Insights into the adsorption/desorption of CO2 and CO on single-atom Fe-nitrogen-graphene catalyst under electrochemical environment

Li, Jiejie; Liu, Jian; Yang, Bo

doi:10.1016/j.jechem.2020.04.016

Cited by 39 publications

(18 citation statements)

References 58 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…Subsequently, to evaluate the CO 2 capture ability of Fe II/III N 4 C, we further calculated the adsorption energies of a CO 2 molecule directly on the surface of Fe II/III N 4 C at the three However, the little change in the geometrical parameters of CO 2 implies that the surface of Fe II/III N 4 C can faintly activate the sluggish CO 2 molecule through the physical adsorption. 34,53,54 It is controversial about which site, Fe or N site of the FeN 4 motif, is the most favorable adsorption site for CO 2 and the intermediates. 11,34,51 Thus, we attempted to systematically compare all the possible adsorption sites for the intermediates to identify the optimal adsorption sites of Fe II/III N 4 C. The optimized adsorption configurations and the Gibbs free energies listed in Table S4 indicate that the N sites can stabilize the formations of the intermediate (COOH) relative to Fe site for all the cases while CO prefers to coordinate to the Fe site.…”

Section: ■ Results and Discussionmentioning

confidence: 99%

The Influence of Single-Atom Fe^2+/3+N₄ Spin State on the Electroreduction of CO₂ to CO/HCOOH by Analyzing Proton/Electron Transfer Mechanisms and Free Energy Evolutions

Xie

Liu

et al. 2021

J. Phys. Chem. C

View full text Add to dashboard Cite

Single-atom catalysts with iron atomically dispersed on nitrogen-doped carbon matrix (FeN 4 C) is attractive for electrochemically converting carbon dioxide (CO 2 ) to carbon monoxide (CO) or formic acid (HCOOH) due to its unique properties and activity. However, the influence of the oxidation state with the different spins of Fe ion in FeN 4 C on the electrochemical mechanisms of conversion of CO 2 to CO/ HCOOH remains unclear. Herein, we got insight into the influence on the CO 2 reduction reaction (CO 2 RR) catalyzed by single-Fe coordinated by four pyridinic N ligands (Fe II/III N 4 C) using density functional theory calculations. Our calculations revealed that the two-electron CO 2 RR takes place via two sequential proton-coupled electron-transfer reactions with proton transfer from a N or C site on the FeN 4 C surface to CO 2 and at the same time electron transfer from FeN 4 C to CO 2 . The potential energy analyses uncovered that the energy barrier (0.72/0.52 eV) of the rate-limiting step for the CO/HCOOH formation catalyzed by the middle spin Fe II N 4 C M is lowest among the two oxidation states with the different spins. In addition, the overpotential (−0.03/0.29 V) of the *CO/*HCOOH formation catalyzed by Fe II N 4 C M is also significantly lower than these of the other cases. Both confirm that the Fe 2+ ion with the middle spin in FeN 4 C is most favorable for the conversion of CO 2 to CO/HCOOH. These findings thus provide valuable information to develop new strategies for designing more efficient Fe single-atom catalysts.

show abstract

Section: ■ Results and Discussionmentioning

confidence: 99%

The Influence of Single-Atom Fe^2+/3+N₄ Spin State on the Electroreduction of CO₂ to CO/HCOOH by Analyzing Proton/Electron Transfer Mechanisms and Free Energy Evolutions

Xie

Liu

et al. 2021

J. Phys. Chem. C

View full text Add to dashboard Cite

show abstract

“…As shown in Table 3, BET and pore volume of slag-based composite powder explosion inhibitors are much lower than those of MSA, because NaHCO 3 , KH 2 PO 4 and Al(OH) 3 can be effectively adsorbed and coated on MSA after the compounding process. As illustrated by Figure 4, the nitrogen adsorption desorption isotherm curve of MSA shows a type IV-H2(a) hysteresis loop in IUPAC classification, which indicates that MSA has relatively uniform channels [24,25]. The isothermal curves of WCSC-MSA-NaHCO 3 composite powder explosion inhibitor and WCSC-MSA-KH 2 PO 4 composite powder explosion inhibitor are type III.…”

Section: Compounding Process Of Industrial Solid-waste Based Composite Powder Explosion Inhibitorsmentioning

confidence: 96%

Study on a New Type of Composite Powder Explosion Inhibitor Used to Suppress Underground Coal Dust Explosion

Liu

Zhang

et al. 2021

Applied Sciences

View full text Add to dashboard Cite

At present, the world is committed to the development of environmentally friendly, sustainable and industrial safety. The effective treatment of industrial solid waste can be applied in the field of industrial safety. It is one of the ways to apply industrial solid waste to industrial safety to modify industrial solid waste and combine active powder to prepare industrial solid waste-based composite powder explosion inhibitors and apply it to underground coal dust explosion. This paper introduces the modification and preparation methods of industrial solid waste, and analyzes the good explosion suppression effect and good economic benefit of industrial solid waste-based composite powder explosion inhibitors on coal dust explosion. In this paper, four kinds of industrial solid wastes (red mud, slag, fly ash and sludge) were modified, and the modified solid waste materials with good carrier characteristics were obtained. Combined with a variety of active powders (NaHCO3, KH2PO4 and Al(OH)3), the industrial solid waste-based composite powder explosion inhibitors were obtained by solvent-crystallization (WCSC) and dry coating by ball milling (DCBM). Those kinds of explosion inhibitors can suppress the explosion of pulverized coal in 40–50% of cases. Compared with the powder explosion inhibitor commonly used in industry, it has a lower production cost and better explosion suppression effect. Those kinds of explosion inhibitors have a good industrial application prospect.

show abstract

“…Therefore, how to adjust the adsorption strength between intermediates and catalysts to obtain ideal catalysts has always been a hot topic for CO 2 RR. 104,145,[160][161][162] To this end, Huang et al 163 reported that NiCo@C 2 N promotes catalysis for CO 2 RR by DFT calculations combined with a computational hydrogen electrode model. It was found that the asymmetric N 2 Ni-CoN 2 bonding configuration is more stable than the symmetric N 2 Ni-CoN 2 bonding configuration.…”

Section: Electrocatalytic Nrrmentioning

confidence: 99%

“…Continuous supply of reactants and rapid product release are conducive to maintaining the high efficiency of the reaction, that is, the mass transfer rate is very important to the catalytic reaction. Therefore, how to adjust the adsorption strength between intermediates and catalysts to obtain ideal catalysts has always been a hot topic for CO 2 RR 104,145,160–162 . To this end, Huang et al 163 reported that NiCo@C 2 N promotes catalysis for CO 2 RR by DFT calculations combined with a computational hydrogen electrode model.…”

Section: Application Of Cn Materialsmentioning

confidence: 99%

Advances of the functionalized carbon nitrides for electrocatalysis

Fan

Sun

et al. 2022

Carbon Energy

View full text Add to dashboard Cite

Over the past few decades, the design and development of carbon materials have occurred at a rapid pace. In particular, these porous graphene-like carbon nitride materials have received considerable attention due to their superior structures and performances in the energy transformation field. In this review, nitrogenated holey two-dimensional graphene and polymeric carbon nitride will be discussed in depth. The structural properties, synthetic methods, and applications including electrocatalytic reactions, such as hydrogen evolution reaction, oxygen reduction reaction, oxygen evolution reaction, and nitrogen reduction reaction, will be presented in detail. Finally, we will present the outlooks on the current obstacles to the development of carbon nitride materials. This comprehensive understanding will help guide and motivate researchers to develop and modify carbon nitride materials with better properties in the future.

show abstract

Insights into the adsorption/desorption of CO2 and CO on single-atom Fe-nitrogen-graphene catalyst under electrochemical environment

Cited by 39 publications

References 58 publications

The Influence of Single-Atom Fe^2+/3+N₄ Spin State on the Electroreduction of CO₂ to CO/HCOOH by Analyzing Proton/Electron Transfer Mechanisms and Free Energy Evolutions

The Influence of Single-Atom Fe^2+/3+N₄ Spin State on the Electroreduction of CO₂ to CO/HCOOH by Analyzing Proton/Electron Transfer Mechanisms and Free Energy Evolutions

Study on a New Type of Composite Powder Explosion Inhibitor Used to Suppress Underground Coal Dust Explosion

Advances of the functionalized carbon nitrides for electrocatalysis

Contact Info

Product

Resources

About

Insights into the adsorption/desorption of CO2 and CO on single-atom Fe-nitrogen-graphene catalyst under electrochemical environment

Cited by 39 publications

References 58 publications

The Influence of Single-Atom Fe2+/3+N4 Spin State on the Electroreduction of CO2 to CO/HCOOH by Analyzing Proton/Electron Transfer Mechanisms and Free Energy Evolutions

The Influence of Single-Atom Fe2+/3+N4 Spin State on the Electroreduction of CO2 to CO/HCOOH by Analyzing Proton/Electron Transfer Mechanisms and Free Energy Evolutions

Study on a New Type of Composite Powder Explosion Inhibitor Used to Suppress Underground Coal Dust Explosion

Advances of the functionalized carbon nitrides for electrocatalysis

Contact Info

Product

Resources

About

The Influence of Single-Atom Fe^2+/3+N₄ Spin State on the Electroreduction of CO₂ to CO/HCOOH by Analyzing Proton/Electron Transfer Mechanisms and Free Energy Evolutions

The Influence of Single-Atom Fe^2+/3+N₄ Spin State on the Electroreduction of CO₂ to CO/HCOOH by Analyzing Proton/Electron Transfer Mechanisms and Free Energy Evolutions