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基于CaO的吸附剂在二氧化碳捕集循环过程中的热活化和自活化

Thermal activation of CaO-based sorbent and self-reactivation during CO2 capture looping cycles.

作者信息

Manovic Vasilije, Anthony Edward J

机构信息

CANMET Energy Technology Centre-Ottawa, Natural Resources Canada, 1 Haanel Drive, Ottawa, Ontario, Canada K1A 1M1.

出版信息

Environ Sci Technol. 2008 Jun 1;42(11):4170-4. doi: 10.1021/es800152s.

Abstract

In this study, the thermal activation of different types of CaO-based sorbents was examined. Pretreatments were performed at different temperatures (800--1300 degrees C) and different durations (6--48 h) using four Canadian limestones. Sieved fractions of the limestones, powders obtained by grinding, and hydroxides produced following multiple carbonation/calcination cycles achieved in a tube furnace were examined. Pretreated samples were evaluated using two types of thermogravimetric reactors/ analyzers. The most important result was that thermal pretreatment could improve sorbent performance. In comparison to the original, pretreated sorbents showed better conversions over a longer series of CO2 cycles. Moreover, in some cases, sorbent activity actually increased with cycle number, and this effectwas especially pronounced for powdered samples preheated at 1000 degrees C. In these experiments, the increase of conversion with cycle number (designated as self-reactivation) after 30 cycles produced samples that were approximately 50% carbonated for the four sorbents examined here, and there appeared to be the potential for additional increase. These results were explained with the newly proposed pore--skeleton model. This model suggests, in addition to changes in the porous structure of the sorbent, that changes in the pore--skeleton produced during pretreatment strongly influence subsequent carbonation/ calcination cycles.

摘要

在本研究中,对不同类型的氧化钙基吸附剂的热活化进行了研究。使用四种加拿大石灰石在不同温度(800 - 1300摄氏度)和不同持续时间(6 - 48小时)下进行预处理。对石灰石的筛分部分、研磨得到的粉末以及在管式炉中经过多次碳酸化/煅烧循环后产生的氢氧化物进行了研究。使用两种类型的热重反应器/分析仪对预处理后的样品进行评估。最重要的结果是热预处理可以提高吸附剂性能。与原始吸附剂相比,预处理后的吸附剂在更长的一系列二氧化碳循环中表现出更好的转化率。此外,在某些情况下,吸附剂活性实际上随着循环次数的增加而增加,这种效应在1000摄氏度下预热的粉末样品中尤为明显。在这些实验中,经过30次循环后转化率随循环次数的增加(称为自再活化)使得此处研究的四种吸附剂产生的样品碳酸化程度约为50%,并且似乎还有进一步增加的潜力。这些结果用新提出的孔 - 骨架模型进行了解释。该模型表明,除了吸附剂多孔结构的变化外,预处理过程中产生的孔 - 骨架变化对后续的碳酸化/煅烧循环有强烈影响。

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