Materials design for electrocatalytic carbon capture

Tan, Xin; Tahini, Hassan A.; Smith, Sean C.

doi:10.1063/1.4942635

Cited by 24 publications

(11 citation statements)

References 49 publications

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“…We investigated the relationship of the different boxes ( a × b × c , a = b , c = 40 Å) of the graphene cell and energy (Figure S1). We finally adopted a unit cell of parameters a = 17.06 Å, b = 17.06 Å, and c = 40 Å composed of 112 carbon atoms in subsequent calculations . On the basis of the unit cell of this nondefective graphene sheet, two different types of N-doped graphene surfaces were constructed.…”

Section: Computational Methods and Detailsmentioning

confidence: 99%

Structure and Catalytic Activity of Gold Clusters Supported on Nitrogen-Doped Graphene

Zhao

et al. 2021

J. Phys. Chem. C

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Controlling the charge types of metal clusters on supports is of great importance in designing a noble-metal-free catalyst. Here, we designed two different types of N-doped graphene surfaces, the graphitic-like nitrogen-doped graphene G nN and the pyridinic-like nitrogen-doped graphene G nN,n′V. We found that in the Au28/G nN system, the Au atoms interact with C atoms. However, in the Au28/G nN,n′V system, the Au atoms interact with the N atoms. Specifically, the different bonding modes result in the charge state of the Au cluster being negative on the G nN surface, whereas on the G nN,n′V surface, the Au cluster is of positive charge. Therefore, it is possible to change the type of carbon–nitrogen bonding structure to control the charge types of gold clusters on nitrogen-doped graphene. In these two systems, the O2 molecules prefer to be activated at the unsaturated and electron-rich bridge sites of the Au cluster. O2 adsorption further enhances the charge transfer along the original directions at the Au28 cluster/N-doped graphene substrate interfaces. However, the charge states of Au clusters slightly affect the activation of O–O bonds. The negatively charged Au cluster surface (Au28/G nN) exhibits better catalytic activity to CO oxidation under the trimolecular Eley–Rideal (3ER) mechanism and electrocatalytic reduction of CO2 compared with the positively charged Au cluster surface (Au28/G nN,n′V). Our results are beneficial for accelerating the industrial application of nanometer-sized gold catalysts and provide a theoretical basis for the design and development of new catalysts.

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Section: Computational Methods and Detailsmentioning

confidence: 99%

Structure and Catalytic Activity of Gold Clusters Supported on Nitrogen-Doped Graphene

Zhao

et al. 2021

J. Phys. Chem. C

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“…The idea can be well applied and generalized to other 2D materials like electron charged graphitic carbon nitrides (C 3 N 4 ) and N-doped graphene, both of which have been proposed for the CO 2 capture (Tan, Kou, Tahini, & Smith, 2015;Tan, Tahini, & Smith, 2016b), where the charged nitrogen as the active capturing sites. Most of the cases, gas sensing materials can be also used for gap capture if the adsorption strength is strong enough due to the same mechanism, namely electron transfer.…”

Section: Two-dimensional Materials For Gas Capturementioning

confidence: 99%

Gas sensing and capturing based on two‐dimensional layered materials: Overview from theoretical perspective

Tang

Kou

2018

WIREs Comput Mol Sci

120

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Toxic gas detection and capture are two important topics, which are highly related with human health and environments. Recently, theoretical simulations based on first‐principles calculations have suggested two‐dimensional (2D) materials to be as ideal candidates for gas sensing and capturing due to the large surface–volume ratio and reactive surface. Starting from graphene, which was firstly proposed for 2D gas sensing, the family currently has been extended to transition metal dichalcogenides, phosphorene, silicene, germanene, MXene, and so on. In this review, we give a comprehensive overview of recent progress in computational investigations of 2D gas sensing/capture materials. We then offer perspectives on possible directions for further fundamental exploration of gas sensor and caption based on 2D materials, which are expected to offer tremendous new opportunities for future research and development. This article is categorized under: Structure and Mechanism > Computational Materials Science

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“…found that borophene achieved a CO 2 capacity of 6.73×10 14 molecules per cm −2 with a charge density of 57.2×10 13 e − cm −2 , and the desorption of CO 2 was exothermic by 1.99 eV when rejecting charges [18] . They also reported that the CO 2 adsorption energy increased from 0.17 to 0.58 eV when 4 e − was injected into N‐doped graphene [19] . Carbon nitrides such as C 2 N and C 3 N have also been demonstrated as efficient charge‐modulated CO 2 capture and separation materials [20,21] .…”

Section: Introductionmentioning

confidence: 96%

Can Charge‐Modulated Metal‐Organic Frameworks Achieve High‐Performance CO₂ Capture and Separation over H₂, N₂, and CH₄?

Wang

Kong

et al. 2021

ChemSusChem

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CO2 capture and separation by using charge‐modulated adsorbent materials is a promising strategy to reduce CO2 emissions. Herein, three TM‐HAB (TM=Co, Ni, and Cu; HAB=hexa‐aminobenzene) metal‐organic frameworks (MOFs) were evaluated as charge‐modulated CO2 capture and separation materials by using density functional theory and grand canonical Monte Carlo simulations. The results showed that each TM‐HAB presented a high electrical conductivity and structural stability when injecting charges. The CO2 adsorption energy increased from 0.211 to 2.091 eV on Co‐HAB, 0.262 to 2.119 eV on Ni‐HAB, and 0.904 to 2.803 eV on Cu‐HAB, respectively, with the increase in charge state from 0.0 to 3.0 e−. Co‐HAB and Ni‐HAB were better charge‐modulated CO2 capture materials with less structure deformation based on energy decomposition analyses. The kinetic process demonstrated that considerably low energy consumptions of 0.911 and 1.589 GJ ton−1 CO2 were observed for a complete adsorption–desorption cycle on Co‐HAB and Ni‐HAB. All charged MOFs, especially Co‐HAB and Ni‐HAB, exhibited higher CO2 adsorption energies and adsorption capacities than those of H2, N2, and CH4, thereby exhibiting high CO2 selectivities. Interaction analysis confirmed that the injecting charges had a more pronounced enhancement in the coulombic interactions between CO2 and MOFs. The results of this work highlight Co‐HAB and Ni‐HAB as promising charge‐modulated CO2 capture and separation materials with controllable CO2 capture, high selectivity, and low energy consumption.

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Materials design for electrocatalytic carbon capture

Cited by 24 publications

References 49 publications

Structure and Catalytic Activity of Gold Clusters Supported on Nitrogen-Doped Graphene

Structure and Catalytic Activity of Gold Clusters Supported on Nitrogen-Doped Graphene

Gas sensing and capturing based on two‐dimensional layered materials: Overview from theoretical perspective

Can Charge‐Modulated Metal‐Organic Frameworks Achieve High‐Performance CO₂ Capture and Separation over H₂, N₂, and CH₄?

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Materials design for electrocatalytic carbon capture

Cited by 24 publications

References 49 publications

Structure and Catalytic Activity of Gold Clusters Supported on Nitrogen-Doped Graphene

Structure and Catalytic Activity of Gold Clusters Supported on Nitrogen-Doped Graphene

Gas sensing and capturing based on two‐dimensional layered materials: Overview from theoretical perspective

Can Charge‐Modulated Metal‐Organic Frameworks Achieve High‐Performance CO2 Capture and Separation over H2, N2, and CH4?

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Can Charge‐Modulated Metal‐Organic Frameworks Achieve High‐Performance CO₂ Capture and Separation over H₂, N₂, and CH₄?