Catalysis Science & Technology
·
2020
·Vol. 11
·期 5
·1914-1921
·
IF 5.721
Xiaoxiao Qin,Xueyan Chen,Min Chen,Jianghao Zhang,Hong He,Changbin Zhang
Formaldehyde (HCHO) elimination at low temperature is of great interest for indoor air purification. In this work, 1 wt% Ru supported on CeO2 and Al2O3 catalysts were prepared by an impregnation method and subsequently tested for the catalytic oxidation of HCHO at low temperature. The activity of the Ru/CeO2 catalyst was significantly superior to the Ru/Al2O3 catalyst, achieving complete conversion of 130 ppm HCHO at 90 °C with a GHSV of 100 000 mL gcat−1 h−1. Brunauer–Emmett–Teller (BET) measurements, X-ray powder diffraction (XRD), high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), X-ray photoelectron spectroscopy (XPS) and H2-temperature-programmed reduction (H2-TPR) were carried out to characterize the physical and chemical properties of the catalysts. The results revealed that RuOx species, rather than Ru0, were directly responsible for the HCHO oxidation over Ru/CeO2, and the excellent performance of Ru/CeO2 was mainly attributed to the strong interaction between Ru and CeO2, which induced a high dispersion and high redox capacity of RuOx species. The reaction mechanism of HCHO oxidation was also investigated using in situ diffuse reflectance infrared Fourier transform spectroscopy (in situ DRIFTS). It was shown that the HCHO oxidation over the Ru/CeO2 and Ru/Al2O3 catalysts followed the same pathway of the direct formate oxidation (HCHO → HCOO + OH → H2O + CO2).
研究领域:
环境科学
·
催化化学
✓ 已验证
DOI
高影响因子
CATALYSIS COMMUNICATIONS
·
2014
·
IF 3.32
Qian Han,Xingquan Xiong,Sizhong Li
An efficient, green and scale-up synthesis of amides from esters and amines has been developed using Ru-MACHO as a readily available catalyst. A diverse range of amides were obtained in moderate to excellent yields (55–98%). Furthermore, when the scale of the amidation reaction was increased to 240.0 mmol, the desired amide still could be obtained in high yield (48.2 g of N -benzylbenzamide, 95%).
研究领域:
有机化学
·
催化化学
✓ 已验证
DOI
高影响因子
Molecular Catalysis
·
2025
·
IF 4.9
Jiali Chen,Chen Huang,Yuqing Zhang,Liya Zhou,Li Ma,Lihui Wang,Yanjun Jiang,Yunting Liu
The conversion of racemic alcohols to enantiopure alcohols and amines is of significant importance yet presents considerable challenges. Herein, we achieved this goal by developing continuous-flow chemoenzymatic systems. In chemical module, a ruthenium (II)-N-heterocyclic carbene (Ru-NHC) catalyst immobilized on dendritic organosilica nanoparticle (DON) was prepared, which exhibited high activity and selectivity in the dehydrogenative oxidation of racemic alcohols to ketones. In enzymatic module, a ketoreductase and an amine dehydrogenase were individually co-immobilized with a cofactor-regenerating enzyme (glucose dehydrogenase) on DON for the enantioselective conversion of ketones to chiral alcohols and amines, respectively. The integration of the two modules in continuous-flow systems enabled the efficient chemoenzymatic deracemization and asymmetric amination of racemic alcohols (9 examples) with the maximum space-time yields of 6.8 and 5.8 g L -1 h -1 , respectively, underscoring the practical utility of the continuous-flow chemoenzymatic systems.
研究领域:
生物化学
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有机化学
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合成生物学
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产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Jin-Jian Pan,Jia Huang,Yuan-Hang Qin,Zhen Chen,Li Yang,Cun-Wen Wang,Xingmao Jiang
Ba-based perovskite oxides rich in oxygen vacancies (OVs) are anticipated to possess robust electron-donating capabilities and other favourable properties, rendering them a promising support for Ru catalysts in NH 3 synthesis. Herein, a glucose-urea deep eutectic solvent calcinating method was developed to synthesize an OV-rich BaTiO 3 (BTO-H) support for Ru catalysts. The BTO-H-supported Ru (Ru/BTO-H) catalyst achieves an impressive NH 3 synthesis rate of 5133 μmol g cat –1 h −1 (256.7 mmol g R u –1 h −1 ) at 400 °C and 0.1 MPa, surpassing the performance of Ru catalysts supported on OV-poor BTO supports and other supported Ru catalysts. Physical characterizations and kinetic experiments reveal the multifaceted influence of OVs on enhancing the catalytic performance of Ru/BTO-H in NH 3 synthesis. OVs serve as electron donors to Ru catalyst, facilitating the activation and dissociation of N 2 . Simultaneously, OVs act as hydrogen acceptors from the Ru surface, mitigating hydrogen poisoning effects. Additionally, OVs stimulate the formation of surface hydrides, not only providing active sites for N 2 activation but also bestowing an electron-donating effect on the supported Ru catalyst. The combined positive effects of OVs establish BTO-H as an outstanding support for Ru catalysts in NH 3 synthesis.
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
GREEN CHEMISTRY
·
2019
·Vol. 21
·期 15
·4152-4158
·
IF 9.405
Bernard Baffour Asare Bediako,Qingli Qian,Jingjing Zhang,Ying Wang,Xiaojun Shen,Jinbiao Shi,Meng Cui,Guanying Yang,Zhen Wang,Shengrui Tong,Buxing Han
Synthesis of ethanol from cheap and renewable CO2 is of great importance, but is still a challenge. Because it involves CO2 hydrogenation with simultaneous C–C bond formation, and the synergy of two or more transition metals is usually required for catalyzing the reaction effectively. Moreover, higher temperature is needed to drive the reaction. In this work, we found that the monometallic Ru3(CO)12 catalyst could efficiently catalyze the synthesis of ethanol from CO2, methanol and H2 in the ionic liquid, 1-butyl-3-methylimidazolium chloride ([bmim]Cl), using LiCl and LiI as promoters. Ethanol could form at 120 °C, which is among the lowest temperatures reported to date. A detailed study indicated that ionic liquids play an important role in monometallic catalysis. High ethanol selectivity and activity were obtained under optimized conditions. In addition, the catalyst could be easily recycled and the TON of ethanol reached 180 after five cycles. To our knowledge, this is the first time that an ionic liquid has been used as a reaction medium to produce ethanol using CO2 and H2.
研究领域:
化学
·
可再生资源利用
✓ 已验证
产品关联
DOI
高影响因子
Chemistry-An Asian Journal
·
2019
·Vol. 14
·期 16
·2815-2821
·
IF 3.698
Wei Li,Shuang Wang,Jinping Li
Graphical Be well supported ! Two BaCeO 3 supports with strong basic sites were synthesized by a co-precipitation route under different calcination temperatures. BaCeO 3 -a has a high basic density and Ru/BaCeO 3 -a has more oxygen vacancies, which are beneficial for the dissociation of N 2 . Therefore, the 1.25 % Ru/BaCeO 3 -a catalyst exhibits superior performance in ammonia synthesis (see figure). BaCeO 3 -a and BaCeO 3 -b, with strong basic sites, were synthesized by using a co-precipitation method at different calcination temperatures, and used as supports to evaluate their performance in ammonia synthesis. The ammonia synthesis rate with the 1.25 % Ru/BaCeO 3 -a catalyst is 24 mmol g −1 h −1 , which is higher than that of 1.25 % Ru/BaCeO 3 -b catalyst (18 mmol g −1 h −1 ) at 3 MPa and 450 °C. Moreover, the performance of the 4 % Cs-1.25 % Ru/BaCeO 3 -a catalyst was further improved to 28 mmol g −1 h −1 , and no sign of deactivation was observed after a reaction time of 120 h. The XPS and H 2 temperature-programmed reduction analyses indicated that the Ru/BaCeO 3 -a catalyst has more oxygen vacancies than the Ru/BaCeO 3 -b catalyst. In addition, the average Ru particle size of the Ru/BaCeO 3 -a catalyst is closer to 2 nm than the Ru/BaCeO 3 -b catalyst, which promotes the generation of B 5 -type sites (the active site for N 2 dissociation). The CO 2 temperature-programmed desorption analysis indicates that BaCeO 3 -a has a high basic density, which is beneficial for electron transfer to Ru and further facilitates the dissociation of N≡N bonds.
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
RSC Advances
·
2014
·Vol. 4
·期 94
·52402-52409
·
IF 3.708
Yong Liu,Lungang Chen,Tiejun Wang,Ying Xu,Qi Zhang,Longlong Ma,Yuhe Liao,Ning Shi
Non-edible cellulose has attracted considerable attention to be converted into valuable platform chemicals. Direct transformation of cellulose to C6 alditols (mannitol and sorbitol) provides a sustainable route. A productive approach is presented in this work using a Ru/C catalyst combined with H+-released boron phosphate in an aqueous phase. A yield of C6 alditols as high as 74.9% with a 91% conversion of cellulose is achieved. By adding silica–alumina materials, the yield of C6 alditols can be improved to 93.5% with complete conversion. The acid sites gradually released from boron phosphate under hydrothermal conditions could promote the hydrolysis of cellulose without significant degradation of glucose. Furthermore, the interaction of boric acid with C6 alditols may form borate–polyol complexes, which can enhance the stability of the C6 alditols to avoid further hydrogenolysis and dehydration of the C6 alditols formed. Due to the adsorption ability of the substrate, the addition of silica–alumina materials with a high content of silica leads to improved performance.
研究领域:
化学工程
·
可再生资源利用
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2017
·
IF 9.446
Fei Li,Yong Wang,Jian Du,Yong Zhu,Congying Xu,Licheng Sun
Water oxidation as a multi-electron transfer and endothermal reaction has been considered to be the bottleneck of solar-driven water splitting into oxygen and hydrogen. Herein, an alternative approach for solar energy conversion is developed by coupling H 2 generation with the selective oxidation of alcohol. In a closed redox system containing molecular ruthenium catalyst (RuCat) and Pt modified g-C 3 N 4 (Pt-g-C 3 N 4 ) composite, hydrogen production is concomitant with the oxidation of benzyl alcohols to aldehydes with over 99% selectivity in the presence of visible light and pure water. By contrary, the system lacking molecular catalyst only exhibits low to moderate selectivities towards aldehydes. The remarkably improved selectivity is attributed to the formation of highly active Ru(IV) = O intermediate through efficient hole transfer from g-C 3 N 4 to RuCat.
研究领域:
化学
·
能源科学
·
光催化
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产品关联
DOI
高影响因子
Catalysts
·
2017
·Vol. 7
·期 10
·311
·
IF 3.082
Xing Li,Haiyang Zhang,Baochang Man,Lijuan Hou,Chuanming Zhang,Hui Dai,Mingyuan Zhu,Bin Dai,Yanzhao Dong,Jinli Zhang
The Ru-based catalysts, including Ru/AC (activated carbon), TPAP (tetrapropylammonium perruthenate)/AC, TPAP/AC-HNO3, and TPAP/AC-HCl, were prepared and assessed for the direct synthesis of vinyl chloride monomer. The results indicate that the TPAP/AC-HCl catalyst exhibits the best performance with the conversion falling from 97% to 91% in 48 hours’ reaction under the conditions of 180 °C, a GHSV(C2H2) of 180 h−1, and the feed ratioVHCl/VC2H2of 1.15. The substitution of RuCl3precursor with high valent TPAP species leads to more ruthenium oxides active species in the catalysts; the acidification treatment of carrier in TPAP/AC catalyst can produce an enhanced interaction between the active species and the modified functional groups on the carrier, and it is beneficial to inhibit the carbon deposition and sintering of ruthenium species in the reaction process, greatly increase the adsorption ability of reactants, and further increase the amount of dominating active species in the catalysts, thus improving the catalytic performance. This also provides a promising strategy to explore high efficient and economic mercury-free catalysts for the hydrochlorination of acetylene.Keywords:tetrapropylammonium perruthenate;acetylene hydrochlorination;Ru catalysts
研究领域:
催化化学
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环境科学
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材料科学
✓ 已验证
DOI
高影响因子
INDUSTRIAL CROPS AND PRODUCTS
·
2024
·
IF 5.6
Wenwei Zhang,Tianjin Li,Xinping Ouyang,Xueqing Qiu
To cope with the challenge of insufficient interaction between lignin macromolecules and catalytic active sites in heterocatalysis systems which hindered the efficient hydrogenolysis of lignin, a lignin-derived N-doped macroporous carbon supported Ru catalyst (Ru/LNPC) was prepared via the pyrolysis of alkali lignin with potassium hydroxide as the activator and ammonium oxalate as the pore forming agent. The LNPC carrier featured a hierarchical porous structure with the diameter of macropores ranging from 50 nm to 10 μm, enhancing the adequately contact between the lignin macromolecules and Ru NPs. The doping nitrogen in the carbon carrier led to well dispersed Ru nanoparticles with average size of 1.08 nm, providing abundant active metallic centers. Therefore, Ru/LNPC exhibited excellent catalytic activity and stability to hydrogenolysis of lignin. Under the condition of 1.0 MPa H 2 at 280 ºC for 2 h, Ru/LNPC contributed to the yield of 45.6 % aromatic monomers from the depolymerization of lignin. After five recycling, Ru/LNPC still showed significant activity. This work provided a new strategy for designing catalysts for efficient hydrogenolysis of lignin and further facilitating its high-value utilization.
研究领域:
化学工程
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材料科学
·
可再生能源
✓ 已验证
产品关联
DOI
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
·
环境科学
✓ 已验证
DOI
高影响因子
BIORESOURCE TECHNOLOGY
·
2018
·
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
·
生物质转化
✓ 已验证
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）