Designing main-group catalysts for low-temperature methane combustion by ozone
Abstract The catalytic combustion of methane at a low temperature is becoming increasingly key to controlling unburned CH4 emissions from natural gas vehicles and power plants, although the low activity of benchmark platinum-group-metal catalysts hinders its broad application. Based on automated rea...
| Main Authors: | , , , , , , , , |
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| Format: | Article |
| Language: | English |
| Published: |
Nature Portfolio
2023-07-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-023-39541-y |
| _version_ | 1797784468088422400 |
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| author | Shunsaku Yasumura Kenichiro Saita Takumi Miyakage Ken Nagai Kenichi Kon Takashi Toyao Zen Maeno Tetsuya Taketsugu Ken-ichi Shimizu |
| author_facet | Shunsaku Yasumura Kenichiro Saita Takumi Miyakage Ken Nagai Kenichi Kon Takashi Toyao Zen Maeno Tetsuya Taketsugu Ken-ichi Shimizu |
| author_sort | Shunsaku Yasumura |
| collection | DOAJ |
| description | Abstract The catalytic combustion of methane at a low temperature is becoming increasingly key to controlling unburned CH4 emissions from natural gas vehicles and power plants, although the low activity of benchmark platinum-group-metal catalysts hinders its broad application. Based on automated reaction route mapping, we explore main-group elements catalysts containing Si and Al for low-temperature CH4 combustion with ozone. Computational screening of the active site predicts that strong Brønsted acid sites are promising for methane combustion. We experimentally demonstrate that catalysts containing strong Bronsted acid sites exhibit improved CH4 conversion at 250 °C, correlating with the theoretical predictions. The main-group catalyst (proton-type beta zeolite) delivered a reaction rate that is 442 times higher than that of a benchmark catalyst (5 wt% Pd-loaded Al2O3) at 190 °C and exhibits higher tolerance to steam and SO2. Our strategy demonstrates the rational design of earth-abundant catalysts based on automated reaction route mapping. |
| first_indexed | 2024-03-13T00:40:18Z |
| format | Article |
| id | doaj.art-14a0cb7e5b724fec926f48c1c1c152e5 |
| institution | Directory Open Access Journal |
| issn | 2041-1723 |
| language | English |
| last_indexed | 2024-03-13T00:40:18Z |
| publishDate | 2023-07-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj.art-14a0cb7e5b724fec926f48c1c1c152e52023-07-09T11:19:07ZengNature PortfolioNature Communications2041-17232023-07-0114111110.1038/s41467-023-39541-yDesigning main-group catalysts for low-temperature methane combustion by ozoneShunsaku Yasumura0Kenichiro Saita1Takumi Miyakage2Ken Nagai3Kenichi Kon4Takashi Toyao5Zen Maeno6Tetsuya Taketsugu7Ken-ichi Shimizu8Institute for Catalysis, Hokkaido UniversityDepartment of Chemistry, Faculty of Science, Hokkaido UniversityInstitute for Catalysis, Hokkaido UniversityInstitute for Catalysis, Hokkaido UniversityInstitute for Catalysis, Hokkaido UniversityInstitute for Catalysis, Hokkaido UniversitySchool of Advanced Engineering, Kogakuin UniversityDepartment of Chemistry, Faculty of Science, Hokkaido UniversityInstitute for Catalysis, Hokkaido UniversityAbstract The catalytic combustion of methane at a low temperature is becoming increasingly key to controlling unburned CH4 emissions from natural gas vehicles and power plants, although the low activity of benchmark platinum-group-metal catalysts hinders its broad application. Based on automated reaction route mapping, we explore main-group elements catalysts containing Si and Al for low-temperature CH4 combustion with ozone. Computational screening of the active site predicts that strong Brønsted acid sites are promising for methane combustion. We experimentally demonstrate that catalysts containing strong Bronsted acid sites exhibit improved CH4 conversion at 250 °C, correlating with the theoretical predictions. The main-group catalyst (proton-type beta zeolite) delivered a reaction rate that is 442 times higher than that of a benchmark catalyst (5 wt% Pd-loaded Al2O3) at 190 °C and exhibits higher tolerance to steam and SO2. Our strategy demonstrates the rational design of earth-abundant catalysts based on automated reaction route mapping.https://doi.org/10.1038/s41467-023-39541-y |
| spellingShingle | Shunsaku Yasumura Kenichiro Saita Takumi Miyakage Ken Nagai Kenichi Kon Takashi Toyao Zen Maeno Tetsuya Taketsugu Ken-ichi Shimizu Designing main-group catalysts for low-temperature methane combustion by ozone Nature Communications |
| title | Designing main-group catalysts for low-temperature methane combustion by ozone |
| title_full | Designing main-group catalysts for low-temperature methane combustion by ozone |
| title_fullStr | Designing main-group catalysts for low-temperature methane combustion by ozone |
| title_full_unstemmed | Designing main-group catalysts for low-temperature methane combustion by ozone |
| title_short | Designing main-group catalysts for low-temperature methane combustion by ozone |
| title_sort | designing main group catalysts for low temperature methane combustion by ozone |
| url | https://doi.org/10.1038/s41467-023-39541-y |
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