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基于Na2ZrO3基CO2吸附剂的燃煤烟气碳捕集技术研究进展

Research progress of Na2ZrO3-based CO2 sorbents for carbon capture from coal-fired flue gas

  • 摘要: 碳捕集与封存技术的迭代革新为“3060”双碳目标的实现奠定了坚实基础。其中,基于高温固体吸附法的流化床反应技术凭借其与工业烟气体系的高适配性和能耗经济性优势,在未来烟气CO2脱除中彰显出极强的应用前景。Na2ZrO3基吸附剂是一种具备卓越循环稳定性且在低浓度CO2气氛下吸附性能卓越的高温固体吸附剂,在水泥、冶金等难减排行业的碳捕集应用中展现出显著的工程化应用价值。本综述系统梳理了Na2ZrO3基吸附剂在高温CO2捕集中的研究进展。首先,合成工艺会显著影响Na2ZrO3的理化性质,而采用更温和的“湿法”工艺与有机前驱体改性可制备出高比表面积的高气固反应活性的吸附剂材料。其次,引入杂质金属可在一定程度上改变Na2ZrO3内部的晶格结构,进而影响其高温碳捕集性能。此外,通过先进表征技术、吸脱附动力学分析以及密度泛函理论可从宏观、微观以及原子尺度描述Na2ZrO3对CO2的物理吸附和化学吸附行为,进而评估或验证不同改性方法的应用效果。最后,在含水蒸气的混合吸附气氛下,Na2ZrO3基吸附剂的碳捕集性能会根据吸附温度区间的不同产生较大差异。对此,后续工作应从三个方面进行技术突破。首先,应面向工业固废增值化利用开发低成本吸附剂合成工艺。其次,应开展真实烟气组分耦合效应下的Na2ZrO3基吸附剂对复杂气体竞争吸附实验研究,利用多尺度原位表征技术、密度泛函理论计算等先进技术手段系统解析Na2ZrO3基吸附剂吸附/脱附机制。最后,应着力解决Na2ZrO3基吸附剂再生能耗较高的应用痛点,以推动其在实际大规模工业烟气CO2脱除中的应用。

     

    Abstract: The iterative innovation of carbon capture and storage (CCS) technologies has laid a robust foundation for achieving the ‘3060’ dual-carbon targets. Among these advancements, fluidized bed reactor technology based on high-temperature solid sorbents stands out due to its exceptional compatibility with industrial flue gas systems and superior energy-economic efficiency, demonstrating strong application prospects for future CO2 removal from flue gases. The Na2ZrO3-based sorbents, one of the high-temperature solid sorbents with outstanding cyclic stability and excellent CO2 sorption performance—particularly under low-concentration CO2 conditions—has shown significant engineering application value in carbon capture systems for hard-to-abate industries such as cement and metallurgy. This review systematically summarizes current research progress on Na2ZrO3-based sorbents for high-temperature CO2 capture. Firstly, synthesis methods critically influence the physicochemical properties of Na2ZrO3 and employing milder wet-chemical routes and organic precursor modification can yield high-surface-area sorbents with enhanced gas-solid reactivity. Secondly, doping metal elements modifies the internal crystal lattice structure, impacting high-temperature CO2 capture performance. Furthermore, advanced characterization techniques, sorption/desorption kinetic analysis, and density functional theory (DFT) calculations enable the description of CO2 physisorption and chemisorption behavior across macro-, micro-, and atomic scales, facilitating the evaluation of various modification strategies. Finally, CO2 capture performance under H2O-contained atmospheres varies significantly across different temperature regimes. Future research should prioritize three key breakthroughs: (1) developing low-cost synthesis processes utilizing industrial solid waste for value-added adsorbent production; (2) investigating competitive sorption experiments of Na2ZrO3-based sorbents under complex gas components in real flue gas environments and elucidating CO2 sorption/desorption mechanisms using multi-scale in-situ characterization and DFT; (3) addressing the high regeneration energy consumption to enable large-scale industrial deployment.

     

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