Abstract
A freestanding 3D graphdiyne–cobalt nitride (GDY/Co2N) with a highly active and selective interface is fabricated for the electrochemical nitrogen reduction reaction (ECNRR). Density function theory calculations reveal that the interface-bonded GDY contributes an unique p-electronic character to optimally modify the Co-N compound surface bonding, which generates as-observed superior electronic activity for NRR catalysis at the interface region. Experimentally, at atmospheric pressure and room temperature, the electrocatalyst creates a new record of ammonia yield rate (Y (Formula presented.)) and Faradaic efficiency (FE) of 219.72 μg h−1 mgcat.−1 and 58.60 %, respectively, in acidic conditions, higher than reported electrocatalysts. Such a catalyst is promising to generate new concepts, new knowledge, and new phenomena in electrocatalytic research, driving rapid development in the field of electrocatalysis. © 2020 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.
| Original language | English |
|---|---|
| Pages (from-to) | 13021-13027 |
| Journal | Angewandte Chemie - International Edition |
| Volume | 59 |
| Issue number | 31 |
| Online published | 24 Apr 2020 |
| DOIs | |
| Publication status | Published - 27 Jul 2020 |
| Externally published | Yes |
Funding
This work was supported by the National Nature Science Foundation of China (21790050, 21790051, and 21771156), the National Key Research and Development Project of China (2016YFA0200104 and 2018YFA0703501), the Key Program of the Chinese Academy of Sciences (QYZDY-SSW-SLH015), and the Early Career Scheme (ECS) fund (Grant No.: PolyU 253026/16P) from the Research Grant Council (RGC) in Hong Kong. We would like to thank the XAFS station (beam line 1W1B) of the Beijing Synchrotron Radiation Facility for the XAS measurements.
Research Keywords
- 2D carbon allotropes
- ammonia synthesis
- graphdiyne
- heterostructures
- self-supporting electrocatalysts