Highly Accurate Determination of the Total Amount of Pb 2+ and Pb(OH) + in a Natural Water Environment Revealed by Dynamic Simulation and DFT Calculation: Benefit from the Electron Inverse Effect of Pt Nanoclusters over Defective g-C 3 N 4

• Published in: Analytical chemistry (Washington) 2024-04, Vol.96 (13), p.5232-5241
• Main Authors: Zhao, Yong-Huan, Xia, Rui-Ze, Liang, Bo, Gao, Zhi-Wei, Song, Zong-Yin, Yang, Meng, Chen, Shi-Hua, Li, Pei-Hua, Xiao, Xiangyu, Huang, Xing-Jiu
• Format: Article
• Language: English
• ISSN: 0003-2700; 1520-6882
• DOI: 10.1021/acs.analchem.3c05707

Although utilizing nanomaterial-modified electrodes for lead ion detection has achieved great success, most of them are carried out under acidic conditions and ignore the variation of Pb(II) speciation at different pH conditions, leading to the potential inaccuracy of Pb(II) detection in a neutral natural water environment. Thus, designing a novel catalyst with high accuracy for the detection of various forms of the total amount of Pb(II) (Pb and Pb(OH) ) in neutral waters is significant. Herein, Pt nanoclusters (Pt NCs) were elaborately constructed and stabilized on the Co single-atom-doped g-C N with abundant N vacancies (Pt NCs/V -C N ), which achieved the ultrasensitive detection (102.16 μM μA ) of Pb(II) in neutral conditions. The dynamic simulation and theoretical calculations reveal that the parallel deposition of Pb and Pb(OH) occurs on the electrode surface modified by Pt NCs/V -C N , and the current peaks of Pb(II) are cocontributed by Pb and Pb(OH) species. An "electron inverse" phenomenon in Pt NCs/V -C N from the V -C N substrate to Pt NCs endows Pt NCs in an electron-rich state, serving as active centers to promote rapid and efficient reduction for both Pb and Pb(OH) , facilitating the accurate detection of the total amount of Pb(II) in all forms in the actual water environment.