Yang Chong, Zhang Cheng, Chen Zheng-Jie, Li Yu, Yan Wen-Yuan, Yu Hai-Bin, Liu Lin
School of Materials Science and Engineering, State Key Lab for Materials Processing and Die & Mold Technology, Huazhong University of Science and Technology, Wuhan 430074, China.
Wuhan National High Magnetic Field Center and School of Physics, Huazhong University of Science and Technology, Wuhan 430074, China.
ACS Appl Mater Interfaces. 2021 Feb 17;13(6):7227-7237. doi: 10.1021/acsami.0c20832. Epub 2021 Feb 8.
Finding highly efficient and reusable catalysts for advanced oxidation processes is a crucial endeavor to resolve the severe water pollution problems. Although numerous nanocatalysts have been developed in the past few decades, their recyclability along with sustainably high catalytic efficiency still remain challenging. Here, we propose a new strategy for designing efficient and reusable catalysts, that is, introducing Cu as a reductant into a metallic glass-based catalyst and constructing three-dimensional hierarchical porous architectures via a laser 3D printing technique. The as-printed 3D porous MG/Cu catalysts exhibit exceptional catalytic efficiency in degrading RhB with a normalized rate constant approximately 620 times higher than commercial nano zero-valent iron, outperforming most reported Fenton-type catalysts so far. Strikingly, the catalysts exhibit an excellent reusability and can be used more than 100 times (the highest record so far) without apparent efficiency decay. It is revealed that Cu-doping could improve the surface reducibility and promote the electronic transfer, rendering the 3D-printed MG/Cu catalysts with a sustainably active Fe(II)-rich surface and, therefore, unprecedented reusability. This work offers a broadly applicable design route for the development of advanced catalysts with an outstanding combination of activity and reusability for wastewater treatments.
寻找用于高级氧化过程的高效且可重复使用的催化剂是解决严重水污染问题的关键努力。尽管在过去几十年中已经开发了许多纳米催化剂,但它们的可回收性以及可持续的高催化效率仍然具有挑战性。在此,我们提出了一种设计高效且可重复使用催化剂的新策略,即把铜作为还原剂引入金属玻璃基催化剂中,并通过激光3D打印技术构建三维分级多孔结构。所打印的3D多孔MG/Cu催化剂在降解罗丹明B方面表现出卓越的催化效率,其归一化速率常数比商业纳米零价铁高约620倍,优于目前报道的大多数芬顿型催化剂。引人注目的是,这些催化剂表现出出色的可重复使用性,并且可以使用100多次(这是目前的最高记录)而没有明显的效率衰减。研究表明,铜掺杂可以提高表面还原性并促进电子转移,使3D打印的MG/Cu催化剂具有富含铁(II)的可持续活性表面,从而具有前所未有的可重复使用性。这项工作为开发具有出色活性和可重复使用性组合的先进催化剂用于废水处理提供了一条广泛适用的设计路线。