锡和锌改性的HZSM-5，用于一步一步催化甘油转化为增值芳烃：浸渍锡颗粒，ALD引入的ZnO膜和HZSM-5沸石的协同组合,Applied Catalysis A: General

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锡和锌改性的HZSM-5，用于一步一步催化甘油转化为增值芳烃：浸渍锡颗粒，ALD引入的ZnO膜和HZSM-5沸石的协同组合
Applied Catalysis A: General ( IF 4.7 ) Pub Date : 2017-04-18 14:02:15
Fei Wang, Xuan Kang, Ma-xi Zhou, Xing-hui Yang, Li-jing Gao, Guo-min Xiao

甘油化学选择性催化转化为高附加值芳烃（GTA）可以大大提高生物柴油和生物质产业链的经济效益。为了提高GTA工艺过程中甘油中碳的芳构化活性，稳定性和转化效率，将可通过脱氢反应将甘油脱氧反应中的烯烃直接转化为芳烃的Zn引入到Sn / HZSM-5中通过原子层沉积（ALD）和初期湿法浸渍（IWI）方法制备沸石。与浸渍的ZnO改性的Sn / HZSM-5相比，通过20次ALD循环引入的ZnO以薄膜形式沉积在Sn / HZSM-5中，不仅完全覆盖了HZSM-5的内外表面，而且部分覆盖了浸渍的锡颗粒。该薄膜稳定了充当催化活性材料的负载SnOx物种的氧化态，并进一步修复了HZSM-5结构缺陷，从而在HZSM-5沸石，浸渍的Sn颗粒和ALD引入的ZnO薄膜之间产生了更好的协同作用。此外，由于引入的ALD ZnO膜具有保护作用，可以防止HZSM-5骨架在GTA反应和再生过程中暴露于蒸汽中而导致HZSM-5不可逆脱铝，因此可大大提高该催化剂的可重复使用性。但是，当沉积的ZnO ALD循环数达到40时，HZSM-5上的Sn颗粒可以完全被ZnO膜包裹，这时Sn不能参与GTA工艺，从而导致芳烃收率和催化剂寿命的降低。。

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Sn and Zn modified HZSM-5 for one-step catalytic upgrading of glycerol to value-added aromatics: Synergistic combination of impregnated Sn particles, ALD introduced ZnO film and HZSM-5 zeolite

The chemoselective catalytic conversion of glycerol into high value-added aromatics (GTA) can greatly enhance the economic profits in biodiesel and biomass industry chain. In order to enhance the aromatization activity, stability and conversion efficiency of carbon in glycerol into aromatics during the GTA process, Zn species, which could directly convert alkenes originated from deoxygenation of glycerol into aromatics through dehydrogenation reaction, was introduced into Sn/HZSM-5 zeolite via atomic layer deposition (ALD) and incipient wet impregnation (IWI) method. Compared with impregnated ZnO modified Sn/HZSM-5, ZnO introduced by 20 ALD cycles into Sn/HZSM-5 deposited in the form of thin film, which not only fully coated both HZSM-5 external and internal surface, but also partially covered impregnated Sn particles. This film stabilized the oxidation state of loaded SnOx species which acted as catalytically active materials and further healed HZSM-5 structural defects, leading to the better synergistic effect among HZSM-5 zeolite, impregnated Sn particles and ALD introduced ZnO films. Besides, the reusability of this catalyst could be tremendously improved due to the protective effect of introduced ALD ZnO film which could prevent irreversible dealumination of HZSM-5 from exposure of HZSM-5 framework to steam during GTA reaction and regeneration procedure. However, when the deposited ZnO ALD cycle number reached 40, Sn particles on HZSM-5 could be completely packaged by ZnO film, on which occasion Sn could not participate in the GTA process, thereby leading to the reduction in both aromatics yields and catalyst lifetime.

更新日期：2017-04-19

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