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Adsorbing and Activating N 2 on Heterogeneous Au–Fe 3 O 4 Nanoparticles for N 2 Fixation
Author(s) -
Zhang Jin,
Ji Yujin,
Wang Pengtang,
Shao Qi,
Li Youyong,
Huang Xiaoqing
Publication year - 2020
Publication title -
advanced functional materials
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 6.069
H-Index - 322
eISSN - 1616-3028
pISSN - 1616-301X
DOI - 10.1002/adfm.201906579
Subject(s) - x ray photoelectron spectroscopy , materials science , faraday efficiency , electrochemistry , nanoparticle , adsorption , reversible hydrogen electrode , redox , desorption , catalysis , yield (engineering) , analytical chemistry (journal) , chemical engineering , nanotechnology , electrode , chemistry , reference electrode , organic chemistry , engineering , metallurgy
Electrochemical nitrogen reduction reaction (NRR) is a promising approach to convert earth‐adundant N 2 into highly value‐added NH 3 . Herein, it is demonstrated that the heterogeneous Au–Fe 3 O 4 nanoparticles (NPs) can be adopted as highly efficient catalysts for NRR. Due to the synergistic effect of the strong N 2 fixation ability of Fe 3 O 4 and the charge transfer capability of Au, the Au–Fe 3 O 4 NPs show excellent performance with a high yield (NH 3 : 21.42 µg mg cat −1 h −1 ) and a favorable faradaic efficiency (NH 3 : 10.54%) at −0.2 V (vs reversible hydrogen electrode), both of which are much better than those of the Au NPs, Fe 3 O 4 NPs, as well as core@shell Au@Fe 3 O 4 NPs. It also exhibits good stability with largely maintained performance after six cycles. The N 2 temperature‐programmed desorption, surface valance band spectra, and X‐ray photoelectron spectroscopy collectively confirm that Au–Fe 3 O 4 NPs have a strong adsorption capacity for the reaction species and suitable surface structure for electronic transfer. The theoretical calculations reveal that Fe provides the active site to fix N 2 into *N 2 H while introducing Au optimizes the adsorption of NRR intermediates, making the NRR pathway on Au–Fe 3 O 4 along an energetic‐favorable process and enhancing the NRR.