Journal
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
Volume 7, Issue 12, Pages 10214-10220Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acssuschemeng.9b00983
Keywords
Electrochemical N-2 reduction reaction; Generalized coordination number; Coordination-activity plot; First-principle calculation; Nanoporous gold
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Funding
- National Natural Science Foundation of China [21603161, 51671145]
- NSFC [51761165012]
- Macau Science and Technology Fund (FDCT) [002/2017/AFJ]
- Tianjin Municipal Science and Technology Commission [16JCYBJC41600, 15JCYBJC52700]
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Exploration of efficient catalysts is a priority for the electrochemical nitrogen reduction reaction (NRR) under ambient temperature and pressure. Recently, several nano-structured gold (Au) catalysts have shown impressive catalytic activities toward NRR However, the atomic origin of high catalytic activities of Au catalysts is vague. In this work, a quantitative relationship between the generalized coordination number (GCN) and NRR activity is established. In particular, the NRR activity is linearly increased with the decrease of GCN values of Au surface atoms. As a proof-of-concept experiment, the NRR activity of nanoporous gold (NPG) with a high proportion of low-coordinated surface atoms is investigated and compared with that of Au octahedra (OCTA) enclosed with (111) facets. As expected, NPG exhibits a high NH3 production rate of 30.5 mu g h(-1) mg(-1), which is 5.8 times larger than that of Au OCTA. In addition, the excellent catalytic performance of NPG can be retained for 21 h by showing constant current density, NH3 production rate, and faradaic efficiency. The findings in this work would provide guiding principles for designing efficient NRR catalysts.
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