{"title":"用于痕量H2S检测的高灵敏度和选择性锌基金属-有机框架衍生物气体传感器。","authors":"Wei Wang,Li Chen,Leif Riemenschneider,Chen-Chen Wang,Luis-Antonio Panes-Ruiz,Martin Hantusch,Yun-Xu Chen,Jian-Jun Zhang,Shivam Singh,Yana Vaynzof,Markus Löffler,Arezoo Dianat,Naisa Chandrasekhar,Shi-Rong Huang,Gianaurelio Cuniberti","doi":"10.1021/acssensors.5c01743","DOIUrl":null,"url":null,"abstract":"High sensitivity and selectivity are never-ending points of interest in the gas sensing field. Herein, the novel functionalized N-doped graphitic carbon is derived from Zn-MOF by modulating the pyrolysis temperature toward H2S sensing application. The results demonstrate excellent sensing performance toward H2S gas with a limit of detection (LOD) of 56.9 ppb, faster response and recovery time (18 and 29 s), and high selectivity with a 20-fold response difference than other interfering gases. The expected stability with stable multiple consecutive responses and a strong response toward 1 ppm of H2S after 4 months were reached. Functionalized groups pyridinic nitrogen (PD-N) and pyrrolic nitrogen (PR-N) that make MOF-derived carbon stand out in H2S gas sensing are mainly attributed to dual active sites: (i) N-C bonds on graphitic carbon undergo surface redox reactions, forming oxidized carbon species (C═O or C═S), and (ii) PD/PR-N-Zn coordination centers facilitate the formation of SO42--based surface complexes through reaction with H2S and adsorbed oxygen. Notably, DFT calculation was employed to confirm both PR-N and PD-N bonding with zinc, yielding the largest charge transfer and binding energy among simulated factors, which attributes to the generation of significant sensing performance for H2S. Consequently, this work will provide a novel strategy for the advancement of gas sensing applications.","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":"28 1","pages":""},"PeriodicalIF":9.1000,"publicationDate":"2025-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Highly Sensitive and Selective Zinc-Based Metal-Organic Framework Derivatives Gas Sensors for Trace H2S Detection.\",\"authors\":\"Wei Wang,Li Chen,Leif Riemenschneider,Chen-Chen Wang,Luis-Antonio Panes-Ruiz,Martin Hantusch,Yun-Xu Chen,Jian-Jun Zhang,Shivam Singh,Yana Vaynzof,Markus Löffler,Arezoo Dianat,Naisa Chandrasekhar,Shi-Rong Huang,Gianaurelio Cuniberti\",\"doi\":\"10.1021/acssensors.5c01743\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"High sensitivity and selectivity are never-ending points of interest in the gas sensing field. Herein, the novel functionalized N-doped graphitic carbon is derived from Zn-MOF by modulating the pyrolysis temperature toward H2S sensing application. The results demonstrate excellent sensing performance toward H2S gas with a limit of detection (LOD) of 56.9 ppb, faster response and recovery time (18 and 29 s), and high selectivity with a 20-fold response difference than other interfering gases. The expected stability with stable multiple consecutive responses and a strong response toward 1 ppm of H2S after 4 months were reached. Functionalized groups pyridinic nitrogen (PD-N) and pyrrolic nitrogen (PR-N) that make MOF-derived carbon stand out in H2S gas sensing are mainly attributed to dual active sites: (i) N-C bonds on graphitic carbon undergo surface redox reactions, forming oxidized carbon species (C═O or C═S), and (ii) PD/PR-N-Zn coordination centers facilitate the formation of SO42--based surface complexes through reaction with H2S and adsorbed oxygen. Notably, DFT calculation was employed to confirm both PR-N and PD-N bonding with zinc, yielding the largest charge transfer and binding energy among simulated factors, which attributes to the generation of significant sensing performance for H2S. Consequently, this work will provide a novel strategy for the advancement of gas sensing applications.\",\"PeriodicalId\":24,\"journal\":{\"name\":\"ACS Sensors\",\"volume\":\"28 1\",\"pages\":\"\"},\"PeriodicalIF\":9.1000,\"publicationDate\":\"2025-10-02\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ACS Sensors\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1021/acssensors.5c01743\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, ANALYTICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Sensors","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1021/acssensors.5c01743","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, ANALYTICAL","Score":null,"Total":0}
Highly Sensitive and Selective Zinc-Based Metal-Organic Framework Derivatives Gas Sensors for Trace H2S Detection.
High sensitivity and selectivity are never-ending points of interest in the gas sensing field. Herein, the novel functionalized N-doped graphitic carbon is derived from Zn-MOF by modulating the pyrolysis temperature toward H2S sensing application. The results demonstrate excellent sensing performance toward H2S gas with a limit of detection (LOD) of 56.9 ppb, faster response and recovery time (18 and 29 s), and high selectivity with a 20-fold response difference than other interfering gases. The expected stability with stable multiple consecutive responses and a strong response toward 1 ppm of H2S after 4 months were reached. Functionalized groups pyridinic nitrogen (PD-N) and pyrrolic nitrogen (PR-N) that make MOF-derived carbon stand out in H2S gas sensing are mainly attributed to dual active sites: (i) N-C bonds on graphitic carbon undergo surface redox reactions, forming oxidized carbon species (C═O or C═S), and (ii) PD/PR-N-Zn coordination centers facilitate the formation of SO42--based surface complexes through reaction with H2S and adsorbed oxygen. Notably, DFT calculation was employed to confirm both PR-N and PD-N bonding with zinc, yielding the largest charge transfer and binding energy among simulated factors, which attributes to the generation of significant sensing performance for H2S. Consequently, this work will provide a novel strategy for the advancement of gas sensing applications.
期刊介绍:
ACS Sensors is a peer-reviewed research journal that focuses on the dissemination of new and original knowledge in the field of sensor science, particularly those that selectively sense chemical or biological species or processes. The journal covers a broad range of topics, including but not limited to biosensors, chemical sensors, gas sensors, intracellular sensors, single molecule sensors, cell chips, and microfluidic devices. It aims to publish articles that address conceptual advances in sensing technology applicable to various types of analytes or application papers that report on the use of existing sensing concepts in new ways or for new analytes.