{"title":"c60支持的单Pt原子选择性活化CH4。","authors":"Jiao-Jiao Chen*, Xi-Guan Zhao, Bo-Han Zang, Hui-Ru Jia, Qing-Yu Liu, Xun-Lei Ding and Sheng-Gui He*, ","doi":"10.1021/acs.jpclett.5c01340","DOIUrl":null,"url":null,"abstract":"<p >Supported single-atom catalysts (SACs) exhibit great potential for the selective activation of C–H bonds, enabling the direct conversion of methane (CH<sub>4</sub>) into high value-added chemical products. Herein, benefiting from state-of-the-art mass spectrometry coupled with newly designed variable-temperature double ion trap reactors, we successfully immobilized a single Pt<sup>–</sup> atom on a unique zero-dimensional carbon support (C<sub>60</sub>) and observed a significantly enhanced reactivity of C<sub>60</sub>Pt<sup>–</sup> toward CH<sub>4</sub> activation at room temperature compared to inert bare Pt<sup>–</sup>. The crucial role of the C<sub>60</sub> support in modifying the electronic state of the single metal site (Pt<sup>–</sup> → Pt<sup>0</sup>) was highlighted as a key factor in enhancing orbital interactions with CH<sub>4</sub>. Furthermore, the electron-buffering capability of C<sub>60</sub> also facilitates selective CH<sub>4</sub> activation by cleaving only one C–H bond. This finding not only provides atomic-scale insights into supported SACs for CH<sub>4</sub> activation but also underscores the importance of considering the positive support effects of C<sub>60</sub> in designing related catalysts for direct CH<sub>4</sub> conversion.</p>","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":"16 25","pages":"6463–6469"},"PeriodicalIF":4.6000,"publicationDate":"2025-06-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"C60-Supported Single Pt Atom for Selective CH4 Activation\",\"authors\":\"Jiao-Jiao Chen*, Xi-Guan Zhao, Bo-Han Zang, Hui-Ru Jia, Qing-Yu Liu, Xun-Lei Ding and Sheng-Gui He*, \",\"doi\":\"10.1021/acs.jpclett.5c01340\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >Supported single-atom catalysts (SACs) exhibit great potential for the selective activation of C–H bonds, enabling the direct conversion of methane (CH<sub>4</sub>) into high value-added chemical products. Herein, benefiting from state-of-the-art mass spectrometry coupled with newly designed variable-temperature double ion trap reactors, we successfully immobilized a single Pt<sup>–</sup> atom on a unique zero-dimensional carbon support (C<sub>60</sub>) and observed a significantly enhanced reactivity of C<sub>60</sub>Pt<sup>–</sup> toward CH<sub>4</sub> activation at room temperature compared to inert bare Pt<sup>–</sup>. The crucial role of the C<sub>60</sub> support in modifying the electronic state of the single metal site (Pt<sup>–</sup> → Pt<sup>0</sup>) was highlighted as a key factor in enhancing orbital interactions with CH<sub>4</sub>. Furthermore, the electron-buffering capability of C<sub>60</sub> also facilitates selective CH<sub>4</sub> activation by cleaving only one C–H bond. This finding not only provides atomic-scale insights into supported SACs for CH<sub>4</sub> activation but also underscores the importance of considering the positive support effects of C<sub>60</sub> in designing related catalysts for direct CH<sub>4</sub> conversion.</p>\",\"PeriodicalId\":62,\"journal\":{\"name\":\"The Journal of Physical Chemistry Letters\",\"volume\":\"16 25\",\"pages\":\"6463–6469\"},\"PeriodicalIF\":4.6000,\"publicationDate\":\"2025-06-17\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"The Journal of Physical Chemistry Letters\",\"FirstCategoryId\":\"1\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/acs.jpclett.5c01340\",\"RegionNum\":2,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"The Journal of Physical Chemistry Letters","FirstCategoryId":"1","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acs.jpclett.5c01340","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
C60-Supported Single Pt Atom for Selective CH4 Activation
Supported single-atom catalysts (SACs) exhibit great potential for the selective activation of C–H bonds, enabling the direct conversion of methane (CH4) into high value-added chemical products. Herein, benefiting from state-of-the-art mass spectrometry coupled with newly designed variable-temperature double ion trap reactors, we successfully immobilized a single Pt– atom on a unique zero-dimensional carbon support (C60) and observed a significantly enhanced reactivity of C60Pt– toward CH4 activation at room temperature compared to inert bare Pt–. The crucial role of the C60 support in modifying the electronic state of the single metal site (Pt– → Pt0) was highlighted as a key factor in enhancing orbital interactions with CH4. Furthermore, the electron-buffering capability of C60 also facilitates selective CH4 activation by cleaving only one C–H bond. This finding not only provides atomic-scale insights into supported SACs for CH4 activation but also underscores the importance of considering the positive support effects of C60 in designing related catalysts for direct CH4 conversion.
期刊介绍:
The Journal of Physical Chemistry (JPC) Letters is devoted to reporting new and original experimental and theoretical basic research of interest to physical chemists, biophysical chemists, chemical physicists, physicists, material scientists, and engineers. An important criterion for acceptance is that the paper reports a significant scientific advance and/or physical insight such that rapid publication is essential. Two issues of JPC Letters are published each month.