Atomic alkali metal anchoring on graphdiyne as single-atom catalysts for capture and conversion of CO2 to HCOOH

Feng, Zhen; Su, Guang; Hai, Ding; Ma, Yaqiang; Li, Yang; Tang, Yanan

doi:10.1016/j.mcat.2020.111142

Cited by 23 publications

(10 citation statements)

References 68 publications

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“…Based on adsorption free energy, the binding between *OCHO and alkali metals is stronger than that between *COOH and alkali metals. This indicates that *HCCOH is preferentially formed via the CO 2 RR, and Li@GDY required a limiting potential of −0.56 V, while Na@GDY required a lower overpotential of −0.16 V. 140 Fe anchored on graphdiyne has been shown to achieve high selectivity and activity in the CO 2 RR towards CH 4 production. The reduction of CO to *COH is the rate determining step, which requires a limiting potential of −0.33 V. 141…”

Section: Insights From Computational Studiesmentioning

confidence: 99%

Mechanistic understanding and design of non-noble metal-based single-atom catalysts supported on two-dimensional materials for CO₂ electroreduction

et al. 2022

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Section: Insights From Computational Studiesmentioning

confidence: 99%

Mechanistic understanding and design of non-noble metal-based single-atom catalysts supported on two-dimensional materials for CO₂ electroreduction

et al. 2022

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“…PBE tends to overestimate the adsorption energy, suggesting that hybrid DFT should be preferred when studying GDY electronic properties [ 97 ]. Similar studies, including Li-decorated GDY, or Li@GDY, show that it could capture CO 2 molecules while investigating the possible conversion of CO 2 into beneficial—or at least less nocive—chemicals via carbon dioxide electrochemical reduction reaction (CO 2 RR) [ 98 ].…”

Section: Adsorption Of Molecules On Pristine or Nonmetal Functionalized Systemsmentioning

confidence: 99%

Carbon Nanostructures Doped with Transition Metals for Pollutant Gas Adsorption Systems

2021

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The adsorption of molecules usually increases capacity and/or strength with the doping of surfaces with transition metals; furthermore, carbon nanostructures, i.e., graphene, carbon nanotubes, fullerenes, graphdiyne, etc., have a large specific area for gas adsorption. This review focuses on the reports (experimental or theoretical) of systems using these structures decorated with transition metals for mainly pollutant molecules’ adsorption. Furthermore, we aim to present the expanding application of nanomaterials on environmental problems, mainly over the last 10 years. We found a wide range of pollutant molecules investigated for adsorption in carbon nanostructures, including greenhouse gases, anticancer drugs, and chemical warfare agents, among many more.

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“…The modification of Rh/Al 2 O 3 with K changes the surroundings of the Rh particles, which influences the strength of CO adsorption and the activation ability of Rh for H 2 dissociation [ 9 ]. The modification of Mo 2 C with alkali metals changes the structural and electronic properties of these catalysts and promotes the performances of Mo 2 C in CO 2 conversions [ 25 , 26 , 27 , 28 , 29 ]. For example, the addition of 2 wt% K to Mo 2 C/γ-Al 2 O 3 increases the CO selectivity to 95% from 73.5% [ 30 ], and the incorporation of K into Cu/Mo 2 C results in high CO 2 dissociation activity (almost 1.5 times higher than Cu/Mo 2 C) but also reduces H 2 adsorption, thus resulting in a low H 2 /CO x ratio and low CH 4 production [ 31 ].…”

Section: Introductionmentioning

confidence: 99%

Unveiling the Origin of Alkali Metal (Na, K, Rb, and Cs) Promotion in CO2 Dissociation over Mo2C Catalysts

et al. 2022

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Molybdenum carbide (Mo2C) is a promising and low-cost catalyst for the reverse water−gas shift (RWGS) reaction. Doping the Mo2C surface with alkali metals can improve the activity of CO2 conversion, but the effect of these metals on CO2 conversion to CO remains poorly understood. In this study, the energies of CO2 dissociation and CO desorption on the Mo2C surface in the presence of different alkali metals (Na, K, Rb, and Cs) are calculated using density functional theory (DFT). Alkali metal doping results in increasing electron density on the Mo atoms and promotes the adsorption and activation of CO2 on Mo2C; the dissociation barrier of CO2 is decreased from 12.51 on Mo2C surfaces to 9.51–11.21 Kcal/mol on alkali metal-modified Mo2C surfaces. Energetic and electronic analyses reveal that although the alkali metals directly bond with oxygen atoms of the oxides, the reduction in the energy of CO2 dissociation can be attributed to the increased interaction between CO/O fragments and Mo in the transition states. The abilities of four alkali metals (Na, K, Rb, and Cs) to promote CO2 dissociation increase in the order Na (11.21 Kcal/mol) < Rb (10.54 Kcal/mol) < Cs (10.41 Kcal/mol) < K (9.51 Kcal/mol). Through electronic analysis, it is found that the increased electron density on the Mo atoms is a result of the alkali metal, and a greater negative charge on Mo results in a lower energy barrier for CO2 dissociation.

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Atomic alkali metal anchoring on graphdiyne as single-atom catalysts for capture and conversion of CO2 to HCOOH

Cited by 23 publications

References 68 publications

Mechanistic understanding and design of non-noble metal-based single-atom catalysts supported on two-dimensional materials for CO₂ electroreduction

Mechanistic understanding and design of non-noble metal-based single-atom catalysts supported on two-dimensional materials for CO₂ electroreduction

Carbon Nanostructures Doped with Transition Metals for Pollutant Gas Adsorption Systems

Unveiling the Origin of Alkali Metal (Na, K, Rb, and Cs) Promotion in CO2 Dissociation over Mo2C Catalysts

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Atomic alkali metal anchoring on graphdiyne as single-atom catalysts for capture and conversion of CO2 to HCOOH

Cited by 23 publications

References 68 publications

Mechanistic understanding and design of non-noble metal-based single-atom catalysts supported on two-dimensional materials for CO2 electroreduction

Mechanistic understanding and design of non-noble metal-based single-atom catalysts supported on two-dimensional materials for CO2 electroreduction

Carbon Nanostructures Doped with Transition Metals for Pollutant Gas Adsorption Systems

Unveiling the Origin of Alkali Metal (Na, K, Rb, and Cs) Promotion in CO2 Dissociation over Mo2C Catalysts

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Mechanistic understanding and design of non-noble metal-based single-atom catalysts supported on two-dimensional materials for CO₂ electroreduction

Mechanistic understanding and design of non-noble metal-based single-atom catalysts supported on two-dimensional materials for CO₂ electroreduction