Metal-free boron carbonitride with tunable boron Lewis acid sites for enhanced nitrogen electroreduction to ammonia

Bin Chang, Lili Li, Dong Shi, Hehe Jiang, Zizheng Ai, Shouzhi Wang, Yongliang Shao, Jianxing Shen, Yongzhong Wu, Yanlu Li*, Xiaopeng Hao

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

106 Scopus citations

Abstract

From a thermodynamic point of view, electrocatalytic nitrogen reduction reaction (NRR) is possible for the carbon-based metal-free catalysts, which are gradually becoming a class of potential alternatives to metal-based catalysts. However, the clarification of true active sites and corresponding exact catalytic mechanism of metal-free catalysts is urgently required. Taking full advantage of boron “Lewis acid”, a series of boron carbonitride (BCN) materials were designed and synthesized and the “Lewis acid catalysis” sites were tuned easily by adjusting the relative contents of boron and nitrogen atoms. Boron-enriched BCN exhibited outstanding NRR performance with an ammonia yield of −8.39 μg h−1.cm−2cat. (−41.9 μg h−1.mg−1cat.) and Faradaic efficiency of −9.87 %, together with excellent stability. Density functional theory calculations indicate that the boron sites of BCN enable the low energy barrier of the NRR rate-determining steps and the spontaneity of nitrogen adsorption. Our philosophy opens a new possible avenue to explore high-performance metal-free materials for nitrogen activation.

Original languageEnglish (US)
Article number119622
JournalApplied Catalysis B: Environmental
Volume283
DOIs
StatePublished - Apr 2021

Bibliographical note

Funding Information:
B. Chang and L. L. Li contributed equally to this work. This work is supported by the National Natural Science Foundation of China (Contract No. 51872162 , 11890700 ), the Natural Science Foundation of Shandong Province (Contract ZR2018MEM013 ).

Publisher Copyright:
© 2020 Elsevier B.V.

Keywords

  • Ammonia production
  • Density functional theory
  • Electrochemical nitrogen reduction
  • Lewis acid catalysis site tuning
  • Metal-free boron carbonitride

ASJC Scopus subject areas

  • Catalysis
  • General Environmental Science
  • Process Chemistry and Technology

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