Journal of CO2 Utilization
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2018
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IF 5.503
Jianyang Wang,Anfeng Zhang,Xiao Jiang,Chunshan Song,Xinwen Guo
Although many researchers have reported CO 2 hydrogenation to various C1 chemicals, it is still challenging to directly and selectively convert CO 2 to C 2 -C 4 hydrocarbons in terms of overcoming the extreme inertness of CO 2 and a high C C coupling barrier. In the present work, we report an efficient integration of methanol-synthesis and the methanol-to-hydrocarbons with the bifunctional catalyst component of In 2 O 3 -ZrO 2 and SAPO-5. These tandem reactions exhibit an excellent relative selectivity of C 2 -C 4 (83%) with a suppressed CH 4 relative selectivity less than 3% at T = 300 °C. A detailed analysis indicates that the partially reduced indium oxide surface (In 2 O 3 -ZrO 2 ) can better activate CO 2 and promote the synthesis of methanol than In 2 O 3 alone, and C C coupling is subsequently manipulated within the confined acidic pores of SAPO-5 according to XRD, H 2 -TPR, CO 2 -TPD, SEM and TEM. Furthermore, the proximity of two components and the content of Si also play an important role in such outstanding selectivity to C 2 -C 4 . Our study paves a new path for the direct synthesis of lower hydrocarbons.
研究领域:
化学工程
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催化化学
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能源化学
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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
Wenhui Li,Jiaxing Zhang,Xiao Jiang,Minchen Mu,Anfeng Zhang,Chunshan Song,Xinwen Guo
Carbon dioxide (CO2) hydrogenation to gasoline through the methanol-mediate route using the metal oxide/ZSM-5 tandem catalyst has attracted considerable attention to reduce the pernicious effect of CO2 on global climate change and to reduce our dependence on fossil fuels. The C5+ molecules are preferred to pass through the straight channels of ZSM-5 zeolite, where side reactions may occur on the acid sites and the catalyst is deactivated due to pore blockage. Thus, the thickness of ZSM-5 along the straight channel, namely the b-axis direction, is crucial to manipulating the product distribution and catalyst lifetime. Here, HZSM-5 nanosheets with different thicknesses (2 nm to 2 μm) along the b-axis were synthesized controllably and composited with In2O3/ZrO2 as tandem catalysts for CO2 hydrogenation to gasoline. In2O3–ZrO2/HZSM-5 with a thickness of 20 nm shows the highest selectivity toward C5+ hydrocarbons under isoconversional conditions and no deactivation after 150 h of reaction with less carbon deposition compared with the 2 μm one. Comparative activity tests and characterization results demonstrate that an appropriate length of straight channels can benefit the production of C5+ hydrocarbons through the polymerization of short-chain molecules while preventing the cracking of long-chain hydrocarbons on acid sites. Adding an appropriate loading of Co into tandem catalysts with optimal composition gives rise to further enhancement in CO2 conversion by 10%, and a slight increase in C5+ selectivity. This can be attributed to the Co-induced hydrogen spillover from metallic Co to support ZrO2, facilitating the formation of the key intermediate and its subsequent hydrogenation steps. This study provides insights into designing effective and anti-carbon deposition tandem catalysts for CO2-to-gasoline by manipulating the channel length–resident time–acidity relationship and the promoter effect.
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
APPLIED SURFACE SCIENCE
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2022
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IF 7.392
Zhuping Li,Yong Men,Shuang Liu,Jinguo Wang,Keye Qin,Dandan Tian,Tianle Shi,Li Zhang,Wei An
The crystalline phases of support have great influence on their surface and structure properties. Therefore, adjusting the crystalline structure of heterogeneous catalysts imposes a significant impact on the catalytic performance. Herein, a suite of Pd/In 2 O 3 /ZrO 2 catalysts with different crystalline phases of ZrO 2 were prepared and evaluated for CO 2 hydrogenation to CH 3 OH using the same amount of metal loading. The activity data showed the distinct superior reactivity of Pd/In 2 O 3 /ZrO 2 catalyst used mixed monoclinic and tetragonal phases ZrO 2 (Mix-ZrO 2 ) as support as compared to respective single phase of monoclinic ZrO 2 (m-ZrO 2 ) and tetragonal ZrO 2 (t-ZrO 2 ). The catalysts are extensively characterized through BET, XRD, HRTEM, UV–vis, H 2 -TPR, CO 2 /H 2 -TPD and XPS. Combining the characterization results and activity data, the superior activity of Pd/In 2 O 3 /Mix-ZrO 2 catalyst can be correlated with large particle size of Pd nanoparticles, the concentration of oxygen vacancies, and the abundant medium basic sites, which were essential for activation of H 2 and inert CO 2 and enhancement of catalytic performance. The best-performing Pd/In 2 O 3 /Mix-ZrO 2 catalyst exhibited a remarkable reactivity with space time yield (STY) of 0.54 g methanol ·h −1 ·g cat −1 at 573 K and 5 MPa, and stability without noticeable deactivation after 100 h of time on stream, demonstrating its potential as catalyst used in CH 3 OH synthesis from CO 2 hydrogenation.
研究领域:
催化化学
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材料科学
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能源化学
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DOI
高影响因子
Greenhouse Gases-Science and Technology
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2022
·Vol. 12
·期 2
·305-320
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IF 2.518
Zichen Liu,Shuman Xu,Jing Hao,Lina Song,Mingben Chong,Dang-Guo Cheng,Fengqiu Chen
The conversion of CO 2 into high-value chemicals has drawn a great deal of consideration, of which the most ideal product is lower olefins. However, the modified Fischer–Tropsch (F-T) synthesis with CO as an intermediate shows poor selectivity for lower olefins. Here, a list of bifunctional catalysts consisting of SAPO-34 zeolites with adjustable silicon contents and In 2 O 3 /ZrO 2 were synthesized. In the reaction process, CO 2 is first hydrogenated to methanol over an In 2 O 3 /ZrO 2 catalyst, and then the generated methanol rapidly diffuses to the adjacent zeolite catalyst to react to lower olefins. The selectivity of lower olefins (88.3%) and conversion rate of CO 2 (23.3%) was achieved over In 2 O 3 /ZrO 2 and SAPO-34-0.05 at 633 K, a gas hourly space velocity (GHSV) of 4500 ml·gcat –1 ·h –1 , and H 2 /CO 2 /Ar = 3:1:1. The catalytic performance remained stable after 50 h of reaction. Characterization analysis showed that Si content affected the content of Brønsted acid sites (BAS) and morphology of SAPO-34, resulting in different distribution of reaction intermediates. Tetramethyl-benzenes, as important intermediate species, had a slower conversion rate on the SAPO-34 with low Si content and nanosheet morphology, which led to high lower olefins selectivity. © 2022 Society of Chemical Industry and John Wiley & Sons, Ltd.
研究领域:
催化
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化学工程
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材料科学
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环境化学
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DOI
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2026
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IF 4.6
Weijie Zhou,Yuzi Zhang,Chaoyue Li,Xiangyang He,Zhichao Miao,Jinglin Mu,Manfen Liang,Jin Zhou
In 2 O 3 supported on ZrO 2 and CeO 2 was developed for CO 2 -to-formate electroreduction. • Distinct support effects of ZrO 2 and CeO 2 on In 2 O 3 active site were identified. • CeO 2 tunes electronic structure of In species and boosts the catalytic performance. • In 2 O 3 /CeO 2 delivers higher current density and Faradaic efficiency than In 2 O 3 /ZrO 2 . • The In 2 O 3 /CeO 2 catalyst maintains stable operation for 50 h at 100 mA cm −2 . Developing efficient electrocatalysts for the selective CO 2 electroreduction to formate is important for achieving carbon neutrality. Herein, In 2 O 3 /ZrO 2 and In 2 O 3 /CeO 2 catalysts were fabricated by combining MOF-derived oxide supports with incipient wetness impregnation and subsequent thermal treatment. Comparative studies reveal that CeO 2 affords a more favorable catalyst-support interface than the ZrO 2 support, resulting in enhanced activity and selectivity for formate production. In a flow cell, the optimized In 2 O 3 /CeO 2 catalyst achieves a formate Faradaic efficiency of 90.0% at −1.37 V vs. RHE with a current density of 177 mA cm −2 , significantly outperforming the In 2 O 3 /ZrO 2 catalyst. Combined structural characterization and kinetic analysis indicate that the CeO 2 support improves the electronic structure of In species, thereby facilitating the adsorption and conversion of key intermediates and thereby improving the intrinsic reactivity for formate formation. Moreover, the In 2 O 3 /CeO 2 catalyst maintains stable operation for 50 h at 100 mA cm −2 . This work highlights the critical role of support effects in regulating In-based active sites and provides insights into the rational design of efficient catalysts for the selective CO 2 -to-formate electroreduction. A series of In 2 O 3 /ZrO 2 and In 2 O 3 /CeO 2 catalysts were prepared for ECR to formate. The CeO 2 affords a more favorable catalyst-support interface than the ZrO 2 support, resulting in enhanced activity and selectivity for formate production. Download: Download high-res image (117KB) Download: Download full-size image
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高影响因子
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