Deng Kai, Zhou Tongqing, Mao Qiqi, Wang Shengqi, Wang Ziqiang, Xu You, Li Xiaonian, Wang Hongjing, Wang Liang
State Key Laboratory Breeding Base of Green-Chemical Synthesis Technology, College of Chemical Engineering, Zhejiang University of Technology, Hangzhou, 310014, P. R. China.
Adv Mater. 2022 May;34(18):e2110680. doi: 10.1002/adma.202110680. Epub 2022 Mar 28.
The design of defects and porous structures into metallene with functional surfaces is highly desired to improve its permeability, surface area, and active sites, but remains a great challenge. In this work, polyallylamine-encapsulated Ir metallene with defects and porous structure (Ir@PAH metallene) is easily fabricated by a one-step wet chemical reduction method. The Ir@PAH metallene exhibits excellent hydrogen evolution reaction (HER) performance with an overpotential of only 14 mV at 10 mA cm , a low Tafel slope of 31.2 mV dec , and almost no activity decay after stability test. The abundant defects and pores as well as several-atomic-layer nanosheet structures of Ir@PAH metallene provide a large specific surface area, high conductivity, and efficient mass transport/diffusion. In addition, surface-functionalized PAH molecules can modulate the electronic structure through strong Ir-N interaction and act as proton carriers to capture hydrogen ions, which is very beneficial for the HER in acidic media. This work provides a useful strategy for the synthesis of the defective and porous metallene with functionalized surfaces for various catalytic applications.
在具有功能表面的金属烯中设计缺陷和多孔结构以提高其渗透性、表面积和活性位点是非常理想的，但仍然是一个巨大的挑战。在这项工作中，通过一步湿化学还原法轻松制备了具有缺陷和多孔结构的聚烯丙胺封装的铱金属烯（Ir@PAH金属烯）。Ir@PAH金属烯表现出优异的析氢反应（HER）性能，在10 mA cm 时过电位仅为14 mV，塔菲尔斜率低至31.2 mV dec ，稳定性测试后几乎没有活性衰减。Ir@PAH金属烯丰富的缺陷和孔隙以及几个原子层的纳米片结构提供了大的比表面积、高导电性和高效的质量传输/扩散。此外，表面功能化的PAH分子可以通过强烈的Ir-N相互作用调节电子结构，并作为质子载体捕获氢离子，这对酸性介质中的HER非常有利。这项工作为合成具有功能化表面的缺陷和多孔金属烯用于各种催化应用提供了一种有用的策略。
