Chen Li Xin, Jiang Ming, Lu Zhuole, Gao Chan, Chen Zhi Wen, Singh Chandra Veer
Department of Materials Science and Engineering, University of Toronto, 184 College Street, Suite 140, Toronto, Ontario M5S 3E4, Canada.
Department of Mechanical and Industrial Engineering, University of Toronto, 5 King's College Road, Toronto, Ontario M5S 3G8, Canada.
ACS Appl Mater Interfaces. 2021 Oct 13;13(40):47541-47548. doi: 10.1021/acsami.1c12054. Epub 2021 Sep 28.
Pt-based materials are the state-of-the-art catalysts for hydrogen evolution reaction (HER) and oxygen reduction reaction (ORR); however, there is still much room to improve the catalytic activity and enhance the stability of Pt-based catalysts. In this work, two-dimensional (2D) graphdiyne (GDY) with uniform distributed pores was applied to cover the Pt surface for catalyzing HER and ORR through density functional theory (DFT) calculations. The 2D confinement induced by GDY was found to improve the catalytic performance of the Pt catalyst from three aspects: (1) the 2D covering layer increases the stability of the Pt catalyst through forming the heterogeneous interface of GDY/Pt(111); (2) GDY/Pt(111) shows better catalytic activities of HER and ORR, with the smaller average overpotential values of 0.26 and 0.51 V, respectively, compared with those (0.29 V for HER, 0.62 V for ORR) on the Pt catalyst; (3) the confinement effect of GDY weakens the adsorption energy of CO to -1.81 eV (average value) from -2.14 eV on Pt(111), inhibiting CO poisoning. This work sheds new light on 2D confinement effects for HER and ORR, which opens up a new strategy for improving the catalytic performance of Pt-based catalysts.
基于铂的材料是析氢反应（HER）和氧还原反应（ORR）的先进催化剂；然而，提高基于铂的催化剂的催化活性和增强其稳定性仍有很大空间。在这项工作中，通过密度泛函理论（DFT）计算，将具有均匀分布孔隙的二维（2D）石墨炔（GDY）应用于覆盖铂表面以催化HER和ORR。发现由GDY引起的二维限制从三个方面提高了铂催化剂的催化性能：（1）二维覆盖层通过形成GDY/Pt(111)的异质界面提高了铂催化剂的稳定性；（2）GDY/Pt(111)表现出更好的HER和ORR催化活性，与铂催化剂上的平均过电位值（HER为0.29 V，ORR为0.62 V）相比，分别为更小的0.26和0.51 V；（3）GDY的限制效应将CO在Pt(111)上的吸附能从-2.14 eV减弱至-1.81 eV（平均值），抑制了CO中毒。这项工作为HER和ORR的二维限制效应提供了新的见解，为提高基于铂的催化剂的催化性能开辟了新策略。
