Background: In the context of modern agriculture, the proliferation of chemical use calls for enhanced pesticide detection to safeguard food quality and public health. The development of accurate testing methodologies is imperative to mitigate the environmental impact of pesticides and ensure the integrity of ecosystems, thereby reflecting the pressing need for advancements in agricultural safety protocols. Therefore, the development of highly sensitive monitoring technology for detecting pesticide residues in agricultural products is necessary for safeguarding human health, ensuring food safety, and maintaining environmental sustainability.
Results: Herein, a controllable surface charge on single tungsten atom-modified gold nanoparticles was used to create an electrostatic force with positively charged pesticide residues. Moreover, hydrogen bonds formed by single-atom sites can induce analyte-adsorbed nanoparticle aggregation, and the sizes of single-tungsten-atom-decorated AuNPs can maintain a gap between each other, resulting in improved SERS detection sensitivity through analyte enrichment at gold nanoparticle hotspots. In terms of the detection limits for pesticide residue analysis, we can effectively achieve an ultrahigh sensitivity of 0.1 ppb for acetamiprid, paraquat and carbendazim, which is among the best SERS sensitivities at the state of the art. For apple sample analysis, our work demonstrated good reproductivity (RSD<6 %) and a strong linear relationship (R2 ≥ 0.97) for 4 pesticide residues after optimizing the pretreatment process, which proves the enormous potential in quantitative analysis.
Significance: Single-atom sites hotspot are firstly successfully achieved and uniformly dispersed between Au nanoparticle, which can effectively increase the sensitivity, keep stability of the Raman scattering signals and possess a significant improvement beyond that of undecorated hotspots when applied in pesticide residue detection. This method can be employed as a universal strategy to capture pesticide residues at hotspots for SERS detection.
Keywords: Enrichment; Pesticide residue; Single atom site; Surface enhanced Raman scattering.
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