Catalysts
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2019
·Vol. 9
·期 3
·218
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IF 3.444
Shaoxia Guo,Guilong Liu,Tong Han,Ziyang Zhang,Yuan Liu
Owing to the outstanding catalytic performance for higher alcohol synthesis, Ga-Co catalysts have attracted much attention. In view of their unsatisfactory stability and alcohol selectivity, herein, K-modulated Co nanoparticles trapped in La-Ga-O catalysts were prepared by the reduction of La1−xKxCo0.65Ga0.35O3perovskite precursor. Benefiting from the atomic dispersion of all the elements in the precursor, during the reduction of La1−xKxCo0.65Ga0.35O3, Co nanoparticles could be confined into the K-modified La-Ga-O composite oxides, and the confinement of La-Ga-O could improve the anti-sintering performance of Co nanoparticles. In addition, the addition of K modulated parts of La-Ga-O into La2O3, which ameliorated the anti-carbon deposition performance. Finally, the addition of K increased the dispersion of cobalt and provided more electron donors to metallic Co, resulting in a high activity and superior selectivity to higher alcohols. Benefiting from the above characteristics, the catalyst possesses excellent activity, good selectivity, and superior stability.Keywords:perovskite-type oxide (PTO);cobalt;gallium;potassium;higher alcohols;syngas
研究领域:
化学工程
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催化材料
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DOI
高影响因子
CATALYSIS LETTERS
·
2019
·Vol. 149
·期 6
·1651-1659
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IF 2.372
Bao Jingxian,Fan Yonghui,Zhang Shuyi,Zhong Liangshu,Wu Minghong,Sun Yuhan
Abstract An atomically economical green protocol for the hydrofunctionalization of olefins to higher aliphatic alcohols with 100% anti-Markovnikov regioselectivity was developed via visible-light photocatalytic coupling. This method employs cheap, readily available and abundant methanol as both the C1 feedstock and the hydrogen source under visible light irradiation over CdS photocatalyst. A wide scope of olefin substrates could be hydrofunctionalized successfully to the corresponding higher alcohols with high selectivity. Besides alcohol, acetone and acetonitrile can also couple with olefins to generate the corresponding hydrofunctionalization products, suggesting promising potential industrial application. Graphical Abstract Hydrofunctionalization of olefins to value-added chemicals with high selectivity was achieved via visible-light photocatalytic cross-coupling.
研究领域:
化学
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绿色化学
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光催化
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DOI
高影响因子
ACS Catalysis
·
2025
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IF 13.1
Guihua Yan,Paulina Pršlja,Gaofeng Chen,Jiahui Kang,Yongde Liu,Miguel A. Caro,Xi Chen,Xianhai Zeng,Bo Peng
Syngas conversion into higher alcohols represents a promising avenue for transforming coal or biomass into liquid fuels. However, the commercialization of this process has been hindered by the high cost, low activity, and inadequate C2+OH selectivity of the catalysts. Herein, we have developed Cu/Co carbon wood catalysts, offering a cost-effective and stable alternative with superior selectivity for catalytic conversion. The formation of Cu/Co nanoparticles was found, influenced by water-1,2-propylene glycol ratios in the solution, resulting in bidisperse nanoparticles. The Cu/Co-CW-W1P1 catalyst (the ratio between water and 1,2-propanediol is 0.5:0.5) exhibited a remarkable CO conversion rate of 74.8% and a selectivity of 58.7% for C2+OH, primarily comprising linear primary alcohols. This catalyst demonstrated enduring stability and selectivity under industrial conditions, maintaining its efficacy for up to 350 h of operation. We also employed density functional theory (DFT) to analyze selectivity, particularly focusing on the binding strength of CO, a crucial intermediate for subsequent reactions leading to the formation of alcohols. DFT identified the pathway of CHx and CO coupling, ultimately yielding C2H5OH. This computational understanding, coupled with the high performance of the Cu/Co-carbon wood catalyst, paves the way to develop catalytically selective materials tailored for higher alcohol production from a nature-based source.
研究领域:
化学工程
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催化材料科学
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DOI
高影响因子
FUEL PROCESSING TECHNOLOGY
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2022
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IF 8.129
Xiudong Zhu,Yunshan Shang,Jingyun Chen,Hui Wei,Deping Xu,Xiongchao Lin,Yonggang Wang
A series of lanthanum oxide modified Cu Co based catalysts for the direct conversion of syngas to higher alcohols were synthesized via the coprecipitation method. The influence of lanthanum on the textural properties and catalytic performance was investigated. It was found that lanthanum-modified Cu Co based catalysts possessed a novel nanosheet structure to form more oxygen vacancies . Compared with CuCo catalyst, the dissociative CO adsorption and associative CO adsorption capacities of La x CuCo catalysts were improved markedly, and formate and methoxy intermediates were more easily formed on the surface of La x CuCo catalysts, which is attributed to the proper synergy of the surface active sites (Cu 0 , Co 0 , and oxygen vacancies). In particular, the addition of lanthanum species reduced the thickness of the nanosheets and facilitated the high dispersion of La x CuCo after reaction by acting as isolation islands to restrain the aggregation and growth of crystal grain. The evaluation results showed that optimized La 0.3 CuCo catalyst exhibited the highest CO conversion of 25.4%, superior total alcohols selectivity of 61.4%, and C 2+ alcohols selectivity of 79.03% among the total alcohol products, and excellent stability.
研究领域:
催化化学
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材料科学
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DOI
高影响因子
Food Analytical Methods
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2017
·Vol. 10
·期 10
·3338-3349
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IF 2.038
Tang Zhong-Sheng,Zeng Xin-An,Brennan Charles S.,Xie Wei-Qi
Fusel oils (FOs) are higher alcohols (including propanol, isobutanol, isoamylol, and active amyl alcohol), which affect the aroma profiles and flavor profiles of wine. A novel method for determination of FOs in lychee wine was developed using headspace gas chromatography (HS-GC). Results showed that 12% standard curve (SC) can be used to determinate the FOs of low alcoholic beverages, yet 40% SC can be used for high alcoholic beverages (e.g., brandy). Optimization of the parameters of equilibrium temperature at 50 °C was maintained for 30 min. The stabilized gas-liquid phase ratio of 3:1 for further research had no significant differences with others, which is caused by the distribution coefficient of K ≫ 100. The addition of sodium chloride (NaCl) decreased the partition coefficient of FOs markedly, and an inverse situation was observed for the extraction of FOs saturating at 1.25 g NaCl in 5 mL LW. Relative standard deviations (RSD) of reproducibility tests were in the range of 1.03–4.91%. Meanwhile, the mean recoveries of low, middle, and high concentration levels were 100.94, 103.2, and 96.74%, respectively. HS-GC was a stabilized, concise, and efficient method compared with the International Organization of Vine and Wine (OIV) method of OIV-MA-BS-14. These findings provide a foundation to determine higher alcohols of alcoholic beverages.
研究领域:
食品科学
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分析化学
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DOI
高影响因子
ACTA PHYSICO-CHIMICA SINICA
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2017
·Vol. 33
·期 8
·1672-1680
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IF 0.767
LIAO Pei-Yi,ZHANG Chen,ZHANG Li-Jun,YANG Yan-Zhang,ZHONG Liang-Shu,GUO Xiao-Ya,WANG Hui,SUN Yu-Han
A series of Cu/Co/Mn/Al catalysts derived from hydrotalcite precursors with different Cu/Co molar ratios (0, 0.1, 0.5, 1.0, and 2.0) were prepared and used for the synthesis of higher alcohols from syngas. N2 physical adsorption desorption, inductively coupled plasma atomic
emission spectrometry (ICP-AES), X-ray diffraction (XRD), scanning electron microscopy (SEM), hydrogen temperature-programmed reduction (H2-TPR), thermogravimetry (TG), and high-resolution transmission electron microscopy (HRTEM) techniques were employed to investigate the physical
and chemical properties of the Cu/Co/Mn/Al catalysts. The results show that the optimum Cu content can increase specific surface area, improve reducibility, and form regular layered structure to provide more uniform distribution of active sites, thereby enhancing catalytic activity and alcohol
selectivity. When the Cu/Co molar ratio was 0.5, the yield of alcohol and the alcohol selectivity reached the maximum values of 0.071 g·g-1·h-1 and 35.9%, respectively.
研究领域:
催化化学
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材料科学
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DOI
高影响因子
Foods
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2024
·Vol. 13
·期 20
·3316
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IF 4.7
Xiaonian Cao,Yunfei Hou,Qingqing Liu,Qian Yang,Min Liu,Haixu Lin,Qingxi Ren,Jian Mao
The unique flavour contribution of higher alcohols in alcoholic beverages has received growing attention; however, there is a dearth of information on their in vivo metabolic kinetics. In this study, the composition and content of higher alcohols in different alcoholic beverages from ChineseBaijiuandLujiuwere studied via in vivo analysis using Bama pigs to elucidate the mechanisms for intoxication of alcohol in vitro and in drinkers. Direct injection combined with gas chromatography–mass spectrometry (GC-MS) were used to accurately quantify a total of 14 higher alcohols in five alcoholic beverages. Based on the external standard method, a total content of 289.37–938.33 mg/L was detected, mainly 1-butanol, 3-methyl-1-butanol, 1-hexanol, 2-methyl-1-propanol and 2-butanol. Then, headspace solid-phase microextraction (HS-SPME) and solid-phase extraction (SPE) combined with GC-MS analysis strategy, respectively, were adopted to continuously monitor the changes in the concentrations of ethanol and 11 higher alcohols in the blood within 24 h after gavage of different alcoholic beverages, and the key pharmacokinetic parameters were analysed. The peak concentration (Cmax) and area under curve (AUC) of blood higher alcohols were significantly lower than those of ethanol (p <0.05), accompanied by a later peak time (Tmax) and a larger apparent clearance rate (CL_F), and there were certain differences between the same higher alcohols in different alcoholic beverages and between different higher alcohols in the same alcoholic beverage. This work provides valuable insights into the metabolism of alcoholic beverages.
研究领域:
食品科学
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动物生理学
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代谢组学
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DOI
PubMed
高影响因子
RSC Advances
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2015
·Vol. 5
·期 72
·58804-58812
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IF 3.84
Ang Cao,Guilong Liu,Yizhi Yue,Lihong Zhang,Yuan Liu
A series of layered double hydroxides (LDHs) with different Cu/Co ratios were prepared according to the co-precipitation method and used as catalyst precursors for higher alcohol synthesis. The prepared samples were characterized by XRD, TPR, SEM, TEM and BET techniques. After calcination, the LDHs were transformed into a mixture of CuO, Co3O4, CuCo2O4 and alumina, and these oxides were mixed uniformly with sizes of several nanometers. For the sample with a ratio of Cu/Co = 1/2, the copper and cobalt species are mainly in the CuCo2O4 phase. In the reduction process, the superior mixed copper and cobalt species in nanoscale were reduced to Cu–Co alloy, which was confirmed by the XRD and TEM results. The prepared bimetallic catalysts showed high activity, good stability and very high selectivity to C2+ alcohols. With the best catalyst, CO conversion of 51.8%, selectivity to alcohols of 45.8% and 94.3 wt% of C2+OH in the total alcohols were obtained at 250 °C, 3 MPa and GHSV of 3900 mL (gcat h)−1.
研究领域:
材料科学
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催化化学
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DOI
高影响因子
Molecular Catalysis
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2024
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IF 3.9
Sihui He,Hao Qu,Jiadong Liu,Jian Sun,Yue Su,Ruijue Hu,Yulong Zhang,Haiquan Su
Higher alcohols synthesis (HAS) is an important branch of syngas conversion, and Mo 2 C-based catalyst is a promising system for this reaction. However, the CO conversion and alcohols selectivity of current Mo 2 C-based catalysts are still low, which hinders their industrial application. Here, a series of Mo 2 C with three-dimensional hierarchically porous (3DHP) structures were prepared via a hard template method and their catalytic performance in HAS was investigated. The CO conversion and higher alcohols proportion of the optimal 3DHP catalyst were increased from 5.1 % and 60.4 % to 17.6 % and 70.5 %, respectively, compared with that of bulk Mo 2 C under similar total alcohols selectivity. The enhancement of the catalytic performance could be related to the increased number of active sites and the synergistic effect between multivalent Mo species. Additionally, the optimal 3DHP catalyst demonstrated good stability over a period of 200 h. This study provides a potential application for 3DHP materials and an alternative for designing efficient Mo 2 C catalysts for the HAS reactions.
研究领域:
材料科学
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化学工程
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DOI
高影响因子
ACS Sustainable Chemistry & Engineering
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2021
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IF 8.198
Zhuang Zeng,Zhuoshi Li,Shaoxia Guo,Jing Lv,Shouying Huang,Yue Wang,Xinbin Ma
Higher alcohol synthesis (HAS) direct from syngas using Fe-based catalysts is quite promising, but there are still problems in the construction of intimate-contact and stable dual sites to obtain satisfactory higher alcohol selectivity and space time yield (STY). Herein, a series of Au–Fe2.2C catalysts derived from monodisperse Janus Au–Fe3O4 nanoparticles with different Fe/Au ratios were prepared. The optimal catalyst with a Fe/Au molar ratio of 11.6 achieved the most Janus nanoparticles and exhibited the highest STY toward higher alcohols of 0.195 g gcat–1 h–1 and excellent catalytic stability over 200 h. The superior performance of this catalyst was attributed to the unique Au–Fe2.2C Janus structure, which could enhance both CO insertion and CO dissociation as well as their synergistic effect. The correlation of the CO adsorption behavior and STY toward alcohols was established as well, indicating that the balance between CO nondissociated adsorption and CO dissociated adsorption played an important role in enhancing the alcohol formation. Moreover, the strong interaction between Au and iron species in Janus nanoparticles could facilitate the formation of ε′-Fe2.2C and benefit the stability of the catalyst. These results may provide new ideas for the design and fabrication of high-performance catalysts with dual sites for HAS.
研究领域:
催化化学
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材料科学
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DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
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2020
·
IF 5.006
Wanliang Yang,Meng Chen,Jiayuan Zhou,Yingnan Duan,Yinmin An,Mao Liu,Mengkui Tian
Porous carriers play an important role in the catalytic transformation of syngas into higher alcohols, which promises higher sustainability in C1 chemistry. In this work, a series of hierarchical hollow silica spheres (HHSS) supported Cu-Fe bimetal catalysts were successfully prepared through ultrasonic-assisted impregnation for higher alcohols synthesis from syngas. Structural characterization results indicate that the hierarchical hollow structure of HHSS support can be maintained and the Cu-Fe bimetallic nanoparticles are highly dispersed on HHSS surface. The catalytic performances of samples in the test of CO hydrogenation for higher alcohols synthesis were investigated. The results revealed that the conversion rate of CO and the selectivity of C 2+ OH alcohol increased first and then decreased with the decrease of the amount of Cu content in the Cu x Fe y @HHSS catalyst. The highest CO conversion, alcohol selectivity and STY ROH over Cu-Fe@HHSS catalyst are 65.1 %, 46.6 %, and 118.1 gkg −1 h −1 , respectively. It was found that a large number of CuFe 2 O 4 were formed in Cu-Fe@HHSS catalyst and also confirmed that the CuFe 2 O 4 spinel and CuO-CuFe 2 O 4 were converted to Cu-Fe 5 C 2 composite in the spent Cu-Fe@HHSS catalyst, which can enhance the synergy between Cu-Fe bimetals. Furthermore, copper and iron are highly dispersed on HHSS after the reaction, which enhances the structural stability of the catalyst. Based on the development and utilization of low-cost catalysts and the production of clean liquid fuels, HHSS has a great prospect of catalyst support in the energy field.
研究领域:
催化化学
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能源化学
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材料科学
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产品关联
DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE
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2016
·Vol. 51
·期 11
·5216-5231
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IF 2.302
Cao Ang,Liu Guilong,Wang Lianfang,Liu Jingge,Yue Yizhi,Zhang Lihong,Liu Yuan
Abstract Nanostructured CuCo-LDH/CNT composites were successfully synthesized according to the co-precipitation method and firstly used for higher alcohol synthesis. The structural characterization and morphological observation demonstrated that CuCo-LDHs were in situ grown on the CNTs surface, and the CNTs support favored the dispersion of LDHs; meanwhile, a mechanism for growing the LDHs on CNTs was proposed, and the reported methods could be expanded to prepare other LDHs/CNT composites. After reduction, due to the strong interaction between CuCo-LDHs and CNTs, Cu–Co alloy, nanoparticles with small and uniform size were obtained and highly dispersed on the Al 2 O 3 matrix and CNTs surface. In particular, the high thermal conductivity of CNTs suppressed the formation of hot spots, thus effectively inhibited the generation of hydrocarbons and CO 2 . The resultant CuCo-LDHs/CNTs composite exhibited better catalytic performance and higher selectivity to C 2+ alcohols than the pristine LDHs did, which turned out to be one of the best catalysts for HAS. Graphical Abstract
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
危险品化学品经营许可证（带存储）