Molten Salt-Directed Catalytic Synthesis of 2D Layered Transition-Metal Nitrides for Efficient Hydrogen Evolution
Molten Salt-Directed Catalytic Synthesis of 2D Layered Transition-Metal Nitrides for Efficient Hydrogen Evolution
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DOI：
10.1016/j.chempr.2020.06.037
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发表时间：
2020-09-10
期刊：
影响因子：
23.5
通讯作者：
Qiao, Shi-Zhang
中科院分区：
文献类型：
--
作者：
Jin, Huanyu;Gu, Qinfen;Qiao, Shi-Zhang
二维层状过渡金属氮化物(TMN)的快速合成对于超导、电磁干扰屏蔽和能源相关应用等新技术的发展具有重要意义。然而，制备具有天然2D层状结构的TMN在热力学上是困难的，严格的合成限制限制了对这类重要功能材料的探索。在这里，我们使用碱性熔盐作为催化剂，在常压下实现了一系列2D层状TMN的简单和大规模(超过十克)的合成，如MoN1.2，WN1.5和Mo0.7W0.3N1.2。非原位实验表明，熔盐通过保证气-液合成和形成TMN-盐-TMN超结构作为中间体，降低了二维层状TMN的形成能。得到的2D层状TMN在析氢反应中表现出优异的性能，展示了2D层状TMN在能源相关应用和其他领域的巨大潜力。
Facile synthesis of single-crystal 2D layered transition-metal nitrides (TMNs) is of crucial importance for the development of forthcoming technologies, such as superconducting, electromagnetic interference shielding, and energy-related applications. However, the fabrication of TMNs with natural 2D layered structure is thermodynamically difficult, in which stringent synthesis constraints have limited the exploration of this important class of functional materials. Here, we employed alkali molten salts as catalysts to achieve facile and large-scale (over decagram) synthesis of a family of 2D layered TMNs, such as MoN1.2, WN1.5, and Mo0.7W0.3N1.2, under atmospheric pressure. Ex-situ experiments reveal that the molten salt can lower the formation energy of 2D layered TMNs by assuring a liquid-gas synthesis and forming a TMN-salt-TMN superstructure as an intermediate. The resultant 2D layered TMNs show superior performance in hydrogen evolution reaction, demonstrating the immense potential of 2D layered TMNs for energy-related applications and beyond.