{"title":"Single-atom nanozyme immunoassay with electron-rich property for clinical patient cancer detection","authors":"Qingshan Liu, Guo Li, Yang Cao, Yaoyao Ren, Qiong Qin, Lei Li, Hao Zhang, Qi Xin, Xiaoqun Gong, Lingyu Zhao, Shu Zhang, Yonghui Li, Jiang Yang, Jianning Zhang, Xiaoyu Mu, Xiao-Dong Zhang","doi":"10.1016/j.cej.2025.159940","DOIUrl":null,"url":null,"abstract":"Biocatalytic activity of artificial nanozymes is strongly correlated with the detection sensitivity of lateral flow immunoassays (LFIA). Modulating the electronic structure is a promising and effective strategy to improve the catalytic activity of nanozymes, but remains a challenge. In this study, we develop a single-atom nanozyme LFIA platform with high active and electron-rich Pt single atoms onto AuPd support (Pt<sub>1</sub>/PA). The Pt<sub>1</sub>/PA nanozymes exhibit superior peroxidase (POD)-like activity with the catalytic efficiency (<em>K<sub>cat</sub>/K<sub>m</sub></em>) of 9.29 × 10<sup>6</sup> mM<sup>−1</sup>·min<sup>−1</sup>, which is 315-fold higher than natural horseradish peroxidase (HRP). Density Functional Theory calculations reveal that the remarkable activity is attributed to the formation of electron-rich site of Pt single atoms through electron transfer from support to Pt 5<em>d</em> orbitals, as well as <em>d</em>-band center modulation. Moreover, more electron transfer numbers are available for Pt single atoms at the surface in the lattice than outside the lattice. Benefiting from excellent biocatalytic activity, the limits of detection (LOD) of Pt<sub>1</sub>/PA-LFIA for carcinoembryonic antigen (CEA) and prostate-specific antigen (PSA) are 1.21pg mL<sup>−1</sup> and 0.6pg mL<sup>−1</sup>, which are 20.4 and 13.3-fold lower than commercial enzyme-linked immunosorbent assay kits (CEA: ab264604, 24.68pg mL<sup>−1</sup>; PSA: ab264615, 8pg mL<sup>−1</sup>), respectively. More importantly, Pt<sub>1</sub>/PA-LFIA achieves the accurate detection of prostate cancer and lung cancer clinical patients. This work presents a paradigm for ultrasensitive biomarker diagnostics based on single-atom nanozyme immunoassays.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"47 1","pages":""},"PeriodicalIF":13.3000,"publicationDate":"2025-01-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Chemical Engineering Journal","FirstCategoryId":"5","ListUrlMain":"https://doi.org/10.1016/j.cej.2025.159940","RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
引用次数: 0
Abstract
Biocatalytic activity of artificial nanozymes is strongly correlated with the detection sensitivity of lateral flow immunoassays (LFIA). Modulating the electronic structure is a promising and effective strategy to improve the catalytic activity of nanozymes, but remains a challenge. In this study, we develop a single-atom nanozyme LFIA platform with high active and electron-rich Pt single atoms onto AuPd support (Pt1/PA). The Pt1/PA nanozymes exhibit superior peroxidase (POD)-like activity with the catalytic efficiency (Kcat/Km) of 9.29 × 106 mM−1·min−1, which is 315-fold higher than natural horseradish peroxidase (HRP). Density Functional Theory calculations reveal that the remarkable activity is attributed to the formation of electron-rich site of Pt single atoms through electron transfer from support to Pt 5d orbitals, as well as d-band center modulation. Moreover, more electron transfer numbers are available for Pt single atoms at the surface in the lattice than outside the lattice. Benefiting from excellent biocatalytic activity, the limits of detection (LOD) of Pt1/PA-LFIA for carcinoembryonic antigen (CEA) and prostate-specific antigen (PSA) are 1.21pg mL−1 and 0.6pg mL−1, which are 20.4 and 13.3-fold lower than commercial enzyme-linked immunosorbent assay kits (CEA: ab264604, 24.68pg mL−1; PSA: ab264615, 8pg mL−1), respectively. More importantly, Pt1/PA-LFIA achieves the accurate detection of prostate cancer and lung cancer clinical patients. This work presents a paradigm for ultrasensitive biomarker diagnostics based on single-atom nanozyme immunoassays.
期刊介绍:
The Chemical Engineering Journal is an international research journal that invites contributions of original and novel fundamental research. It aims to provide an international platform for presenting original fundamental research, interpretative reviews, and discussions on new developments in chemical engineering. The journal welcomes papers that describe novel theory and its practical application, as well as those that demonstrate the transfer of techniques from other disciplines. It also welcomes reports on carefully conducted experimental work that is soundly interpreted. The main focus of the journal is on original and rigorous research results that have broad significance. The Catalysis section within the Chemical Engineering Journal focuses specifically on Experimental and Theoretical studies in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. These studies have industrial impact on various sectors such as chemicals, energy, materials, foods, healthcare, and environmental protection.