Catalysts
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2020
·Vol. 10
·期 11
·1304
·
IF 3.52
Qiang Yuan,Jifeng Pang,Wenguang Yu,Mingyuan Zheng
A high-performance Pt catalyst supported on SBA-15 was developed for furfural decarbonylation. Compared to Pt catalysts loaded on microporous DeAl-Hbeta zeolite and hierarchical micro-mesoporous MFI nanosheet (NS) materials, the 1%Pt/SBA-15 catalyst afforded notably higher activity, furan selectivity and stability owing to the negligible acid sites and proper mesopores on the SBA-15 support. Among a set of 1%Pt/SBA-15 catalysts bearing Pt nanoparticles (NPs) with sizes of 2.4–4.3 nm, the catalyst with 3.7 nm Pt NPs afforded the highest furan selectivity. Over the optimal catalyst, 88.6% furan selectivity and ca. 90% furfural conversion were obtained at 573 K and a high weight hourly space velocity (WHSV) of 16.5 h−1. Moreover, the reaction temperatures at 440–573 K and the ratios of H2to furfural at 0.79–9.44 did not affect the reaction selectivity notably, showing that the reaction over 1%Pt/SBA-15 can be conducted over a wide range of conditions. The catalyst was stable under the harsh reaction conditions and lasted for 90 h without significant deactivation, demonstrating the superior property of SBA-15 as a catalyst support for furfural decarbonylation.Keywords:decarbonylation;furfural;furan;platinum;SBA-15
研究领域:
催化化学
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能源化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ORGANIC CHEMISTRY
·
2022
·
IF 4.198
Tianhao Xu,Xingyu Zhou,Xiong Xiao,Yan Yuan,Long Liu,Tianzeng Huang,Chunya Li,Zhi Tang,Tieqiao Chen
A nickel-catalyzed decarbonylative thioetherification of carboxylic acids with thiols was developed. Under the reaction conditions, benzoic acids, cinnamic acids, and benzyl carboxylic acids coupled with various thiols including both aromatic and aliphatic ones produce the corresponding thioethers in up to 99% yields. Moreover, this reaction was applicable to the modification of bioactive molecules such as 3-methylflavone-8-carboxylic acid, probenecid, and flufenamic acid, and the synthesis of acaricide chlorbenside. These results well demonstrated the potential synthetic value of this new reaction in organic synthesis.
研究领域:
有机化学
·
合成化学
✓ 已验证
DOI
高影响因子
JOURNAL OF ORGANIC CHEMISTRY
·
2023
·
IF 3.6
Qi Dang,Jiani Chen,Tianbao Li,Long Liu,Tianzeng Huang,Chunya Li,Tieqiao Chen
A palladium-catalyzed decarbonylative annulation of 2-arylbenzoic acids with internal alkynes via C(sp2)–H activation has been developed. A series of phenanthrenes were produced in moderate to good yield with good functional group tolerance. The mechanism study indicated that the C(sp2)–H activation should be the rate-determining step during the reaction.
研究领域:
有机化学
·
催化化学
✓ 已验证
DOI
PubMed
高影响因子
Green Chemical Engineering
·
2025
·
IF 7.6
Jiankun Yu,Weixiao Sun,Kuan Huang,Jin Xu,Fuzeyu Zhong,Xiaohu Ge,Wenyao Chen,Gang Qian,Yueqiang Cao,Jianrong Zeng,Jianbo Ma,Xinggui Zhou,Xuezhi Duan,Jing Zhang,Lilong Jiang
Due to escalating carbon emissions, increasing attention is being focused on the synthesis of biomass-derived liquid fuels with a low CO 2 footprint. Currently, the dominant biobased liquid fuel in the diesel range is green diesel, produced via deoxygenation of non-edible natural/waste oils and their free fatty acid components into engine-compatible diesel-range alkanes. Industrially, sulfided NiMo or CoMo catalysts are typically used, leading to total hydrocarbon yields of 70-80 wt%. However, their inevitable sulfur leaching often contaminates the products and requires the addition of sulfur-containing agents. Here, we developed a highly selective sulfur-free Ni-Cu alloy catalyst by disentangling the electronic and size effects, to enable green diesel synthesis through the decarbonylation of palmitic acid—the most common fatty acid in these feedstocks. An unprecedented decarbonylation product (pentadecane) yield of 98% (on a molar basis) was achieved using a Ni-Cu alloy catalyst with a Ni/Cu ratio of 1:1 under mild reaction conditions (2 MPa H 2 , 250 °C). Minimal metal sintering or leaching was observed after multiple reuses. Kinetic studies show that incorporating Cu into Ni markedly reduces both the apparent activation energy and the reaction order for the conversion of palmitic acid. These results, combined with catalyst characterization, reveal that introducing Cu into Ni not only facilitates the adsorption and activation of the carboxylic hydroxyl group to promote the reductive deoxygenation of palmitic acid into aldehyde/alcohol intermediates—the slow step in decarbonylation—but also weakens the adsorption of C–C bonds on Ni by enhancing its electron density.
研究领域:
能源化学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
FUEL PROCESSING TECHNOLOGY
·
2022
·
IF 8.129
Hao Zhu,Fei Wang,Jianchun Jiang,Zeng Zhang,Yuchan Du,Junfeng Feng,Xiaoxiang Jiang
In order to deal with the deficiency of active sites in Ni catalyst, Ni Fe nanosheet (Ni-Fe/Al 2 O 3 -NS) catalyst was synthesized by using Ni-Fe-Al LDH as the precursor. The catalyst was further utilized in the lipid hydrotreatment for green diesel production. With a lamellar structure and large Ni loading (more than 60%), the Ni-Fe/Al 2 O 3 -NS catalyst possessed abundant Ni sties with high dispersion, large surface area, and strong acidity. Moreover, in Ni-Fe/Al 2 O 3 -NS the highly active Ni 3 Fe phase was formed, which promoted the decarbonylation route in hydrotreatment. The Ni-Fe/Al 2 O 3 -NS catalyst achieved 98.7% conversion with 98.1% alkane yield in oleic acid hydrotreatment under very mild conditions (220 °C, 2 MPa of hydrogen pressure, 3 h). The catalytic performance of Ni-Fe/Al 2 O 3 -NS was much higher than traditional Ni-Fe/Al 2 O 3 and other catalysts reported in current related studies.
研究领域:
催化化学
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能源材料科学
✓ 已验证
产品关联
DOI
高影响因子
GREEN CHEMISTRY
·
2015
·Vol. 17
·期 5
·2888-2895
·
IF 8.02
Jian-hua Guo,Guang-yue Xu,Fei Shen,Yao Fu,Ying Zhang,Qing-xiang Guo
The long-chain alkanes obtained from the hydrodeoxygenation of plant oils are ideal substitutes for diesel. In this work, a new efficient catalytic system was established for the conversion of plant oil to long-chain alkanes under mild conditions with a bi-functional Ru/La(OH)3 catalyst. The hydrodeoxygenation of stearic acid was performed in an autoclave with Ru-based catalysts with different supports (HZSM-5, ZSM-5, SiO2–Al2O3, SiO2, ZrO2, Mg(OH)2, La(OH)3, and La2O3). Among these catalysts, Ru supported on basic La(OH)3 showed a remarkable catalytic performance for the reaction. Over 98% of long-chain alkanes were obtained with 100% conversion of stearic acid at 200 °C and 4 MPa H2. When crude Jatropha oil was hydrogenated, about 80.7 wt% of long chain alkanes were obtained under the optimized conditions (200 °C, 4 MPa H2, 8 h). The high efficiency of the Ru/La(OH)3 catalyst could be due to a co-effect of the high hydrogenation activity of Ru and the basic La(OH)3 support which can attract the acidic raw material. Additionally, the Ru/La(OH)3 catalyst was recycled four times and maintained a good activity and stability. The reaction pathway was also explored by using stearic acid as a model compound. Hydrogenation–decarbonylation could be the main pathway to produce n-heptadecane, which has one carbon atom less than stearic acid.
研究领域:
化学工程
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催化
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可再生能源
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生物燃料
✓ 已验证
产品关联
DOI
高影响因子
Green Energy & Environment
·
2023
·
IF 13.3
Lin Yuan,Yancheng Hu,Guangyi Li,Fengan Han,Aiqin Wang,Yu Cong,Tao Zhang,Feng Wang,Ning Li
The production of industrial chemicals with renewable biomass feedstock holds potential to aid the world in pursuing a carbon-neutral society. Trimellitic and trimesic acids are important commodity chemicals in industry that are prepared by the oxidation of petroleum-derived trimethylbenzene. To reduce the dependence on the limited oil source, we develop a potential sustainable alternative towards trimellitic and trimesic acids using biomass-based 2-methyl-2,4-pentandiol (MPD), acrylate and crotonaldehyde as starting materials. The process for trimellitic acid includes dehydration/D-A reaction of MPD and acrylate, flow aromatization over Pd/C catalyst, hydrolysis and catalytic aerobic oxidation (60% overall yield). The challenging regioselectivity issue of D-A reaction is tackled by a matched combination of temperature and deep eutectic solvent ChCl/HCO 2 H. Crotonaldehyde can also participate in the reaction, followed by Pd/C-catalyzed decarbonylation/dehydrogenation and oxidation to provide trimesic acid in 54% overall yield. Life cycle assessment implies that compared to conventional fossil process, our biomass-based routes present a potential in reducing carbon emissions.
研究领域:
生物化学
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绿色化学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF THE ENERGY INSTITUTE
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2024
·
IF 5.6
Haonan Shi,Sihao Shu,Zhongze Wang,Xing Zhang,Xiaoyu Gu,Jixiang Chen
Deoxygenation of fatty acid esters in aqueous phase using in-situ generated H 2 has emerged as a promising approach to producing sustainable diesel-like hydrocarbons. In this study, we employed a solvothermal method to synthesize novel Ni–Sn metal–organic frameworks (MOFs) with a homogeneous distribution of Ni and Sn elements. Subsequently, various Ni–Sn intermetallic compounds (IMCs) encapsulated with a porous carbon layer (<3 nm) (Ni–Sn IMC@C) were prepared through the facile pyrolysis of metal–organic frameworks under a controlled N 2 atmosphere. Applying methyl palmitate as model reactant and methanol as hydrogen donor, Ni 3 Sn 2 IMC@C gives approximately 100% conversion and 93% yield towards n-C 15 and n-C 16 alkanes at 330 °C, without significant deactivation during the recycling for five times. The deoxygenation pathway is dominated by decarbonylation (DeCO) on Ni–Sn IMCs. In Ni–Sn IMCs, the oxophilic nature of Sn, along with its charge transfer with Ni, enhances the adsorption of an η 2 (C, O)-aldehyde configuration. The strategic isolation of adjacent Ni by Sn effectively inhibits methanation and C–C bond hydrolysis, reducing H 2 consumption and increasing carbon yield. Moreover, the ultrathin porous carbon encapsulation not only prevents the loss and sintering of Ni 3 Sn 2 IMC under harsh hydrothermal condition but also mitigates mass transfer limitation. Surface oxidation of Ni 3 Sn 2 IMC, particularly the formation of SnO 2 , is detrimental to deoxygenation. Additionally, Ni 3 Sn 2 IMC@C exhibits high hydrocarbon yields (>89.6%) in in-situ aqueous phase deoxygenation of methyl laurate, methyl stearate and methyl oleate. These findings highlight the remarkable potential of MOF-derived catalysts for hydrothermal deoxygenation.
研究领域:
材料科学
·
催化
·
化学工程
·
可持续能源
✓ 已验证
产品关联
DOI
高影响因子
ChemSusChem
·
2025
·
IF 6.6
Zixuan Tan,Yihong Cai,Bo Yang,Hao Huang,Haijun Guo,Min Zhuang,Hui Luo,Qingwei Meng,Shaoqu Xie
Graphical Monohydric alcohols are a potential fuel, and herein, monohydric alcohols have been selectively synthesized from multicarbon sugars by modulating the electron distribution of Ru and enhancing the hydrodeoxygenation process of biomass. Ru-based catalysts are widely used in catalytic reactions, but the electron-deficient nature promotes strong decarbonylation, leading to complete deoxygenation during the conversion of polyhydroxy biomass. Despite extensive research, effectively suppressing this decarbonylation activity remains challenging. Herein, electron-rich Ru and electron-deficient Ni formed due to the electron migration of Ni → Ru have a synergistic catalytic effect, controlling the precise cleavage of C N bonds by Ru 0 and retaining most of the C O bonds. The amorphous Al 2 O 3 is sufficiently bound to the substrate to promote rapid hydrogenation. This modification effectively suppresses the intrinsic decarbonylation activity of Ru and improves selectivity for hydrodeoxygenation. Using carbohydrates as substrates, the Ru–Ni bimetallic catalysts preferentially promote the hydrodeoxygenation pathway, resulting in a significant increase in C3+ monohydric alcohol yields. This work presents a new strategy for modulating reaction pathways via electronic structure engineering, offering valuable insights into the potential of Ru–Ni systems for biomass conversion and sustainable alcohol synthesis.
研究领域:
催化化学
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材料科学
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化学工程
·
生物质转化
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可持续化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Yanxi Chen,Renli Yin,Lixi Zeng,Wanqian Guo,Mingshan Zhu
To investigate the effects of hydroxyl groups on the degradation of tetracycline antibiotics (TCs), three kinds of TCs [tetracycline (TC), oxytetracycline (OTC), and doxycycline (DTC)] were chosen as the target molecules and then degraded in the carbon black (CB)-activated peroxydisulfate (PDS) oxidation process . The degradation ratios of the TC, OTC, and DTC in the CB/PDS oxidation process reached 52%, 60%, and 87% within 40 min, respectively, with the degradation rate following the order of DTC > OTC > TC. According to the density functional theory calculations, these three TCs have different charge distributions, electrostatic potential distributions and average local ionization energy, which are caused by the distinct hydroxyl group position, thus contribute to the different degradation ratios and reaction rate constants. The hydrogenation of TC was slower special degradation pathway relative to those of OTC and DTC, while the decarbonylation of OTC was slower special degradation pathway relative to that of DTC, which adversely resulted in the degradation rate following the order of DTC > OTC > TC. This presentation gives a knowledge that the position and numbers of hydroxyl groups are pivotal to the degradation efficiency toward TCs.
研究领域:
环境化学
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分析化学
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药学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
·
2021
·
IF 5.541
Fangqi Wang,Fengwen Yu,Yi Wei,Ao Li,Shenzheng Xu,Xianghong Lu
Oleaginous biomass conversion to liquid hydrocarbon biofuels has emerged as an effective solution to the energy crisis and environmental problems. In this process, the removal of oxygenated compounds will directly affect the effectiveness of subsequent biofuel applications. Herein, deoxygenation of oleic acid by catalytic cracking was conducted using five various elements (La, Ni, P, Zr and Ce) modified Al-MCM-41. The related characterizations were carried out for these catalysts, including N 2 physisorption, XRD, XPS, pyridine-FTIR and NH 3 -TPD techniques. The results showed the mesoporous structure of Al-MCM-41 was maintained after different modifications, and these catalysts greatly improved the hydrocarbons content and physiochemical properties of biofuels. The modified catalysts tended to facilitate the decarbonylation pathway and showed high selectivity to alkane and aromatic hydrocarbons. Besides, La/Al-MCM-41 presented excellent anti-coking activity. Ni/Al-MCM-41 showed both high dehydrogenation and deoxygenation activities. The Zr modification and Ce modification had a promotion effect in the deoxidizing activity of the catalyst, owing to the formation of oxophilic metal oxides. Noteworthily, P/Al-MCM-41 displayed the best deoxidizing performance due to its high Brönsted acidity, which caused the highest hydrocarbons content (82.30 %) and the lowest fatty acids content (around 0 %) of the biofuel. Moreover, the resulting biofuel had not only low oxygen content (3.88 wt.%) and acid value (5.47 mgKOH g −1 ) but also a high calorific value (44.50 MJ kg −1 ), which could be processed into green diesel. Hence, the catalytic cracking of fatty acid over P/Al-MCM-41 has excellent potential to produce high-quality renewable fuels.
研究领域:
化学工程
·
可再生能源
·
催化
·
生物化学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）