Song Zong-Yin, Xiao Xiang-Yu, Chen Shi-Hua, Li Yong-Yu, Yang Yuan-Fan, Huang Cong-Cong, Duan Wanchun, Yang Meng, Li Pei-Hua, Huang Xing-Jiu
Key Laboratory of Environmental Optics and Technology, and Environmental Materials and Pollution Control Laboratory, Institute of Solid State Physics, HFIPS, Chinese Academy of Sciences, Hefei 230031, China.
Department of Materials Science and Engineering, University of Science and Technology of China, Hefei 230026, China.
Anal Chem. 2022 Apr 26;94(16):6225-6233. doi: 10.1021/acs.analchem.1c05617. Epub 2022 Apr 11.
Interference among multiple heavy metal ions (HMIs) is a significant problem that must be solved in electroanalysis, which extremely restricts the practical popularization of electrochemical sensors. However, due to the limited exploration of the intrinsic mechanism, it is still difficult to confirm the influencing factors. In this work, a series of experimental and theoretical electroanalysis models have been established to investigate the electroanalysis results of Cu(II), Cd(II), As(III), and their mixtures, which were based on the simple structure and stable coordination of nickel single-atom catalysts. X-ray absorption spectroscopy and density functional theory calculations were used to reveal the underlying detection mechanism of the 50-fold boosting effect of Cu(II) on As(III) while Cd(II) inhibits As(III). Combining the application of the thermodynamic model and Fourier transform infrared reflection, the specific interaction of the nanomaterials and HMIs on the interface is considered to be the fundamental source of the interference. This work opens up a new way of thinking about utilizing the unique modes of interplay between nanomaterials and HMIs to achieve anti-interference intelligent electrodes in stripping analysis.
多种重金属离子(HMI)之间的干扰是电分析中必须解决的一个重大问题,这极大地限制了电化学传感器的实际推广。然而,由于对内在机制的探索有限,仍然难以确定影响因素。在这项工作中,基于镍单原子催化剂的简单结构和稳定配位,建立了一系列实验和理论电分析模型,以研究Cu(II)、Cd(II)、As(III)及其混合物的电分析结果。利用X射线吸收光谱和密度泛函理论计算揭示了Cu(II)对As(III)有50倍增强效应而Cd(II)抑制As(III)的潜在检测机制。结合热力学模型和傅里叶变换红外反射的应用,纳米材料与HMI在界面上的特定相互作用被认为是干扰的根本来源。这项工作为利用纳米材料与HMI之间独特的相互作用模式来实现溶出分析中的抗干扰智能电极开辟了一条新的思路。