Theoretical study on the synthesis of methane by CO2 hydrogenation on Ni3Fe(111) surface

Kang, Liming; Chen, Xin; Ke, Qiang

doi:10.1016/j.jngse.2021.104114

Cited by 14 publications

(3 citation statements)

References 45 publications

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“…Since the industrial revolution, the massive consumption of fossil fuels has led to the increasing concentration of carbon dioxide (CO 2 ) in the atmosphere, which has caused a series of environmental problems such as global warming and the melting of polar glaciers, thereby seriously threatening the sustainable development of human society. − In this context, achieving carbon neutrality has become a common goal of all humanity . Therefore, how to rationally utilize the excess CO 2 in the atmosphere has become a research hotspot .…”

Section: Introductionmentioning

confidence: 99%

Graphene-Supported Tin Single-Atom Catalysts for CO₂ Hydrogenation to HCOOH: A Theoretical Investigation of Performance under Different N Coordination Numbers

Liang

Zhao

et al. 2023

ACS Appl. Nano Mater.

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The effects of the adjustment of the N coordination number in Sn single-atom catalysts toward the activity and selectivity of CO2 hydrogenation to HCOOH are systematically explored via density functional theory calculations. The stability of the studied catalysts was evaluated by formation energy calculations, and the calculated results indicated that Sn-N x C4–x -G (x = 1–4) are structurally stable. Through the discussion of the reaction mechanism, the optimal path of CO2 hydrogenation to HCOOH on all the studied catalysts is via CO2* + H2* → HCOO* + H* → HCOOH*. In addition, they have different speed limit steps. For Sn-N1C3-G and Sn-N2C2-G, the rate-determining step of CO2 to HCOOH is CO2* + H2* → HCOO* + H*, while the rate-determining step of the other two catalysts is HCOO* + H* → HCOOH*. Meanwhile, the order of catalytic activities of Sn-N x C4–x -G is determined to be Sn-N1C3-G > Sn-N2C2-G > Sn-N3C1-G > Sn-N4-G. Furthermore, the origin of the catalytic activities for HCOOH synthesis on Sn-N x C4–x -G is revealed through the calculated p-band center. It demonstrated that the p-band center of the Sn atom is a good descriptor to evaluate the catalytic activity for HCOOH synthesis in the Sn-N x C4–x -G system.

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Section: Introductionmentioning

confidence: 99%

Graphene-Supported Tin Single-Atom Catalysts for CO₂ Hydrogenation to HCOOH: A Theoretical Investigation of Performance under Different N Coordination Numbers

Liang

Zhao

et al. 2023

ACS Appl. Nano Mater.

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“…For almost a century, the carbon emissions generated by burning fossil fuels and anthropogenic activities have contributed to the sharp increase in greenhouse gases. − Reducing carbon dioxide (CO 2 ) to high-value chemicals (methanol, methane, formic acid, etc.) has great potential in solving the energy crisis and mitigating global warming simultaneously. − As one of the possible products for CO 2 reduction, formic acid (HCOOH) is recognized as an important chemical raw material and a hydrogen storage material, which is widely used in the rubber, pharmaceutical, and leather industries. − Commercial HCOOH production is achieved by the hydrolysis of methyl formate or direct synthesis from carbon monoxide and water.…”

Section: Introductionmentioning

confidence: 99%

Theoretical Investigation of Graphene Supported Sn–M (M = Fe, Co, Ni, Cu, Zn) Dual-Atom Catalysts for CO₂ Hydrogenation to HCOOH

Ma,

Chen

2023

ACS Appl. Nano Mater.

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This work selects a series of transition metals (Fe, Co, Ni, Cu, and Zn) and Sn metal to construct a series of Sn−M dual-atom catalysts (SnMN 6 /G). Formation energy calculations are conducted to evaluate the stability of the studied catalyst. The calculated results demonstrate that SnMN 6 /G (M = Fe, Co, Ni, Cu, Zn) dual-atom catalysts exhibit high structural stability. From the calculated electrostatic potential and Fukui(−) index, it is determined that the Sn atom is the main reaction site for CO 2 hydrogenation. Based on the analysis, the optimal path of HCOOH synthesis is CO 2 * → HCOO* → HCOOH* on SnMN 6 /G. In addition, the rate-determining step of the reaction CO 2 → HCOOH is CO 2 * → HCOO* on all SnMN 6 /G. Furthermore, the catalytic activity of SnMN 6 /G is ranked in the following order: SnZnN 6 /G > SnNiN 6 /G > SnCoN 6 /G > SnCuN 6 /G > SnFeN 6 /G. Moreover, the activity origin of the catalyst is explored through Mulliken charge analysis, which SnZnN 6 /G exhibits stronger charge fluctuation during the reaction process, which may be the source of its high activity. This work clarifies that SnZnN 6 /G is a highly active dual-atom catalyst for HCOOH synthesis.

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“…The substitution of CH 4 with CO 2 , namely CO 2 -enhanced shale gas recovery (CO 2 -ESGR) technology, is currently considered a promising approach for CH 4 extraction and CO 2 storage. , The technique displaces CH 4 in shale pores by injecting CO 2 into shale reservoirs, where injected CO 2 remains. This method can not only effectively improve shale gas recovery but also achieve geological storage of CO 2 , thereby effectively alleviating the problem of global warming caused by excessive CO 2 emission. − However, the CO 2 -ESGR technology is affected by complex shale reservoirs, temperature, pressure, and other factors, especially the differences in the adsorption capacity of CO 2 and CH 4 in different shale reservoirs, making the application of this technology challenging. Therefore, understanding the adsorption mechanisms of CO 2 and CH 4 in shale is significant for improving shale gas recovery and the effectiveness of CO 2 sequestration.…”

Section: Introductionmentioning

confidence: 99%

Effect of the Water Content on the Adsorption of CO₂ and CH₄ in Calcite Slit Nanopores: Insights from GCMC, MD, and DFT

Guo,

Zhang,

et al. 2023

Langmuir

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It is significant to understand the adsorption mechanisms of shale gas (CH4) and CO2 in shale formations to enhance CH4 recovery rates and enable geological CO2 storage. This study provides a comprehensive investigation into the adsorption behaviors of CO2 and CH4 within dry and hydrous calcite nanopores, utilizing a combination of grand canonical Monte Carlo simulations, molecular dynamics simulations, and density functional theory calculations. In dry calcite slits, the calculated results for the adsorption capacity, density profile, and isosteric heat of CO2 and CH4 reveal that CO2 possesses a stronger adsorption affinity, making it preferentially adsorb on the pore surface compared to CH4. In hydrous calcite slits, calculating the adsorption capacity and density profile of CO2 and CH4, the results show that the gas adsorption sites become progressively occupied by H2O molecules, leading to a substantial decrease in the adsorption capacity of CO2 and CH4. Furthermore, by analysis of the adsorption energy and electronic structure, the reason for the reduction of gas adsorption capacity caused by H2O is further revealed. This work has a deep understanding of the adsorption mechanisms of shale gas and CO2 in calcite and can offer valuable theoretical insights for the development of a CO2-enhanced shale gas recovery technology.

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Theoretical study on the synthesis of methane by CO2 hydrogenation on Ni3Fe(111) surface

Cited by 14 publications

References 45 publications

Graphene-Supported Tin Single-Atom Catalysts for CO₂ Hydrogenation to HCOOH: A Theoretical Investigation of Performance under Different N Coordination Numbers

Graphene-Supported Tin Single-Atom Catalysts for CO₂ Hydrogenation to HCOOH: A Theoretical Investigation of Performance under Different N Coordination Numbers

Theoretical Investigation of Graphene Supported Sn–M (M = Fe, Co, Ni, Cu, Zn) Dual-Atom Catalysts for CO₂ Hydrogenation to HCOOH

Effect of the Water Content on the Adsorption of CO₂ and CH₄ in Calcite Slit Nanopores: Insights from GCMC, MD, and DFT

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Theoretical study on the synthesis of methane by CO2 hydrogenation on Ni3Fe(111) surface

Cited by 14 publications

References 45 publications

Graphene-Supported Tin Single-Atom Catalysts for CO2 Hydrogenation to HCOOH: A Theoretical Investigation of Performance under Different N Coordination Numbers

Graphene-Supported Tin Single-Atom Catalysts for CO2 Hydrogenation to HCOOH: A Theoretical Investigation of Performance under Different N Coordination Numbers

Theoretical Investigation of Graphene Supported Sn–M (M = Fe, Co, Ni, Cu, Zn) Dual-Atom Catalysts for CO2 Hydrogenation to HCOOH

Effect of the Water Content on the Adsorption of CO2 and CH4 in Calcite Slit Nanopores: Insights from GCMC, MD, and DFT

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Product

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Graphene-Supported Tin Single-Atom Catalysts for CO₂ Hydrogenation to HCOOH: A Theoretical Investigation of Performance under Different N Coordination Numbers

Graphene-Supported Tin Single-Atom Catalysts for CO₂ Hydrogenation to HCOOH: A Theoretical Investigation of Performance under Different N Coordination Numbers

Theoretical Investigation of Graphene Supported Sn–M (M = Fe, Co, Ni, Cu, Zn) Dual-Atom Catalysts for CO₂ Hydrogenation to HCOOH

Effect of the Water Content on the Adsorption of CO₂ and CH₄ in Calcite Slit Nanopores: Insights from GCMC, MD, and DFT