鈣循環(CaL)涉及應用二氧化碳對氧化鈣進行碳酸化,並通過將捕獲的二氧化碳轉化為有用的產品來再生氧化鈣。通過結合CaL與甲烷重組(DRM),捕獲的二氧化碳可轉化為合成氣,具有高價值的化學原料和燃料。本研究已開發出由氧化鈣(CO2吸附劑),金屬鎳(DRM催化劑)和二氧化鈰(DRM助催化劑)組成的多功能材料(DFM)來驅動CaL-DRM串聯反應。在研究的第一部分,我們應用共沉澱法合成的CaO-Ni-CeO2 多功能材料的CO2吸收效率為10.3 mmolCO2/gCaO,H2 和CO產率分別為754.4 mmolH2/gNi和454.6 mmolCO/gNi,甲烷重組所需的起始溫度為680 °C。氧化鈣的碳酸化反應受材料的鹼度影響,而甲烷與二氧化碳的轉化率則被材料中金屬鎳的分散度所影響。第二部分採用氣溶膠合成方法合成了CaO-Ni-CeO2 多功能材料。氣溶膠納米粒子的利用對催化領域非常有益,因為它可以產生大量有效的金屬-載體-助催化劑相互作用以促進界面催化(例如DRM)。 此氣溶膠合成的CaO-Ni-CeO2納米結構對於CaL-DRM的性能方面有著極大的改進:高CO2吸收效率(~12.1 mmolCO2/gCaO), 高CO2轉化率(~97.2 %), 低甲烷重組起始溫度(600 °C)和足夠高的運行穩定性。總體而言，我們的工作展示了使用程序升溫反應平台對 CaL-DRM 動力學進行定量實時分析的原型研究。

Calcium looping (CaL), which involves carbonation of CaO by CO2 and regeneration of CaO through the conversion of the captured CO2 into useful products, shows promise for carbon capture and utilization. By integrating CaL with methane dry reforming (DRM), the captured CO2 can be converted into syngas, a valuable chemical feedstock and fuel. Herein, a dual functional material (DFM) composed of CaO (CO2 adsorbent), Ni (DRM catalyst) and CeO2 (promoter for DRM) had been developed to drive the CaL-DRM tandem processes. In the first part of study, the CaO-Ni-CeO2 DFM synthesized using co-precipitation method possessed CO2 uptake efficiency of 10.3 mmolCO2/gCaO, H2 and CO yields of 754.4 mmolH2/gNi and 454.6 mmolCO/gNi, respectively, and a moderate required temperature for methane dry reforming (680 °C). The carbonation of CaO was strongly influenced by the basicity of the material, and the conversions of CH4 with the captured CO2 were affected by the Ni dispersion in the material. In the second part, aerosol-based synthetic approach was employed for the synthesized of CaO-Ni-CeO2 DFM. The utilization of aerosol nanoparticles is highly beneficial to catalysis field by the creation of strong metal-support-promoter interaction for promoting an interfacial catalysis (i.e., such as DRM). The CaO-Ni-CeO2 hybrid nanostructure showed great improvement in the performance of cyclic CaL-DRM: high CO2 uptake efficiency (~12.1 mmolCO2/gCaO), high CO2 conversion (~97.2 %), low required temperature for methane dry reforming (600 °C) and sufficiently high operational stability. Overall, our work demonstrates a prototype study of using a temperature-programmed reaction platform for a quantitative, real-time analysis on CaL-DRM kinetics. The mechanistic understanding of CaL-DRM by the CaO-Ni-CeO2 DFM were elucidated, showing promise for the catalyst optimizations.

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