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The most convenient method for the clinical routine analysis of disease biomarkers is homogeneous immunoassay, which minimizes the requirements for automation and time-/lab-consumption. Despite great success, because sample constituents are not removed by a separation or washing step, a major challenge in conducting homogeneous immunoassays for the practical application is the matrix effect-related inaccuracy. Herein, to guarantee an accurate quantification, a self-validated homogeneous immunoassay was proposed, by simultaneously scrutinizing both frequency and intensity of single gold nanoparticles. The two analytical modes of single particle inductively coupled plasma mass spectrometry (ICPMS) correlated well with each other, resulting in a self-validation mechanism for the accurate immunoassay. Both two modes of the proposed method provided linear ranges of 2 orders of magnitude and LODs of pM level. Thanks to the self-validated strategy and the high tolerance of the matrix effect of ICPMS, the proposed homogeneous immunoassay was successfully demonstrated in a series of human serum samples, with results in good accordance with clinical routine methods.

Pancreatic cancer is one of the foremost malignant gastrointestinal tumors, with prognosis and postoperative prediction remaining challenging because of the lack of facile, sensitive diagnostic methods and a specific single biomarker. Combined-biomarker analysis which provides a promising strategy to conquer such dilemma still requires developments in methodologies to gain accurate and reliable outcomes with wash-/separationfree scenarios and minimal interferences. Herein, a multiplex single-particle homogeneous immunoassay was proposed by simultaneously evaluating three pancreatic cancer-related biomarkers. Owing to the excellent resolution and multielement detectors without mass spectra overlapping, single-particle ICP-MS simultaneously provided biomarkers (CA125, CEA, and CA199) with three to four order-of-magnitude linear ranges and low-level limits of detection from specific antibody-labeled noble metal nanoparticles (AuNPs, AgNPs, and PtNPs). By scrutinizing both intensity and frequency signals, the proposed method was successfully applied in patients' serological evaluation, with results correlating well with those measured by the clinical routine method. The proposed method provides a potential tool in risk assessment of disease recurrence and survival.

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ISOBAM-104 protected Rh/Ni bimetallic nanoparticles (BNPs) of 3.1 nm in diameter were synthesized by a co-reduction method with a rapid injection of KBH 4 solution. The catalytic activities of as-prepared BNPs for hydrogen generation from hydrolysis of a basic KBH 4 solution were evaluated. Ultraviolet-visible spectrophotometry (UV-Vis), transmission electron microscopy (TEM), and high-resolution transmission electron microscopy (HRTEM) were employed to characterize the structure, particle size, and chemical composition of the resultant BNPs. Catalytic activities for hydrolysis of KBH 4 and catalytic kinetics of prepared BNPs were also investigated. It was shown that Rh/Ni BNPs displayed much higher catalytic activities than that of Rh or Ni monometallic nanoparticles (MNPs), and the prepared Rh 10 Ni 90 BNPs possessed the highest catalytic activities, with a value of 11,580 mol-H 2 ·h −1 ·mol-Rh −1 . The high catalytic activities of Rh/Ni BNPs could be attributed to the electron transfer effect between Rh and Ni atoms, which was confirmed by a density functional theory (DFT) calculation. The apparent activation energy for hydrogen generation of the prepared Rh 10 Ni 90 BNPs was about 47.2 ± 2.1 kJ/mol, according to a kinetic study.