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Oxygen vacancy engineering in spinel-structured nanosheet wrapped hollow polyhedra for electrochemical nitrogen fixation under ambient conditions
Ist Teil von
Journal of materials chemistry. A, Materials for energy and sustainability, 2020-01, Vol.8 (4), p.1652-1659
Ort / Verlag
Cambridge: Royal Society of Chemistry
Erscheinungsjahr
2020
Quelle
Alma/SFX Local Collection
Beschreibungen/Notizen
Electrochemical nitrogen-to-ammonia conversion by the nitrogen reduction reaction (NRR) under ambient conditions is regarded as a potential approach to tackle the energy-intensive Haber-Bosch process with excessive CO
2
emission. However, the NRR is still restricted by low faradaic efficiency and NH
3
yield, which is due to the chemical inertness of N-related groups for efficient adsorption/activation on the electrocatalysts. Here, a series of spinel-structured nanosheet wrapped hollow nitrogen-doped carbon polyhedra with abundant oxygen vacancies are constructed successfully. From theoretical aspects, these materials show increased charge density on their surface for enhanced capture and activation of N
2
molecules. As a result, oxygen vacancy-rich NiCo
2
O
4
on hollow N-carbon polyhedra (
V
o
-rich NiCo
2
O
4
@HNCP) shows outstanding electrocatalytic NRR performance with high production yield (NH
3
: 4.1 μg h
−1
cm
−2
/17.8 μg h
−1
mg
−1
; faradaic efficiency: 5.3%) and high stability under ambient conditions and is superior to the counterpart oxygen vacancy-poor electrocatalysts. Oxygen vacancy engineering introduces a new concept for rational design of advanced NRR catalysts for energy conversion systems.
Electrochemical nitrogen-to-ammonia conversion under ambient conditions is realized by an oxygen vacancy-rich spinel structured materials, showing relatively high faradaic efficiency and yields.