ACS Catalysis
·
2017
·
IF 10.614
Guangyue Xu,Ying Zhang,Yao Fu,Qingxiang Guo
A catalytic system over Ru-HAP catalyst is established to hydrodeoxygenate various oils to long-chain alkanes in water, for potential large-scale renewable diesel production, which has the following advantages. (i) This system is versatile to different oil sources, including Jatropha oil, palm oil, waste cooking oil, and cooking waste. (ii) Ru-HAP is highly efficient at achieving full conversion from stearic acid to alkanes at as low as 100 °C, and the isolated yield from Jatropha oil, palm oil, and waste cooking oil to long-chain alkanes reached up to 95, 96, and 87 mol % at 180 °C and 2 MPa H2 within 4–4.5 h, respectively. (iii) The catalyst showed high stability during five runs of recycling, ICP-OES analysis, and a hydrothermal treatment. The activity decreased less than 5% after the catalyst was treated in water at 200 °C for 24 h with a stirring speed of 1000 rpm due to the strong metal and hydrothermally stable support interaction. (iv) Ru-HAP is compatible with most impurities such as various salts, sugars, and macromolecules. (v) The system required low cost for operation since no dehydration before the reaction was necessary and the alkane product can be easily separated from water. The reaction route was investigated and indicated that the coexisting hydrodehydration and hydrodecarbonylation are affected by water, temperature, and H2 pressure. The catalyst was also characterized in detail, and its high reactivity and stability may result from the fact that highly distributed Ru nanoclusters anchored on the HAP support absorbed fatty acids by forming a metastable calcium carboxyl phosphate.
研究领域:
催化化学
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可再生能源
✓ 已验证
DOI
高影响因子
Chem
·
2021
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IF 22.804
Lingling Li,Ya-Fei Jiang,Tianhua Zhang,Hongfang Cai,Yanliang Zhou,Bingyu Lin,Xingyi Lin,Ying Zheng,Lirong Zheng,Xiuyun Wang,Cong-Qiao Xu,Chak-tong Au,Lilong Jiang,Jun Li
Summary Ammonia synthesis is structure sensitive, and a minute change in the catalyst structure would cause a dramatic change in activity. To date, none of the studies reveal the metal size effect at a subnanometer scale on NH 3 synthesis, and such investigation remains a challenge. Here, we report the synthesis of Ru catalysts with sizes ranging from single atoms, atomic clusters (ACCs), sub-nanometric clusters, to nanoparticles (NPs) by adjusting precursor and/or loading of Ru. Sub-nanometric Ru catalysts not only exhibit performance different from that of NPs but also follow a different route for N 2 activation. The strong intra-cluster interaction of Ru atomic clusters enables the formation of strong interactions of Ru d -orbitals with the σ and π orbitals of N 2 molecules, resulting in N 2 activation over Ru ACCs to occur more easily than that over Ru NPs. Consequently, Ru ACCs display an unprecedentedly high NH 3 synthesis rate and large turnover frequency at mild conditions.
研究领域:
催化化学
·
材料科学
✓ 已验证
DOI
高影响因子
JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
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2020
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IF 4.192
Xiao-Jian Zhang,Hai-Wei Li,Wang Bin,Bao-Juan Dou,De-Shui Chen,Xin-Ping Cheng,Mian Li,Hong-Yan Wang,Kai-Qian Chen,Li-Qun Jin,Zhi-Qiang Liu,Yu-Guo Zheng
Sugar alcohols are the prominent alternatives of sugars in food, medical, and health industries. The ruthenium supported on multiwalled carbon nanotubes (Ru/MWCNTs) catalysts were prepared based on the Ru valence regulation strategy and applied for selective sugar hydrogenation to prepare various sugar alcohols including xylitol, arabinitol, sorbitol, mannitol, and galactitol for the first time, with high selectivity (>99.0%) and yield (>98.0%) under mild conditions (≤110 °C, 3.0 MPa H2 pressure). The hydrogenation reaction of xylose was further optimized and under mild conditions (100 °C, 3.0 MPa H2 pressure, and 500 rpm), which were lower than ever reported for high efficient synthesis of xylitol, 99.8% xylose conversion and 99.0% xylitol yield were achieved after 120 min of reaction.
研究领域:
食品科学
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化学工程
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Sustainable Chemistry & Engineering
·
2018
·
IF 6.14
Guangce Jiang,Yinghui Hu,Guoqiang Xu,Xindong Mu,Huizhou Liu
Hydrodeoxygenation of phenolic components in pyrolysis bio-oil is considered to be a potential strategy for producing renewable aromatic chemicals. The key issue of this process is the establishment of an effective catalytic system that can cleave the CAr–O bonds without affecting the aromatic structure. To achieve this goal, an efficient heterogeneous catalyst with solid acid support (WOx/ZrO2) and active metal (Ru) was prepared in this study. The Ru–WOx/ZrO2 catalyst can effectively convert model phenolic compounds into aromatic hydrocarbons. For a mixed phenolic sample, the conversion to and selectivity for arenes were all around 90%. The good selectivity was proved to be strongly related to the surface adsorption and acid properties of the catalyst as well as the reaction pathway. Moreover, the hydrodeoxygenation of a pretreated bio-oil was also conducted and presented a satisfactory yield of arenes at 240 °C with 1 MPa of H2 reacted for 5 h. The depolymerization of high-molecular-weight phenolic oligomers was found to be significant during the catalytic process, which further enhanced the yield of aromatic monomers.
研究领域:
能源化学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
ChemCatChem
·
2017
·Vol. 9
·期 19
·3646-3654
·
IF 4.803
Bin Zhang,Qifan Wu,Chao Zhang,Xinluona Su,Ruhui Shi,Weiwei Lin,Yan Li,Fengyu Zhao
Graphical Stability from the support : The excellent stability of a Ru/ZSM-5 catalyst for levulinic acid hydrogenation in water relies on the higher tetrahedral-coordinated Al content and preferable pore connectivity in well-crystallized ZSM-5 zeolite, which suppress Ru aggregation and leaching and the formation of carbonaceous residues in the acidic environment. A long-life topic in the field of heterogeneous catalysis has been to develop supported catalysts that are stable against the aggregation of active metal and carbon deposition. Herein, we report a highly stable Ru/ZSM-5 catalyst for the hydrogenation of levulinic acid in water, which can be recycled at least 10 times without apparent loss of activity (conv. >95 %, yield >85 %). The influences of types of Al species, structure of support, Ru sizes, Ru leaching, and carbon deposition, etc. on activity and stability were discussed in detail. It was confirmed that the tetrahedral-coordinated framework Al in ZSM-5 contributed to the favorable metal–support interaction, and thus suppressed the aggregation and leaching of ruthenium during recycling. Besides, the suitable pore volume and channel network connectivity successfully prevent from deposition of carbonaceous residues.
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2023
·
IF 7.4
Licheng Liang,Linyan Bian,Yanping Fan,Shuyan Guan,Xianyun Liu,Qunying Sun,Baozhong Liu
The research and development of efficient catalysts is very important for the sustainable utilization of hydrogen energy. Herein, we designed the Ru/Ti 3 C 2−x N x catalysts using N -doped two-dimensional material MXene (Ti 3 C 2−x N x ) as support toward hydrogen generation from ammonia borane (AB) hydrolysis. Due to the confinement and anchoring effects of Ti 3 C 2−x N x , the as-prepared Ru/Ti 3 C 2−x N x catalysts show an ultrafine particle size of 1.55 nm and remarkable AB hydrolysis activity with high turnover frequency (TOF) value of 1334 min −1 and r B value of 297 × 10 3 mL·min −1 ·g Ru −1 at 298 K. XPS results show that the doped N atoms in Ti 3 C 2−x N x support provide electron-feeding effect for Ru in the reaction to form electron-rich Ru. The isotope experiments confirm that the dissociation of H 2 O is the rate-determining step (RDS) in AB hydrolysis reaction catalyzed by Ru/Ti 3 C 2−x N x . According to the density functional theory (DFT) calculations, the N atoms introduced into Ti 3 C 2−x N x decrease the dissociation energy of O–H bond in H 2 O molecules, accelerating the desorption of H* from Ti 3 C 2−x N x surface. This research provides a strategy to enhance synergistic interaction between support and metal through N -doping, so as to effectively improve the catalytic performance of heterogeneous catalysts.
研究领域:
催化化学
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材料科学
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能源化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2023
·
IF 8.4
Yingqiao Zhou,Yining Liang,Xiaoning Liu,Xinhua Qi
As one of the important value-added chemicals that has wide applications, the catalytic hydrogenation of glucose to sorbitol has been a hot topic in biomass upgrading. In order to support the prosperity of the sorbitol industry, catalysts with superior activity, higher selectivity, longer life, and lower cost are desirable. Herein, tremelliform graphene-like carbon-encapsulated Ru catalysts (Ru/GLC) were synthesized from 4-nitrocatechol by using solvent evaporation-induced self-assembly and KHCO3 chemical activation processes. The Ru/GLC materials were used for the catalytic hydrogenation of glucose to sorbitol, and the best Ru/GLC-600 sample prepared at a 600 °C activation temperature exhibited both high glucose conversion of 100% and sorbitol yield of 96.8% at 140 °C and 3 MPa H2 in 120 min. The Ru/GLC-600 catalyst exhibited excellent stability and durability that sorbitol yield could be remained at 95.4% after recycling five runs. The catalyst was applicable to concentrated glucose solutions (50 wt %) with 95.6% sorbitol yield. Compared with previously reported catalysts, Ru/GLC catalyst had lower apparent activation energy (Ea = 30.66 kJ/mol) and higher turnover frequency (TOF = 1680.6 h–1). This work provides a simple one-pot synthesis strategy for graphene-like carbon materials for metal encapsulating, and the prepared materials exhibited high catalytic activity and stability for glucose hydrogenation to sorbitol.
研究领域:
化学工程
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催化材料科学
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2023
·
IF 7.2
Jiayao Chen,Yuan Gao,Wenwen Yang,Zhiwei Li,Kun Xiong
Designing highly active and durable catalysts is considered to be crucial for enhancing hydrogen evolution reaction (HER) from water electrolysis . Although some studies indicate that anatase TiO 2 is a promising candidate for electrolytic hydrogen evolution reaction, the influence of different crystalline phases of TiO 2 on the supported Ru catalysts for electrocatalytic HER performance is rarely systematically explored. Herein, a series of Ru/TiO 2 -X (X = R (Rutile), A (Anatase), and P25) catalysts were prepared to investigate the influence of the rutile and anatase phases of TiO 2 on the catalytic activity of Ru catalysts in HER. The findings demonstrate that the HER activity is much affected by the variation of the titania structure, when other factors are kept constant. The 15Ru/TiO 2 -R-H 2 has superior HER performance with a small overpotential of 63 mV to achieve a current density of 10 mA cm −2 in acidic electrolyte and 99 mV in alkaline electrolyte compared to 15Ru/TiO 2 -A-H 2 and 15Ru/TiO 2 -P25-H 2 . This might be attributed to the faster electron transfer and lower Fermi level caused by the oxygen vacancy (V O ) and strong metal-support interaction (SMSI), along with the exposure of active sites afforded by the highly dispersed ruthenium nanoparticles on the rutile TiO 2 . Our results indicate that the presence of rutile TiO 2 support alone is adequate to maintain Ru in its most active form and make it a more performing catalyst, compared to anatase titania and P25.
研究领域:
化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2024
·
IF 2.7
Tiantian Liu,Jing Li,Xiaorui Yan,Kairui Li,Wenhua Wang,Haisheng Wei
The availability of catalytic sites for contact with reactants is a key issue to improve the performance of a catalyst, where constructing hollow structured nanomaterials has been considered as an effective strategy. Here, an N-doped carbon supported Ru catalyst with an interior cavity was synthesized by etching a MOF-derived core–shell precursor, in which metal Ru can be highly dispersed in the porous shell. This catalyst shows 98.7% conversion and >99% selectivity towards p-chloroaniline in the hydrogenation of p-chloronitrobenzene, which is better than the corresponding supported catalyst. Moreover, it also displays excellent stability with 5 cycle runs and good substrate universality for the hydrogenation of extensive substituted nitroarenes. Various characterization techniques and control experiments reveal the advantage of the unique structure to promote the mass transport and adsorption of reactant molecules on Ru sites. This work provides a novel strategy to design an efficient Ru-based catalyst for chemoselective hydrogenation.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2024
·
IF 6.7
Ranlei Shao,Lu Zhang,Luyuan Wang,Jianmei Wang,Xingyu Zhang,Shiwang Han,Xingxing Cheng,Zhiqiang Wang
In this study, Ru catalysts supported on Ce-Al composite carriers were prepared using the precipitation-hydrothermal method, significantly enhancing ammonia decomposition efficiency. The test results show that the Ru/3Ce-Al catalyst, with a Ru loading of only 0.8 wt%, achieves a reaction rate of 14.17 mmol g cat −1 min −1 at 500 °C, and reaches a 95 % conversion rate at 525 °C. No decline in efficiency was observed after 48 h of durability testing, which significantly reduces the usage of Ru. The RuO 2 particle size in the samples was only 2–4 nm. Ce-Al composite increased the specific surface area and pore volume of the catalyst, facilitating the uniform distribution of Ru. Additionally, it increased the number of surface acidic sites and strengthened the metal-support interaction. The unique low redox potential and oxygen vacancies of CeO 2 allowed for faster electron transfer to the Ru surface. DFT calculations revealed that bridge site adsorption was more stable, with the rate-determining step of the ammonia decomposition reaction being the formation of N 2 . Ce-Al composite catalysts enhanced NH 3 adsorption strength and lowered the reaction energy barrier.
研究领域:
催化化学
·
材料科学
·
理论计算
✓ 已验证
产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2024
·
IF 2.7
Shufeng Lin,Zhonghua Sun,Zhenzhen Wang,Qiumin Zhou,Anwei Wang,zhong wu,Junfeng Qian,Ming-Yang He,Qun Chen
Bisphenol A (BPA) is ubiquitous in industrial production and daily life. However, BPA is harmful to the health of fetuses and children due to its potential endocrine-disrupting effects. Hydrogenated bisphenol A (HBPA), an alicyclic diol generated from hydrogenating the double bonds of two benzene rings in the BPA molecule, is supposed to be a perfect substitute for BPA due to its stability and non-toxicity. Nevertheless, the rational design of high-performance catalysts for selectively converting BPA into HBPA remains a significant challenge. In this work, highly dispersed Ru immobilized by Al2O3 modified with Ni promoter (Ru/Ni-Al2O3) have been constructed, enabling BPA selective hydrogenation to produce HBPA under mild conditions. The doping of Ni promoter around Ru active sites effectively regulated the selectivity of target reaction. Both characterization and experimental results validated that the Ni promoter manipulated the electronic state of Ru through strong electron interaction between Ni and Ru, and thus the catalytic performance. In addition, the catalytic performance was also dependent on other reaction parameters such as H2 pressure, reaction temperature, liquid hourly space velocity (LHSV), and hydrogen-oil volume ratio. The optimized Ru/0.1Ni-Al2O3 catalyst achieved a BPA conversion of 100% and an HBPA selectivity of 96.4% under optimal reaction conditions (6 MPa H2, 140 oC, 0.42 h-1 LHSV, and 1500:1 hydrogen-oil volume ratio).
研究领域:
催化化学
·
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
ORGANIC PROCESS RESEARCH & DEVELOPMENT
·
2014
·
IF 2.549
Liang Xu,Zhi-Hong Huang,Christian A. Sandoval,Lian-Quan Gu,Zhi-Shu Huang
A novel efficient asymmetric hydrogenation (AH) process was developed for the preparation of (R)-1-(3,5-bis(trifluoromethyl)phenyl)ethanol (3), using a catalyst Ru/(4R,5R)-(+)-4,5-bis(diphenylphosphinomethyl)-2,2-dimethyl-1,3-dioxoane-(R,R-Diop)-2R-(α-methylmethanamine)-4,7-dimethyl-1H-benzo[d]imidazole (R-D-Me-BIMAH) in toluene in the presence of potassium t-butoxide. Various hydrogenation parameters, such as ligand, solvent, and substrate-to-catalyst (S/C) ratio, were investigated. The hydrogenation was carried out for four times on a 5 kg scale at 30 atm and 25 °C with S/C of 20 000 with an enantiomeric excess of >89%.
研究领域:
有机化学
·
催化化学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）