利用 Cu/CaO 双功能材料实现二氧化碳的综合捕集与转化:原位转化对 CaO 烧结及其二氧化碳捕获性能的影响

Rui Han , Yang Wang , Lifei Wei , Mingke Peng , Zhiyong Li , Caixia Liu , Qingling Liu
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摘要

综合碳捕集与利用(ICCU)技术一直被认为是缓解碳排放问题的一项前瞻性战略。与传统的二氧化碳捕集与利用相比,ICCU 工艺可降低运输、产品净化、建设和运营成本。然而,很少有研究集中于研究 CO2 原位转化对 CaO 高温烧结的影响。在这项工作中,合成了 Cu/CaO 双功能材料 (DFM),并将其用于 650 °C 下的钙循环-反向水气转换(CaL-RWGS)工艺。结果表明,将 CaL 与 RWGS 反应耦合在一起在热力学上是可行的。在循环二氧化碳捕集试验中,Ca1Cu0.1 DFMs 表现出理想的二氧化碳捕集性能(11.34 mmol/gDFMs),并在前 15 个循环中出现自激活现象。此外,DFMs 中的 Cu 纳米粒子催化剂通过加速 CaO 表面对 CO2 的解吸并在转化阶段将其转化为 CO,从而有效抑制了 CaO 的烧结。对 Ca1Cu0.1 DFMs 的原位 DRIFTS 显示,甲酸盐可能是 CaL-RWGS 的 RWGS 中间体。
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Integrated CO2 capture and conversion by Cu/CaO dual function materials: Effect of in-situ conversion on the sintering of CaO and its CO2 capture performance

The integrated carbon capture and utilization (ICCU) technology has been considered a prospective strategy for mitigating carbon emissions issues. Compared to conventional CO2 capture and utilization, the ICCU process reduces transporting, product purification, construction, and operation costs. However, few works focus on investigating the effect of in-situ CO2 conversion on the sintering of CaO at high temperatures. In this work, Cu/CaO dual functional materials (DFMs) were synthesized and used in the Calcium Looping-Reverse Water-Gas Shift (CaL-RWGS) process at 650 °C. The results showed that it is thermodynamically feasible to couple the CaL with the RWGS reaction. In the cyclic CO2 capture test, Ca1Cu0.1 DFMs showed desirable CO2 capture performance (11.34 mmol/gDFMs) and self-activated phenomenon in the first 15 cycles. Moreover, Cu nanoparticle catalysts in the DFMs effectively inhibited the sintering of CaO by accelerating the desorption of CO2 from the CaO surface and converting it to CO during the conversion stage. In-situ DRIFTS of Ca1Cu0.1 DFMs revealed that formates might be the RWGS intermediates in CaL-RWGS.

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