Gou Zhaolin, Qu Huiqi, Liu Hanfang, Ma Yiru, Zong Lingbo, Li Bin, Xie Congxia, Li Zhenjiang, Li Wei, Wang Lei
Key Laboratory of Eco-chemical Engineering, Taishan Scholar Advantage and Characteristic Discipline Team of Eco-Chemical Process and Technology, Qingdao, 266042, China.
College of Chemistry and Molecular Engineering, Qingdao University of Science and Technology, Qingdao, 266042, China.
Small. 2022 Apr;18(15):e2106581. doi: 10.1002/smll.202106581. Epub 2022 Feb 28.
2D heterostructures provide a competitive platform to tailor electrical property through control of layer structure and constituents. However, despite the diverse integration of 2D materials and their application flexibility, tailoring synergistic interlayer interactions between 2D materials that form electronically coupled heterostructures remains a grand challenge. Here, the rational design and optimized synthesis of electronically coupled N-doped mesoporous defective carbon and nitrogen modified titanium carbide (Ti C ) in a 2D sandwiched heterostructure, is reported. First, a F127-polydopamine single-micelle-directed interfacial assembly strategy guarantees the construction of two surrounding mesoporous N-doped carbon monolayers assembled on both sides of Ti C nanosheets. Second, the followed ammonia post-treatment successfully introduces N elements into Ti C structure and more defective sites in N-doped mesoporous carbon. Finally, the oxygen reduction reaction (ORR) and theoretical calculation prove the synergistic coupled electronic effect between N-Ti C and defective N-doped carbon active sites in the 2D sandwiched heterostructure. Compared with the control 2D samples (0.87-0.88 V, 4.90-5.15 mA cm ), the coupled 2D heterostructure possesses the best onset potential of 0.90 V and limited density current of 5.50 mA cm . Meanwhile, this catalyst exhibits superior methanol tolerance and cyclic durability. This design philosophy opens up a new thought for tailoring synergistic interlayer interactions between 2D materials.
二维异质结构提供了一个具有竞争力的平台，可通过控制层结构和成分来调整电学性质。然而，尽管二维材料有多种集成方式及其应用灵活性，但调整形成电子耦合异质结构的二维材料之间的协同层间相互作用仍然是一个巨大的挑战。在此，报道了二维夹心异质结构中电子耦合的氮掺杂介孔缺陷碳和氮改性碳化钛（TiC）的合理设计与优化合成。首先，一种F127-聚多巴胺单胶束导向的界面组装策略确保了在TiC纳米片两侧构建两个环绕的介孔氮掺杂碳单层。其次，随后的氨后处理成功地将氮元素引入TiC结构以及氮掺杂介孔碳中更多的缺陷位点。最后，氧还原反应（ORR）和理论计算证明了二维夹心异质结构中N-TiC与缺陷氮掺杂碳活性位点之间的协同耦合电子效应。与对照二维样品（0.87 - 0.88 V，4.90 - 5.15 mA cm）相比，耦合的二维异质结构具有最佳的起始电位0.90 V和有限密度电流5.50 mA cm。同时，这种催化剂表现出优异的甲醇耐受性和循环耐久性。这种设计理念为调整二维材料之间的协同层间相互作用开辟了新思路。
