{"title":"Ru单原子/纳米粒子双位点催化剂接力催化甲苯加氢研究","authors":"Lingxia Zheng, Lubo Zhang, Jiawei Bai, Yifeng Zhang, Sentao Wei, Chenlong Zhang, Guojing Zhang, Yongbing Ma, Xin Wang, Yi Jia","doi":"10.1002/smll.202501665","DOIUrl":null,"url":null,"abstract":"<p>The methylcyclohexane-toluene-hydrogen (MTH) cycle is one of the most promising liquid organic hydrogen carrier (LOHC) systems. Despite the good performance of carbon-supported Pt nanoparticles, the drawbacks of noble metals, such as high cost and limited availability, hinder the industrial applications of these catalyst technologies. Herein, a ruthenium single-atom/nanoparticle (Ru SA/NP) dual-site electrocatalyst is developed with low metal loadings and notable electrochemical hydrogenation (ECH) efficiency of toluene (TL) to methylcyclohexane (MCH) in an electrochemical microreactor. The results reveal that within a wide potential window (∆V = 500 mV), the optimal catalyst Ru4-CN exhibits ≈100% Faraday efficiency (FE), high MCH selectivity, and significant inhibition of the hydrogen evolution reaction (HER). At a cell voltage of 2.0 V, the yield of MCH reaches 657.12 µmol h<sup>−1</sup> mg<sub>Ru</sub><sup>−1</sup>, which is ≈28 times higher than that of commercial Ru/C catalyst. Experimental and theoretical analyses indicate that TL preferentially adsorbs on Ru NP, while hydrogen atoms adsorb on Ru-SA to form H<sup>*</sup>, which is then delivered to Ru-NP to hydrogenate TL. This work brings forth a special design of Ru SA/NP dual-sites on the electrochemical hydrogenation of organic substrates and sheds light on the structure-activity relationships for future studies.</p>","PeriodicalId":228,"journal":{"name":"Small","volume":"21 24","pages":""},"PeriodicalIF":12.1000,"publicationDate":"2025-05-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Efficient Electrochemical Hydrogenation of Toluene by Relay Catalysis Over a Ru Single Atom/Nanoparticle Dual-Site Catalyst\",\"authors\":\"Lingxia Zheng, Lubo Zhang, Jiawei Bai, Yifeng Zhang, Sentao Wei, Chenlong Zhang, Guojing Zhang, Yongbing Ma, Xin Wang, Yi Jia\",\"doi\":\"10.1002/smll.202501665\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p>The methylcyclohexane-toluene-hydrogen (MTH) cycle is one of the most promising liquid organic hydrogen carrier (LOHC) systems. Despite the good performance of carbon-supported Pt nanoparticles, the drawbacks of noble metals, such as high cost and limited availability, hinder the industrial applications of these catalyst technologies. Herein, a ruthenium single-atom/nanoparticle (Ru SA/NP) dual-site electrocatalyst is developed with low metal loadings and notable electrochemical hydrogenation (ECH) efficiency of toluene (TL) to methylcyclohexane (MCH) in an electrochemical microreactor. The results reveal that within a wide potential window (∆V = 500 mV), the optimal catalyst Ru4-CN exhibits ≈100% Faraday efficiency (FE), high MCH selectivity, and significant inhibition of the hydrogen evolution reaction (HER). At a cell voltage of 2.0 V, the yield of MCH reaches 657.12 µmol h<sup>−1</sup> mg<sub>Ru</sub><sup>−1</sup>, which is ≈28 times higher than that of commercial Ru/C catalyst. Experimental and theoretical analyses indicate that TL preferentially adsorbs on Ru NP, while hydrogen atoms adsorb on Ru-SA to form H<sup>*</sup>, which is then delivered to Ru-NP to hydrogenate TL. This work brings forth a special design of Ru SA/NP dual-sites on the electrochemical hydrogenation of organic substrates and sheds light on the structure-activity relationships for future studies.</p>\",\"PeriodicalId\":228,\"journal\":{\"name\":\"Small\",\"volume\":\"21 24\",\"pages\":\"\"},\"PeriodicalIF\":12.1000,\"publicationDate\":\"2025-05-08\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Small\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://onlinelibrary.wiley.com/doi/10.1002/smll.202501665\",\"RegionNum\":2,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Small","FirstCategoryId":"88","ListUrlMain":"https://onlinelibrary.wiley.com/doi/10.1002/smll.202501665","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
Efficient Electrochemical Hydrogenation of Toluene by Relay Catalysis Over a Ru Single Atom/Nanoparticle Dual-Site Catalyst
The methylcyclohexane-toluene-hydrogen (MTH) cycle is one of the most promising liquid organic hydrogen carrier (LOHC) systems. Despite the good performance of carbon-supported Pt nanoparticles, the drawbacks of noble metals, such as high cost and limited availability, hinder the industrial applications of these catalyst technologies. Herein, a ruthenium single-atom/nanoparticle (Ru SA/NP) dual-site electrocatalyst is developed with low metal loadings and notable electrochemical hydrogenation (ECH) efficiency of toluene (TL) to methylcyclohexane (MCH) in an electrochemical microreactor. The results reveal that within a wide potential window (∆V = 500 mV), the optimal catalyst Ru4-CN exhibits ≈100% Faraday efficiency (FE), high MCH selectivity, and significant inhibition of the hydrogen evolution reaction (HER). At a cell voltage of 2.0 V, the yield of MCH reaches 657.12 µmol h−1 mgRu−1, which is ≈28 times higher than that of commercial Ru/C catalyst. Experimental and theoretical analyses indicate that TL preferentially adsorbs on Ru NP, while hydrogen atoms adsorb on Ru-SA to form H*, which is then delivered to Ru-NP to hydrogenate TL. This work brings forth a special design of Ru SA/NP dual-sites on the electrochemical hydrogenation of organic substrates and sheds light on the structure-activity relationships for future studies.
期刊介绍：
Small serves as an exceptional platform for both experimental and theoretical studies in fundamental and applied interdisciplinary research at the nano- and microscale. The journal offers a compelling mix of peer-reviewed Research Articles, Reviews, Perspectives, and Comments.
With a remarkable 2022 Journal Impact Factor of 13.3 (Journal Citation Reports from Clarivate Analytics, 2023), Small remains among the top multidisciplinary journals, covering a wide range of topics at the interface of materials science, chemistry, physics, engineering, medicine, and biology.
Small's readership includes biochemists, biologists, biomedical scientists, chemists, engineers, information technologists, materials scientists, physicists, and theoreticians alike.
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