Enhancing CO2 methanation via synergistic multi-valence Pd0− Pdδ+ interactions on TiO2

Yawei Wu; Jui-Cheng Kao; Yu-Chieh Lo; Haolin Li; Alice Hu; Jyh-Pin Chou; Tsan-Yao Chen

doi:10.1016/j.apsusc.2024.160627

Enhancing CO₂ methanation via synergistic multi-valence Pd⁰− Pd^δ+ interactions on TiO₂

Yawei Wu, Jui-Cheng Kao, Yu-Chieh Lo, Haolin Li^*, Alice Hu^*, Jyh-Pin Chou^*, Tsan-Yao Chen^*

^*Corresponding author for this work

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

4 Citations (Scopus)

Abstract

Converting CO₂ waste into valuable chemicals through hydrogenation is promising for reducing atmospheric CO₂ and promoting sustainable carbon recycling. Supported Pd catalysts are commonly studied for CO₂ methanation, yet the pivotal role of interfacial Pd species remains unclear due to ambiguous experimental results, impeding further catalyst enhancements. This study uses theoretical calculations to explore how interfacial Pd sites influence catalytic performance in Pd-PdO_x@TiO₂ catalysts during CO₂ methanation. Our findings show that H₂ preferentially dissociates at Pd⁰ sites, while Pd^δ+ sites primarily activate CO₂. Adjusting the Pd⁰/Pd^δ+ ratios optimizes the electronic properties of these sites, enhancing CO₂ activation efficiency. The designed Pd₂₁-Pd₈O₉@TiO₂ nanocatalyst with adjusted electronic states significantly promotes electron transfer to CO₂, favoring CH₄ formation by stabilizing the *CH₃ intermediate and reducing the activation barrier for its conversion to *CH₄. These insights advance understanding of interface engineering in metal-support systems for CO₂ hydrogenation. © 2024 Elsevier B.V.

Original language	English
Article number	160627
Journal	Applied Surface Science
Volume	670
Online published	2 Jul 2024
DOIs	https://doi.org/10.1016/j.apsusc.2024.160627
Publication status	Published - 15 Oct 2024

Funding

The authors would like to thank the National Center for High- performance Computing (NCHC) of National Applied Research Laboratories (NARLabs) in Taiwan for providing computational and storage resources. J.-P. Chou is thankful for the funding support from the National Science and Technology Council, Taiwan (NSTC 112-2112-M-018-005-). T.-Y. Chen acknowledges the funding support from the National Science and Technology Council, Taiwan (NSTC 112-2112-M-007-026-) and the industrial collaboration projects from the MA-tek (MA-tek 2023-T-004 ) and the Taiwan Space Agency ( TASA-S-1120691 ). Y.-C. Lo gratefully acknowledges the funding support from the National Science and Technology Council, Taiwan ( 112-2221-E-A49-030 ) and extends thanks the Center for Advanced Semiconductor Technology Research from The Featured Areas Research Center Program within the framework of the Higher Education Sprout Project by the Ministry of Education in Taiwan. A. Hu gratefully acknowledges the sponsorship from Research Grants Council of the Hong Kong Special Administrative Region, China (Project No. CityU 11200120 ), City University of Hong Kong (Project No. 7005615 , 7006103 ), CityU Seed Fund in Microelectronics (Project No. 9229135 ). H. Li acknowledges the funding support by Zhejiang Provincial Natural Science Foundation of China, China (Grant No. LQ23E020008 ) and Science Foundation of Zhejiang Sci-Tech University (ZSTU), China (Grant No. 22212153-Y ).

Research Keywords

Catalytic performance
CO2 hydrogenation
Interface engineering
Interfacial Pd species
Pd catalysts
Pd-PdOx@TiO2 catalysts

RGC Funding Information

RGC-funded

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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10.1016/j.apsusc.2024.160627

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title = "Enhancing CO2 methanation via synergistic multi-valence Pd0− Pdδ+ interactions on TiO2",

abstract = "Converting CO2 waste into valuable chemicals through hydrogenation is promising for reducing atmospheric CO2 and promoting sustainable carbon recycling. Supported Pd catalysts are commonly studied for CO2 methanation, yet the pivotal role of interfacial Pd species remains unclear due to ambiguous experimental results, impeding further catalyst enhancements. This study uses theoretical calculations to explore how interfacial Pd sites influence catalytic performance in Pd-PdOx@TiO2 catalysts during CO2 methanation. Our findings show that H2 preferentially dissociates at Pd0 sites, while Pdδ+ sites primarily activate CO2. Adjusting the Pd0/Pdδ+ ratios optimizes the electronic properties of these sites, enhancing CO2 activation efficiency. The designed Pd21-Pd8O9@TiO2 nanocatalyst with adjusted electronic states significantly promotes electron transfer to CO2, favoring CH4 formation by stabilizing the *CH3 intermediate and reducing the activation barrier for its conversion to *CH4. These insights advance understanding of interface engineering in metal-support systems for CO2 hydrogenation. {\textcopyright} 2024 Elsevier B.V.",

keywords = "Catalytic performance, CO2 hydrogenation, Interface engineering, Interfacial Pd species, Pd catalysts, Pd-PdOx@TiO2 catalysts",

author = "Yawei Wu and Jui-Cheng Kao and Yu-Chieh Lo and Haolin Li and Alice Hu and Jyh-Pin Chou and Tsan-Yao Chen",

year = "2024",

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doi = "10.1016/j.apsusc.2024.160627",

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TY - JOUR

T1 - Enhancing CO2 methanation via synergistic multi-valence Pd0− Pdδ+ interactions on TiO2

AU - Wu, Yawei

AU - Kao, Jui-Cheng

AU - Lo, Yu-Chieh

AU - Li, Haolin

AU - Hu, Alice

AU - Chou, Jyh-Pin

AU - Chen, Tsan-Yao

PY - 2024/10/15

Y1 - 2024/10/15

N2 - Converting CO2 waste into valuable chemicals through hydrogenation is promising for reducing atmospheric CO2 and promoting sustainable carbon recycling. Supported Pd catalysts are commonly studied for CO2 methanation, yet the pivotal role of interfacial Pd species remains unclear due to ambiguous experimental results, impeding further catalyst enhancements. This study uses theoretical calculations to explore how interfacial Pd sites influence catalytic performance in Pd-PdOx@TiO2 catalysts during CO2 methanation. Our findings show that H2 preferentially dissociates at Pd0 sites, while Pdδ+ sites primarily activate CO2. Adjusting the Pd0/Pdδ+ ratios optimizes the electronic properties of these sites, enhancing CO2 activation efficiency. The designed Pd21-Pd8O9@TiO2 nanocatalyst with adjusted electronic states significantly promotes electron transfer to CO2, favoring CH4 formation by stabilizing the *CH3 intermediate and reducing the activation barrier for its conversion to *CH4. These insights advance understanding of interface engineering in metal-support systems for CO2 hydrogenation. © 2024 Elsevier B.V.

AB - Converting CO2 waste into valuable chemicals through hydrogenation is promising for reducing atmospheric CO2 and promoting sustainable carbon recycling. Supported Pd catalysts are commonly studied for CO2 methanation, yet the pivotal role of interfacial Pd species remains unclear due to ambiguous experimental results, impeding further catalyst enhancements. This study uses theoretical calculations to explore how interfacial Pd sites influence catalytic performance in Pd-PdOx@TiO2 catalysts during CO2 methanation. Our findings show that H2 preferentially dissociates at Pd0 sites, while Pdδ+ sites primarily activate CO2. Adjusting the Pd0/Pdδ+ ratios optimizes the electronic properties of these sites, enhancing CO2 activation efficiency. The designed Pd21-Pd8O9@TiO2 nanocatalyst with adjusted electronic states significantly promotes electron transfer to CO2, favoring CH4 formation by stabilizing the *CH3 intermediate and reducing the activation barrier for its conversion to *CH4. These insights advance understanding of interface engineering in metal-support systems for CO2 hydrogenation. © 2024 Elsevier B.V.

KW - Catalytic performance

KW - CO2 hydrogenation

KW - Interface engineering

KW - Interfacial Pd species

KW - Pd catalysts

KW - Pd-PdOx@TiO2 catalysts

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U2 - 10.1016/j.apsusc.2024.160627

DO - 10.1016/j.apsusc.2024.160627

M3 - RGC 21 - Publication in refereed journal

SN - 0169-4332

VL - 670

JO - Applied Surface Science

JF - Applied Surface Science

M1 - 160627

ER -

Enhancing CO₂ methanation via synergistic multi-valence Pd⁰− Pd^δ+ interactions on TiO₂

Abstract

Funding

Research Keywords

RGC Funding Information

UN SDGs

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DON_RMG: A Quantum-classical Hybrid Clustering Algorithm for Excited States Preparation - RMGS

GRF: Sparks When Quantum Computing Meet Ab Initio Calculation

Cite this

Enhancing CO2 methanation via synergistic multi-valence Pd0− Pdδ+ interactions on TiO2

Abstract

Funding

Research Keywords

RGC Funding Information

UN SDGs

Access Output

Other Access Options

Permanent Link

Other Files and Links

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Projects

DON_RMG: A Quantum-classical Hybrid Clustering Algorithm for Excited States Preparation - RMGS

GRF: Sparks When Quantum Computing Meet Ab Initio Calculation

Cite this

Enhancing CO₂ methanation via synergistic multi-valence Pd⁰− Pd^δ+ interactions on TiO₂