3D Spiderweb-like nanowire networks loading single-atom catalysts in capillary array as high-efficiency microreactor
3D Spiderweb-like nanowire networks loading single-atom catalysts in capillary array as high-efficiency microreactor
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DOI：
10.1016/j.cej.2022.139700
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发表时间：
2022-10
影响因子：
15.1
通讯作者：
Gonggang Liu;Zhaocai He;Yuanjuan Bai;Yanran Li;Chongqing Wang;Jinbo Hu;Xian-jun Li;Yongfeng Luo;Daoyong Chen
中科院分区：
文献类型：
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作者：
Gonggang Liu;Zhaocai He;Yuanjuan Bai;Yanran Li;Chongqing Wang;Jinbo Hu;Xian-jun Li;Yongfeng Luo;Daoyong Chen
快速流体输送和高反应效率是设计高性能单片微反应器不可调和的指标。本文从微观结构设计和单原子催化剂（SACs）利用两方面同时着手，在木材毛细管阵列中开发了具有高渗透率的三维蛛网状纳米线网络，并将成功合成的SACs集成为高效去除水中有机污染物的微反应器。超长、柔性的peg113 -b- p4vp104蠕虫状胶束在木材毛细管中形成松散的微气凝胶，通过非共价和物理纠缠相互作用获得三维蛛网状纳米线网络。直线型微通道阵列中丰富的纳米线网络允许大量的催化剂活性组分加载位点，大大提高了接触反应效率。同时，纳米线网络的网格状多孔结构较好地保持了木毛细管阵列的良好渗透性。此外，吡啶在P4VP嵌段中的强配位相互作用和核-壳结构蠕虫状胶束的约束作用使SACs具有高密度、均匀分布的特点。作为概念验证，我们展示了木材毛细管阵列中三维蜘蛛网状纳米线网络和分散良好的Pd-N4/Fe-N4SACs的独特微观结构的集成，实现了亚甲基蓝的高去除效率和水的快速传质。重要的是，这项工作为原子分散催化剂提供了一种简单且可扩展的方法，为在其他潜在重要反应中设计高性能微反应器铺平了道路。
Rapid fluid transport and high reaction efficiency are known as irreconcilable indicators for designing high-performance monolithic microreactors. Here, proceeding from microstructure design and single-atom catalysts (SACs) utilization simultaneously, we developed 3D spiderweb-like nanowire networks in wood capillary array owning high permeability integrated with successfully synthesized SACs as high-efficiency microreactor for organic pollutant removal from water. The 3D spiderweb-like nanowire networks could be obtained by noncovalent and physical entanglement interactions of ultralong and flexible PEG113-b-P4VP104worm-like micelles forming loosened micro-aerogel in the wood capillary. Abundant nanowire networks in straight microchannels array allow vast quantities of catalyst active component loading sites and greatly increase contact reaction efficiency. Meanwhile, the grid-like porous structure of the nanowire networks preferably maintains good permeability of the wood capillary array. Furthermore, strong coordination interaction of pyridine in P4VP block and confinement effect from core-shell structured worm-like micelles afford uniformly distributed SACs with high density. As a proof of concept, we demonstrate an integration of unique microstructure from 3D spiderweb-like nanowire networks in wood capillary array and well dispersed Pd-N4/Fe-N4SACs enables high removal efficiency for methylene blue and fast mass transfer for water. Importantly, this work provides a facile and scalable method for atomically dispersed catalysts, paving the way for designing high-performance microreactors in other potentially important reactions.