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Effect of Mesoporosity, Acidity and Crystal Size of Zeolite ZSM‐5 on Catalytic Performance during the Ex‐situ Catalytic Fast Pyrolysis of Biomass
ChemCatChem ( IF 3.8 ) Pub Date : 2020-12-01 , DOI: 10.1002/cctc.202001778 Ana M. Hernández‐Giménez 1 , Eleni Heracleous 2, 3 , Eleni Pachatouridou 2 , Andrej Horvat 4 , Héctor Hernando 5 , David P. Serrano 5, 6 , Angelos A. Lappas 2 , Pieter C. A. Bruijnincx 1, 7 , Bert M. Weckhuysen 1
ChemCatChem ( IF 3.8 ) Pub Date : 2020-12-01 , DOI: 10.1002/cctc.202001778 Ana M. Hernández‐Giménez 1 , Eleni Heracleous 2, 3 , Eleni Pachatouridou 2 , Andrej Horvat 4 , Héctor Hernando 5 , David P. Serrano 5, 6 , Angelos A. Lappas 2 , Pieter C. A. Bruijnincx 1, 7 , Bert M. Weckhuysen 1
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The catalytic performance of a set of technical, zeolite ZSM‐5 extruded materials have been studied in a bench scale unit for the ex‐situ Catalytic Fast Pyrolysis (CFP) of lignocellulosic biomass. The set of catalysts include micro‐ and mesoporous materials, with and without ZrO2‐promotion, with different Si/Al ratios and with micro‐ and nanosized zeolite crystals. Mesoporosity, acidity and crystal size play a key role on the overall catalytic performances in terms of activity and selectivity (i. e., in their ability to obtain the highest bio‐oil fraction with the lowest oxygen content), and also importantly, stability. Detailed post‐mortem bulk and micro‐spectroscopic studies of the solid catalysts complement the catalytic testing. The obtained results point towards coke deposits as the main cause for catalyst deactivation. Details of the nature, formation and evolution of these coke deposits revealed essential insights, which serve to evaluate the design of catalysts for the ex‐situ CFP of biomass. In particular the mesoporous catalysts are overall better preserved with increasing time‐on‐stream and deactivate later than their microporous counterparts, which suffer from pore blockage. Likewise, it was seen that ZrO2‐promotion contributed positively in the prevention against deactivation by hard coke spreading, thanks to its enhanced Lewis acidity. The zeolite's crystal size is another important characteristic to combine the different components within catalyst bodies, ensuring the proper interaction between zeolite, promoter and binder. This is illustrated by the nanocrystalline ZrO2/n‐ZSM‐5‐ATP material, which shows the best catalytic performance.
中文翻译：
ZSM-5分子筛的介孔度，酸度和晶体尺寸对生物质异位催化快速热解过程中催化性能的影响
在台式规模的装置中，对木质纤维素生物质的异位催化快速热解（CFP），研究了一组技术性ZSM-5沸石挤压材料的催化性能。这套催化剂包括带和不带ZrO 2的微孔和中孔材料促进，具有不同的Si / Al比以及微米和纳米尺寸的沸石晶体。中孔度，酸度和晶体尺寸在活性和选择性（即以最低的氧含量获得最高的生物油级分的能力）和稳定性方面对整体催化性能起关键作用。固体催化剂的详细事后本体和显微光谱研究补充了催化测试。获得的结果表明焦炭沉积是催化剂失活的主要原因。这些焦炭沉积物的性质，形成和演化的细节揭示了重要的见解，这些见解可用于评估生物质异位CFP催化剂的设计。尤其是，中孔催化剂的整体保存时间更长，并且比起孔隙阻塞的微孔催化剂要更迟钝化。同样，可以看到ZrO2-促进作用增强了路易斯酸度，对防止硬焦炭扩散引起的失活起到了积极作用。沸石的晶体尺寸是在催化剂体内结合不同组分的另一个重要特征，可确保沸石，促进剂和粘合剂之间的适当相互作用。纳米晶ZrO 2 / n-ZSM-5-ATP材料说明了这一点，该材料显示出最佳的催化性能。
更新日期：2020-12-01
中文翻译：
ZSM-5分子筛的介孔度，酸度和晶体尺寸对生物质异位催化快速热解过程中催化性能的影响
在台式规模的装置中，对木质纤维素生物质的异位催化快速热解（CFP），研究了一组技术性ZSM-5沸石挤压材料的催化性能。这套催化剂包括带和不带ZrO 2的微孔和中孔材料促进，具有不同的Si / Al比以及微米和纳米尺寸的沸石晶体。中孔度，酸度和晶体尺寸在活性和选择性（即以最低的氧含量获得最高的生物油级分的能力）和稳定性方面对整体催化性能起关键作用。固体催化剂的详细事后本体和显微光谱研究补充了催化测试。获得的结果表明焦炭沉积是催化剂失活的主要原因。这些焦炭沉积物的性质，形成和演化的细节揭示了重要的见解，这些见解可用于评估生物质异位CFP催化剂的设计。尤其是，中孔催化剂的整体保存时间更长，并且比起孔隙阻塞的微孔催化剂要更迟钝化。同样，可以看到ZrO2-促进作用增强了路易斯酸度，对防止硬焦炭扩散引起的失活起到了积极作用。沸石的晶体尺寸是在催化剂体内结合不同组分的另一个重要特征，可确保沸石，促进剂和粘合剂之间的适当相互作用。纳米晶ZrO 2 / n-ZSM-5-ATP材料说明了这一点，该材料显示出最佳的催化性能。
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