Pd nanocatalysts engineering for direct oxidation methane-to-methanol with 99.7% selectivity
Abstract Pd catalysts demonstrate remarkable activity and selectivity for the direct oxidation methane-to-methanol (DOMM) under mild conditions. However, understanding the structure–performance relationship is challenging because Pd catalysts used in existing studies have complex polycrystalline str...
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| Main Authors: | , , , , , , , |
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| Format: | Article |
| Language: | English |
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Nature Portfolio
2025-08-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-025-63067-0 |
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| _version_ | 1849226159858909184 |
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| author | Peilin Deng Yueshan Xu Daoxiong Wu Ying Liang Xue Zhang Zhitong Wang Jing Li Xinlong Tian |
| author_facet | Peilin Deng Yueshan Xu Daoxiong Wu Ying Liang Xue Zhang Zhitong Wang Jing Li Xinlong Tian |
| author_sort | Peilin Deng |
| collection | DOAJ |
| description | Abstract Pd catalysts demonstrate remarkable activity and selectivity for the direct oxidation methane-to-methanol (DOMM) under mild conditions. However, understanding the structure–performance relationship is challenging because Pd catalysts used in existing studies have complex polycrystalline structures. In this work, well-defined Pd nanocrystals with controlled morphologies are synthesized and used as model systems to investigate the origins of the observed structure-activity differences. Our findings indicate that DOMM activity is primarily governed by crystal facet type rather than nanocrystal size. The lower d-band center of the Pd {111} facet weakens the adsorption strength of critical intermediates, including *O2 and *OH species, promoting H2O2 generation and CH3OH formation, respectively. Consequently, {111}-dominated octahedral Pd nanocrystals achieve an exceptional CH3OH yield of 201.8 mmol·gPd −1·h−1, three times higher than that of their {100}-dominated hexahedral counterparts. These results provide key insights into the structure-dependent behavior of Pd catalysts and pave the way for designing high-performance catalysts for DOMM. |
| format | Article |
| id | doaj-art-b849065fc89d4d4a8dfaa1c150729ba3 |
| institution | Kabale University |
| issn | 2041-1723 |
| language | English |
| publishDate | 2025-08-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj-art-b849065fc89d4d4a8dfaa1c150729ba32025-08-24T11:36:55ZengNature PortfolioNature Communications2041-17232025-08-011611810.1038/s41467-025-63067-0Pd nanocatalysts engineering for direct oxidation methane-to-methanol with 99.7% selectivityPeilin Deng0Yueshan Xu1Daoxiong Wu2Ying Liang3Xue Zhang4Zhitong Wang5Jing Li6Xinlong Tian7State Key Laboratory of Tropic Ocean Engineering Materials and Materials Evaluation, School of Marine Science and Engineering, Hainan UniversityState Key Laboratory of Tropic Ocean Engineering Materials and Materials Evaluation, School of Marine Science and Engineering, Hainan UniversityState Key Laboratory of Tropic Ocean Engineering Materials and Materials Evaluation, School of Marine Science and Engineering, Hainan UniversityState Key Laboratory of Tropic Ocean Engineering Materials and Materials Evaluation, School of Marine Science and Engineering, Hainan UniversityState Key Laboratory of Tropic Ocean Engineering Materials and Materials Evaluation, School of Marine Science and Engineering, Hainan UniversityState Key Laboratory of Tropic Ocean Engineering Materials and Materials Evaluation, School of Marine Science and Engineering, Hainan UniversityState Key Laboratory of Tropic Ocean Engineering Materials and Materials Evaluation, School of Marine Science and Engineering, Hainan UniversityState Key Laboratory of Tropic Ocean Engineering Materials and Materials Evaluation, School of Marine Science and Engineering, Hainan UniversityAbstract Pd catalysts demonstrate remarkable activity and selectivity for the direct oxidation methane-to-methanol (DOMM) under mild conditions. However, understanding the structure–performance relationship is challenging because Pd catalysts used in existing studies have complex polycrystalline structures. In this work, well-defined Pd nanocrystals with controlled morphologies are synthesized and used as model systems to investigate the origins of the observed structure-activity differences. Our findings indicate that DOMM activity is primarily governed by crystal facet type rather than nanocrystal size. The lower d-band center of the Pd {111} facet weakens the adsorption strength of critical intermediates, including *O2 and *OH species, promoting H2O2 generation and CH3OH formation, respectively. Consequently, {111}-dominated octahedral Pd nanocrystals achieve an exceptional CH3OH yield of 201.8 mmol·gPd −1·h−1, three times higher than that of their {100}-dominated hexahedral counterparts. These results provide key insights into the structure-dependent behavior of Pd catalysts and pave the way for designing high-performance catalysts for DOMM.https://doi.org/10.1038/s41467-025-63067-0 |
| spellingShingle | Peilin Deng Yueshan Xu Daoxiong Wu Ying Liang Xue Zhang Zhitong Wang Jing Li Xinlong Tian Pd nanocatalysts engineering for direct oxidation methane-to-methanol with 99.7% selectivity Nature Communications |
| title | Pd nanocatalysts engineering for direct oxidation methane-to-methanol with 99.7% selectivity |
| title_full | Pd nanocatalysts engineering for direct oxidation methane-to-methanol with 99.7% selectivity |
| title_fullStr | Pd nanocatalysts engineering for direct oxidation methane-to-methanol with 99.7% selectivity |
| title_full_unstemmed | Pd nanocatalysts engineering for direct oxidation methane-to-methanol with 99.7% selectivity |
| title_short | Pd nanocatalysts engineering for direct oxidation methane-to-methanol with 99.7% selectivity |
| title_sort | pd nanocatalysts engineering for direct oxidation methane to methanol with 99 7 selectivity |
| url | https://doi.org/10.1038/s41467-025-63067-0 |
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