Journal
JOURNAL OF MATERIALS CHEMISTRY A
Volume 9, Issue 2, Pages 1230-1239Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/d0ta10696h
Keywords
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Funding
- Ministry of Science and Technology of Taiwan [MOST 106-2113-M-029-006-MY2, MOST 107-2622-M-029-001-CC2, MOST 109-2113-M-029-002-]
- Tunghai University
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The study demonstrates that molybdenum sulfide on nickel foil (1T-MoS2-Ni) with low crystallinity is an active NRR electrocatalyst with high faradaic efficiency. In situ X-ray diffraction and ex situ X-ray photoemission analyses show that lithium ions are intercalated into the 1T-MoS2 layers during the NRR process.
The Haber-Bosch process is widely used to convert atmospheric nitrogen (N-2) into ammonia (NH3). However, the extreme reaction conditions and abundant carbon released by this process make it important to develop a greener NH3 production method. The electrochemical nitrogen reduction reaction (NRR) is an attractive alternative to the Haber-Bosch process. Herein, we demonstrated that molybdenum sulfide on nickel foil (1T-MoS2-Ni) with low crystallinity was an active NRR electrocatalyst. 1T-MoS2-Ni achieved a high faradaic efficiency of 27.66% for the NRR at -0.3 V (vs. RHE) in a LiClO4 electrolyte. In situ X-ray diffraction and ex situ X-ray photoemission analyses showed that lithium ions were intercalated into the 1T-MoS2 layers during the NRR. Moreover, theoretical calculations revealed the differences between six membered rings formed in the 1T-MoS2 and 2H-MoS2 systems with Li intercalation. The bond distances of d(Mo-N) and d(N-Li) of in Li-1T-MoS2 were found to be shorter than those in Li-2H-MoS2, resulting in a lower energy barrier of N-2 fixation and higher NRR activity. Therefore, 1T-MoS2-Ni is promising as a scalable and low-cost NRR electrocatalyst with lower power consumption and carbon emission than the Haber-Bosch process.
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