DFT insights into electrocatalytic CO2 reduction to methanol on α-Fe2O3(0001) surfaces

Kumar, Nandha; Seriani, Nicola; Gebauer, Ralph

doi:10.1039/c9cp06453b

Cited by 23 publications

(12 citation statements)

References 47 publications

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“…Among thousands of possible reaction pathways, the key steps are CO formation and C-C coupling. Typically, the first CO 2 reduction reaction step is the hydrogenation of CO 2 , which results in the generation of formate (*HCOO) or carboxyl (*COOH) (Kumar et al 2020). Subsequently, CO would be formed from *COOH, and further reduced to other carbon-based fuels.…”

Section: Intermediates and Reaction Pathwaysmentioning

confidence: 99%

Photoelectrochemical technology for solar fuel generation, from single photoelectrodes to unassisted cells: a review

et al. 2021

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Photoelectrochemical solar fuel generation requires a highly integrated technology for converting solar energy into chemical fuels. Dihydrogen (H 2 ) and carbon-based fuels can be produced by water splitting and CO 2 reduction, respectively. Material synthesis, device assembly, and performance of photoelectrochemical systems have rapidly improved in the last decade. More recently, research has shifted from developing single photoelectrodes to fabricating tandem photoelectrochemical cells. Here we review photoelectrochemical systems for solar fuel generation, with focus on photocathodes, photoanodes, protective layers and cocatalysts. We also present strategies for unassisted solar fuel generation.

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Section: Intermediates and Reaction Pathwaysmentioning

confidence: 99%

Photoelectrochemical technology for solar fuel generation, from single photoelectrodes to unassisted cells: a review

et al. 2021

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“…Several types of 2D MXene materials with M 2 X, M 3 X 2 , and M 4 X 3 stoichiometry have been synthesized using fluorine and hydrogen from precursor MAX phases and found to exhibit large surface areas in the range of 250–1000 m 2 g –1 . Interestingly, MXenes possess high adsorption energies when compared to other 2D materials, as shown in Figure . − Zhang et al studied O surface-functionalized MXene Ti 2 C (Ti 2 CO 2 ) and found enhanced photocatalytic performance for CO 2 reduction to formic acid. Later, Li et al theoretically observed M 3 C 2 -type (Mo 3 C 2 and Cr 3 C 2 ) MXenes as most promising candidates for CO 2 conversion into hydrocarbon fuels …”

Section: Introductionmentioning

confidence: 99%

“…Adsorption energies of CO 2 on various 2D materials collected from literature. − The purple balls correspond to MXenes (M 2 C, M 3 C 2 , and M 4 C 3 (M = Ti, V, Zr, Nb, and Mo) and orange balls represent other 2D materials such as Cu 2 O, MoS 2 , MoSe 2 , WTe 2 , WSe 2 , MgO, In 2 O 3 , Fe 2 O 3 , ZnO, SnO 2 , GaN, Ga 2 O 3 , and X-AlC (X = B, N, P, Si). This analysis clearly indicates that the E ads of CO 2 on MXenes are highly negative when compared to other 2D materials.…”

Section: Introductionmentioning

confidence: 99%

High-Throughput Screening of Atomic Defects in MXenes for CO₂ Capture, Activation, and Dissociation

Parey

Abraham

Mir³

et al. 2021

ACS Appl. Mater. Interfaces

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The capture, activation, and dissociation of carbon dioxide (CO2) is of fundamental interest to overcome the ramifications of the greenhouse effect. In this regard, high-throughput screening of two-dimensional MXenes has been examined using well-resolved first-principles simulations through DFT-D3 dispersion correction. We systematically investigated different types of structural defects to understand their influence on the performance of M2X-type MXenes. Defect calculations demonstrate that the formation of M2C(VMC) and M2N(VMN) vacancies require higher energy, while M2C(VC) and M2N(VN) vacancies are favorable to form during the synthesis of M2X-type MXenes. The M2X-type MXenes from group III to VII series show remarkable behavior for active capturing of CO2, especially group IV (Ti2X and Zr2X) MXenes exhibit unprecedentedly high adsorption energies and charge transfer (>2e) from M2X to CO2. The potential CO2 capture, activation, and dissociation abilities of MXenes are emanated from Dewar interactions involving hybridization between π orbitals of CO2 and metal d-orbitals. Our high-throughput screening demonstrates chemisorption of CO2 on pure and defective MXenes, followed by dissociation into CO and O species.

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“…Lately, DFT-based calculations have been found to be useful in predicting various mechanisms of the ERC using modeled surfaces. [127,128] The DFT-based calculations are equally applicable both for predicting the product selectivity as well as the mechanistic insights in the case of Cu electrocatalysts. Hussain et al [129] obtained calculated reaction rates using combined DFT and rate theory, and compared their results with the experimental findings.…”

Section: Theoretical Investigations On Cu-based Electrodesmentioning

confidence: 99%

Strategies for Improved Electrochemical CO₂ Reduction to Value‐Added Products by Highly Anticipated Copper‐Based Nanoarchitectures

Khan

2021

The Chemical Record

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Uncontrolled CO 2 emission from various industrial and domestic sources is a considerable threat to environmental sustainability. Scientists are trying to develop multiple approaches to not only reduce CO 2 emissions but also utilize this potent pollutant to get economically feasible products. The electrochemical reduction of CO 2 (ERC) is one way to effectively convert CO 2 to more useful products (ranging from C1 to C5). Nevertheless, this process is kinetically hindered and less selective towards a specific product and, consequently, requires an efficient electrocatalyst with characteristics like selectivity, stability, reusability, low cost, and environmentally benign. Owing to specified commercial features, copper (Cu)-based materials are highly anticipated and widely investigated for the last two decades. However, their non-modified polycrystalline Cu forms usually lack selectivity and lower overpotential of CO 2 reduction. Therefore, extensive research is in progress to induce various alterations ranging from morphological and surface chemistry tuning to structural and optoelectrical characteristics modifications. This review provides an overview of those strategies to improve the CO 2 conversion efficiency through Cu-based ERC into valuable C1, C2 , and higher molecular weight hydrocarbons. The thermodynamics and kinetics of CO 2 reduction via Cu-based electrocatalysts are discussed in detail with the support of the first principle DFT-based models. In the last portion of the review, the reported mechanisms for various products are summarized, with a short overview of the outlook. This review is expected to provide important basics as well as advanced information for experienced as well as new researchers to develop various strategies for Cu and related materials to achieve improved ERC.

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DFT insights into electrocatalytic CO₂ reduction to methanol on α-Fe₂O₃(0001) surfaces

Abstract: Electrocatalytic reduction of CO2 to manufacture fuels and other useful chemicals is one of the appealing methods to reuse CO2.

Cited by 23 publications

References 47 publications

Photoelectrochemical technology for solar fuel generation, from single photoelectrodes to unassisted cells: a review

Photoelectrochemical technology for solar fuel generation, from single photoelectrodes to unassisted cells: a review

High-Throughput Screening of Atomic Defects in MXenes for CO₂ Capture, Activation, and Dissociation

Strategies for Improved Electrochemical CO₂ Reduction to Value‐Added Products by Highly Anticipated Copper‐Based Nanoarchitectures

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DFT insights into electrocatalytic CO2 reduction to methanol on α-Fe2O3(0001) surfaces

Abstract: Electrocatalytic reduction of CO2 to manufacture fuels and other useful chemicals is one of the appealing methods to reuse CO2.

Cited by 23 publications

References 47 publications

Photoelectrochemical technology for solar fuel generation, from single photoelectrodes to unassisted cells: a review

Photoelectrochemical technology for solar fuel generation, from single photoelectrodes to unassisted cells: a review

High-Throughput Screening of Atomic Defects in MXenes for CO2 Capture, Activation, and Dissociation

Strategies for Improved Electrochemical CO2 Reduction to Value‐Added Products by Highly Anticipated Copper‐Based Nanoarchitectures

Contact Info

Product

Resources

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DFT insights into electrocatalytic CO₂ reduction to methanol on α-Fe₂O₃(0001) surfaces

High-Throughput Screening of Atomic Defects in MXenes for CO₂ Capture, Activation, and Dissociation

Strategies for Improved Electrochemical CO₂ Reduction to Value‐Added Products by Highly Anticipated Copper‐Based Nanoarchitectures