A new adsorption energy-barrier relation and its application to CO2 hydrogenation to methanol over In2O3-supported metal catalysts

Yang, Deshuai; Lu, Huili; Zeng, Guixiang; Chen, Zhao-Xu

doi:10.1039/d2cc05571f

Cited by 7 publications

(3 citation statements)

References 49 publications

(18 reference statements)

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“…Different from our previously discovered ADBS relation, which correlates energy barriers with the separate adsorption energies of one reactant, the ADTS relation discovered here reflects the correlation between the adsorption energies of TSs having two reactants (here CO 2 and H) and the separate adsorption energies of only one reactant (here CO 2 ). To understand this counterintuitive phenomenon, interaction analysis was performed on the two transition-state structures (TS1 and TS2) for CO 2 * + H* → HCOO* + * and CO 2 * + H* → COOH* + *, see Figure S14.…”

Section: Resultscontrasting

confidence: 98%

“…According to the conventional TSS relation,36−38 the adsorption energies of TSs are expected to correlate with the adsorption energies of ISs that contain both reactants CO 2 and H. Equations 1 and 2 show that the adsorption energies of TSs are linearly correlated with the separate adsorption energies of only one reactant CO 2 . Here, we name such a linear relation the adsorbatedependent transition-state (ADTS) scaling relation to distinguish it from the conventional TSS relation.Different from our previously discovered ADBS relation,69 which correlates energy barriers with the separate adsorption energies of one reactant, the ADTS relation discovered here reflects the correlation between the adsorption energies of TSs having two reactants (here CO 2 and H) and the separate adsorption energies of only one reactant (here CO 2 ). To understand this counterintuitive phenomenon, interaction analysis was performed on the two transition-state structures (TS1 and TS2) forCO 2 * + H* → HCOO* + * and CO 2 * + H* → COOH* + *, see Figure S14.…”

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confidence: 96%

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CO₂ Hydrogenation to Methanol and Ethanol on In₂O₃-Based Single-Atom Catalysts and a New Scaling Relation

Yang,

Lu,

Zeng

et al. 2023

J. Phys. Chem. C

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Conversion of CO2 into high-value chemicals is a hot issue both industrially and scientifically, and the development of suitable catalysts is the key problem. Using density functional theory (DFT) calculations and microkinetic simulations, we investigated the mechanisms for reduction of CO2 to methanol and ethanol on the iridium-doped In2O3 single-atom catalyst, which exhibits high selectivity to ethanol. The favorable pathways and two key steps controlling the formation and selectivity of methanol and ethanol were identified. Further calculations of the energy barriers for the two key steps on the other nine single-metal-atom-doped In2O3 show that Mn-doped In2O3 may possess higher selectivity to ethanol than Ir-doped In2O3, while Ru-, Fe-, and Rh-doped In2O3 might be good catalysts for methanol. Furthermore, we found that there exists a linear relation (ADTS relation) between the CO2 separate adsorption energies and the adsorption energies of transition states. It is demonstrated that for a bimolecular (A + B) surface reaction, the ADTS relation holds true when the sum of the interactions of B with A and B with the surface are constant. The present work also outlines a methodology to identify reaction descriptors to screen catalysts on the basis of reaction mechanisms and microkinetic analysis.

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Section: Resultscontrasting

confidence: 98%

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confidence: 96%

CO₂ Hydrogenation to Methanol and Ethanol on In₂O₃-Based Single-Atom Catalysts and a New Scaling Relation

Yang,

Lu,

Zeng

et al. 2023

J. Phys. Chem. C

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“…38–40 Recently, we investigated the BEP and TSS relationships of diatomic species dissociation on strained metal surfaces and found that these relationships can be nonlinear. 41 Under some specific condition, variants of the TSS relationship, such as ADBS (the adsorbate-dependent barrier scaling) 42 may emerge.…”

Section: Resultsmentioning

confidence: 99%

The mechanism of CO₂ hydrogenation to CH₃OH on MZrO_x (M = Ga, Cr) solid-solution catalysts and effects of lattice strain

Lu,

Yang,

Chen

2024

Catal. Sci. Technol.

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Nano‐alloy Catalysts for Methanol Synthesis from CO₂ Hydrogenation

Zhang,

Lian,

Sun

et al. 2024

Chemistry An Asian Journal

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Nano‐alloy catalysts (NACs), which differ appreciably from monometallic catalysts, take on superior intrinsic features in surface microstructure, surface electronic properties, homogeneity in nanoscale, etc., endowing them with attractive prospects in heterogeneous catalysis. In particular, methanol synthesis from CO2 exhibits high potentials in terms of alternative energy sources to fossil fuels and NACs have shown promising performance in promoting the reaction. However, there still lacks of the bottom‐up catalysts design as well as the unanimous insight regarding the mechanistic understanding. Herein, we present a comprehensive overview of the physico‐chemical properties and the fabrication approach to NACs with high catalytic performance in the CO2 hydrogenation to methanol. Additionally, the progresses of NACs were comprehensively summarized in terms of mechanisms. Finally, some thinking about the further relevant studies on NACs is outlooked with the aim to provide new insights for achieving the precise design and controllable properties of NACs.

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A new adsorption energy-barrier relation and its application to CO₂ hydrogenation to methanol over In₂O₃-supported metal catalysts

Abstract: Herein, we report a new adsortpion energy-barrier relation, adsorbate-dependent barrier scaling (ADBS) relation, with which the catalytic activity of In2O3-supported metal catalysts for CO2 hydrogenation to methanol is predicted. It...

Cited by 7 publications

References 49 publications

CO₂ Hydrogenation to Methanol and Ethanol on In₂O₃-Based Single-Atom Catalysts and a New Scaling Relation

CO₂ Hydrogenation to Methanol and Ethanol on In₂O₃-Based Single-Atom Catalysts and a New Scaling Relation

The mechanism of CO₂ hydrogenation to CH₃OH on MZrO_x (M = Ga, Cr) solid-solution catalysts and effects of lattice strain

Nano‐alloy Catalysts for Methanol Synthesis from CO₂ Hydrogenation

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A new adsorption energy-barrier relation and its application to CO2 hydrogenation to methanol over In2O3-supported metal catalysts

Abstract: Herein, we report a new adsortpion energy-barrier relation, adsorbate-dependent barrier scaling (ADBS) relation, with which the catalytic activity of In2O3-supported metal catalysts for CO2 hydrogenation to methanol is predicted. It...

Cited by 7 publications

References 49 publications

CO2 Hydrogenation to Methanol and Ethanol on In2O3-Based Single-Atom Catalysts and a New Scaling Relation

CO2 Hydrogenation to Methanol and Ethanol on In2O3-Based Single-Atom Catalysts and a New Scaling Relation

The mechanism of CO2 hydrogenation to CH3OH on MZrOx (M = Ga, Cr) solid-solution catalysts and effects of lattice strain

Nano‐alloy Catalysts for Methanol Synthesis from CO2 Hydrogenation

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A new adsorption energy-barrier relation and its application to CO₂ hydrogenation to methanol over In₂O₃-supported metal catalysts

CO₂ Hydrogenation to Methanol and Ethanol on In₂O₃-Based Single-Atom Catalysts and a New Scaling Relation

CO₂ Hydrogenation to Methanol and Ethanol on In₂O₃-Based Single-Atom Catalysts and a New Scaling Relation

The mechanism of CO₂ hydrogenation to CH₃OH on MZrO_x (M = Ga, Cr) solid-solution catalysts and effects of lattice strain

Nano‐alloy Catalysts for Methanol Synthesis from CO₂ Hydrogenation