Journal
CHEMICAL ENGINEERING JOURNAL
Volume 430, Issue -, Pages -Publisher
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2021.132694
Keywords
Electrochemical ammonia synthesis; Metal-organic framework; Fe2O3@MoS2 composites; Density functional theory
Categories
Funding
- National Natural Science Foundationof China [21203227, 51872173]
- Natural Science Founda-tion of Shandong Province [ZR2016BM33]
- Research Foundation for Talented Scholars of Qingdao Agricultural University [6631120039, 6631113335]
- National College Student Inno-vation and Entrepreneurship Training Program [S202010435041]
- University of Science and Technology of China
- Taishan Scholars Program of Shan-dong Province [tsqn201812068]
- Science and Technology Special Project of Qingdao City [20-3-4-3-nsh]
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This study presents a highly efficient electrocatalyst Fe2O3@-MoS2 for electrochemical ammonia synthesis (EAS) at ambient conditions. The Fe2O3@-MoS2 catalyst demonstrates remarkable ammonia yield and high faradaic efficiency, along with superior electrochemical stability. Density functional theory (DFT) calculations reveal that Fe2O3@-MoS2 is capable of activating inert N-2 molecules more effectively than MoS2.
Electrochemical ammonia synthesis (EAS) is considered to be an ecofriendly and sustainable method for artificial N-2 fixation. It is urgent to develop cost-effective and efficient electrocatalysts for EAS because present catalysts have low activity and poor selectivity. Herein, Fe2O3 nanoparticles anchored on MoS2 nanoflowers (Fe2O3@-MoS2) were developed as a highly efficient EAS electrocatalyst under ambient conditions. Electrochemical measurements indicate that Fe2O3@MoS2 achieves a remarkable NH3 yield of 112.15 mu g h(-1) mgcat(-1) at -0.6 V vs. reversible hydrogen electrode (RHE) and a high faradaic efficiency (FE) of 8.62% at -0.4 V vs. RHE in 0.1 M Na2SO4, much better than the EAS performance of separate MoS2 and Fe2O3. The superior electrochemical stability is confirmed by long-term (at least 24 h) continuous tests. Density functional theory (DFT) calculations show that Fe2O3@MoS2, compared to MoS2, is better able to activate inert N-2 molecules, as reflected by its greater adsorption energy (-0.32 eV vs. -0.10 eV), greater N equivalent to N bond distance (1.223 angstrom vs. 1.159 angstrom), lower energy barrier (0.40 eV vs. 0.78 eV), and greater charge transfer from active sites to N-2 molecules (1.16 e(-) vs. 0.62 e(-)). Thus, this work provides new perspectives on the development of efficient EAS catalysts using MoS2-based materials as the substrate.
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