Xiaojun Liu, Xiaoyu Chen, Yao Xiao, Ziming Yang, Yong Xu, Andrew P. Ault and Xiangqun Zeng*,
{"title":"PtNi纳米晶体-离子液体界面:高效可靠的H2检测创新平台","authors":"Xiaojun Liu, Xiaoyu Chen, Yao Xiao, Ziming Yang, Yong Xu, Andrew P. Ault and Xiangqun Zeng*, ","doi":"10.1021/acssensors.4c03564","DOIUrl":null,"url":null,"abstract":"<p >The transition to hydrogen (H<sub>2</sub>) as a clean alternative energy source demands rigorous safety, especially in its storage, transportation, and application due to its inherently explosive nature. Moreover, H<sub>2</sub> emissions into the atmosphere can disrupt the atmospheric balance of greenhouse gases, such as methane, ozone, and water vapor, leading to indirect contributions to short-term global temperature increases. To address this, the development of high-performance H<sub>2</sub> gas sensors is crucial for the early detection and warning of potential leakages, both ensuring safety and assessing their environmental impact. In this study, we present a real-time, high-performance electrochemical H<sub>2</sub> sensor featuring an innovative electrochemical interface between octahedral PtNi alloy nanocrystals and two distinct ionic liquid electrolytes: 1-butyl-1-methylpyrrolidinium bis(trifluoromethylsulfonyl)imide ([Bmpy][NTf<sub>2</sub>]) and 1-butyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide ([Bmim][NTf<sub>2</sub>]). We demonstrated that the PtNi/[Bmpy][NTf<sub>2</sub>] interface achieves exceptional sensitivity, with a limit of detection of 107.1 ppm, as well as rapid response time of 17 s and recovery time of 21 s, excellent selectivity, and long-term stability, with only a 1.1% degradation observed over a 120 day test period. Experimental analysis and theoretical calculations reveal that [Bmpy][NTf<sub>2</sub>] surpasses [Bmim][NTf<sub>2</sub>] due to its better wettability, lower H<sub>2</sub> solvation energy, and favorable H<sub>2</sub> dissociation kinetics for the H<sub>2</sub> oxidation reaction (HOR). These characteristics enhance H<sub>2</sub> solubility and facilitate H<sub>2</sub> oxidation on the PtNi nanocrystal surface, making [Bmpy][NTf<sub>2</sub>] superior to [Bmim][NTf<sub>2</sub>] as the electrolyte for H<sub>2</sub> sensing application. This study advances high-sensitivity durable H<sub>2</sub> sensor technology and offers insights into the interactions between metal alloy nanocrystals and ionic liquids, guiding the design of next-generation H<sub>2</sub> sensors for environmental monitoring, industrial safety, and sustainable energy systems.</p>","PeriodicalId":24,"journal":{"name":"ACS Sensors","volume":"10 6","pages":"3993–4005"},"PeriodicalIF":9.1000,"publicationDate":"2025-06-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"PtNi Nanocrystal–Ionic Liquid Interfaces: An Innovative Platform for High-Performance and Reliable H2 Detection\",\"authors\":\"Xiaojun Liu, Xiaoyu Chen, Yao Xiao, Ziming Yang, Yong Xu, Andrew P. Ault and Xiangqun Zeng*, \",\"doi\":\"10.1021/acssensors.4c03564\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >The transition to hydrogen (H<sub>2</sub>) as a clean alternative energy source demands rigorous safety, especially in its storage, transportation, and application due to its inherently explosive nature. Moreover, H<sub>2</sub> emissions into the atmosphere can disrupt the atmospheric balance of greenhouse gases, such as methane, ozone, and water vapor, leading to indirect contributions to short-term global temperature increases. To address this, the development of high-performance H<sub>2</sub> gas sensors is crucial for the early detection and warning of potential leakages, both ensuring safety and assessing their environmental impact. In this study, we present a real-time, high-performance electrochemical H<sub>2</sub> sensor featuring an innovative electrochemical interface between octahedral PtNi alloy nanocrystals and two distinct ionic liquid electrolytes: 1-butyl-1-methylpyrrolidinium bis(trifluoromethylsulfonyl)imide ([Bmpy][NTf<sub>2</sub>]) and 1-butyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide ([Bmim][NTf<sub>2</sub>]). We demonstrated that the PtNi/[Bmpy][NTf<sub>2</sub>] interface achieves exceptional sensitivity, with a limit of detection of 107.1 ppm, as well as rapid response time of 17 s and recovery time of 21 s, excellent selectivity, and long-term stability, with only a 1.1% degradation observed over a 120 day test period. Experimental analysis and theoretical calculations reveal that [Bmpy][NTf<sub>2</sub>] surpasses [Bmim][NTf<sub>2</sub>] due to its better wettability, lower H<sub>2</sub> solvation energy, and favorable H<sub>2</sub> dissociation kinetics for the H<sub>2</sub> oxidation reaction (HOR). These characteristics enhance H<sub>2</sub> solubility and facilitate H<sub>2</sub> oxidation on the PtNi nanocrystal surface, making [Bmpy][NTf<sub>2</sub>] superior to [Bmim][NTf<sub>2</sub>] as the electrolyte for H<sub>2</sub> sensing application. This study advances high-sensitivity durable H<sub>2</sub> sensor technology and offers insights into the interactions between metal alloy nanocrystals and ionic liquids, guiding the design of next-generation H<sub>2</sub> sensors for environmental monitoring, industrial safety, and sustainable energy systems.</p>\",\"PeriodicalId\":24,\"journal\":{\"name\":\"ACS Sensors\",\"volume\":\"10 6\",\"pages\":\"3993–4005\"},\"PeriodicalIF\":9.1000,\"publicationDate\":\"2025-06-06\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ACS Sensors\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/acssensors.4c03564\",\"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://pubs.acs.org/doi/10.1021/acssensors.4c03564","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, ANALYTICAL","Score":null,"Total":0}
PtNi Nanocrystal–Ionic Liquid Interfaces: An Innovative Platform for High-Performance and Reliable H2 Detection
The transition to hydrogen (H2) as a clean alternative energy source demands rigorous safety, especially in its storage, transportation, and application due to its inherently explosive nature. Moreover, H2 emissions into the atmosphere can disrupt the atmospheric balance of greenhouse gases, such as methane, ozone, and water vapor, leading to indirect contributions to short-term global temperature increases. To address this, the development of high-performance H2 gas sensors is crucial for the early detection and warning of potential leakages, both ensuring safety and assessing their environmental impact. In this study, we present a real-time, high-performance electrochemical H2 sensor featuring an innovative electrochemical interface between octahedral PtNi alloy nanocrystals and two distinct ionic liquid electrolytes: 1-butyl-1-methylpyrrolidinium bis(trifluoromethylsulfonyl)imide ([Bmpy][NTf2]) and 1-butyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide ([Bmim][NTf2]). We demonstrated that the PtNi/[Bmpy][NTf2] interface achieves exceptional sensitivity, with a limit of detection of 107.1 ppm, as well as rapid response time of 17 s and recovery time of 21 s, excellent selectivity, and long-term stability, with only a 1.1% degradation observed over a 120 day test period. Experimental analysis and theoretical calculations reveal that [Bmpy][NTf2] surpasses [Bmim][NTf2] due to its better wettability, lower H2 solvation energy, and favorable H2 dissociation kinetics for the H2 oxidation reaction (HOR). These characteristics enhance H2 solubility and facilitate H2 oxidation on the PtNi nanocrystal surface, making [Bmpy][NTf2] superior to [Bmim][NTf2] as the electrolyte for H2 sensing application. This study advances high-sensitivity durable H2 sensor technology and offers insights into the interactions between metal alloy nanocrystals and ionic liquids, guiding the design of next-generation H2 sensors for environmental monitoring, industrial safety, and sustainable energy systems.
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.