Delicate Tuning of the Ni/Co Ratio in Bimetal Layered Double Hydroxides for Efficient N2 Electroreduction

Zhi Zou, Lei Wu, Fangqi Yang, Chenliang Cao, Qiangguo Meng, Junhui Luo, Weizhen Zhou, Zhikun Tong, Jingwen Chen, Shixia Chen, Shaodong Zhou, Jun Wang, Shuguang Deng

Research output: Contribution to journalArticlepeer-review

Abstract

Electroreduction of N2 to NH3 at ambient conditions using renewable electricity is promising, but developing efficient electrocatalysts is still challenging due to the inertness of N≡N bonds. Layer double hydroxides (LDHs) composed of first-row transition metals with empty d-orbitals are theoretically promising for N2 electroreduction (NRR) but rarely reported. Herein, hollow NiCo-LDH nanocages with different Ni/Co ratios were prepared, and their electronic structures and atomic arrangements were critical. The synergetic mechanisms of Ni and Co ions were revealed, and the optimized catalytic sites were proposed. Besides, in-situ Raman spectroscopy and 15N2 isotopic labeling studies were applied to detect reaction intermediates and confirm the origin of NH3. As a result, high NH3 yield of 52.8 μg h−1 mgcat−1 and faradaic efficiency of 11.5 % were obtained at −0.7 V, which are top-ranking among Co/Ni-based NRR electrocatalysts. This work elucidates the structure–activity relationship between LDHs and NRR and is instructive for rational design of LDH-based electrocatalysts.

Original languageEnglish (US)
Article numbere202200127
JournalChemSusChem
Volume15
Issue number6
DOIs
StatePublished - Mar 22 2022
Externally publishedYes

Keywords

  • N electroreduction
  • Raman spectroscopy
  • electrode materials
  • layered double hydroxides
  • structure–activity relationship

ASJC Scopus subject areas

  • Environmental Chemistry
  • Chemical Engineering(all)
  • Materials Science(all)
  • Energy(all)

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