FUEL
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2024
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IF 6.7
Shenghua Liu,Xiaoqian Feng,JinXin Xu,Jiaxin Wang,Yonghua Zhao,Huan Wang,Qijian Zhang
CO 2 methanation is a potential way for the re-utilization of CO 2 . MOF derivations are promising candidates for commonly used Ni-based catalysts due to their high porosity and confinement effect. Herein, we systematically investigated the synthetic pathway of Zr-MOF-derived Ni-based catalysts. It is found that Ce addition can effectively improve the thermostability, specific surface area and Ni dispersion of the derived Ni/CeO 2 -ZrO 2 catalyst. It can also enhance the adsorption of CO 2 by the generation of O v and improve CO 2 methanation activity. Calcination the MOF in inert gas leads to the formation of CNTs and amorphous carbon. Amorphous carbon results in less interaction between NiO and CeO 2 as well as low amount of O v , leading to lower catalytic activity than the catalyst calcinated in air. Compared with impregnation method, one-pot solvothermal method leads to much higher specific surface area for both MOF and derived oxides. It also benefits the uniform dispersion of NiO and higher amount of O v . Therefore, it shows better catalytic activity and is proved to be a better method for Ni introduction. In the catalysts we discussed, St-ZrCeNi (Ce addition, one-pot solvothermal method, calcination in air) shows the highest CO 2 conversion and good CH 4 selectivity due to its high specific area and more O v . It also shows good stability (>50 h) and good intrinsic activity. This research reveals the roles of several important factors in the synthesis process of Zr-MOF derived Ni-based catalysts. It also gives new insights for the design and synthesis for other MOF derived catalysts.
研究领域:
材料科学
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催化化学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
Inorganic Chemistry Frontiers
·
2019
·Vol. 6
·期 7
·1799-1812
·
IF 5.934
Xiaosong Hu,Chaoyue Zhao,Qingxin Guan,Xin Hu,Wei Li,Jun Chen
The chemical transformation of CO2 not only mitigates CO2 released into the atmosphere but also produces fuels and chemicals with important additional value. The activation of stable CO2 molecules is the key difficulty for the efficient conversion of CO2. Herein, we designed a ternary catalyst containing Cu, ZnO, and CeOx and dispersed them in SBA-15 using incipient wetness impregnation. Interestingly, the catalytic performances were improved greatly when the related active components were dispersed inside and outside the pore channels of SBA-15 using the incipient wetness impregnation method. Methanol and CO were controllably produced on the interface of Cu and metal oxides (ZnO and CeOx) due to the synergistic effects between the three active components. The metal oxides play a more important role in CO2 conversion as well as the product selectivity compared to Cu. CeO2 is more efficient than ZnO in promoting the dispersion of Cu nanoparticles and methanol generation. The suitable pore channels of SBA-15 promote the mass transfer and heat transfer while the high specific surface area is favorable to the dispersion of active components, which will facilitate the production of methanol and CO. After continuous hydrogenation evaluation for 100 h, the catalytic performance of the catalyst was still very stable. This work provides a viable strategy to prepare a supported catalyst with highly dispersed active sites, and the catalyst exhibits an efficient catalytic effect on producing methanol and CO.
研究领域:
化学工程
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催化科学
✓ 已验证
产品关联
DOI
高影响因子
Catalysis Science & Technology
·
2016
·Vol. 6
·期 14
·5656-5667
·
IF 5.287
Fufeng Cai,Guomin Xiao
In this work, a series of Cu–Co–Al catalysts with different Ce loadings were applied to the hydrogenolysis of glycerol to 1,2-propanediol in a fixed-bed flow reactor. The physicochemical properties of the synthesized catalysts were analyzed using BET, N2O chemisorption, SEM, TEM, XRD, H2-TPR, NH3-TPD and XPS techniques. Systematic characterization demonstrated that the incorporation of Ce into the Cu–Co–Al catalyst could effectively restrain the aggregation of active metal species as well as the growth of metallic particles during calcination and reduction, which resulted in the formation of highly dispersed active metals. Large amounts and superior strength of acid sites were present in the Ce-promoted Cu–Co–Al catalysts, as confirmed by NH3-TPD analysis. The reducible nature of the Cu–Co–Al catalyst greatly increased after the addition of Ce. The higher concentration of acid sites, excellent reducibility and highly dispersed active metals were responsible for the superior catalytic activity of the 8Ce/Cu–Co–Al catalyst and it attained 91.6% glycerol conversion and 92.4% 1,2-propanediol selectivity. In addition, the effects of different process parameters such as the solvent, reaction temperature, operating pressure, catalyst loading, glycerol concentration and liquid flow rate on glycerol hydrogenolysis together with the catalyst stability were studied in detail, showing that the Ce-promoted Cu–Co–Al catalyst had high efficiency and stability for glycerol hydrogenolysis.
研究领域:
化学工程
·
催化科学
✓ 已验证
产品关联
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2024
·
IF 15.7
Tianhua Zhang,Haihui Hu,Jiaxin Li,Yinglong Gao,Lingling Li,Mingyuan Zhang,Xuanbei Peng,Yanliang Zhou,Jun Ni,Bingyu Lin,Jianxin Lin,Bing Zhu,Dongshuang Wu,Linjie Zhang,Lili Han,Lirong Zheng,Xiuyun Wang,Lilong Jiang
Ammonia (NH 3 ) is an excellent candidate for hydrogen storage and transport. However, producing NH 3 under mild conditions is a long-term, arduous task. Atomic cluster catalysts (ACCs) have been shown to be effective for catalytic N 2 -to-NH 3 conversion, opening the door to the development of efficient catalysts under mild conditions. Still, ACC formation with thermally stable catalytic sites remains a challenge because of their high surface free energy . Herein, we report anchoring Ba and/or Ce onto Ru ACCs (2 wt% Ru atomic clusters supported on N-doped carbon) to form so-called clusters–metal oxide promoters electronic interaction (CMEI) to stabilize the Ru atomic clusters. The resulting Ba/Ce/Ru ACCs significantly boost the NH 3 synthesis rate to 56.2 mmol NH3 g cat −1 h −1 at 400 °C and 1 MPa, which is 7.5-fold higher than that of Ru ACC. The strengthened CMEI between the Ba/Ce and Ru atomic clusters across the Ba/Ce/Ru ACC enables electron transfer from Ba and/or Ce to Ru atomic clusters. As such, the electron-enriched Ru atom could facilitate electron transfer to N≡N bond π* orbitals, which would weaken the N≡N bond and drive the eventual conversion of N 2 to NH 3 . This study offers insight into the role of CMEI in Ru ACCs and provides an effective approach for designing stable atomic cluster catalysts for NH 3 synthesis.
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
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