Fe-embedded Au (111) monolayer as an electrocatalyst for N2 reduction reaction: A first-principles investigation

Fu, Ling; Yan, Longbin; Lin, Long; Xie, Kun; Zhu, Linghao; He, Chaozheng; Zhang, Zhanying

doi:10.1016/j.jallcom.2021.159907

Cited by 62 publications

(11 citation statements)

References 70 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…4 In recent years, electrocatalysis has been applied to various catalytic reactions, including the oxygen reduction reaction (ORR), [5][6][7][8] oxygen evolution reaction (OER), [9][10][11][12] CO 2 reduction reaction (CO 2 RR), [13][14][15] hydrogen evolution reaction (HER), 16 and nitrogen reduction reaction (NRR). [17][18][19][20][21][22][23][24][25] Among these electrocatalytic processes, the NRR process can be used for the production of ammonia. Crucially, the NRR can be carried out using renewable electricity and allows NH 3 synthesis under ambient conditions, making it suitable for alleviating the growing energy and environmental crises.…”

Section: Introductionmentioning

confidence: 99%

Density functional theory study of a two-atom active site transition-metal/iridium electrocatalyst for ammonia synthesis

Song

Liu

et al. 2022

J. Mater. Chem. A

Self Cite

View full text Add to dashboard Cite

show abstract

Section: Introductionmentioning

confidence: 99%

Density functional theory study of a two-atom active site transition-metal/iridium electrocatalyst for ammonia synthesis

Song

Liu

et al. 2022

J. Mater. Chem. A

Self Cite

View full text Add to dashboard Cite

show abstract

“…The adjunction between the (111) plane of NPG and the (101) plane of SnS 2 was made possible through the S atoms of SnS 2 , as mostly this particular plane of Au actively interacts with the S atoms (soft− soft interaction) at the cost of the low energy barrier, which in turn facilitates the electrocatalytic NRR process as shown in several reports. 15,48 It was presumed that this interface formation apparently affected the out of plane stretching vibration of the S atoms, 49,50 bonded to the Au atoms of NPG as reflected in the peak shifting of the A 1g phonon mode 51 at ∼311 cm −1 in the Raman spectrum of NPG@SnS 2 in Figure 2b, which was positioned at ∼307 cm −1 for pristine SnS 2 . However, the elemental composition (Table S1) from the EDS analysis (Figure S5) at the visible interface of NPG@SnS 2 corroborated the formation of phase-pure SnS 2 over NPG with the atomic weight percentage of Sn being 7.68% and that of S being almost its double, that is 13.04%.…”

Section: Resultsmentioning

confidence: 99%

Alteration of Electronic Band Structure via a Metal–Semiconductor Interfacial Effect Enables High Faradaic Efficiency for Electrochemical Nitrogen Fixation

Biswas¹,

Nandi

Kamboj³

et al. 2021

ACS Nano

View full text Add to dashboard Cite

The interface engineering strategy has been an emerging field in terms of material improvisation that not only alters the electronic band structure of a material but also induces beneficial effects on electrochemical performances. Particularly, it is of immense importance for the environmentally benign electrochemical nitrogen reduction reaction (NRR), which is potentially impeded by the competing hydrogen evolution reaction (HER). The main problem lies in the attainment of the desired current density at a negotiable potential where the NRR would dominate over the HER, which in turn hampers the Faradaic efficiency for the NRR. To circumvent this issue, catalyst development becomes necessary, which would display a weak affinity for H-adsorption suppressing the HER at the catalyst surface. Herein, we have adopted the interfacial engineering strategy to synthesize our electrocatalyst NPG@SnS2, which not only suppressed the HER on the active site but yielded 49.3% F.E. for the NRR. Extensive experimental work and DFT calculations regarded that due to the charge redistribution, the Mott–Schottky effect, and the band bending of SnS2 across the contact layer at the interface of NPG, the d-band center for the surface Sn atoms in NPG@SnS2 lowered, which resulted in favored adsorption of N2 on the Sn active site. This phenomenon was driven even forward by the upshift of the Fermi level, and eventually, a decrease was seen in the work function of the heterostructure that increased the conductivity of the material as compared to pristine SnS2. This strategy thus provides a field to methodically suppress the HER in the realm of improving the Faradaic efficiency for the NRR.

show abstract

“…Graphene-based devices, including photovoltaics [ 7 ], spintronic devices [ 8 ], gas sensors [ 9 ] and graphene-based composite materials [ 10 ], have attracted wide attention in the field of two-dimensional materials owing to their excellent electronic, mechanical, photonic and thermal characters [ 11 , 12 , 13 , 14 , 15 , 16 , 17 , 18 , 19 , 20 , 21 , 22 ]. In addition, graphene has been proved to be a promising carrier for single-atom catalysts (SACs) due to its orbital hybridization and charge transfer between the substrate and single atoms [ 23 , 24 ].…”

Section: Introductionmentioning

confidence: 99%

Adsorption Characteristics of Gas Molecules Adsorbed on Graphene Doped with Mn: A First Principle Study

et al. 2022

Self Cite

View full text Add to dashboard Cite

Herein, the adsorption characteristics of graphene substrates modified through a combined single manganese atom with a vacancy or four nitrogen to CH2O, H2S and HCN, are thoroughly investigated via the density functional theory (DFT) method. The adsorption structural, electronic structures, magnetic properties and adsorption energies of the adsorption system have been completely analyzed. It is found that the adsorption activity of a single vacancy graphene-embedded Mn atom (MnSV-GN) is the largest in the three graphene supports. The adsorption energies have a good correlation with the integrated projected crystal overlap Hamilton population (-IpCOHP) and Fermi softness. The rising height of the Mn atom and Fermi softness could well describe the adsorption activity of the Mn-modified graphene catalyst. Moreover, the projected crystal overlap Hamilton population (-pCOHP) curves were studied and they can be used as the descriptors of the magnetic field. These results can provide guidance for the development and design of graphene-based single-atom catalysts, especially for the support effect.

show abstract

Fe-embedded Au (111) monolayer as an electrocatalyst for N2 reduction reaction: A first-principles investigation

Cited by 62 publications

References 70 publications

Density functional theory study of a two-atom active site transition-metal/iridium electrocatalyst for ammonia synthesis

Density functional theory study of a two-atom active site transition-metal/iridium electrocatalyst for ammonia synthesis

Alteration of Electronic Band Structure via a Metal–Semiconductor Interfacial Effect Enables High Faradaic Efficiency for Electrochemical Nitrogen Fixation

Adsorption Characteristics of Gas Molecules Adsorbed on Graphene Doped with Mn: A First Principle Study

Contact Info

Product

Resources

About