Operando XAS and DFT Uncover Structure-Performance Relationships in Re/TiO ₂ for Selective CO ₂ Hydrogenation to Methanol Article Swipe

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Maitê L. Gothe , Adriano H. Braga , Laís Reis Borges , Jiyun Hong , Giliandro Farias , Alvaro David Torrez Baptista , Bryan Alberto Laura Larico , Ana Bárbara Moulin Cansian , Caetano R. Miranda , Simon R. Bare , Liane M. Rossi , Pedro Vidinha ·

YOU? · · 2025 · Open Access · · DOI: https://doi.org/10.1021/acscatal.5c05984

The conversion of CO₂ into value-added chemicals, such as methanol, offers a promising pathway toward a renewable energy future. However, a precise kinetic control and a highly selective catalyst are necessary to overcome the thermodynamic preference for CO₂ hydrogenation to methane. Rhenium-based catalysts, particularly Re/TiO₂, demonstrate high activity and selectivity for methanol under high-pressure conditions. For example, at 100 bar and 200 °C, a methanol selectivity of 97-99% was obtained. Catalysts with 1 wt % Re and 5 wt % Re/TiO₂ were used to study the effect of cluster sizes. At 250 °C, the 1 wt % catalyst achieves 97% selectivity at 23% conversion, whereas 5 wt % Re/TiO₂ achieves 74% selectivity at 40% conversion, corresponding to a drop in space-time yield from 65 to 16 g_CH₃OH·g_Re ^-1·h^-1, respectively. X-ray absorption spectroscopy provided insights into the structure of the active sites, while density functional theory calculations revealed the effects of cluster size on the energy barriers for H₂ activation, CH₃OH dissociation, and CH₃OH desorption, all of which directly influence conversion and selectivity. These results underscore the importance of balancing cluster size for optimal catalyst performance and provide insights into the design of efficient and selective catalysts for renewable methanol production.

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Type: article
Language: en
Landing Page: https://doi.org/10.1021/acscatal.5c05984
OA Status: hybrid
References: 79
OpenAlex ID: https://openalex.org/W4415869859

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DOI: https://doi.org/10.1021/acscatal.5c05984

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Title: Operando XAS and DFT Uncover Structure-Performance Relationships in Re/TiO ₂ for Selective CO ₂ Hydrogenation to Methanol

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Type: article

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Language: en

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Publication year: 2025

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Publication date: 2025-11-04

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Authors: Maitê L. Gothe, Adriano H. Braga, Laís Reis Borges, Jiyun Hong, Giliandro Farias, Alvaro David Torrez Baptista, Bryan Alberto Laura Larico, Ana Bárbara Moulin Cansian, Caetano R. Miranda, Simon R. Bare, Liane M. Rossi, Pedro Vidinha

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Landing page: https://doi.org/10.1021/acscatal.5c05984

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Cited by: 0

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References (count): 79

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abstract_inverted_index.These	172
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abstract_inverted_index.study	84
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abstract_inverted_index.97-99%	67
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abstract_inverted_index.energy	17, 154
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abstract_inverted_index.offers	10
abstract_inverted_index.sites,	140
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abstract_inverted_index.future.	18
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abstract_inverted_index.directly	167
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abstract_inverted_index.desorption,	163
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abstract_inverted_index.calculations	145
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abstract_inverted_index.selectivity.	171
abstract_inverted_index.spectroscopy	131
abstract_inverted_index.H<sub>2</sub>	157
abstract_inverted_index.Rhenium-based	41
abstract_inverted_index.corresponding	115
abstract_inverted_index.dissociation,	160
abstract_inverted_index.high-pressure	53
abstract_inverted_index.hydrogenation	38
abstract_inverted_index.respectively.	128
abstract_inverted_index.thermodynamic	34
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citation_normalized_percentile

Operando XAS and DFT Uncover Structure-Performance Relationships in Re/TiO 2 for Selective CO 2 Hydrogenation to Methanol Article Swipe

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Operando XAS and DFT Uncover Structure-Performance Relationships in Re/TiO ₂ for Selective CO ₂ Hydrogenation to Methanol Article Swipe