Catalytic Teflon AF-2400 membrane reactor with adsorbed ex situ synthesized Pd-based nanoparticles for nitrobenzene hydrogenation
Catalytic Teflon AF-2400 membrane reactor with adsorbed ex situ synthesized Pd-based nanoparticles for nitrobenzene hydrogenation
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DOI：
10.1016/j.cattod.2020.03.062
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发表时间：
2021-02
期刊：
影响因子：
5.3
通讯作者：
B. Venezia;L. Panariello;Daniel Biri;Juhun Shin;S. Damilos;Anand N. P. Radhakrishnan;C. Blackman;A. Gavriilidis
中科院分区：
文献类型：
--
作者：
B. Venezia;L. Panariello;Daniel Biri;Juhun Shin;S. Damilos;Anand N. P. Radhakrishnan;C. Blackman;A. Gavriilidis
在负载催化剂纳米颗粒的非常规方法中，用于纳米颗粒吸附的聚电解质多层的逐层组装是一种简单方便的方法。它能够沉积单一吸附的纳米颗粒并防止它们聚集。在这项工作中，聚多巴胺被接枝到 Teflon AF-2400 管状膜的内表面上，该膜以其对轻气体的优异渗透性和对化学品的惰性而闻名。将聚丙烯酸和聚烯丙胺盐酸盐依次吸附到膜的改性表面上。然后掺入非原位合成的球形、立方体、截头八面体钯或树枝状铂-钯纳米颗粒。将催化膜组装成管中管结构，并用分子氢对硝基苯连续氢化进行 6 小时以上的测试。观察到截短八面体和树枝状纳米颗粒的稳定转化，而其他纳米颗粒则发生逐渐失活。由于尺寸小，3.7nm 球形纳米粒子表现出最高的反应速率，629molreactant/(molcatalyst⋅h)，而立方体纳米粒子表现出最高的周转频率，∼3000h−1。这项工作中开发的反应器概念展示了这种设计如何作为使用单一吸附和精细调节的纳米粒子在流动中进行连续多相催化反应的平台。与间歇式工艺相比，管中管反应器中存在的少量加压气体提高了工艺安全性，而 Teflon AF-2400 膜可控制反应过程中的气体渗透。
Among the unconventional approaches of supporting catalyst nanoparticles, the layer-by-layer assembly of polyelectrolyte multilayers for nanoparticle adsorption represents an easy and convenient method. It enables the deposition of singularly adsorbed nanoparticles and prevents them from aggregating. In this work, polydopamine was grafted onto the internal surface of a Teflon AF-2400 tubular membrane, known for its excellent permeability to light gases and inertness to chemicals. Poly(acrylic acid) and poly(allylamine hydrochloride) were sequentially adsorbed onto the modified surface of the membrane.Ex situsynthesized spherical, cubical, truncated octahedral palladium or dendritic platinum-palladium nanoparticles were then incorporated. The catalytic membranes were assembled in a tube-in-tube configuration and tested over 6 h of continuous nitrobenzene hydrogenation with molecular hydrogen. Stable conversion was observed for the truncated octahedral and dendritic nanoparticles, while a progressive deactivation occurred for the other nanoparticles. Due to their small size, the 3.7 nm spherical nanoparticles exhibited the highest reaction rate, 629molreactant/(molcatalyst⋅h), while the cubical nanoparticles showed the highest turnover frequency, ∼3000 h−1. The reactor concept developed in this work demonstrates how such a design can serve as a platform for conducting continuous multiphase catalytic reactions in flow using singularly adsorbed and finely tuned nanoparticles. The small volume of pressurized gas present in the tube-in-tube reactor offers improved process safety compared to a batch process, while the Teflon AF-2400 membrane provides control over the gas permeation during reaction.