脂肪族单氢取代多氟羧酸位置异构体的单分子检测研究

程梦源; 汤雯; 赵娴; 杨泽楷; 李洪双; 田思语; 罗丹; 谢雪迎; 李浦风; 邱恺培

doi:10.13205/j.hjgc.202506015

脂肪族单氢取代多氟羧酸位置异构体的单分子检测研究

doi: 10.13205/j.hjgc.202506015

程梦源¹,
汤雯¹,
赵娴¹,
杨泽楷¹,
李洪双¹,
田思语¹,
罗丹¹,
谢雪迎¹,
李浦风¹,
邱恺培^1,2,3,4, ,

1. 华东理工大学资源与环境工程学院国家环境保护化工过程环境风险评价与控制重点实验室, 上海 200237;
2. 煤液化气化及高效低碳利用全国重点实验室, 上海 200237;
3. 上海市环境保护化学污染物环境标准与风险管理重点实验室, 上海 200237;
4. 上海污染控制与生态安全研究院, 上海 200092

基金项目:

国家自然科学基金项目“超痕量全氟羧酸异构体的单分子精准检测研究”（22006037）；上海市自然科学基金项目“新污染物单分子监测”（23ZR1416300）

详细信息

作者简介:
程梦源（1999—），女，硕士研究生，主要研究方向为新污染物单体环境分析化学。13966374958@163.com

通讯作者:
邱恺培（1990—），男，副教授，主要研究方向为新污染物单体环境分析化学。kaipeiqiu@gmail.com

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出版历程
- 收稿日期: 2024-06-04
- 录用日期: 2024-08-06
- 修回日期: 2024-07-10

Single-molecule sensing of aliphatic monohydrogen-substituted polycarboxylic acid positional isomers

1. State Environmental Protection Key Laboratory of Environmental Risk Assessment and Control on Chemical Processes, School of Resources and Environmental Engineering, East China University of Science and Technology, Shanghai 200237, China;
2. State Key Laboratory of Coal Liquification, Gasification and Utilization with High Efficiency and Low Carbon Technology, Shanghai 200237, China;
3. Shanghai Environmental Protection Key Laboratory for Environmental Standard and Risk Management of Chemical Pollutants, Shanghai 200237, China;
4. Shanghai Institute of Pollution Control and Ecological Security, Shanghai 200092, China

摘要

摘要: 全氟和多氟羧酸（per- and polyfluorinated carboxylic acids， PFCAs）及异构体种类繁多、环境风险大，近年来受到广泛关注。现有检测方法在缺乏标准品的前提下，难以满足PFCAs异构体精准分析需求。基于待测分子体积与阻断电流线性响应关系的单分子检测方法，能够实现无需标准品的PFCAs检测，但对PFCAs异构体的分辨能力尚待验证。以脂肪族单氢取代PFCAs位置异构体为研究对象，发展了一种耦合频率调制的多维特征单分子算法，实现了野生型Aerolysin纳米孔对上述PFCAs异构体待测物近100%的准确识别。
- 多氟羧酸位置异构体 /
- 脂肪族氢取代 /
- 单分子检测 /
- 多维特征参数 /
- 频率调制
Abstract: Per- and polyfluorinated carboxylic acids （PFCAs） and their isomers have emerged as critical environmental concerns in recent years due to their structural diversity， extreme persistence， and substantial environmental risks. These compounds， characterized by strong carbon-fluorine bonds， are ubiquitously detected in water systems， soil， and even biological tissues， posing significant risks to ecosystems and human health. Current analytical techniques， such as liquid chromatography-mass spectrometry （LC-MS）， heavily depend on standardized reference materials for isomer identification. However， the lack of commercially available isomer-specific standards severely limits their capacity to achieve precise differentiation and quantification of PFCA isomers， particularly in complex environmental matrices. To address this challenge， single-molecule sensing （SMS）， which rely on the linear correlation of analyte volume and blockade current， offer a promising approach for PFCA detection without requiring standard samples. However， the capability of SMS to resolve PFCA isomers still requires further validation. Taking aliphatic monohydrogen-substituted PFCA positional isomers as an example， this study developed a novel single-molecule algorithm incorporating frequency modulation and multi-dimensional feature extraction. This approach enable 100% accurate recognition of the above PFCA isomers using a wild-type Aerolysin nanopore. The method leverages the unique electrical signatures generated by the interaction of the isomers with the nanopore， which are then analyzed using sophisticated signal processing techniques to differentiate between the isomers with high precision.
- polycarboxylic acid positional isomers /
- aliphatic hydrogen substitution /
- single-molecule sensing /
- multi-feature parameters /
- frequency modulation

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