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compare. As shown in Fig. S12, the NH3 generation rate for
JUC-1000/CC||RuO2/CC at 0.4 V with 1.0 M SG shows the
similar growth as JUC-1000/CC||JUC-1000/CC. However,
JUC-1000/CC||JUC-1000/CC behaves a higher NH3 yield rate of
Conflicts of interest
There are no conflicts to declare.
DOI: 10.1039/C9CC04378K
-1
24.7 mg h-1 mgcat compared with JUC-1000/CC||RuO2/CC
Notes and references
(20.3 mg h-1 mgcat-1).
1
2
3
V. Rosc, M. Duca, M. T. de Groot and M. T. Koper, Chem.
To explore the role of ECSG in NRR, the comparison test was
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similar level in the FE values (Fig. 5a). Nevertheless, the NH3
generation rate dramatically decreases over hundredfold with
the same potential. Fig. S12, ESI reveals that the HER
polarization curve exhibits the potential of -0.74 V vs. RHE to
achieve 10 mA cm-2 in the presence of SG, which is a negative
shift of 10 mV compared with that without SG. The results
offer an exciting solution of boosting NRR that the anodic
replacement of the water oxidation significantly improves the
NH3 yield and simultaneously maintains FE value accompanied
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oxidition of SG than pure water, such a hybrid electrolyzer can
deliver higher current density to the cathode for overall
reactions including NH3 and H2 generation with lower cell
voltage input at the anode, hence increasing the conversion
with above experimental observations (Fig.5a, b). H2 evolution
is a competitive reaction, but the NH3 FE value was not
decrease with the increase of H2 yield, indicating that there is
no significant selection for the anodic replacement of ECSG.
Fig. 5c displays that the selective oxidations of SG to GA over
JUC-1000/CC||JUC-1000/CC at 0.4 V increases with the
decreasing concentration of SG during the reaction process.
The GA selectivity can reach the high value of 96.96% for 12 h
reaction with the SG conversion of 100%, suggesting little
side-products in the anode compartment. Impressively, the
NH3 yield and FE do not change significantly after 20 cycles
tested, implying excellent durability and stability of this
JUC-1000/CC catalyst (Fig. 5d).
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In summary, we have demonstrated an ECSG strategy for
promoting ambient electroreduction of N2 to NH3. The
assembled electrolyzer utilizing the catalyst, CuII-MOF/CC as
both cathode and anode, needs a cell potential of only 0.4 V to
achieve the highest NH3 yield rate of 24.7mg h-1 mgcat-1, FE of
11.90% and GA selectivity of 96.96% in 1.0 M Na2SO4
containing 1.0 M SG. Moreover, the NH3 yield is over
hundredfold enhancement and without sacrificing FE value
than that of the absence of SG. This study could be further
extended for development of other anodic replacement
oxidation reaction for energy-efficient NH3 generation.
Acknowledgements
This work was financially supported by the National Key
Scientific Instrument, the Equipment Development Project of
China (No. 21627809), the National Natural Science
Foundation of China (21605058, 21575050 and 21375047) and
the China Postdoctoral Science Foundation (2016M600517).
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