JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
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2025
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IF 2.4
Shiyuan Wang,Fang Wang,Yalong Song,Zelin Ma,Jiulong Wang,Yazhou Shuang,Weihao Zhao,Jie Jian,Pengfei Guo,Hongqiang Wang
BACKGROUND Carbon dioxide-assisted propane dehydrogenation (CO 2 -ODP) is a promising advanced technology for propylene production. However, a significant challenge still remains in advancing the adsorption and activation of propane and CO 2 , as hydrogenolysis and oligomerization isomerization reactions severely constrain propylene production. RESULTS In this work, we introduce Ga as a second metal promoter into Pt/SiO 2 catalysts, effectively promoting the dispersion of active particles and significantly reducing their size, thereby enhancing their catalytic activity. Meanwhile, the impregnation of Ga also promotes the activation of CO 2 , ultimately accelerating the reverse gas–water shift reaction. CONCLUSION The propylene yield and CO 2 conversion of Pt–Ga 1 /SiO 2 catalyst increased up to 40.45% and 45.10%, respectively, which were 17.54 and 6.62 times higher than those of the pristine SiO 2 –Pt catalyst at weight hourly space velocity (WHSV) = 3.1 h −1 . Most notably, the C 3 H 6 selectivity of SiO 2 –Pt/Ga 1 catalyst remarkably achieved an impressive value of 99.04%, which was much higher than that of other bimetallic-based catalysts, thus providing valuable guidance for the rational development of bimetallic highly active CO 2 -ODP catalysts. © 2025 Society of Chemical Industry (SCI).
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
APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Chaokai Xu,Shengdong Tan,Yaxin Tang,Shibo Xi,Bingqing Yao,Austin Wade,Binbin Zhao,Shangchen Lu,Yankun Du,Mingjiao Tian,Chi He,Lu Ma,Xingjie Fu,Jiwei Shi,Jiong Lu,Alexander G.R. Howe,Sheng Dai,Guangfu Luo,Qian He
We investigated the industrially important PtSn/Al 2 O 3 catalysts prepared with uniform particle sizes (∼ 1 nm) and varied compositions using molecular complexes of Pt(II) and Sn(II). Our best catalyst, with a Sn:Pt ratio of around 2, exhibited a high initial propylene productivity of about 1.1 mol C 3 H 6 (g catalyst) −1 h −1 . Elaborate electron microscopy studies revealed significant compositional variations in the catalyst, highlighting the practical challenges in achieving or confirming the theoretically predicted optimum Sn:Pt ratio. It is also found that the catalytic activities correlate well with the Pt dispersion, suggesting the structure-insensitive nature of the dehydrogenation reaction applies to these ultrasmall Pt-Sn nanoparticles . The presence of Pt-rich particles in the catalysts did not produce noticeable degradations in the reaction selectivity, indicating a wide composition range for Pt-Sn nanoparticles to be effective at the 1 nm size range. These findings emphasize the importance of detailed analysis of compositional distributions for understanding and optimizing nanoalloys.
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
Nature Communications
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2023
·Vol. 14
·期 1
·1-12
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IF 16.6
Wang Xianhui,Pei Chunlei,Zhao Zhi-Jian,Chen Sai,Li Xinyu,Sun Jiachen,Song Hongbo,Sun Guodong,Wang Wei,Chang Xin,Zhang Xianhua,Gong Jinlong
Redox catalysts play a vital role in chemical looping oxidative dehydrogenation processes, which have recently been considered to be a promising prospect for propylene production. This work describes the coupling of surface acid catalysis and selective oxidation from lattice oxygen over MoO 3 -Fe 2 O 3 redox catalysts for promoted propylene production. Atomically dispersed Mo species over γ-Fe 2 O 3 introduce effective acid sites for the promotion of propane conversion. In addition, Mo could also regulate the lattice oxygen activity, which makes the oxygen species from the reduction of γ-Fe 2 O 3 to Fe 3 O 4 contribute to selectively oxidative dehydrogenation instead of over-oxidation in pristine γ-Fe 2 O 3 . The enhanced surface acidity, coupled with proper lattice oxygen activity, leads to a higher surface reaction rate and moderate oxygen diffusion rate. Consequently, this coupling strategy achieves a robust performance with 49% of propane conversion and 90% of propylene selectivity for at least 300 redox cycles and ultimately demonstrates a potential design strategy for more advanced redox catalysts.
研究领域:
化学工程
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催化科学
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PubMed
高影响因子
ACS Applied Nano Materials
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2023
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IF 5.9
Xiangyang Ji,Yue Ma,Xiao Sun,Shaojia Song,Kun Yang,Weixin Huang,Chunming Xu,Bohan Feng,Jian Liu,Weiyu Song
Propane direct dehydrogenation (PDH) has received much attention. How to effectively catalyze inert C–H bond activation is of great significance for industrial development. Pt-based catalysts show excellent activity but are limited by their expensive price. Cr-based catalysts are scarcely applied owing to their high toxicity. V-based catalysts are appropriate candidates for their cheap price and low toxicity, but they suffer from high energy consumption. The photothermal synergy effect induced by nonradiative relaxation is expected to make the C–H bond activation and hydrogen coupling process easier compared to bare thermal catalysis. Herein, a set of V/TiO2 nanoscale catalysts were synthesized. The optimized 3 wt % V/TiO2 catalyst (hereafter simplified as 3V) has a particle size of ∼26 nm, achieving a propylene production rate of 342 μmol·g–1·h–1 at 500 °C with UV–vis light radiation, which is 9.2% higher compared with bare thermal conditions. In situ radiation X-ray photoelectron spectroscopy (XPS) shows that photon injection leads to more electron-deficient V atoms (Vδ+, 5 > δ > 3). The strengthened Lewis acidity enhances the C3H8 activation as revealed by kinetic evidence and in situ C3H8-DRIFT measurements. The calculated molecular orbital diagrams show that the V atoms decrease the energy gap between the highest occupied orbital (HOMO) of C3H8 and the lowest unoccupied orbital (LUMO) of the model catalyst. This work describes an efficient photothermal synergy approach, specifically the nonthermal effect for promoting propane dehydrogenation.
研究领域:
化学工程
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催化
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材料科学
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高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2022
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IF 4.326
Wenhao Xu,Xiaofeng Gao,Xian Zhou,Yongkang Huang,Houhong Song,Siyu Yao
Prins condensation of methyl tert-butyl ether (MTBE) with formaldehyde (FA) is an important route for isoprene synthesis. Traditionally, the production capacity of isoprene in a liquid-phase batch reactor is significantly limited due to the high ratio of MTBE/FA and the addition of an excessive amount of solvent. In this study, we evaluated different acid catalysts aiming at enhancing the selectivity and recyclability of catalysts under the condition of stoichiometric MTBE/FA in a concentrated solution. A Brønsted sulfonic ionic liquid ([HSO3-bmin] PTS) showed remarkable performance. The study of the reaction network confirmed that 4,4-dimethyl-1,3-dioxane (DMD) was the key reaction intermediate for isoprene synthesis. Sufficient acid strength of the ionic liquid catalysts was necessary for the conversion of intermediates to isoprene. The influence of reaction conditions including reaction time, reaction temperature, solvent, SO3H-functionalized ionic liquid (SFIL) concentration, and the amount of MTBE and formaldehyde was investigated in detail to maximize the yield of isoprene. Under the optimal conditions, the capacity of isoprene production reached 55.0 g/L, 1 order higher than that in previous studies. The [HSO3-bmin] PTS ionic liquid exhibited excellent recyclability and maintained its activity and selectivity after being reused seven times.
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
ADVANCED MATERIALS
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2023
·Vol. 35
·期 14
·2207955
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IF 29.4
Yong Wang,Tong Li,Libo Li,Rui-Biao Lin,Xiaoxia Jia,Zeyu Chang,Hui-Min Wen,Xiao-Ming Chen,Jinping Li
Propane/propene (C 3 H 8 /C 3 H 6 ) separation is essential in the petrochemical industry but challenging because of their similar physical and chemical properties. Adsorptive separation with C 3 H 8 -selective porous materials can energy-efficiently produce high-purity C 3 H 6 , which is highly promising for replacing conventional cryogenic distillation but suffers from unsatisfactory performance. Herein, through the precise incorporation of fluorinated functional groups into the confined pore space, a new fluorinated metal–organic framework (FDMOF-2) featuring the unique and strong C 3 H 8 -trap is successfully constructed. FDMOF-2 exhibits an unprecedented C 3 H 8 capture capacity of 140 cm 3 cm −3 and excellent C 3 H 8 /C 3 H 6 (1:1, v/v) selectivity up to 2.18 (298 K and 1 bar), thus setting new benchmarks for all reported porous materials. Single-crystal X-ray diffraction studies reveal that the tailored pore confinement in FDMOF-2 provides stronger and multiple attractive interactions with C 3 H 8 , enabling excellent binding affinities. Breakthrough experiments demonstrate that C 3 H 8 can be directly extracted from various C 3 H 8 /C 3 H 6 mixtures with FDMOF-2, affording an outstanding C 3 H 6 production (501 mmol L −1 ) with over 99.99% purity. Benefiting from the robust framework and hydrophobic ligands, the separation performance of FDMOF-2 can be well maintained even under 70% relative humidity conditions.
研究领域:
材料科学
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化学工程
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DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
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IF 20.2
Sen-Wang Wang,Zhen-Hong He,Yue Tian,Zhan-Jun Zhu,Yong-Chang Sun,Kuan Wang,Weitao Wang,Yang Yang,Huan Wang,Zhao-Tie Liu
Photothermal CO 2 oxidative dehydrogenation of propane (CO 2 -ODHP) is an environmentally friendly and sustainable route for propylene production and CO 2 utilization. In the present work, we developed a Pt-GaN/SrTiO 3 dual-functional catalyst to facilitate the reaction. The catalyst achieved propylene and CO yields of 1 mmol·g cat -1 ·h -1 and 1.2 mmol·g cat -1 ·h -1 under photothermal conditions at 320 °C, surpassing the performance of previously reported catalysts. Additionally, control experiments and in situ DRIFTS analyses corroborated that GaN and Pt were primarily responsible for the activation of C-H and C O bonds, respectively, and the photothermal route worked via a distinguished intermediate for CO 2 activation in contrast to the thermal route. DFT calculations supported the reaction route involving the coupling direct dehydrogenation of propane and reverse water-gas shift reaction. The present work shines a light on the design of photothermal catalysts with dual functions, particularly for the activation of CO 2 and light hydrocarbons. Additionally, it proposes a strategy to initiate high-temperature reactions at relatively lower temperatures.
研究领域:
催化
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化学工程
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环境科学
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材料科学
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DOI
高影响因子
FUEL
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2023
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IF 7.4
Linjie Guan,Meiyu Liu,Honghai Liu,Li Zhang,Yiming Zhang,Yucai Qin,Binbin He,Yi Mei,Yun Zu
The regulation of the engineering regionally spatial framework aluminum (Al F ) distribution in MFI channels has been considered as an effective way for the production of light olefins by targeted fluid catalytic cracking (TCO) technology. In this work, ZSM-5 zeolites with controlled Al F distributions are facilely synthesized by tuning the combinations of pentaerythritol (PET), tetrapropylammonium (TPA) and Na cations. The Al F atoms in the prepared HZ5-[PET + Na] and HZ5-[TPA] samples are enriched in the straight channels and intersection channels, respectively, which are favorable to the n-butane monomolecular reaction pathway, promoting the propylene production. Whereas the Al F atoms in the HZ5-[TPA + Na] sample are simultaneously distributed in both the straight and intersection channels, the n-butane molecules preferentially take place monomolecular reaction in the straight channels to generate carbonium ions (e.g., C 2 H 5 + , C 3 H 7 + and C 4 H 9 + ). Subsequently, all of them enter into the intersection channels to induce the occurrence of bimolecular reaction. Such a process is conducive to the formation of ethylene. These insights can help to clarify the catalytic behavior of regional framework acid sites in ZSM-5 channels and then provide an effective approach to design efficient TCO catalysts.
研究领域:
化学工程
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催化
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材料科学
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高影响因子
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