Mn-enhanced performance of the Ni-CaO/γ-Al2O3 dual function material for CO2 capture and in situ methanation

•The impact of Mn on the performance of the Ni-CaO/γ-Al2O3 DFM was investigated.•The Mn-doped DFM performed better than the undoped DFM in the ICCU process.•The CH4 yield of MnNi-DFM-3 is 4 times higher than that of Ni-CaO/γ-Al2O3 DFM.•DFT analysis shows the addition of Mn enhanced the activity of t...

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Published inSeparation and purification technology Vol. 357; p. 130152
Main Authors Xiang, Shu-Xiang, Wang, Jin-Peng, Gao, Su, Guo, Zhan-Kuo, Jiang, Hui-Lin, Dong, Bao-Xia, Teng, Yun-Lei
Format Journal Article
LanguageEnglish
Published Elsevier B.V 01.05.2025
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Summary:•The impact of Mn on the performance of the Ni-CaO/γ-Al2O3 DFM was investigated.•The Mn-doped DFM performed better than the undoped DFM in the ICCU process.•The CH4 yield of MnNi-DFM-3 is 4 times higher than that of Ni-CaO/γ-Al2O3 DFM.•DFT analysis shows the addition of Mn enhanced the activity of the Ni catalyst.•This work offers a method for improving the property of DFMs using cheap metals. The CH4 yield over dual functional materials (DFMs) remains low and requires further improvement. In this work, we first examined the influence of Mn on the performance of the Ni-CaO/γ-Al2O3 DFM for CO2 capture and in situ methanation. Our results showed that the MnNi-DFM-3 (MnNi-CaO/γ-Al2O3 DFM) exhibited the best performance at 350 °C, with a CH4 yield of 0.56 mmol/g which is 4 times higher than that of the Ni-DFM-1 (Ni-CaO/γ-Al2O3 DFM) (0.14 mmol/g). Nanoscale characterization revealed that highly scattered Mn3O4 acted as a barrier preventing the agglomeration of Ni-based catalysts. Furthermore, our density functional theory (DFT) analysis demonstrated that the introduction of Mn enhanced the activation of CO2, promoted the dissociation of H2 and intermediates, and reduced the activation energy needed to produce carboxylic acid intermediates on the Ni catalyst. The prepared MnNi-DFM is promising to be a cheap efficient material for CO2 capture and in situ methanation. This work opens up a new pathway for enhancing the performance of DFMs using inexpensive transition metals.
ISSN:1383-5866
DOI:10.1016/j.seppur.2024.130152