Bifunctional catalysts based on PdZn/ZnO and hierarchical zeolites in the direct synthesis of dimethyl ether from CO-rich syngas: influence of the support and the Zn/Pd molar ratio†

IF 4.4 3区 化学 Q2 CHEMISTRY, PHYSICAL
Bing Wang , Nicola Da Roit , Michael Zimmermann , Markus Boese , Thomas Zevaco , Silke Behrens
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引用次数: 0

Abstract

Following the ‘precursor’ concept, a series of Pd/Zn-based, colloidal nanoparticles (NPs) with different Zn/Pd molar ratios were synthesized by reductive stabilization and used as precursors for the methanol active component in bifunctional catalysts. The bifunctional catalysts for the single-step dimethyl ether synthesis from CO-rich syngas were obtained by immobilizing the NPs on a microporous or hierarchical HZSM-5 zeolite, which were used as dehydration catalysts. The catalysts were characterized, e.g., by (in situ) powder X-ray diffraction, scanning and transmission electron microscopy with energy-dispersive X-ray analysis, N2 physisorption, and NH3 temperature programmed desorption. This study demonstrates the influence of the Zn/Pd molar ratio on the size of PdZn particles formed under reaction conditions, which correlates with the catalytic performance in the STD process. The introduction of mesopores in the hierarchical zeolite by desilication of HZSM-5 increased the DME yield while decreasing the selectivity to hydrocarbons.

Abstract Image

基于PdZn/ZnO和分级沸石的双功能催化剂在富co合成气中直接合成二甲醚:载体和Zn/Pd摩尔比†的影响
遵循“前驱体”的概念,通过还原稳定合成了一系列具有不同Zn/Pd摩尔比的Pd/Zn基胶体纳米颗粒(NPs),并将其用作双功能催化剂中甲醇活性组分的前驱体。通过将NPs固定在微孔或分级HZSM-5沸石上,制备了富co合成气一步法合成二甲醚的双功能催化剂,并将其作为脱水催化剂。通过(原位)粉末x射线衍射,扫描和透射电子显微镜(带有能量色散x射线分析),N2物理吸附和NH3温度程序脱附等方法对催化剂进行了表征。本研究证明了Zn/Pd摩尔比对反应条件下形成的PdZn颗粒大小的影响,这与STD工艺的催化性能有关。通过HZSM-5脱硅在分级沸石中引入介孔,提高了二甲醚的收率,但降低了对烃类的选择性。
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来源期刊
Catalysis Science & Technology
Catalysis Science & Technology CHEMISTRY, PHYSICAL-
CiteScore
8.70
自引率
6.00%
发文量
587
审稿时长
1.5 months
期刊介绍: A multidisciplinary journal focusing on cutting edge research across all fundamental science and technological aspects of catalysis. Editor-in-chief: Bert Weckhuysen Impact factor: 5.0 Time to first decision (peer reviewed only): 31 days
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