fe and Ru (CoFeP@Ru). Such a catalyst exhibits high activity and stability towards the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), with overpotentials of only 38 mV in 0.5 M H 2 SO 4 and 48 mV in 1.0 M KOH for HER, and an overpotential of 340 mV in 0.1 M KOH for OER at 10 mA cm −2 . Finally, as the bifunctional catalyst, an alkali electrolyzer is assembled and delivers at a low cell voltage, with almost 100 % Faradaic efficiency. Our experimental results demonstrate that Fe incorporation can disturb or even break the periodic structure of cobalt phosphides, causing a redistribution of the electronic structure and electron density of activity sites, while Ru can significantly enhance the catalytic kinetics, as well as electrochemical and mechanical stability.
研究领域:
材料科学
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电化学
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产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2023
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IF 13.6
Jia Zhao,Heng Zhang,Yang Shi,Mengfan Luo,Hongyu Zhou,Zhenjun Xie,Ye Du,Peng Zhou,Chuanshu He,Gang Yao,Bo Lai
Ferrate (Fe(VI)) has aroused great research interest in recent years due to its environmental benignancy and lower potential in disinfection by-product generation. However, the inevitable self-decomposition and lower reactivity under alkaline conditions severely restrict the utilization and decontamination efficiency of Fe(VI). Here, we discovered that Ru(III), a representative transition metal, could effectively activate Fe(VI) to degrade organic micropollutants, and its performance on Fe(VI) activation exceeded that of previously reported metal activators. The high-valent metal species (i.e., Fe(IV)/Fe(V) and high-valent Ru species) made a major contribution to SMX removal by Fe(VI)−Ru(III). Density functional theory calculations indicated the function of Ru(III) as a two-electron reductant, leading to the production of Ru(V) and Fe(IV) as the predominant active species. The characterization analyses proved that Ru species was deposited on ferric (hydr)oxides as Ru(III), indicating the possibility of Ru(III) as an electron shuttle with the rapid valence circulation between Ru(V) and Ru(III). This study not only develops an efficient way to activate Fe(VI) but also offers a thorough understanding of Fe(VI) activation induced by transition metals.
研究领域:
环境科学
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化学
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水处理
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产品关联
DOI
PubMed
高影响因子
Biosensors-Basel
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2024
·Vol. 14
·期 10
·512
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IF 4.9
Jiawen Fan,Junjie Qi,Jingkun Li,Fuwei Pi
Arginine has been widely applied in the food industry as coloring agents, flavoring agents, and nutritional fortifiers. It is also one of the major components of feed additives. Currently, methods for the highly selective detection of arginine remain absent. For accurate and sensitive detection of L−arginine, a novel ratiometric fluorescence assay based on Ru@UiO-66-NH2was developed and demonstrated in this study. Under optimized detection conditions, the limit of detection (LOD) of this assay for L-arginine was 2.32 μM, which is superior to most assays reported to date. Meanwhile, Ru@UiO-66-NH2showed good stability within 30 days, demonstrating the wide applicability of the proposed assay. The spike-and-recovery rates of the proposed assay for L-arginine in real samples (e.g., tea, grape juice, and serum) were 84.27–113.09%. Overall, the proposed assay showed high sensitivity, good reproducibility, and excellent stability in the detection of L-arginine in both buffer and real samples.
研究领域:
分析化学
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食品科学
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生物化学
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产品关联
DOI
PubMed
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2020
·
IF 3.573
Bowen Luo,Rongxuan Li,Riyang Shu,Chao Wang,Jingtao Zhang,Ying Chen
Simple and efficient catalytic routes have been explored to upgrade the raw lignin oil. Though homogeneous catalysis is easy to operate and possesses a high reaction rate, it also suffers from the difficulty of product separation. In this work, we used H3BO3 as a novel homogeneous catalyst coupled with Ru/C to overcome the separation problem and carry out the hydrodeoxygenation (HDO) of phenolic compounds and raw lignin oil. H3BO3 showed an outstanding performance over the liquid organic and mineral acids, with a good catalyst recyclability. Phenolic model compounds including monomers and dimers can be efficiently converted into cycloalkanes with yields close to 100%. Moreover, the raw lignin oil also had a good HDO result by using this bifunctional catalyst (H3BO3 and Ru/C). The content of hydrocarbons increased from 7.9% to 93.1% at 260 °C, which promoted the upgraded lignin oil capable to be used as fuel directly.
研究领域:
化学工程
·
可再生能源
✓ 已验证
DOI
高影响因子
HYDROMETALLURGY
·
2019
·
IF 3.465
Shunyan Ning,Shichang Zhang,Wei Zhang,Jie Zhou,Siyi Wang,Xinpeng Wang,Yuezhou Wei
The separation of fission products Ru, Rh, and Pd will benefit both the nuclear fuel cycle and enlarge the platinum group metals source. A silica-based iso Bu-BTP/SiO 2 -P adsorbent was used to separate Ru, Rh, and Pd from nitrate solution. It exhibited good adsorption towards Ru, Rh, and Pd with the uptake rates over 95% at 55 °C in 0.1 M HNO 3 –3 M NaNO 3 solution and no adsorption towards 238 U(VI). The adsorption towards Ru, Rh, and Pd matched well with pseudo-second-order model with the equilibrium obtained within 24 h, 24 h and 0.5 h and Langmuir adsorption isotherm model with the saturation adsorption amounts as high as 0.37 mmol/g, 0.34 mmol/g and 0.71 mmol/g respectively. The adsorbed Pd, Rh, and Ru can be desorbed by 0.1 M HNO 3 –0.1 M thiourea , 2 M HCl and NaClO solution (CP) which is expected to realize their mutual separation in desorption stage using the above-mentioned eluents successively. Both FT-IR and XPS revealed that C N C played key role during adsorption and the adsorption needed the participation of NO 3 − to keep charge balance. In a word, iso Bu-BTP/SiO 2 -P is a promising adsorbent for separation and recovery Ru, Rh, and Pd, especially in the case of separating them from other fission products and actinides from high level liquid waste .
研究领域:
核化学
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材料科学
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放射化学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Jiale Wu,Jiajun Zhang,Liguo Wang,Ziqiang Han,Xiang Hui,Yan Cao,Jianhui Shi,Shuang Xu,Peng He,Huiquan Li
Green production of alicyclic amines is highly desirable but of great challenges. Herein, an efficient one-pot synthesis of alicyclic amines from nitroaromatics was realized with a Pt-Ru bimetallic catalyst. 0.5 %Pt-2.5 %Ru supported on an air-exfoliated C 3 N 4 nanosheet achieved 100.0 % conversion of nitrobenzene (NB) with 98.9 % selectivity of cyclohexylamine (CHA) under mild conditions of 80 °C and 1 MPa, attaining a yield rate for alicyclic amine of 357.9 mmol/g metal ·h. Our study has shown hydrogenation of nitro group and aromatic ring took place in sequence over Pt and Ru in a tandem manner due to the highly selective adsorption. During the hydrogenation, the homolytic dissociation of H 2 occurred on the bimetal sites and the inter-site hydrogen spillover between the bimetal played a crucial role. C 3 N 4 nanosheet as the support not only gave rise to the uniform dispersion of metal nanoparticles, but was crucial in curbing the unnecessary adsorption of intermediate aromatic amines. Our study has also demonstrated the good stability and wide applicability of the Pt-Ru/C 3 N 4 -air catalyst for the hydrogenation of various nitroaromatic derivatives.
研究领域:
催化化学
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绿色化学
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材料科学
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产品关联
DOI
高影响因子
Energy Technology
·
2025
·
IF 3.6
Hui Huang,Qi Xu,Liangyun Yu,Lidong Li,Ying Zhang,Fennv Han,Qi Zhang
Currently, there is a thermodynamic and kinetic mismatch between carbon dioxide methanation. Carbon dioxide is stable in nature and requires a highly active catalyst to facilitate its reduction reaction. In this article, Ru/ZrO 2 catalysts are prepared by a structure-directed derivatization strategy using zirconium-based metal-organic frameworks (MOFs) (UiO-66) as precursors. The porous framework structure of MOFs was utilized to construct Ru nanoparticles with a large size (≈9.7 nm). Photothermal catalysis is employed, and the photoexcitation induced the transfer of electrons from the conduction band of ZrO 2 to Ru, which elevated the electron density of Ru to the enriched state and promoted the activation of CO 2 adsorption, while the photothermal effect facilitated the warming of the catalyst bureau, which provided a favorable condition for CO 2 methanation. The compositional valence, morphology, specific surface area, bandgap and other properties of the catalysts were evaluated by X-ray diffraction, X-ray photoelectron spectroscopy, transmission electron microscpe, Brunner-Emmet-Teller measurements, hydrogen temperature-programmed reduction, CO 2 -TPD, ultraviolet–visible, photoluminescence, and photocurrent response characterization. The experimental results showed that 99% methane selectivity and 120.354 mmol g cat −1 h −1 methane yield were achieved at 1 MPa and photothermal (250 °C) conditions.
研究领域:
材料科学
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催化化学
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环境科学
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产品关联
DOI
高影响因子
GREEN CHEMISTRY
·
2017
·Vol. 19
·期 9
·2201-2211
·
IF 9.125
Wenxiu Cao,Wenhao Luo,Hongguang Ge,Yang Su,Aiqin Wang,Tao Zhang
The hydrogenation of levulinic acid (LA) to γ-valerolactone (GVL) is a crucial reaction included in many biorefinery schemes for the production of renewable chemicals and fuels. The development of highly stable supported Ru-based catalysts in the polar protic liquid phase under hydrothermal conditions is still a major challenge. Here, we prepared a 0.85 wt% Ru/ZrO2@C catalyst using a new stabilization strategy based on the UiO-66 (Zr-MOF) material. The catalytic performance of this Ru/ZrO2@C in LA-to-GVL was tested and compared with commercial 5 wt% Ru/C at 10 bar H2, 413 K in water and also in high protic aqueous solution (pH = 1). The full conversion of LA and quantitative yield of GVL were achieved with both catalysts. However, the 5 wt% Ru/C showed poor resistance to deactivation already after the first run. ICP, XPS, HRTEM, AC-STEM, TPR and physisorption data showed that quick deactivation of Ru/C was mainly caused by the leaching of ruthenium in addition to the loss of surface area via carbonaceous deposition in micro-pores. In contrast, the self-prepared Ru/ZrO2@C catalyst showed no apparent drop in catalytic performance either in water or in high protic aqueous solution upon multiple recycling, and no leaching of ruthenium was found even under harsh conditions (pH = 1). Remarkably, in the Ru/ZrO2@C catalyst, Ru (probable single-atom) was highly dispersed on nanotetragonal ZrO2 (3.3 nm), embedded in the amorphous carbon, and no apparent Ru nanoclusters were observed even after reactions. TPR results indicated that this excellent stability might be attributed to strong metal–support interaction between Ru and nanotetragonal ZrO2.
研究领域:
化学工程
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催化材料科学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Peng Lu,Lyumeng Ye,Xianhui Yan,Jianhang Huang,Zhixiong Tang,Dongyao Chen,Chaoping Cen
It is challenging for catalytic oxidation of volatile organic compounds (VOCs) due to the existence of HCl in municipal solid waste incineration flue gases. A thorough probe into the deactivation mechanism is imperative but still lacking. Herein, the poisoning effect of gaseous HCl on a Ru-based catalyst for toluene catalytic oxidation was investigated. Toluene conversion and CO 2 selectivity decreased dramatically from 89.3 % and 93.8 % to 15.0 % and 8.0 %, respectively at 250 °C under HCl atmosphere. HCl led to a reduction of low-temperature redox properties, as well as a decrease of BET surface area, surface oxygen content and mobility, resulting in a loss of catalytic activity. HCl combined with active Ru and Mn, thereby restricting the electron transfer between Ru 4+ and Mn 2+ . Moreover, HCl could be oxidized by active oxygen species to form Cl• radical, which subsequently reacted with toluene oxidation intermediates, resulting in the generation of chlorinated compounds, such as chlorobenzene, dichlorobenzene, carbon tetrachloride, and benzyl chloride. These harmful chlorinated compounds predominantly deposited on catalyst surface. The protective role of H 2 O against HCl poisoning was mainly attributed to the competitive adsorption between H 2 O and Cl ions, the washing effect, and the promoting of intermediates oxidation and oxygen activation. It is noteworthy that during toluene oxidation in the presence of HCl + H 2 O, a detectable level of 0.048 ng I-TEQ/Nm 3 PCDD/Fs was observed in the off-gas.
研究领域:
环境科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
International Journal of Electrochemical Science
·
2023
·
IF 1.5
Nian Lu,Wen-chang Wang,Xiao-hui Chen,Zhi-dong Chen
In this paper, a PSA/Ru(bpy) 3 2+ modified electrode was prepared by electrochemical polymerization and used as the working electrode in ECL detection of melamine. Under the optimal conditions, the sensor shows a wide linear range of 1.0×10 -7 ~1.0×10 -5 mol/L, detection limit of 2.5×10 -8 mol/L with good reproducibility and stability. The method is expected to be a new method for the detection of melamine, which is simple and convenient.
研究领域:
分析化学
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食品科学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）