Abstract:Electrochemical NO-to-NH3 conversion (NORR) offers a promising pathway to achieve both harmful NO treatment and effective NH3 electrosynthesis. Main group p-block metal catalysts are promising NORR candidates but remain largely...
“…The charge-density difference map (Figure b) shows a remarkable charge transfer (−0.84 |e|) from the bridge Pd site to *NO 3 for effective NO 3 – activation. Meanwhile, both charge accumulation and depletion occur on *NO 3 , suggesting that the bridge Pd site polarizes *NO 3 via a charge “donation–back-donation” mechanism. − In addition, the corresponding partial density of states analysis (Figure S12) displays a pronounced hybridization between the *NO 3 p and Pd d orbitals, indicating a strong Pd–*NO 3 interaction and further confirming the powerful NO 3 – activation on the bridge Pd site of PdP 2 (011). − …”
Palladium phosphides are explored as efficient catalysts
for the
electrocatalytic reduction of nitrate to ammonia (NRA). The explored
PdP2 nanoparticles on reduced graphene oxide exhibit the
maximum NH3 Faradaic efficiency of 98.2% with a corresponding
NH3 yield rate of 7.6 mg h–1 cm–2 at −0.6 V (RHE). Theoretical calculations reveal that a PdP2 (011) surface can not only effectively activate and hydrogenate
NO3
– via a NOH pathway but also retard
H adsorption to inhibit the competitive hydrogen evolution reaction.
“…The charge-density difference map (Figure b) shows a remarkable charge transfer (−0.84 |e|) from the bridge Pd site to *NO 3 for effective NO 3 – activation. Meanwhile, both charge accumulation and depletion occur on *NO 3 , suggesting that the bridge Pd site polarizes *NO 3 via a charge “donation–back-donation” mechanism. − In addition, the corresponding partial density of states analysis (Figure S12) displays a pronounced hybridization between the *NO 3 p and Pd d orbitals, indicating a strong Pd–*NO 3 interaction and further confirming the powerful NO 3 – activation on the bridge Pd site of PdP 2 (011). − …”
Palladium phosphides are explored as efficient catalysts
for the
electrocatalytic reduction of nitrate to ammonia (NRA). The explored
PdP2 nanoparticles on reduced graphene oxide exhibit the
maximum NH3 Faradaic efficiency of 98.2% with a corresponding
NH3 yield rate of 7.6 mg h–1 cm–2 at −0.6 V (RHE). Theoretical calculations reveal that a PdP2 (011) surface can not only effectively activate and hydrogenate
NO3
– via a NOH pathway but also retard
H adsorption to inhibit the competitive hydrogen evolution reaction.
“…[16][17][18] Nevertheless, the NORR conversion efficiency is restricted by the high NORR reaction energy barriers and fierce competition from the hydrogen evolution reaction (HER), 19 and it is necessary to explore high-performance electrocatalysts to promote the NORR while retarding the HER. [20][21][22] Currently, research on the NORR is mainly focused on precious metal and non-precious metal-based materials, [23][24][25][26][27][28][29][30][31][32][33][34][35] while metal-free catalysts still lack adequate exploration. It is known that there are only limited metal reserves on the Earth and the excess use of metal catalysts would largely increase the possibility of metal contamination and environmental pollution.…”
mentioning
confidence: 99%
“…Currently, research on the NORR is mainly focused on precious metal and non-precious metal-based materials, 23–35 while metal-free catalysts still lack adequate exploration. It is known that there are only limited metal reserves on the Earth and the excess use of metal catalysts would largely increase the possibility of metal contamination and environmental pollution.…”
A metal-free boron phosphide (BP) is first explored as an effective catalyst for electrocatalytic NO reduction to NH3, showing a high NH3-Faradaic efficiency of 83.3% with an NH3 yield rate...
“…These results demonstrate that Pd can effectively absorb and activate NO on its hcp site through a mixed pathway with a low energy barrier. Considering that the HER is the major competitive reaction for the NORR, [44][45][46][47][48] we further evaluate the competitive adsorption of NO and H on the hcp site of Pd. Fig.…”
We demonstrate Pd metallene as an efficient catalyst for electrocatalytic NO reduction to NH3, showing the maximum NO-to-NH3 Faradaic efficiency of 89.6% with a corresponding NH3 yield rate of 112.5...
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