Journal of Physical Chemistry C
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2022
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IF 4.177
Jie Zhang,Guanpeng Li,Suyu Jiang,Jing-He Yang
Photocatalytic water splitting is a convenient method to produce hydrogen as a renewable energy resource. GaZnNO solid solution with a controllable band gap of 2.3–2.8 eV is considered a promising photocatalyst, while the specific reaction mechanism is still not clear. In this research, the mechanism of photocatalytic water splitting by RuO2-modified GaZnNO solid solution was investigated. X-ray diffraction and scanning electron microscopy detection were used to verify the crystal form of the prepared photocatalysts. Brunauer–Emmett–Teller test was used to analyze the surface properties, and UV–vis diffuse reflection and photoluminescence spectra were used to investigate the abilities of light. Importantly, the hydroxyl radicals and photocatalytically generated oxygen were quantitively measured under different conditions. In conclusion, H2O2 molecules were speculated to be the intermediates and •OH radicals were generated as the byproducts during the water oxidization reaction with GaZnNO solid solution photocatalysts. Ru deposition enhanced the photocatalytic activity by promoting the decomposition of hydrogen peroxide to oxygen. The photocatalytic organic decomposition of the catalysts was also investigated, and it is believed that the organics were mainly oxidized by photogenerated holes. The effect of Ru deposition on the mechanism of photocatalytic water splitting by GaZnNO solid solution was proposed in the end.
研究领域:
材料科学
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能源化学
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DOI
高影响因子
TALANTA
·
2023
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IF 6.1
Kai Zheng,Jiangfei Pan,Zipei Yu,Changqing Yi,Mei-Jin Li
We have proposed a signal dual-amplification electrochemiluminescence (ECL) strategy based on tris(2,2′-bipyridyl)ruthenium(II) (Ru(bpy) 3 2+ ) as chromophores confined with three-dimensional (3D) zinc oxalate metal−organic frameworks (Ru(bpy) 3 2+ @MOFs) for the detection of miRNA-21. The three-dimensional chromophore connectivity in zinc oxalate MOFs provided a network among Ru(bpy) 3 2+ units, shielding the chromophores from solvent molecules and resulting in high Ru(II) complex emission efficiency. Additionally, we discovered that magnetic beads (MBs) used as carrier for enriched signals contribute to enhanced ECL intensity of the chromophore. To evaluate its clinical application, we applied this method to determine the concentration of miRNA-21 solutions ranging from 1.56 to 100 nM, obtaining a calibration curve of ECL intensity versus logarithm of concentration (logC) of miRNA-21 with a high correlation coefficient. This work demonstrates the construction of a signal amplification strategy ECL biosensor for miRNA using Ru(bpy) 3 2+ @MOF systems and its application in ECL detection for analyte methodology.
研究领域:
生物化学
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分子生物学
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医学诊断
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DOI
PubMed
高影响因子
International Journal of Green Energy
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2024
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IF 3.1
Jiaping Zhao,Xincheng Cao,Peng Liu,Feng Long,Shiyu Wu,Junming Xu,Jianchun Jiang
The hydrogenation of bio-based oil into biodiesel is a key strategy in reducing reliance on fossil fuels. However, efficient catalysts are needed to enable low-temperature hydrogenation reactions due to the current high-temperature requirement for bio-based oil hydrogenation. Here, bimetallic catalysts Rex-Ru/C for low-temperature hydrogenation of bio-based oils were prepared. The presence of Re oxides (ReOx) in the catalyst enhances the abundance of weak and medium acid sites, thereby facilitating the adsorption of H2. The DFT calculation shows the introduction of Re also improved the adsorption capacity of the catalyst for fatty acid methyl ester and H2. The Re0.25-Ru/C catalyst exhibits superior conversion, selectivity, and recyclability at low temperatures compared to the previously reported catalysts, achieving 100% conversion of methyl stearate with 100% selectivity toward n-heptadecane (C17) and n-octadecane (C18) (reaction conditions: 150°C, 4 h, 2.5 MPa H2). Moreover, the catalyst also shows excellent hydrogenation activity toward various fatty acids or esters, including methyl palmitate, stearic acid, and palmitate at low temperatures. The Re0.25-Ru/C catalyst showed consistent recycling performance over 9 cycles. The decline in catalytic performance of the catalyst was primarily caused by a reduction in ReOx content, resulting in a decrease in acid site concentration. Consequently, there was reduced adsorption of H2 and oil on the catalyst.
研究领域:
催化化学
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可再生能源
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材料科学
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DOI
高影响因子
RENEWABLE ENERGY
·
2025
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IF 9.1
Yongyuan Deng,Yichao Ye,Tao Yin,Zhipeng Tian,Chao Wang,Ying Chen,Zhi Yang,Junling Tu,Riyang Shu
Hydrodeoxygenation (HDO) is a common refinery process to convert oxygen-containing lignin pyrolysis oil into high-quality hydrocarbon liquid fuels. In this work, we prepared a core-shell Ru@SiO 2 -Al 2 O 3 catalyst and employed it in the HDO of phenolic compounds and lignin pyrolysis oil. The unique core-shell structure of the catalyst reduces the size of Ru metal particles, which significantly improves the hydrogenation catalytic activity. The high surface area, large pore size, and large pore volume of the SiO 2 shell provide a favorable environment for the substrate transfer during the reactions, meanwhile the doped Al 2 O 3 introduces a substantial number of acid sites for the catalysis of deoxygenation. The synergistic effect between the metal sites and acid sites greatly promotes the HDO reaction efficiency. Under mild conditions of 220 °C and 1 MPa H 2 , Ru@SiO 2 -Al 2 O 3 catalyst achieved a guaiacol conversion of 99.9% and a cyclohexane selectivity of 99.9%. This catalyst also demonstrates an outstanding stability, with catalytic activity little loss after 6 recycles. Furthermore, an efficient HDO performance was obtained in the upgrade of other phenolic compounds and lignin pyrolysis oil. At the temperature of 240 °C, the content of hydrocarbons in lignin pyrolysis oil increased from 15.4% to 92.7%. These results indicate that Ru@SiO 2 -Al 2 O 3 holds significant potential for the efficient HDO refinery, providing a promising avenue for the future biofuel development.
研究领域:
化学工程
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可再生能源
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DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
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IF 19.503
Keying Lin,Li Feng,Dekang Li,Jiawei Zhang,Wei Wang,Baojun Ma
It is urgent to deep understanding the electron transfer mechanism in composite co-catalyst for efficient photocatalytic H 2 evolution. Here, choosing Ru and WC as probes, (Ru/WC)/CdS and Ru/(WC/CdS) are designed. The Ru and WC show a synergistic effect in (Ru/WC)/CdS on photocatalytic H 2 evolution. The optimum (Ru/WC)/CdS shows 16.8 mmol/h/g of H 2 evolution, which are 1.93 and 1.34 times of that Ru / CdS and WC/CdS, respectively. Amazingly, the Ru / (WC/CdS) is inferior to WC/CdS, and the Ru shows harmful to WC in H 2 evolution. The role of WC and Ru in photocatalysts and the electron transfer path of composite catalysts with different assembly methods are demonstrated. This study shows the relationship between activities and transferring paths of photoexited electrons.
研究领域:
材料科学
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能源化学
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催化反应
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DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2022
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IF 7.392
Xianda Han,Zhigang Yu,Yangkejia Xiang,Fengqin Li,Xiaoping Tan,Lan Xu,Guiling Zhang
An electrochemical fabrication method of Ru[bpy] 3 2+ @Cu-MOF(-SH)/Au (MOF = metal–organic framework) was developed with a photo/electrochemical information characterization and a DNA-based biosensing validation for the proposed interface. Applying an anodic synthesis method, a modification layer of Ru[bpy] 3 2+ encapsulated with MOF was formed on the Au electrode surface to fabricate an interface with photo/electrochemical dual-signal response. Combining the scanning electrochemical microscopy (SECM) imaging technology with electrochemical and electrochemiluminescence (ECL) detection, the information about the interfacial photo/electrochemical bi-functional properties was explored from three aspects of the parameter variable, intensity variable, and morphology variable. The results show that the effect of parameter variables on the interfacial response follows an “interference effect” mechanism. Under the optimized conditions, the background and the saturation ECL intensities are 610.0 and 24.0 with a quenching efficiency of 96.1% and a detection limit of 30 fM. The saturation current is 48.8 µA with a detection limit of 330.0 nM. Both ECL and electrochemical imaging methods can corroborate each other, validating the logical correlation between the interface fabrication and the response performance in the regional interfacial distribution and laying a methodological foundation for evaluating the interface fabrication quality based on imaging morphology qualitatively. The proposed interface can construct photo/electrochemical dual-signal DNA-based biosensors.
研究领域:
分析化学
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生物医学工程
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材料科学
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DOI
高影响因子
Journal of Environmental Sciences
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2025
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IF 6.3
Xiaonan Guo,Yuanzhe Yu,Runduo Zhang,Shuting Wei,Bin Kang,Ying Wei,Jingbo Jia,Zhou-jun Wang
The Ru-based catalysts with different preparation methods or supports were achieved and applied in efficiently catalytic elimination of 1,2-dichloroethane (1,2-DCE). It was firstly found that the redox ability and chlorine resistance of the catalyst could be improved by regulating the interaction between Ru and supports. Compared with other supports and conventionally impregnated methods, the Ru@ZSM-5 catalyst synthesized by the in-situ encapsulation strategy exhibited an excellent low-temperature catalytic performance ( T 50 = 262°C, T 90 = 327°C), superior stability in long-term test as well as ideal target products. The acidity, specific surface area, and interaction with precious metals of the supports have significant influences on the catalytic activity, and the Ru clusters inside the pore structures are more closely bound to the framework Al species, which promotes the oxidation behavior. The encapsulation strategy also significantly improves the Ru dispersion thereby facilitates oxygen activation as well as Cl-containing volatile organic compounds (CVOCs) deep oxidation, and preserves large amounts of Brønsted acid sites to optimize the hydrolysis mechanism for purification of CVOCs. Subsequently, the synergistic effect between metal redox and acidity is greatly optimized, thus extremely promoting the catalytic efficiency of 1,2-DCE oxidation.
研究领域:
环境科学
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催化化学
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DOI
PubMed
高影响因子
Nanoscale Research Letters
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2020
·Vol. 15
·期 1
·1-15
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IF 3.578
Fan Li,Sun Qi,Zheng Wei,Tang Qinyuan,Zhang Ting,Tian Mengkui
The rutile Sn x Ti 1− x O 2 ( x = 0, 0.33, 0.5, 0.67, 1) solid solution was synthesized by a one-step hydrothermal method, in which tetrabutyl titanate and Tin (IV) chloride pentahydrate were used as raw materials. A series of Ru/Sn x Ti 1− x O 2 were then prepared by the impregnation process in RuCl 3 to investigate the performance and stability of CO and C 3 H 8 oxidation. These catalysts were characterized through XRD, N 2 adsorption-desorption, FT-IR, TEM, XPS, H 2 -TPR, and O 2 -TPD techniques. The effect of Sn/Ti molar ratio and hydrothermal condition on the low-temperature catalytic oxidized performance and stability of Ru/Sn x Ti 1− x O 2 were investigated. The results indicated that Ru/Sn 0.67 Ti 0.33 O 2 catalyst showed an excellent activity and stability at low temperatures. The CO conversion reached 50% at 180 °C and 90% at 240 °C. Besides, the C 3 H 8 conversion reached 50% at 320 °C, the complete conversion of C 3 H 8 realized at 500 °C, and no deactivation occurs after 12 h of catalytic reaction. The excellent low-temperature activity and stability of the Ru/Sn 0.67 Ti 0.33 O 2 were attributed to the following factors. Firstly, XRD results showed that Sn 4+ was successfully introduced into the lattice of TiO 2 to replace Ti 4+ forming a homogeneous solid solution (containing –Sn 4+ –O–Ti 4+ – species), which was consistent with TEM and N 2 adsorption-desorption results. The introduction of Sn could suppress the growth of anatase crystal and promote the formation of rutile phase, and this phase transition was helpful to improve the low-temperature activity of the catalysts. Secondly, TEM images showed that ultrafine Ru nanoparticles (~ 5 nm) were dispersed on Sn 0.67 Ti 0.33 O 2 support, suggesting that the formation of Sn x Ti 1− x O 2 solid solution was beneficial to the dispersion of Ru particles.
研究领域:
催化化学
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材料科学
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DOI
PubMed
高影响因子
SOLID STATE SCIENCES
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2019
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IF 2.155
Wei Li,Pengcheng Liu,Ruyue Niu,Jinping Li,Shuang Wang
Three CeO 2 supports with different concentration of surface oxygen vacancies were prepared by using C 12 H 29 NO (TPAOH), C 2 H 8 N 2 (EDA) and NaOH as precipitant under hydrothermal conditions, respectively. Catalytic experiments showed that the Ru/CeO 2 -TPAOH catalyst has superior catalytic activity (22000 μmol g −1 h −1 ) than Ru/CeO 2 -EDA (19000 μmol g −1 h −1 ) and Ru/CeO 2 –NaOH (16500 μmol g −1 h −1 ) at 450 °C, 3 MPa. In addition, the introduction of Cs and Ba promoters improve the catalytic activity of the Ru/CeO 2 -TPAOH. However, the introduction of K promoter inhibits the catalytic activity of the Ru/CeO 2 -TPAOH. The 4% Cs promoter can effectively increase the catalytic activity of the Ru/CeO 2 -TPAOH (32000 μmol g −1 h −1 ). BET and TEM indicated that 5.5 nm average pore size of CeO 2 -TPAOH support contributes to the dispersion of active metal Ru. XPS and CO 2 -TPD proved that the Ru/CeO 2 -TPAOH catalyst has higher Ce 3+ concentration, more oxygen vacancies, and higher basic site density, which are important factors for improving ammonia synthesis activity.
研究领域:
化学工程
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材料科学
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DOI
高影响因子
BIOMASS & BIOENERGY
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2025
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IF 5.8
Chunyang Han,Zhen Dong,Yahui Zhang,Haian Xia
Ethylene glycol (EG) and 1,2-propylene glycol (1,2-PG) are very important chemicals that are produced mainly from fossil resources at present. Catalytic hydrogenolysis of biomass (such as cellulose and sugar alcohols) to diols has attracted much attention in recent years. However, compared to sugar alcohols, sugars such as xylose have been scarcely used for the production of EG and PG until now due to their instability and low selectivity of diols. Xylose is an abundant and readily available bio-chemicals that can be produced from the hydrolysis of hemicellulose, but its catalytic hydrogenolysis into diols with high yields remains a great challenge. Herein, bimetallic Ru-Re/CZO(Ce 0.7 Zr 0.3 O 2 ) catalysts were synthesized and used to catalyze the hydrogenolysis of xylose to EG and PG. The nature of the catalysts is thoroughly characterized by XRD, XPS, BET, TEM, etc. It is found that Ru and Re nanoparticles are uniformly distributed on CZO alloy support formed by Ce and Zr. A very high total yield (65.0 %) of EG and 1,2-PG was achieved on the 4 %Ru-1 %Re/CZO catalyst under optimal conditions. Recycling experiments demonstrate that high xylose conversion and diol yields are maintained over four successive cycles under optimal conditions, despite a slight increase in Ru nanoparticle size observed via TEM analysis. The mechanistic study shows that xylose is first isomerized into xylulose, which undergoes retro-aldol cleavage to generate the intermediates, followed by further hydrogenation to EG and 1,2-PG. This work provides a new research avenue for the efficient preparation of diols from xylose.
研究领域:
化学工程
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生物质转化
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催化科学
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DOI
高影响因子
ChemistrySelect
·
2025
·Vol. 10
·期 15
·e202501120
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IF 2
Peipei Ji,Xiuwu Wang,Lianpei Zhou,Guiyang Zhou,Tao Chen
Graphical This study develops polymeric micelles with Brönsted acid and pybox-Ru(II) catalysts encapsulated in hydrophobic cores for efficient one-pot tandem catalysis of deacetalization-transfer hydrogenation. The micelles, prepared via self-assembly of block copolymers, demonstrate excellent catalytic efficiency, offering a simple and effective strategy for tandem catalysis. One-pot tandem catalysis has been favored by researchers for its ability to achieve the advantage of a shortened production process. In this paper, polymeric micelles containing Brönsted acid/pybox-Ru(II) in the hydrophobic cores were prepared for one-pot tandem catalysis of deacetalization-transfer hydrogenation reaction. First, block copolymer P[NHS] 30 - b -P[PEG 2000 ] 68 containing activated ester (NHS) in the suspended chain was successfully synthesized by ring-opening metathesis polymerization (ROMP) using a functional monomer containing norbornene group (NB-NHS) and polyethylene glycol containing norbornene group (NB-PEG 2000 ) as the raw materials. Then, block copolymer P[COOH] 30 - b -P[PEG 2000 ] 68 containing Brönsted acid catalyst and complex P[pybox-Ru] 30 - b -P[PEG 2000 ] 68 containing pybox-Ru(II) catalyst were prepared by the activated ester functionalization strategy. The copolymers and complexes were characterized using nuclear magnetic resonance spectroscopy (NMR), X-ray photoelectron spectroscopy (XPS), and gel permeation chromatography (GPC). Then, polymeric micelles with the catalysts encapsulated in hydrophobic cores were achieved by the self-assembly of the above copolymers in water. The prepared polymeric micelles as catalytic nanoreactors were successfully applied to one-pot tandem catalysis of the deacetalization-transfer hydrogenation reaction, demonstrating excellent catalytic efficiency. This study provided a facile and efficient strategy for tandem catalysis.
研究领域:
化学工程
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材料科学
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催化化学
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DOI
高影响因子
ChemCatChem
·
2017
·Vol. 10
·期 6
·1376-1384
·
IF 4.803
Zhaoxia Zheng,Zhicheng Luo,Chen Zhao
Graphical Taking the cross : Morphologically cross-shaped HZSM-5 loaded Ru nanoparticles demonstrate high activity (rate: 7.8 g g −1 h −1 ) in the selective hydrogenolysis of guaiacol to benzene in water with a nearly quantitative yield accompanied with high durability. Hydrogenolysis of C−O bonds is an important tool for synthesis of valuable fuels and chemicals from biomass. In this contribution, we report that morphologically cross-shaped HZSM-5-loaded Ru nanoparticles have demonstrated high activity in the selective hydrogenolysis of guaiacol to benzene in water with 97 % yield and a rate of 7.8 g g −1 h −1 accompanied with high durability. N 2 sorption analysis showed that Ru/HZSM-5 (cross-shaped) had a large mesoporous surface area and pore volume for loading small and uniform Ru nanoparticles, as confirmed by TEM images. The stronger interaction of Ru and cross-shaped HZSM-5 was simultaneously confirmed by a higher hydrogen reduction temperature of RuO 2 on calcined Ru/HZSM-5, a blueshift of Ru δ+ -(CO) n , Ru δ+ -(CO), and Ru 0 -(CO) species in the IR spectra of adsorbed CO, and a higher Ru 3d 5/2 binding energy in X-ray photoelectron spectroscopy measurements. The reaction constant in guaiacol hydrogenolysis to phenol over cross-shaped Ru/HZSM-5 (0.051 min −1 ) was 3–4 times higher than that on spherical and cuboid Ru/HZSM-5 (0.012–0.029 min −1 ) at identical conditions, attributed to the remarkable hydrogenolysis catalytic capability of Ru nanoparticles on cross-shaped HZSM-5. In addition, adsorption of guaiacol and hydrogen was more substantial on cross-shaped Ru/HZSM-5, as evidenced by of IR and mass spectroscopy, respectively. The higher adsorption of guaiacol is attributed to the abundant Lewis acid sites on cross-shaped Ru/HZSM-5, as the Al−OH enriched Lewis acid sites favor the adsorption of oxygen-containing guaiacol. The higher rate constant in the primary step, together with the adsorbed high concentrated reactant and hydrogen (with nearly first-order reaction kinetics) on cross-shaped Ru/HZSM-5, facilitates the overall tandem reaction, leading to an excellent hydrogenolysis catalyst working at hydrothermal conditions for biomass conversion.
研究领域:
催化化学
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能源化学
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材料科学
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）