Catalysis Science & Technology
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2024
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IF 4.4
Muhammad Faizan,Erum Aamir,Tiong Sieh Kiong,Hua Song
Vanadium phosphorus oxide (VPO) catalysts are synthesized for utilization of lighter alkanes such as n-butane to produce maleic anhydride (MA) by a selective oxidation process. Such a process has received huge global attention because of greater selectivity, eco-friendliness and being a less-expensive process as compared to the benzene oxidation process for the production of MA. Herein, we introduced for the first time 2-D MXene Ti3C2 (Mx) into VPO synthesis and prepared Ti3C2@VPO (MXene@VPO; Mx@VPO) nanocomposites via solvothermal and ball milling processes as a promoter and supporter at different (1–5) wt% for the evolution of n-butane selective oxidation. Among them, the solvothermal based promoted catalyst (5% Mx@VPO) exhibited large MA selectivity (up to 11%) as compared to the unpromoted catalyst. Simultaneously, it will decrease the COx selectivity (CO2 and CO). More importantly, the CO : CO2 ratio is reduced up to 1.5 from 2.01, which is beneficial for the environment and chemical plants. From various characterization techniques such as BET, XPS, SEM, TEM, XRD, FT-IR, NH3-TPD, H2-TPR, EDS, EPR, Raman, and TG/DTA we confirmed the role of MXene as a structure directing agent and electron promoting agent in VPO catalysis.
研究领域:
化学工程
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材料科学
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DOI
高影响因子
ENERGY & FUELS
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2020
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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
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DOI
高影响因子
PROCEEDINGS OF THE COMBUSTION INSTITUTE
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2026
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IF 4.6
Min Liu,Fanggang Zhang,Long Qin,Chung K. Law,Ran Sui
This work presents an experimental and mechanistic study on the catalytic partial oxidation (CPO) of n -butane for syngas production over a Rh/Al 2 O 3 catalyst. Experiments were conducted in a fixed-bed reactor under fuel-rich conditions (equivalence ratios φ = 1.5, 2.5 and 3.5) within a temperature range of 373–1073 K. The process initiates with total oxidation, seamlessly transitioning to partial oxidation and subsequently to steam/dry reforming regimes as temperature increases, with H 2 emerging as the first syngas product followed by CO and CH 4 . Based on the experimental observations, a reduced global reaction mechanism comprising eight irreversible, lumped steps was developed. Kinetic parameters were extracted from experimental data at φ = 1.5 and validated against independent datasets at φ = 2.5 and 3.5, with the model accurately capturing the major species trends. The Rh catalyst exhibits exceptional performance, achieving H 2 selectivity of 99.1% at φ = 3.5 and 873 K, surpassing reported values for methane and propane CPO systems. In addition, trace C 2-6 hydrocarbons were detected at φ = 3.5 and temperatures above 973 K, indicating the occurrence of hydrocarbon cracking under excessively fuel-rich and high-temperature conditions. XPS analysis further reveals a temperature-induced surface transition from oxidized Rh 3+ to metallic Rh 0 , which is associated with the high catalytic activity. These results provide mechanistic insight and useful kinetic parameters for modeling and optimizing Rh-catalyzed CPO of light hydrocarbons. Novelty and significance statement This work provides the first kinetic analysis and reaction mechanism for the catalytic partial oxidation (CPO) of n -butane over rhodium, addressing a significant gap in the literature, which has predominantly focused on methane and propane. The novelty lies in the elucidation of the unique two-stage reaction pathway for n -C 4 H 10 , beginning with total oxidation, sequentially transitioning through partial oxidation, and finally to reforming. A reduced reaction mechanism comprising eight lumped steps was developed, which successfully captured the species formation and the complex non-monotonic dependence on equivalence ratio and temperature. The significance of this research is that it delivers essential theoretical insights and a practical kinetic model for utilizing n -butane, a major component of LPG and NGL, in efficient syngas production. This directly advances the application of these fuels in solid-oxide fuel cell (SOFC) systems and distributed energy technologies, enhancing energy security and reducing emissions. Ultimately, this work provides guidance for the design and optimization of fuel-flexible catalytic reactors, contributing to the transition towards a more sustainable and diversified energy landscape.
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高影响因子
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
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DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2026
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IF 5.1
Yufeng Liu,Xiaofan Yang,Jinghua Hu,Junhao Liu,Peiwen Wu,Huifang Cheng,Huaming Li,Jixing Liu,Wenshuai Zhu
The hydroisomerization of isobutane is of considerable practical significance for the development of low-carbon and high-efficiency ethylene production technologies. However, conventional noble metal-solid superacid catalysts used for this reaction suffer from drawbacks including high cost and catalyst deactivation caused by the loss of halogen species and other active components. Herein, a series of highly dispersed W-Cu/Beta catalysts were designed and prepared via a facile ion-exchange method, and their catalytic performances toward isobutane hydroisomerization were systematically investigated. The results show that the introduction of WO x species effectively suppresses strong Brønsted acid sites of the Beta zeolite and modifies the Brønsted/Lewis acid balance of W-Cu/Beta catalysts. Although both Brønsted and Lewis acid site concentrations decrease with increasing W loading, Brønsted acidity is reduced to a greater extent, resulting in a lower Brønsted/Lewis acid site ratio. This acidity regulation is associated with suppression of undesired cracking reactions and improved selectivity toward n-butane. Under reaction conditions of 2 MPa, 380°C, and a weight hourly space velocity of 2.0 h ‒1 , the 5%W-Cu/Beta catalyst exhibits the best catalytic performance with isobutane conversion of 62.3% and n-butane yield of 32.4%. This enhanced catalytic behavior is attributed to optimized acidity and an appropriate distribution of catalytic active sites. Kinetic analyses indicate that WO x introduction alters the apparent kinetic behavior of the catalysts and is accompanied by an increase in apparent activation energy. The improved catalytic selectivity is correlated with changes in acidity distribution and suppression of cracking pathways rather than direct evidence of carbocation stabilization.
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高影响因子
Surfaces and Interfaces
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2021
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IF 4.837
Ikram Ullah,T.A. Taha,Asma M. Alenad,Ikram Uddin,Asif Hayat,Ashiq Hayat,Muhammad Sohail,Ahmad Irfan,Javid Khan,Arkom Palamanit
In this study, sulfated zirconia with loading of platinum (Pt) and platinum alumina (PA-Al 2 O 3 ) promoted sulfated zirconia (SZ) catalysts were synthesized by hydro-thermal route. The samples were characterized by XRD, BET, FT-IR, NH 3 -TPD, and TGA. The catalytic efficiency of all the synthesized catalysts was tested on the isomerization of n -butane. The results indicated that the conversion of n -butane (71.04%), selectivity to i -butane (98.96%), and yield of i -butane (70.30%) is significantly high for PA/SZ sample than that of Pt modified SZ and bare SZ. The results of this study suggest that the SZ modified by Pt/Al 2 O 3 (PA) provided better catalytic performance and higher stability (within 25 h of TOS), when compared with SZ, and Pt-modified SZ.
研究领域:
化学工程
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催化科学
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DOI
高影响因子
CATALYSIS LETTERS
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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
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DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2024
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IF 3.8
Xinxing Huang,Yong Xu
As one of the most significant chemicals in the industry, 1,3-butadiene has been widely used in various fields. Recently, butane dehydrogenation (BDH) has emerged as a new frontier for the production of 1,3-butadiene. However, this process is limited by the low selectivity to the desired product since BDH experiences a complicated dehydrogenation process and the products consist of various C1–C4 hydrocarbons. Here, we demonstrate that an In2O3-modified Pt-based catalyst can serve as an effective catalyst for the dehydrogenation of n-butane to 1,3-butadiene. The optimum catalyst exhibits n-butane conversion and 1,3-butadiene selectivity of 45.2 and 21.9%, respectively, at 575 °C. Further experimental results indicate that In2O3 can improve the dispersion of Pt, regulate acidity, and suppress n-butane dehydroisomerization (BDI).
研究领域:
催化化学
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工业化学
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高影响因子
CATALYSIS LETTERS
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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
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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
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材料科学
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产品关联
DOI
高影响因子
Green Energy & Environment
·
2022
·
IF 12.781
Muhammad Faizan,Yingwei Li,Xingsheng Wang,Piao Song,Ruirui Zhang,Ruixia Liu
Deep eutectic solvents (DESs) are now considered a new class of ionic liquid analogs that have been generously used in various fields. Herein, vanadium phosphorus oxide (VPO) catalysts are synthesized in combination with a deep eutectic solvent containing rare earth metal (rE-DES), and their catalytic performance in n-butane selective oxidation to produce maleic anhydride (MA) is evaluated. The rE-DES is produced from the interaction of choline chloride (ChCl) and rare earth metal salts (Cerium, Europium, Lanthanum, and Samarium metal salt) (ChCl:rE = 1:0.5–1:3) under mild conditions. It was found that DESs served as structural modifiers and electronic promoters during VPO synthesis. It regulated the chemical state of the catalyst surface, such as the vanadium valence state, acid-base properties, and ratios of V 4+ /V 5+ , Lat–O/Sur–O and P/V. Various characterization techniques, such as FT-IR, DSC, XRD, SEM, EDS, TEM, Raman, TGA, NH 3 -TPD, and XPS, were used to examine its physical and chemical characteristics. These characteristics were correlated with the catalytic performance. The VPO catalyst modified by rE-DES showed a significant enhancement of n-butane conversion and MA selectivity while suppressing the selectivity of CO and CO 2 as well as the CO/CO 2 ratio compared to the unpromoted VPO catalyst. Especially for Ce-DES-VPO, it increased the n-butane conversion and MA mass yield up to approximately 11% and 10%, respectively. In addition, we evaluated the catalytic performance under different activation atmospheres.
研究领域:
化学工程
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催化材料
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高影响因子
AICHE JOURNAL
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2026
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IF 4.4
Ali Raza Khan,Bingxu Chen,Zhongyao Zhang,Yao Shi,Wenyao Chen,Longqin Gu,Xinggui Zhou,Xuezhi Duan
Selective oxidation of n -butane to maleic anhydride (MA) is fundamentally limited by the activity-selectivity trade-off, and the origin of selectivity control remains debated. Here we show that surfactant-mediated modification of vanadium phosphorus oxide catalysts can shift the reaction network toward MA by suppressing competing carbon oxides (CO x ) formation. We establish a kinetic framework that explains this selectivity shift through coupled redox-site balance and product-branching kinetics. Kinetic analysis identifies the CO x to MA branching parameter (
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高影响因子
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