CIESC Journal ›› 2020, Vol. 71 ›› Issue (10): 4820-4825.DOI: 10.11949/0438-1157.20200714

• Material science and engineering, nanotechnology • Previous Articles     Next Articles

Theoretical study on electrocatalytic nitrogen fixation performance of two-dimensional AuP2

Xiaorong ZHU(),Yafei LI()   

  1. School of Chemistry and Materials Science, Nanjing Normal University, Nanjing 210023, Jiangsu, China
  • Received:2020-06-05 Revised:2020-07-24 Online:2020-10-05 Published:2020-10-05
  • Contact: Yafei LI

二维AuP2材料电催化固氮性能的理论研究

朱晓蓉(),李亚飞()   

  1. 南京师范大学化学与材料科学学院,江苏 南京 210023
  • 通讯作者: 李亚飞
  • 作者简介:朱晓蓉(1994—),女,博士研究生,xiaorongzhu_njnu@163.com
  • 基金资助:
    国家自然科学基金面上项目(21873050)

Abstract:

The electrochemical conversion of nitrogen (N2) and water (H2O) into ammonia (NH3) under normal temperature and pressure conditions is a green and environmentally friendly method of ammonia synthesis. However, because N2 has a very high chemical inertness, an electrocatalyst must be used to accelerate the kinetic process of the reaction. In this paper, we use density functional theory calculations to reveal that AuP2, a new type of two-dimensional inorganic material, has good catalytic activity for the electrochemical reduction of N2 to NH3. In the two-dimensional AuP2 material, significant charge transfer occurs between Au and P atoms due to the difference in electronegativity, so that positively charged P can be used as an active site to promote nitrogen reduction. Our calculations show that the rate-determining step of the entire reaction is the process of generating *NNH from N2 with a limiting voltage of 1.2 V, and the catalytic activity can be comparable to some metal catalysts. This work provides new ideas for the design of high-efficiency nitrogen reduction electrocatalysts.

Key words: two-dimensional materials, AuP2, electrocatalysis, nitrogen reduction reaction, density functional theory calculations

摘要:

通过电化学反应将氮气(N2)和水(H2O)在常温常压的条件下转化为氨气(NH3)是一种绿色环保的合成氨方法。但由于N2具有非常高的化学惰性,必须借助电催化剂来加速反应的动力学过程。通过密度泛函理论计算揭示出新型二维无机材料AuP2对N2电化学还原制NH3具有很好的催化活性。在二维AuP2材料中,Au与P之间由于电负性差异发生显著的电荷转移,使带有正电荷的P可作为活性位点促进氮还原。计算表明整个反应的速控步是N2生成*NNH的过程,限制电压为1.2 V,催化活性可以跟部分金属催化剂相媲美。为设计高效氮还原电催化剂提供了新的思路。

关键词: 二维材料, AuP2, 电催化, 氮还原, 密度泛函理论计算

CLC Number: