JOURNAL OF CATALYSIS
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2019
·
IF 7.723
Yu Xin,Lin Dong,Yong Guo,Xiaohui Liu,Yongfeng Hu,Yanqin Wang
Production of aromatic hydrocarbons through lignin hydrodeoxygenation (HDO) is of significant importance. Previously, we found that Ru/Nb 2 O 5 was an excellent catalyst for the conversion of lignin to arenes with relatively high selectivity (71%). Herein, we aim to clarify which properties of Nb 2 O 5 influence the activity and selectivity. Four Ru/Nb 2 O 5 catalysts with different Nb 2 O 5 morphologies were used in the HDO of 4-methylphenol. Intensive studies show that layered Nb 2 O 5 supported Ru has more Nb O groups (unsaturated NbOx sites) and highest Ru dispersion, which led to the highest activity and toluene selectivity, this was further confirmed by loading pre-synthesized Ru colloids in various Nb 2 O 5 . Finally, a Ru/Nb 2 O 5 catalyst with more unsaturated Nb O groups was designed and it was found that even with enzymatic lignin as the feedstock, the selectivity to arenes can reach up to 94.8% with the yield of hydrocarbons of 99.6%. This study provides a promising strategy for catalyst design towards the selective production of aromatic hydrocarbons from lignin.
研究领域:
催化化学
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可再生能源
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DOI
高影响因子
Frontiers in Chemistry
·
2022
·
IF 5.545
Gao Wenran,Wang Ke,Wu Yishuang,Zhu Xun,Wu Yinlong,Zhang Shoujun,Li Bin,Huang Yong,Zhang Shu,Zhang Hong
Doping of heteroatoms into carbon materials is a popular method to modify their physicochemical structures and has been widely used in the fields of energy conversion and storage. This study aims to investigate the effect of doping atmosphere on the catalytic performance of nitrogen and sulfur co-doped biochar supported Ru in the production of phenolic monomers from lignin hydrogenolysis. The results showed that the catalyst prepared under CO2 atmosphere (Ru@CNS-CO2) was able to produce phenolic monomers from corncob lignin with a yield up to 36.41 wt%, which was significantly higher than that from the run over N2-prepared catalyst (Ru@CNS-N2). The characterization of the catalysts demonstrated that the CNS-CO2 support had a larger specific surface area, richer C=S and C-S groups, and higher oxygen content than CNS-N2, resulting in finer Ru particles and more Ru0 content on the CNS-CO2 support. The Ru@CNS-CO2 catalyst exhibited high activity in hydrogenation and fragmentation of β-O-4 linkages.
研究领域:
催化化学
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能源材料科学
✓ 已验证
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Yuying Zhao,Jiahui Zhan,Rui Hu,Gang Luo,Jiajun Fan,James H. Clark,Shicheng Zhang
Extensive use of grey hydrogen in traditional hydrodeoxygenation (HDO) severely reduces the sustainable development of lignin valorization processes. Conversely, the catalytic transfer hydrogenation (CTH) mediated by green hydrogen is an alternative strategy that promotes the sustainability of in-situ hydrogenation of lignin. In this work, a bifunctional catalyst (Ru/NiAl 2 O 4 ) was developed to assist the proposed green hydrogen-driven cosolvent system composed of isopropanol and water for the CTH of guaiacol. Results indicate that 95% conversion of guaiacol and 80% cyclohexanol selectivity can be achieved at 200 ℃ within 3 h with a high water/isopropanol ratio (6/4), significantly increasing the greenness and sustainability. Furthermore, the recycling experiments verify the stability of the catalyst’s active sites. Analysis of the mechanism suggests that the high efficiency of such system can be attributed to the activation of metal and acid dual functional sites of Ru/NiAl 2 O 4 catalyst on aromatic rings and C-O bonds. The acceleration of the in-situ hydrogen supply is due to hydrogen exchange between water and isopropanol. The participation of water in the reaction is also demonstrated by the presence of deuterium in the product after the reaction in D 2 O. This work provided the insights into the development of a strategy for the production of cyclohexanol from lignin derivatives by an in-situ CTH system.
研究领域:
化学工程
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可再生能源
✓ 已验证
产品关联
DOI
高影响因子
Catalysis Science & Technology
·
2025
·
IF 4.2
Chuqiao Song,Wei Cheng,Xiaojie Wu,Shufang Zhao,Ying Tang,Xin Tang,Yao Xu,Lili Lin,Siyu Yao
The one-pot hydrodeoxygenation of lignin-derived (alkyl)-guaiacols to (alkyl)-cyclohexanols with high selectivity is an attractive process for biomass conversion. However, designing catalysts that preferentially cleave etheric CAr–O(R) bonds over hydrogenating aromatic rings under mild conditions remains a significant challenge. In this study, we explore the structure sensitivity of supported Ru catalysts with varying particle sizes (0.6–7.5 nm) and identify the optimal catalyst for selective hydrodeoxygenation. Using a catalyst with 1.5 nm Ru particles, we achieve a ∼95% yield of cyclohexanol from guaiacol under relatively mild conditions (190 °C, 5 bar H2). In situ DRIFTS analysis reveals that the cleavage of CAr–OCH3 bonds occurs preferentially over aromatic ring hydrogenation on the 1.5 nm Ru particles, minimizing side reactions and enhancing cyclohexanol selectivity.
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 & TECHNOLOGY
·
2010
·Vol. 33
·期 12
·2082-2088
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IF 1.266
F. Huang,W. Li,Q. Lu,X. Zhu
A homogeneous RuCl 2 (PPh 3 ) 3 catalyst was prepared for the hydrogenation of bio-oil to improve its stability and fuel quality. Experiments were first performed on three model aldehydes of acetaldehyde, furfural and vanillin selected to represent the linear aldehydes, oxygen heterocyclic aldehydes and aromatic aldehydes in bio-oil. The results demonstrated the high hydrogenation capability of this homogeneous catalyst under mild conditions (55–90 °C, 1.3–3.3 MPa). The highest conversion of the three model aldehydes was over 90 %. Furfural and acetaldehyde were singly converted to furfuryl alcohol and ethanol after hydrogenation, while vanillin was mainly converted to vanillin alcohol, together with a small amount of 2-methoxy-4-methylphenol and 2-methoxyphenol. Further experiments were conducted on a bio-oil fraction extracted by ethyl acetate and on the whole bio-oil at 70 °C and 3.3 MPa. Most of the aldehydes were transformed to the corresponding alcohols, and some ketones and compounds with C–C double bond were converted to more stable compounds.
研究领域:
化学工程
·
可再生能源
✓ 已验证
DOI
高影响因子
FUEL
·
2020
·
IF 5.578
Jing-Pei Cao,Tao Xie,Xiao-Yan Zhao,Chen Zhu,Wei Jiang,Ming Zhao,Yun-Peng Zhao,Xian-Yong Wei
Selective hydrogenolysis, the aromatic ether C-O bonds under mild conditions, is crucial for the valorization of lignin. In this context, the effects of H 2 and solvent on the hydrogenolysis of lignin model compounds over Ru catalysts were explored. With H 2 as hydrogen donor, the Ru/AC exhibited the highest activity for converting lignin model compounds into monomeric compounds, whereas H 2 led to low selectivity of aromatics. However, isopropanol was the good H-donor solvent, which could provide a large amount of active hydrogen to promote the cleavage of C-O bonds. Additionally, the yield of aromatics in isopropanol was higher than that under H 2 atmosphere. It could be ascribed to the fact that isopropanol is the protic solvent which displays Lewis basicity, and is a good H-bond donor and a good H-bond acceptor. The higher electron-releasing inductive effect of isopropanol made it easier to provide active hydrogen. Based on the experiments, the mechanism of benzyl phenyl ether hydrogenolysis in H 2 and isopropanol system was presented.
研究领域:
化学工程
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催化科学
✓ 已验证
DOI
高影响因子
ChemSusChem
·
2020
·Vol. 13
·期 21
·5683-5689
·
IF 7.962
Zhenbing Xie,Bingfeng Chen,Fangfang Peng,Mingyang Liu,Huizhen Liu,Guanying Yang,Buxing Han
Graphical A sustainable conversion : Developing highly efficient catalytic systems for amino acid productions from renewable bio-derived chemicals is very attractive for a sustainable future. N-doped carbon nanotube-supported Ru nanoparticles (Ru/N−CNTs) display excellent performance in the amination of bio-derived hydroxy acids into amino acids. The high-performance can be correlated with high dispersion of Ru nanoparticles and electronic effect resulting from the N-dopant. The amino acids have extensive applications, and their productions from biomass-derived feedstocks are very attractive. In this work, the synthesis of amino acids by amination of bio-derived hydroxy acids with ammonia over different metallic nano-catalysts supported on various supports is studied. It is found that Ru nano-catalysts on the nitrogen-doped carbon nanotubes (Ru/N−CNTs) have an outstanding performance for the reaction. Different hydroxy acids can be catalytically converted into the corresponding amino acids with yields up to 70.0 % under mild conditions, which is higher than those reported. The reasons for the high efficiency of the catalyst are investigated, and the reaction pathway is proposed on the basis of control experiments.
研究领域:
生物化学
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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
Journal of Energy Chemistry
·
2021
·
IF 9.676
Qiaojuan Wang,Yating Gao,Chantsalmaa Tumurbaatar,Tungalagtamir Bold,Fei Wei,Yihu Dai,Yanhui Yang
Carbonate-modified metal-support interfaces allow Ru/MnCO 3 catalyst to exhibit over 99% selectivity, great specific activity and long-term anti-CO poisoning stability in atmospheric CO 2 methanation. As a contrast, Ru/MnO catalyst with metal-oxide interfaces prefers reverse water–gas shift rather than methanation route, along with a remarkably lower activity and a less than 15% CH 4 selectivity. The carbonate-modified interfaces are found to stabilize the Ru species and activate CO 2 and H 2 molecules. Ru-CO* species are identified as the reaction intermediates steadily formed from CO 2 dissociation, which show moderate adsorption strength and high reactivity in further hydrogenation to CH 4 . Furthermore, carbonates of Ru/MnCO 3 are found to be consumed by hydrogenation to form CH 4 and replenished by exchange with CO 2 , which are in a dynamic equilibrium during the reaction. Modification with surface carbonates is proved as an efficient strategy to endow metal-support interfaces of Ru-based catalysts with unique catalytic functions for selective CO 2 hydrogenation.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF RARE EARTHS
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2019
·
IF 2.846
Wenfeng Han,Zhi Li,Huazhang Liu
La 2 Ce 2 O 7 nanoparticles were prepared by citric acid complexation method followed by calcination at varied temperatures. Then, supported with 4 wt% Ru, they were evaluated as the catalysts for ammonia synthesis under conditions similar with industry. With La 2 Ce 2 O 7 being calcinated at 700 or 800 °C, the experimental results indicate that the Ru/La 2 Ce 2 O 7 catalyst exhibits much higher ammonia concentration or ammonia synthesis rate than that of Ru/CeO 2 and Ru/La 2 O 3 . In addition, Ru/La 2 Ce 2 O 7 possesses high stability under over-heating test. In the absence of any promotor, ammonia concentration of Ru/La 2 Ce 2 O 7 catalyst approaches 14% at 450 °C, GHSV of 10000 h −1 and pressure of 10 MPa. The rate-determining step of ammonia synthesis, dissociation of N 2 is significantly facilitated by the strong metal–support interaction (SMSI) between Ru and La 2 Ce 2 O 7 . Due to the interaction, La 2 Ce 2 O 7 tends to donate electrons to Ru, resulting in the high electron density over the surface of Ru active sites which is favorable for the dissociation of N 2 . Consequently, high activity is achieved.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2024
·
IF 4.9
Haijiao Jia,Xiao Zhang,Guirong Borjihan,Shengbo Yang,Youxin Li
Using ruthenium chloride as catalyst precursor, magnetic silicon spheres as support, 4-formylphenylboronic acid and ethylenediaminepentaacetic acid as functional ligands, a magnetic heterogeneous nano-ruthenium catalyst (Fe 3 O 4 @SiO 2 -FPBA-DTPA-Ru) was prepared for the first time. It was nano level with 20.17 emu/g saturation magnetic strength and thermal stability under 249.63 °C. Fe 3 O 4 @SiO 2 -FPBA-DTPA-Ru contained 0.38 mmol/g Ru and was successfully used to catalyze the oxidation reactions of 15 aromatic secondary alcohols. Results proved that Fe 3 O 4 @SiO 2 -FPBA-DTPA-Ru as catalyst had good catalytic activity for the oxidation of secondary aromatic alcohols with yields exceeding 90 % for 12 products and 95 % for 10 products. High TON and TOF values (6386 and 9158 h −1 ) in 1-phenylethanol oxidation were obtained. All the reactions of aromatic alcohols were carried out in a solvent-free system, so the prepared catalyst had the characteristics of green and pollution-free. It was’nt suitable for oxidation of aromatic primary alcohols. If there was steric hindrance around the hydroxyl group in substrate, the catalysis also may be limited. The Fe 3 O 4 @SiO 2 -FPBA-DTPA-Ru catalyst also exhibited the advantages of energy saving, satisfactory reusability and stability in 9 consecutive runs. It showed great potential for future large-scale industrial production.
研究领域:
化学
·
材料科学
·
环境科学
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产品关联
DOI
高影响因子
RSC Advances
·
2019
·Vol. 9
·期 36
·20698-20705
·
IF 3.049
Shulai Liu,Bokai Yu,Zegao Wang,Jie Hu,Mingwen Fu,Yong Wang,Jianhua Liu,Zheng Guo,Xuebing Xu,Yuting Ding
Supported ruthenium (Ru) has the capacity to catalyze the conjugation of double bonds in linoleic acid (LA) into conjugated linoleic acids (CLAs). It has been reported that CLAs have shown a lot of benefits to human health. To enhance the selectivity of cottonseed oil (CSO) to CLAs, various Ru catalysts supported by multiwalled carbon nanotubes (Ru/MWCNTs) were prepared using a microwave-heated ethylene glycol method. All catalysts were characterized by transmission electron microscopy (TEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS) and inductively coupled plasma optical emission spectrometry (ICP-OES). The catalytic efficiency/selectivity of Ru/MWCNTs and two commercially available Ru catalysts (Ru/C and Ru/Al2O3) were investigated in a solvent-free system by catalyzing the isomerization of CSO. TEM analysis showed that Ru nanoparticles with average sizes of 1.0 nm to 1.8 nm were uniformly dispersed on the surface of the supports. Among the as-synthesized Ru/MWCNTs, catalyst S1 (diameter < 8 nm, length 0.5–2 μm) and catalyst S4 (diameter < 8 nm, length 10–30 μm) exhibit excellent catalytic performance for isomerization of CSO with high yield of total CLA (15.91% and 11.56%, respectively) and high turnover frequency (TOF) of 10.39 and 11.38 h−1, which is much better than two typical commercial Ru catalysts (Ru/Al2O3 and Ru/C). It has been revealed that the average particle size and chemical state of Ru on the surface of MWCNTs have influence on the activity and selectivity of the isomerization reaction.
研究领域:
食品科学
·
催化化学
·
营养学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Catalysis Science & Technology
·
2014
·Vol. 4
·期 5
·1286-1292
·
IF 4.76
Bing Liu,Ting Huang,Zehui Zhang,Zheng Wang,Yuhua Zhang,Jinlin Li
The present study reported the results on the water–gas shift (WGS) reaction over a series of Ru/C catalysts. It was found that the reduction method showed a remarkable effect on the catalytic activity of Ru/C catalysts over WGS reaction, which increased in an order of the reduction by NaBH4, ethylene glycol, H2. It has been shown that alkali additives with K2CO3 significantly improved the activity of the Ru/C catalysts. XPS results indicated that Ru species were further oxidized by the addition of K2CO3, which indicated an electron transfer from the alkali metal to the substrate, resulting in stronger bonding of the adsorbed gas. FTIR results showed that the absorption peak intensity of H2O and hydroxyl group increased with the increase of K2CO3 content, due to the strong hygroscopic ability of K2CO3. Through the addition of K2CO3 to the Ru/C catalyst, much more water was adsorbed around the catalytic active sites, reducing the strong adsorption of CO on the active sites. Thus the addition of K2CO3 balanced the concentration of water and CO on the active sites, which was considered to be the key step for low temperature WGS reaction over Ru supported on irreducible activated carbon.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子