{"title":"通过调整钯碳共催化剂的电子态,实现了2,4,6-三氯苯酚的高灵敏度电化学测定。","authors":"Ting-Wei Lee, Chiaying Chen, Chun-Wei Su, Wei-Ling Chen, Chun-Chi Chen, Hsin-Jou Cheng, Shu-Chi Chang","doi":"10.1007/s00604-025-07300-z","DOIUrl":null,"url":null,"abstract":"<div><p>Chlorophenols (CPs) have been identified as priority pollutants due to their ecological persistence, mutagenic, and carcinogenic properties. Among CPs, 2,4,6-trichlorophenol (2,4,6-TCP) is one of the most toxic chlorinated organic compounds. Owing to the detrimental impacts of 2,4,6-TCP, the development of a sensing platform for real-time and on-site monitoring is essential for effective management and pollution control. In this study, a palladium-carbon cocatalyst was utilized to determine 2,4,6-TCP. These results indicate that the anodic current response of 2,4,6-TCP was regulated by the electronic state and dispersity of Pd loaded on two-dimensional reduced graphene oxide (rGO) nanosheets. The resulting Pd with a more electron-deficient nature (i.e., higher-valent Pd) promoted charge polarization of the ring structure of 2,4,6-TCP and facilitated the subsequent nucleophilic attack, leading to superior electrochemical oxidation of 2,4,6-TCP. 2,4,6-TCP is dechlorinated into chlorophenol species at lower voltages, which subsequently oxidize at peak anodic voltages, thereby providing voltage-dependent selectivity. The palladium‒carbon cocatalyst‒modified electrode exhibited a wide sensing concentration range (0.1 to 100 μM) for 2,4,6-TCP, with a low LOD of 16.5 nM and excellent anti-interference ability. Overall, the constructed sensing platform demonstrated high sensitivity, stability, and resistance to interference, which is promising for the on-site determination of 2,4,6-TCP in aqueous environments.</p><h3>Graphical Abstract</h3>\n<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":705,"journal":{"name":"Microchimica Acta","volume":"192 7","pages":""},"PeriodicalIF":5.3000,"publicationDate":"2025-06-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Realizing highly sensitive electrochemical determination of 2,4,6-trichlorophenol by tailoring the electronic state of a palladium‒carbon cocatalyst\",\"authors\":\"Ting-Wei Lee, Chiaying Chen, Chun-Wei Su, Wei-Ling Chen, Chun-Chi Chen, Hsin-Jou Cheng, Shu-Chi Chang\",\"doi\":\"10.1007/s00604-025-07300-z\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>Chlorophenols (CPs) have been identified as priority pollutants due to their ecological persistence, mutagenic, and carcinogenic properties. Among CPs, 2,4,6-trichlorophenol (2,4,6-TCP) is one of the most toxic chlorinated organic compounds. Owing to the detrimental impacts of 2,4,6-TCP, the development of a sensing platform for real-time and on-site monitoring is essential for effective management and pollution control. In this study, a palladium-carbon cocatalyst was utilized to determine 2,4,6-TCP. These results indicate that the anodic current response of 2,4,6-TCP was regulated by the electronic state and dispersity of Pd loaded on two-dimensional reduced graphene oxide (rGO) nanosheets. The resulting Pd with a more electron-deficient nature (i.e., higher-valent Pd) promoted charge polarization of the ring structure of 2,4,6-TCP and facilitated the subsequent nucleophilic attack, leading to superior electrochemical oxidation of 2,4,6-TCP. 2,4,6-TCP is dechlorinated into chlorophenol species at lower voltages, which subsequently oxidize at peak anodic voltages, thereby providing voltage-dependent selectivity. The palladium‒carbon cocatalyst‒modified electrode exhibited a wide sensing concentration range (0.1 to 100 μM) for 2,4,6-TCP, with a low LOD of 16.5 nM and excellent anti-interference ability. Overall, the constructed sensing platform demonstrated high sensitivity, stability, and resistance to interference, which is promising for the on-site determination of 2,4,6-TCP in aqueous environments.</p><h3>Graphical Abstract</h3>\\n<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>\",\"PeriodicalId\":705,\"journal\":{\"name\":\"Microchimica Acta\",\"volume\":\"192 7\",\"pages\":\"\"},\"PeriodicalIF\":5.3000,\"publicationDate\":\"2025-06-24\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Microchimica Acta\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://link.springer.com/article/10.1007/s00604-025-07300-z\",\"RegionNum\":2,\"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":"Microchimica Acta","FirstCategoryId":"92","ListUrlMain":"https://link.springer.com/article/10.1007/s00604-025-07300-z","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, ANALYTICAL","Score":null,"Total":0}
Realizing highly sensitive electrochemical determination of 2,4,6-trichlorophenol by tailoring the electronic state of a palladium‒carbon cocatalyst
Chlorophenols (CPs) have been identified as priority pollutants due to their ecological persistence, mutagenic, and carcinogenic properties. Among CPs, 2,4,6-trichlorophenol (2,4,6-TCP) is one of the most toxic chlorinated organic compounds. Owing to the detrimental impacts of 2,4,6-TCP, the development of a sensing platform for real-time and on-site monitoring is essential for effective management and pollution control. In this study, a palladium-carbon cocatalyst was utilized to determine 2,4,6-TCP. These results indicate that the anodic current response of 2,4,6-TCP was regulated by the electronic state and dispersity of Pd loaded on two-dimensional reduced graphene oxide (rGO) nanosheets. The resulting Pd with a more electron-deficient nature (i.e., higher-valent Pd) promoted charge polarization of the ring structure of 2,4,6-TCP and facilitated the subsequent nucleophilic attack, leading to superior electrochemical oxidation of 2,4,6-TCP. 2,4,6-TCP is dechlorinated into chlorophenol species at lower voltages, which subsequently oxidize at peak anodic voltages, thereby providing voltage-dependent selectivity. The palladium‒carbon cocatalyst‒modified electrode exhibited a wide sensing concentration range (0.1 to 100 μM) for 2,4,6-TCP, with a low LOD of 16.5 nM and excellent anti-interference ability. Overall, the constructed sensing platform demonstrated high sensitivity, stability, and resistance to interference, which is promising for the on-site determination of 2,4,6-TCP in aqueous environments.
期刊介绍:
As a peer-reviewed journal for analytical sciences and technologies on the micro- and nanoscale, Microchimica Acta has established itself as a premier forum for truly novel approaches in chemical and biochemical analysis. Coverage includes methods and devices that provide expedient solutions to the most contemporary demands in this area. Examples are point-of-care technologies, wearable (bio)sensors, in-vivo-monitoring, micro/nanomotors and materials based on synthetic biology as well as biomedical imaging and targeting.