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Photoactive Earth‐Abundant Iron Pyrite Catalysts for Electrocatalytic Nitrogen Reduction Reaction
Author(s) -
Chang ChiaChe,
Li SinRen,
Chou HungLung,
Lee YiCheng,
Patil Shivaraj,
Lin YingSheng,
Chang ChunChih,
Chang Yuan Jay,
Wang DiYan
Publication year - 2019
Publication title -
small
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 3.785
H-Index - 236
eISSN - 1613-6829
pISSN - 1613-6810
DOI - 10.1002/smll.201904723
Subject(s) - catalysis , electrochemistry , electrocatalyst , inorganic chemistry , ammonia production , materials science , reversible hydrogen electrode , faraday efficiency , pyrite , chemical engineering , chemistry , electrode , working electrode , organic chemistry , engineering , metallurgy
Abstract The generation of ammonia, hydrogen production, and nitrogen purification are considered as energy intensive processes accompanied with large amounts of CO 2 emission. An electrochemical method assisted by photoenergy is widely utilized for the chemical energy conversion. In this work, earth‐abundant iron pyrite (FeS 2 ) nanocrystals grown on carbon fiber paper (FeS 2 /CFP) are found to be an electrochemical and photoactive catalyst for nitrogen reduction reaction under ambient temperature and pressure. The electrochemical results reveal that FeS 2 /CFP achieves a high Faradaic efficiency (FE) of ≈14.14% and NH 3 yield rate of ≈0.096 µg min −1 at −0.6 V versus RHE electrode in 0.25 m LiClO 4 . During the electrochemical catalytic reaction, the crystal structure of FeS 2 /CFP remains in the cubic pyrite phase, as analyzed by in situ X‐ray diffraction measurements. With near‐infrared laser irradiation (808 nm), the NH 3 yield rate of the FeS 2 /CFP catalyst can be slightly improved to 0.1 µg min −1 with high FE of 14.57%. Furthermore, density functional theory calculations demonstrate that the N 2 molecule has strong chemical adsorption energy on the iron atom of FeS 2 . Overall, iron pyrite‐based materials have proven to be a potential electrocatalyst with photoactive behavior for ammonia production in practical applications.