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Bimetallic nanoparticles remain a promising avenue to achieve highly reactive catalysts. In this contribution, we demonstrate the use of a photoswitchable peptide for the production of PdAu bimetallic nanoparticles at a variety of Pd : Au ratios. Using this peptide, the biomolecular overlayer structure can be switched between two different conformations ( cis vs. trans ) via light irradiation, thus accessing two different surface structures. The composition and arrangement of the materials was fully characterized, including atomic-level analyses, after which the reactivity of the bimetallic materials was explored using the reduction of 4-nitrophenol as a model system. Using these materials, it was demonstrated that the reactivity was maximized for the particles prepared at a Pd : Au ratio of 1 : 3 and with the peptide in the cis conformation. Such results present routes to a new generation of catalysts that could be remotely activated for on/off reactivity as a function of the ligand overlayer conformation. 

Precise monitoring of specific biomarkers in biological fluids with accurate biodiagnostic sensors is critical for early diagnosis of diseases and subsequent treatment planning. In this work, we demonstrated an innovative biodiagnostic sensor, portable reusable accurate diagnostics with nanostar antennas (PRADA), for multiplexed biomarker detection in small volumes (~50 μl) enabled in a microfluidic platform. Here, PRADA simultaneously detected two biomarkers of myocardial infarction, cardiac troponin I (cTnI), which is well accepted for cardiac disorders, and neuropeptide Y (NPY), which controls cardiac sympathetic drive. In PRADA immunoassay, magnetic beads captured the biomarkers in human serum samples, and gold nanostars (GNSs) “antennas” labeled with peptide biorecognition elements and Raman tags detected the biomarkers via surface‐enhanced Raman spectroscopy (SERS). The peptide‐conjugated GNS‐SERS barcodes were leveraged to achieve high sensitivity, with a limit of detection (LOD) of 0.0055 ng/ml of cTnI, and a LOD of 0.12 ng/ml of NPY comparable with commercially available test kits. The innovation of PRADA was also in the regeneration and reuse of the same sensor chip for ~14 cycles. We validated PRADA by testing cTnI in 11 de‐identified cardiac patient samples of various demographics within a 95% confidence interval and high precision profile. We envision low‐cost PRADA will have tremendous translational impact and be amenable to resource‐limited settings for accurate treatment planning in patients.