Fang Lu, Zhang Sibo, Dai Xinyi, Sun Pengfei, Cao Zhengmao, Wang Wu, Dong Xiaoping, Dong Fan, Chen Si
Department of Chemistry, Zhejiang Sci-Tech University, Hangzhou 310018, China.
Yangtze Delta Region Institute (Huzhou), University of Electronic Science and Technology of China, Huzhou 313000, China.
ACS Sens. 2025 Mar 28;10(3):2038-2048. doi: 10.1021/acssensors.4c03249. Epub 2025 Mar 6.
Accurately detecting low concentrations of ethyl acetate (EA) holds promise for the early screening of rectal and gastric cancer. The primary challenges lie in achieving a high response at parts per billion level concentration and ensuring high selectivity. This study focuses on designing Fe-Ce-O bimetallic oxides with doping and heterogeneous interfaces, which exhibit outstanding redox properties and highly enhanced ability of the adsorption and activation of both O and EA molecules. Benefiting from the violent reaction between EA and the adsorbed oxygen species, the sensor achieves an ultrahigh ethyl acetate sensing response of more than 500,000 at 200 ppm concentration, along with an ultrafast recovery rate (<5 s). In experiments, the response can reach 4.8 even at an extremely low concentration of 10 ppb. Special attention is given to the interfacial chemical reactions through DRIFTS during the sensing process. We propose for the first time that the produced intermediate byproducts (acetaldehyde, ethyl alcohol, acetic acid, and formic acid) coresponse on this sensor, contributing to its ultrahigh sensing response. Furthermore, both EA and the byproducts are effectively classified using linear discriminant analysis with 95% accuracy. This work is expected to elucidate the interfacial sensing mechanisms, particularly the contributions of derived byproducts to the sensor's response, and to propose a novel idea for designing high-performance sensors.
准确检测低浓度乙酸乙酯(EA)有望用于直肠癌和胃癌的早期筛查。主要挑战在于在十亿分之一浓度水平实现高响应并确保高选择性。本研究专注于设计具有掺杂和异质界面的铁铈氧双金属氧化物,其展现出出色的氧化还原特性以及对氧和EA分子的吸附与活化能力的高度增强。受益于EA与吸附氧物种之间的剧烈反应,该传感器在200 ppm浓度下实现了超过500,000的超高乙酸乙酯传感响应,以及超快的恢复速率(<5秒)。在实验中,即使在10 ppb的极低浓度下,响应也能达到4.8。在传感过程中,通过漫反射红外傅里叶变换光谱(DRIFTS)特别关注界面化学反应。我们首次提出,生成的中间副产物(乙醛、乙醇、乙酸和甲酸)在该传感器上共同响应,促成了其超高传感响应。此外,使用线性判别分析对EA和副产物进行有效分类,准确率达95%。这项工作有望阐明界面传感机制,特别是衍生副产物对传感器响应的贡献,并为设计高性能传感器提出新思路。