Journal
NANO ENERGY
Volume 78, Issue -, Pages -Publisher
ELSEVIER
DOI: 10.1016/j.nanoen.2020.105391
Keywords
Boron doping; MoS2 nanosheets; N equivalent to N bond polarization; Nitrogen reduction reaction; Electrocatalysis
Categories
Funding
- Swedish Research Council [2017-00935]
- Swedish Energy Agency
- Knut and Alice Wallenberg Foundation [KAW 2016.0072]
- China Scholarship Council (CSC)
- Swedish National Infrastructure for Computing (SNIC)
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Ammonia production consumes-2% of the annual worldwide energy supply, therefore strategic alternatives for the energy-intensive ammonia synthesis through the Haber-Bosch process are of great importance to reduce our carbon footprint. Inspired by MoFe-nitrogenase and the energy-efficient and industrially feasible electrocatalytic synthesis of ammonia, we herein establish a catalytic electrode for artificial nitrogen fixation, featuring a carbon fiber cloth fully grafted by boron-doped molybdenum disulfide (B-MoS2/CFC) nanosheets. An excellent ammonia production rate of 44.09 mu g h(-1) cm(-2) is obtained at-0.2 V versus the reversible hydrogen electrode (RHE), whilst maintaining one of the best reported Faradaic efficiency (FE) of 21.72% in acidic aqueous electrolyte (0.1 M HCl). Further applying a more negative potential of-0.25 V renders the best ammonia production rate of 50.51 mu g h(-1) cm(-2). A strong-weak electron polarization (SWEP) pair from the different electron accepting and back-donating capacities of boron and molybdenum (2p shell for boron and 5d shell for molybdenum) is proposed to facilitate greatly the adsorption of non-polar dinitrogen gas via N equivalent to N bond polarization and the first protonation with large driving force. In addition, for the first time a visible light driven photo-electrochemical (PEC) cell for overall production of ammonia, hydrogen and oxygen from water + nitrogen, is demonstrated by coupling a bismuth vanadate BiVO4 photo-anode with the B-MoS2/CFC catalytic cathode.
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