JOURNAL OF THE ENERGY INSTITUTE
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2024
·
IF 5.6
Bo Chen,Qing-Pan Du,Zhi-Jun Diao,Hong Yuan,Jia-Meng He,Yi-Qing Xie,Xiao-Ran Wang,Yu Wang
Hydrogenation upgrading is an effective technique that lowers the oxygen content of bio-oil with the aim of improving its quality. In order to fabricate a series of Ru-based catalysts for the hydrodeoxygenation of bio-oil, several all-silica supports with different pore sizes are synthesized and modified with Al and Cs in this work. The physical morphology and electronic structure of the catalysts are characterized using multiple techniques including X-ray diffraction, in-situ pyridine adsorption infrared spectroscopy, in-situ diffuse reflectance Fourier transform infrared spectroscopy , Raman spectroscopy , CO 2 temperature-programmed desorption, scanning electron microscopy, energy-dispersive X-ray spectroscopy, transmission electron microscopy , X-ray photoelectron spectroscopy and N 2 physical adsorption-desorption testing. Phenol , guaiacol , anisole and o-cresol are selected as model compounds to investigate the hydrodeoxygenation reactivity of the catalysts. The results reveal that there is a strong linear correlation between the pore size of the catalysts and the rates of the hydrogenation and hydrodeoxygenation of phenol. Importantly, both the oxygen vacancy density and relative content of Brønsted and Lewis sites (B/L) of the catalysts can be greatly increased by Cs modification, which further linearly promotes the hydrodeoxygenation activity of the catalysts. In addition, the in-situ infrared spectroscopy results show that the catalysts modified by Al and Cs heterolytically cleave H 2 to supply H + for the reaction. This work presents a novel approach for fabricating catalysts employed in the hydrotreatment process of bio-oil.
研究领域:
化学工程
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催化科学
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产品关联
DOI
高影响因子
ACS Applied Energy Materials
·
2024
·
IF 5.4
Hailiang Chu,Guangyao Li,Chuang Liu,Chenhui Cui,Yutong Li,Shujun Qiu,Yongpeng Xia,Yongjin Zou,Fen Xu,Lixian Sun
Currently, ammonia borane (AB, NH3BH3) hydrolysis is considered an available tactic for hydrogen evolution under ambient conditions, which includes many complex reaction steps, such as the activation and adsorption of AB and water molecules on the catalyst. Therefore, exploiting the high-performance catalysts with multiple active sites to match the multistep catalytic processes in AB hydrolysis is a critical and urgent task but a tough challenge. Herein, we propose a synthesis scheme for a high-entropy alloy (HEA) catalyst for hydrogen liberation from AB hydrolysis. The FeCoNiMnRu HEA with face-centered cubic (fcc) phase was synthesized by the polymer fiber nanoreactor method using low-cost transition metals of Co, Fe, Mn, and Ni as basic elements combined with the precious metal Ru, which facilitates the electron transfer and enhances the synergistic interaction between these elements, hence enhancing the catalytic activity toward AB hydrolysis to release hydrogen. For instance, the as-synthesized Fe23Co27Ni27Mn12Ru11 HEA catalyst shows superior activity in catalyzing AB hydrolysis with an apparent activation energy (Ea) of 42.3 kJ·mol–1 and a turnover frequency (TOF) of 55.3 molH2·molRu–1·min–1 at 298 K. This work affords a facile approach for the synthesis of low-cost and high-efficiency catalysts for AB hydrolysis to produce hydrogen.
研究领域:
材料科学
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化学工程
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产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Lemeng Ding,Bingwei Zhong,Xiao Kong,Lingmei Wang,Chao Li,Qingyang Du,Conghua Liu,Wuzhu Sun
Elevated nitrate levels in natural water bodies significantly disrupt the global nitrogen cycle and pose a substantial environmental and human health risk. This study investigates the selective conversion of nitrate to ammonia via catalytic hydrogenation. This highly efficient and selective process offers a sustainable alternative to traditional ammonia production methods while simultaneously addressing nitrate pollution. Ruthenium (Ru) catalysts supported on ceria (CeO 2 ), titania (TiO 2 ), and tin dioxide (SnO 2 ) were synthesized using a simple impregnation method, incorporating oxygen vacancies and low Palladium (Pd) loadings (0.25–0.5 wt%) to enhance catalytic performance. Ru-Pd/CeO 2 exhibited superior activity and selectivity, maintaining near 100 % ammonia selectivity across various nitrate concentrations. At 75 °C, complete conversion of 2000 ppm nitrate to ammonia was achieved within 80 min using Ru-Pd/CeO 2 , and the yield of ammonia can reach up to 16440 mg•h −1 •g Ru -1 . Subsequent ammonia enrichment through evaporation yielded pure ammonia solutions up to 3.6 wt%. Characterization and theoretical calculations suggest that abundant oxygen vacancies on the CeO 2 surface and efficient hydrogen spillover from Pd nanoparticles synergistically contribute to the Ru-Pd/CeO 2 catalyst’s superior performance. The catalyst exhibited excellent stability and reusability, maintaining high activity and selectivity over four cycles. This research presents a promising strategy for addressing nitrate pollution in water bodies while offering a sustainable and environmentally friendly route for ammonia synthesis. The findings of this study lay the foundation for further advancing and potentially implementing catalytic hydrogenation technology for nitrate pollution remediation and ammonia synthesis.
研究领域:
环境科学
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催化化学
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产品关联
DOI
高影响因子
ChemElectroChem
·
2020
·Vol. 7
·期 5
·1207-1212
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IF 4.154
Abubakar Abdussalam,Yiran Guan,Guobao Xu
Graphical Simplify to amplify : Isatin is investigated as a new efficient co-reactant for Ru(bpy) 3 2+ electrochemiluminescence (ECL), and the ECL response of the Ru(bpy) 3 2+ /isatin system in borate buffer solution is about 12 times more intense than in phosphate buffer of the same pH, enabling sensitive ECL detection of isatin. Isatin is an endogenous indole derivative that has been reported to possess various pharmacological and therapeutic activities of clinical importance. To date, isatin has been detected mainly by mass spectrometry. Here, we report for the first time the intense anodic electrochemiluminescence (ECL) of tris(2,2′-bipyridyl)ruthenium(II) with isatin as an efficient co-reactant. Interestingly, the ECL response of the Ru(bpy) 3 2+ /isatin system in borate buffer solution is about 12 times more intense than in phosphate buffer of the same pH; and approximately 114 times greater than the ECL intensity of the luminophore. Under the optimal conditions, the ECL of Ru(bpy) 3 2+ increases linearly with the concentration of the isatin in the range of 1.0 μM to 1.0 mM (R 2 =0.998) with a limit of detection (LOD) of 0.28 μM (3σ/m). Moreover, the method has been successfully applied to the detection of isatin in human urine. The developed method has shown excellent recoveries in the range of 99.7–101.3 %. The anodic ECL assay reported in this work is superior in terms of linear range and selectivity than the previously reported methods and can be applied for the detection of isatin in real samples.
研究领域:
分析化学
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生物医学
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DOI
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2021
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IF 4.464
Muhammad Saqib,Shahida Bashir,Sajjad Ali,Rui Hao
Developing highly specific, rapid, and cost-effective electrochemiluminescence (ECL) methods capable of detecting multiple analytes remains a compelling research goal but it is still a substantial challenge due to narrow choice of ECL systems. In this study, efficient ECL detections were achieved by using anodic Ru(bpy) 3 2+ -acridine orange (AO) ECL system. In present system, dimethylamino substituent on acridine ring acts as active sites for strong ECL generation, while heterocyclic nitrogen atom (–N–) contributes to specific complex formation with metal ion. Accordingly, this anodic ECL method was exploited for highly sensitive detection of both mercury (II) (Hg 2+ ) and dopamine (DA), with detection limits as low as 0.36 nM (linear range 0.01–50 μM) and 1.0 nM (linear range 0.01–10 μM), respectively. The mechanism of Hg 2+ detection was supported by density functional theory (DFT) calculations. Notably, the ECL method exhibit superior selectivity over numerous competing interfering agents. Moreover, the method achieved the detection of both targets in practical media with excellent recoveries (96.0–103.8%). Importantly, the method demonstrates potential advantages in terms of selectivity, sensitivity, rapidity, simplicity, and low cost. This work realizes a successful attempt to further expand the analytical applications of ECL systems and may initiate new thoughts in utilizing acridines in diverse ECL-based sensing and imaging applications.
研究领域:
分析化学
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环境科学
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生物医学
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DOI
高影响因子
RSC Advances
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2018
·Vol. 8
·期 45
·25802-25807
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IF 2.936
Jinyu Gu,Gangbin Yan,Yuebin Lian,Qiaoqiao Mu,Huidong Jin,Zaichao Zhang,Zhao Deng,Yang Peng
Inorganic defect halide compounds such as Cs3Bi2I9 have been regarded as promising alternatives to overcome the instability and toxicity issues of conventional perovskite solar cells. However, their wide indirect bandgaps and deep defect states severely limit their photoelectronic conversion efficiency when implemented in devices. Trivalent cation substitution has been proposed by previous calculations allowing the engineering of their band structures, but experimental evidences are still lacking. Herein we use the trivalent cation Ru3+ to partially replace Bi3+ in Cs3Bi2I9, and reveal their structural and optoelectronic properties, as well as the environmental stability. The Ru-doped Cs3Bi2I9 shows a decreasing bandgap with the increasing doping levels and an overall up-shift of band structure, owing to the dopant-induced defect states and thus enhanced phonon–electron coupling. As a result, upon Ru3+ doping, the narrowed bandgap and the upward shift of the band structures might facilitate and broaden their applications in optoelectronic devices.
研究领域:
材料科学
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能源科学
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光电子学
✓ 已验证
DOI
PubMed
高影响因子
Frontiers of Chemical Science and Engineering
·
2024
·Vol. 18
·期 5
·1-10
·
IF 4.3
Li Kaile,Yu Shijie,Li Qinghai,Zhang Yanguo,Zhou Hui
Lignin, an abundant aromatic polymer in nature, has received significant attention for its potential in the production of bio-oils and chemicals owing to increased resource availability and environmental issues. The hydrodeoxygenation of guaiacol, a lignin-derived monomer, can produce cyclohexanol, a nylon precursor, in a carbon-negative and environmentally friendly manner. This study explored the porous properties and the effects of activation methods on the Ru-based catalyst supported by environmentally friendly and cost-effective hydrochar. Highly selective cleavage of C aryl -O bonds was achieved under mild conditions (160 °C, 0.2 MPa H 2 , and 4 h), and alkali activation further improved the catalytic activity. Various characterization methods revealed that hydrothermal treatment and alkali activation relatively contributed to the excellent performance of the catalysts and influenced their porous structure and Ru dispersion. X-ray photoelectron spectroscopy results revealed an increased formation of metallic ruthenium, indicating the effective regulation of interaction between active sites and supports. This synergistic approach used in this study, involving the valorization of cellulose-derived hydrochar and the selective production of nylon precursors from lignin-derived guaiacol, indicated the comprehensive and sustainable utilization of biomass resources.
研究领域:
化学工程
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环境科学
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DOI
高影响因子
ACS Applied Materials & Interfaces
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2021
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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.
研究领域:
材料科学
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催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
BIORESOURCE TECHNOLOGY
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2018
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IF 5.807
Zengyong Li,Ying Liu,Chuanfu Liu,Shubin Wu,Weiqi Wei
The conversion of cellulose into sorbitol has been recognized as one of most promising biomass valorization routes for the production of high added-value chemicals. In this work, Sulfonic acid-functionalized carbonized cassava dregs supported ruthenium bifunctional catalyst (Ru/CCD-SO 3 H) was prepared. The Ru/CCD-SO 3 H catalyst was employed for direct conversion of cellulose into sorbitol in a neutral aqueous solution. A sorbitol yield of 63.8% could be obtained at 180 °C for 10 h. The acidic sites and metal hydrogenation sites of the Ru/CCD-SO 3 H catalyst played an important role in hydrolytic hydrogenation of cellulose. Particularly, there presented a strong synergistic effect between sulfonic groups and Ru nanoparticles in conversion of cellulose into sorbitol. This synergistic effect was favorable to enhancing the sorbitol yield. Besides, the stability of Ru/CCD-SO 3 H catalyst was investigated under the optimal reaction conditions. The catalytic performance of catalyst was decreased after being used five times.
研究领域:
化学工程
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生物质转化
✓ 已验证
DOI
PubMed
高影响因子
ACS Sustainable Chemistry & Engineering
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2021
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IF 8.198
Xiaoqing Cao,Jun Zhou,Zhipeng Zhai,Song Li,Guo Yuan,Gaowu Qin
Development of efficient and sustainable monolithic catalysts for NaBH4 hydrolysis remains an important goal for hydrogen cycling. In this work, the structured catalyst Ru/MgO with an on–off feature has been prepared by directly growing a nano-Ru-embedded MgO coating layer on a Mg substrate via an instant high-temperature plasma oxidation process. The porous MgO framework provides an ideal space for the access of reactants and diffusion of mass transport, which facilitates reaction triggering and the expulsion of byproducts to avoid poisoning the catalyst. Importantly, Ru nanoparticles (NPs) are monodisperse with ultrasmall particle size deriving from a concurrent rapid arcing and fast quenching. The hierarchical structured Ru NP catalysts are highly active for hydrolysis of sodium borohydride by achieving a high hydrogen generation rate (HGR) of 101,189 mL min–1 g–1 and exhibit attractive stability. In addition, it is facile to realize the “on–off” functionality based on simple separation that could accurately control the hydrogen generation, suggesting the structured catalyst to be of great potential for practical applications. This simple method opens valuable opportunities for fast synthesis of the high-quality structured catalyst and could be extended to various noble metals on oxides of valve metals with high catalytic performance.
研究领域:
材料科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2016
·Vol. 6
·期 81
·77499-77506
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IF 3.289
Kai Zhang,Shubin Wu,He Yang,Huimin Yin,Gang Li
As promising and environmentally friendly catalysts, tungsten-containing heteropoly acids combined with supported noble metals were used for one-pot hydrothermal conversion of cellulose into polyols in the presence of pressurized hydrogen. The microcrystalline cellulose was completely converted over a mixed catalyst consisting of a low concentration of phosphotungstic acid (PTA) (0.03 wt%) and Ru/activated carbon (Ru/AC) via an one-pot hydrothermal reaction, with an ethylene glycol (EG) yield of up to 53.1% under optimal conditions. The catalytic activity of the mixed catalyst gradually decreased with increasing reaction runs, which could be mainly ascribed to the aggregation of Ru/AC particles, and to the coverage of the active sites of Ru due to the deposition of organic materials. Cellobiose was used as a model feedstock for a comparative study on the reaction pathways of the conversion of cellulose, and the results revealed that catalytic conversion of cellobiose consisted of at least three important parallel reactions under the present hydrothermal conditions, which were also most likely involved during the catalytic conversion of cellulose for EG production. Effective control of these reactions would be helpful to further maximize the EG yield during the catalytic conversion of cellulose.
研究领域:
化学工程
·
可再生资源转化
✓ 已验证
产品关联
DOI
高影响因子
Journal of CO2 Utilization
·
2019
·
IF 5.189
Shanshan Chai,Yong Men,Jinguo Wang,Shuang Liu,Qiaoling Song,Wei An,Gunther Kolb
Catalytic reduction of CO 2 to methane has been recognized as one of the most important strategic reactions to produce highly valuable chemicals and for storage of renewable energy (power-to-gas). This study demonstrates a crystal facet-dependent catalytic reduction of CO 2 to CH 4 on ruthenium nanoparticles deposited over TiO 2 nanocrystal with exposed (001) and (101) facets. Compared with TiO 2 (101) nanocrystal with the same Ru loading, Ru nanoparticles supported by TiO 2 (001) exhibited a highly enhanced CO 2 conversion rate and significantly improved methanation reactivity, along with a considerable durability. The physicochemical properties of the samples were characterized by HR-TEM, XRD, BET, FT-IR, UV–vis, Raman, ICP, and temperature-programmed reaction with CO 2 , and CO 2 + H 2 . In view of the difference in catalytic activity and the physicochemical properties of the supported Ru/TiO 2 catalysts, the results uncovered that the nature of the catalyst support of Ru/TiO 2 strongly affected the dispersion of Ru species and the synergistic effect between Ru and underlying TiO 2 supporting materials due to the strong metal-support interaction, and thus affected their capability to activate CO 2 and determined the catalytic activity for CO 2 methanation. Our work demonstrated the important role of the exposed crystal facets of the underlying support and the resulting Ru particle which had a large effect on CO 2 methanation.
研究领域:
催化化学
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材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
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