Wang Shuang, Bai Pu, Sun Mingzhe, Liu Wei, Li Dongdong, Wu Wenzheng, Yan Wenfu, Shang Jin, Yu Jihong
State Key Laboratory of Inorganic Synthesis and Preparative Chemistry College of Chemistry Jilin University Changchun 130012 China.
School of Energy and Environment City University of Hong Kong Tat Chee Ave Kowloon Hong Kong China.
Adv Sci (Weinh). 2019 Jul 1;6(17):1901317. doi: 10.1002/advs.201901317. eCollection 2019 Sep 4.
3D-printing technology is a promising approach for rapidly and precisely manufacturing zeolite adsorbents with desirable configurations. However, the trade-off among mechanical stability, adsorption capacity, and diffusion kinetics remains an elusive challenge for the practical application of 3D-printed zeolites. Herein, a facile "3D printing and zeolite soldering" strategy is developed to construct mechanically robust binder-free zeolite monoliths (ZM-BF) with hierarchical structures, which can act as a superior configuration for CO capture. Halloysite nanotubes are employed as printing ink additives, which serve as both reinforcing materials and precursor materials for integrating ZM-BF by ultrastrong interfacial "zeolite-bonds" subjected to hydrothermal treatment. ZM-BF exhibits outstanding mechanical properties with robust compressive strength up to 5.24 MPa, higher than most of the reported structured zeolites with binders. The equilibrium CO uptake of ZM-BF reaches up to 5.58 mmol g (298 K, 1 bar), which is the highest among all reported 3D-printed CO adsorbents. Strikingly, the dynamic adsorption breakthrough tests demonstrate the superiority of ZM-BF over commercial benchmark zeolites for flue gas purification and natural gas and biogas upgrading. This work introduces a facile strategy for designing and fabricating high-performance hierarchically structured zeolite adsorbents and even catalysts for practical applications.
3D打印技术是一种快速精确制造具有理想结构的沸石吸附剂的有前景的方法。然而，对于3D打印沸石的实际应用而言，在机械稳定性、吸附容量和扩散动力学之间进行权衡仍然是一个难以解决的挑战。在此，开发了一种简便的“3D打印与沸石焊接”策略，以构建具有分级结构的机械坚固的无粘结剂沸石整体材料（ZM-BF），其可作为CO捕获的优异结构。埃洛石纳米管用作打印油墨添加剂，其既是增强材料又是通过水热处理形成的超强界面“沸石键”整合ZM-BF的前驱体材料。ZM-BF表现出出色的机械性能，抗压强度高达5.24 MPa，高于大多数已报道的含粘结剂的结构化沸石。ZM-BF的平衡CO吸附量高达5.58 mmol g（298 K，1 bar），这在所有已报道的3D打印CO吸附剂中是最高的。引人注目的是，动态吸附突破测试证明了ZM-BF在烟气净化以及天然气和沼气升级方面优于商业基准沸石。这项工作引入了一种简便策略，用于设计和制造用于实际应用的高性能分级结构沸石吸附剂甚至催化剂。
