INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2020
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IF 3.573
Jun Jiang,Teng Li,Kexin Huang,Guangyu Sun,Jing Zheng,Jinlong Chen,Weiran Yang
As a bio-based platform chemical, it is desirable to convert levulinic acid (LA) to varieties of value-added biochemicals. n-Butane, mainly from nonrenewable fossil resources, is a basic chemical to produce some important chemicals, such as butadiene and ethylene. In this paper, 95.5% yield of n-butane was obtained from LA in one-step over base-treated Pt/C at around 300 °C in 4 h. The reaction pathway was confirmed to be the hydrodeoxygenation of LA to valeric acid (VA) and then the VA decarboxylation to n-butane by kinetic studies. Base-treated Pt/C had better reactivity due to its improved decarboxylation activity. Detailed characterization of the catalyst revealed that the Pt particle size is the key reason for the activity improvement, and further studies showed that Pt nanoparticles with a size of 2–4 nm showed the highest decarboxylation activity. This is the first report on the direct conversion of LA to n-butane.
研究领域:
化学工程
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可再生资源
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催化科学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2023
·
IF 4.7
Xia Zhang,Haibo Wang,Lianke Gou,Lanpeng Li,Aijun Duan,Zhengkai Cao
Serial VPO catalysts with different crystal structures were prepared by adjusting the ratios of air and N 2 in the calcination process. The precursors and vanadium phosphorus oxide (VPO) catalysts were characterized by various measurements. As the air and N 2 ratios were lower than 1:1, the ordered VOHPO 4 ·0.5H 2 O phase was mainly formed in the precursors during calcination. However, as the ratio of air to N 2 reached 3:1, amorphous VOPO 4 phases were formed over the surface of the precursor during calcination, which prevented the formation of ordered V5+ species over the surface of the VPO catalyst after activation. Meanwhile, a high proportion of VOHPO 4 ·0.5H 2 O in the precursor could facilitate more formation of the ordered α 1 -VOPO 4 phase over the surface of the VPO catalyst. Interestingly, the crystal structure over the surface of active VPO catalysts was totally different from the core of VPO catalysts. There were more P species and V species with 5+ existing over the surface of the VPO catalysts. The evaluation results of n-butane oxidation showed that when the ratio of air to N 2 was 1:3, the corresponding VPO-1A catalyst presented the highest conversion of n-butane and yield of the MA product (57.6 m% at 412 °C). The reason should be related to the fact that the VPO-1A catalyst possessed the highest acidity and proportions of surface V5+ species and Sur-O species. As the ratio of air to N 2 reached 3:1, the VPO-3A catalyst showed the poorest performance in the oxidation of n-butane, which could be due to the formation of inactive and amorphous VOPO 4 phases over the surface of the VPO catalyst. Finally, kinetic and thermodynamic models were established and calculated to investigate the characteristics of n-butane oxidation reactions for various VPO catalysts.
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
ENERGY & FUELS
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2020
·
IF 3.421
Wei Zhao,Shanshan Ruan,Siyu Qian,Beibei Feng,Chengcheng Ao,Lei Wang,Fuyi Liu,Lidong Zhang
Catalytic combustion has become a promising technology to address the accelerating volatile organic compounds (VOCs) emissions. In this work, cobalt modified ZSM-5 zeolite catalysts (3–18 wt % Co) were prepared to investigate the combustion of n-butane (one typical model component of VOCs). The performances of catalysts were evaluated by conducting experiments in a flow tube reactor. XRD, BET, FT-IR, and XPS were also utilized to characterize their physicochemical properties. A significant enhancement of the catalytic activity was demonstrated in terms of the cobalt supported over ZSM-5, with an optimal cobalt loading of 7 wt %. The excellent catalytic activity of 7 wt % Co-ZSM-5 is mainly attributed to a higher concentration of active surface Co3+ species. Furthermore, DFT calculations indicated that the role of Co can enhance the activity by decreasing the activation barriers for C–H bond cleavage. In addition, the primary reaction mechanism of n-butane combustion on Co-ZSM-5 was also revealed.
研究领域:
环境科学
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催化化学
✓ 已验证
DOI
高影响因子
CATALYSIS LETTERS
·
2022
·Vol. 153
·期 1
·271-284
·
IF 2.936
Faizan Muhammad,Zhang Ruirui,Liu Ruixia
Recently, global warming is proving to be an increasing challenge for the sustainable human survival on planet earth. Worldwide, researchers are putting their efforts into controlling carbon emissions and have set the aim to achieve levels of overall carbon neutrality. Different industrial processes, especially oil refinery processes, release large amounts of low-carbon alkanes as gaseous byproducts directly into the air and pollute clean environments, which is one of the major reasons for sudden climate changes, ocean acidification, loss of biodiversity, and rising sea levels. The conversion of lighter alkanes, especially n-butane, into value-added chemicals can be beneficial for green economies and green environments. Presently, heterogeneous vanadium phosphorus oxide catalysts (VPOs) are considered potential candidates for n-butane selective oxidation toward maleic anhydride (MA). In this research, we developed a VPO catalyst with the assistance of copper-based ionic liquids (Cu-ILs), including [Bmim][OAc]–[Cu(OAc) 2 ], [Bmim][Cl]–[CuCl], and [Bmim][Cl]–[CuCl 2 ]. We observed significant improvement in the MA selectivity; meanwhile, the CO x (CO and CO 2 ) selectivity was decreased. Compared to the unpromoted catalyst (Blank-VPO), the Cu-IL-promoted catalyst, i.e., [Bmim][Cl]–[CuCl 2 ]-VPO remarkably increased the MA selectivity (11%) and n-butane conversion (9.2%) and minimized the CO x selectivity (11%). In addition to this the ratio of CO/CO 2 has been reduced from 2.01 to 1.32. Therefore, this can be a helpful process for achieving carbon neutrality goals. Graphical Abstract
研究领域:
化学工程
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环境科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
CATALYSIS LETTERS
·
2022
·Vol. 153
·期 10
·3074-3091
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IF 2.936
Faizan Muhammad,Saeed Aamir,Song Piao,Zhang Ruirui,Liu Ruixia,Chang Zhi,Wu Liuzhu,Zhang Manyuan
Vanadium phosphorous oxide (VPO) catalysts have been recognized as heterogeneous catalyst for selective oxidation of low-carbon alkanes i.e., n -butane toward maleic anhydride. This process has widely gained attention globally due to its highly selective and cost-effective process. Herein, we employed Cd 0 . 2 Zn 0 . 8 S as a support for the VPO catalyst and evaluated its n -butane catalytic performance. Compared to the unpromoted catalyst (Blank-VPO), a higher n -butane conversion and MA yield were successfully obtained from the promoted catalyst (Cd 0 . 2 Zn 0 . 8 S@VPO). Interestingly, it reduces the byproducts, i.e., CO 2 and CO emission. Characterization methods such as TGA, XRD, EDS, SEM, FTIR, NH 3 -TPD, XPS, TEM, and Raman spectroscopy were used to characterize the Cd 0 . 2 Zn 0 . 8 S, VPO precursor and catalyst. Graphical Abstract
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
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
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2022
·
IF 6.76
Muhammad Faizan,Hao Li,Yumei Liu,Kexin Li,Shuang Wei,Ruirui Zhang,Ruixia Liu
Currently, deep eutectic solvents (DESs), as an exclusive class of ionic liquid analogs, are extensively employed in various fields. Herein, vanadium phosphorus oxide (VPO) catalysts assisted by copper-based deep eutectic solvent (Cu-DES) as an electronic promoter and structure directing agent were ingeniously synthesized and exploited in the selective oxidation of n-butane to maleic anhydride (MA). The DES is efficient, cost effective and highly green compared to conventionally use metal inorganic modifiers. Cu-DES was prepared from a eutectic mixture of an organic salt (ChCl) and a metal salt hydrate/metal salt of cupric (Cu(NO 3 ) 2 .3H 2 O, CuCl 2 ) and cuprous (CuCl) salt with a molar ratio of 1:1–1:3, which notably improved the catalytic performance compared to that of an unpromoted VPO catalyst. The MA selectivity and n-butane conversion of Cu–DES–VPO increased significantly, while the CO x (CO and CO 2 ) selectivity decreased. FTIR, DSC , XRD, SEM, EDS, TEM, Raman, TGA, XPS, and NH 3 -TPD characterization techniques were utilized to fully analyze the DES, precursor and catalyst to explore MA selectivity. This work shifts the significant increase of 13% n-butane conversion, 11% MA selectivity and 16% MA mass yield, which greatly influences low carbon alkane utilization. Importantly, the CO: CO 2 ratio is reduced from 2.02 to 1.62, which is more beneficial for chemical plants as well as green environments.
研究领域:
化学工程
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2021
·
IF 5.455
Linjie Guan,Chengming Huang,Dingmei Han,Linhua Zhu,Yi Mei,Dedong He,Yun Zu
Three zeolites ZSM-5, ZSM-35 and ZSM-22 are applied in n -butane cracking to reveal the influence of regional differences in Brønsted acid sites on reaction pathways. The Brønsted acid sites located in the channels of ZSM-5 exhibit a higher catalytic activity and yields to light olefins (especially the ethylene), which can be attributed to more relative contribution of bimolecular pathway. In comparison, more Brønsted acid sites are situated on the external surface or micropore mouths of ZSM-35 and ZSM-22, which are beneficial to propylene production. Note-worthily, almost no propane production on the two zeolites implies the predomination of monomolecular pathway. In situ FTIR technique further discloses that the difference in the reaction pathways is tailored by adsorption configurations of n -butane at two types of Brønsted acid sites. Under comparable conditions, the ZSM-5 performs a relatively good catalytic stability through bimolecular pathway. Furthermore, the correlation between deactivation rate and light olefins reveals that the enhancement of propylene selectivity accelerates the deactivation of ZSM-35 and ZSM-22. While, promotion on the ethylene selectivity is a significant inducement for the deactivation of ZSM-5.
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
CHEMICAL ENGINEERING SCIENCE
·
2021
·
IF 4.311
Zenan Ni,Yuming Li,Yaoyuan Zhang,Yajun Wang,Guoqing Cui,Guiyuan Jiang,Zhen Zhao,Chunming Xu
Ga species with high dehydrogenation capability were prepared by H 2 -O 2 atmosphere treatment, and efficient balance of bifunctionality (dehydrogenation/cracking) was realized between Ga species and ZSM-5 over Ga/ZSM-5 based catalysts. Compared with parent Ga/ZSM-5, the conversion rate of n -butane was increased from 0.53 to 2.59 mmol·g −1 ·min −1 on Ga/ZSM-5 with H 2 -O 2 treatment. Kinetic analysis revealed that the apparent activation energy of n -butane catalytic cracking decreased largely from 141 to 47 kJ·mol −1 , which is attributed to the formation of new interaction between Ga species and ZSM-5 upon such an atmosphere treatment. It was also found Butane-O 2 treatment acted as a similar role with H 2 -O 2 treatment in enhancing the catalytic performance. On this basis, different Ga species were correlated with activity and kinetic data, and the effect of practical reaction atmosphere on Ga species was also investigated.
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
危险品化学品经营许可证（带存储）