Carbon-resistant bifunctional catalyst composed of LaFeO3 enhanced Ni-CaO for integrated CO2 capture and conversion

Hengyu Wei , Min Lin , Juping Zhang , Di Gao , Yuhao Chen , Liang Zhang , Xing Zhu
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Abstract

Coupled calcium cycling and dry reforming of methane (CaL-DRM) process has garnered significant attention in recent years as a promising technique for the CO2 capture and in-situ conversion. However, traditional Ni-CaO catalysts with substantial CaL-DRM activity are susceptible to severe carbon deposition, which greatly hinders their industrial application. A combination of sol-gel and impregnation methods to include LaFeO3 into Ni-CaO to enhance CO2 capture and conversion is utilized. The characterization results indicate that the incorporation of LaFeO3 significantly improves the dispersion of Ni and CaO, increases the concentration of oxygen vacancies, effectively suppresses the sintering and carbon deposition, and improves the cycling stability of Ni-CaO. In addition, LaFeO3 promotes the outward diffusion of lattice oxygen, thereby facilitating CO2 capture and CH4 conversion to syngas. At 700 ℃, up to 86.5 % CO2 conversion, 87.6 % CO selectivity, and syngas yield close to the theoretical value of 1.0 were achieved over 5Ni-30CaO-LFO (30 wt% CaO). More importantly, the activity of catalyst remains almost unchanged after 30 cycles. This study introduces an innovative approach for CaL-DRM, showing significant potential for effective and stable CO2 capture and in-situ conversion.
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由LaFeO3组成的抗碳双功能催化剂增强Ni-CaO集成CO2捕获和转化
近年来,钙循环耦合甲烷干重整(CaL-DRM)工艺作为一种很有前途的CO2捕集和原位转化技术受到了广泛关注。然而,具有较强CaL-DRM活性的传统Ni-CaO催化剂容易发生严重的积碳,这极大地阻碍了其工业应用。采用溶胶-凝胶和浸渍相结合的方法将LaFeO3加入Ni-CaO中,以增强CO2的捕获和转化。表征结果表明,LaFeO3的掺入显著改善了Ni和CaO的分散性,增加了氧空位浓度,有效抑制了Ni-CaO的烧结和积碳,提高了Ni-CaO的循环稳定性。此外,LaFeO3促进晶格氧向外扩散,从而促进CO2捕获和CH4转化为合成气。在700℃条件下,5Ni-30CaO-LFO (CaO质量分数为30%)的CO2转化率高达86.5%,CO选择性高达87.6%,合成气收率接近理论值1.0。更重要的是,经过30次循环后,催化剂的活性几乎保持不变。本研究介绍了一种创新的CaL-DRM方法,显示出有效和稳定的CO2捕获和原位转换的巨大潜力。
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阿拉丁
La(NO3)3·6H2O
阿拉丁
Fe(NO3)3·9H2O
阿拉丁
C6H8O7
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