Amorphization‐Modulated Metal Sulfides with Boosted Active Sites and Kinetics for Efficient Enzymatic Colorimetric Biodetection

Abstract

Colorimetric biosensing has become a popular sensing method for the portable detection of a variety of biomarkers. Artificial biocatalysts can replace traditional natural enzymes in the fields of enzymatic colorimetric biodetection; however, the exploration of new biocatalysts with efficient, stable, and specific biosensing reactions has remained challenging so far. Here, to enhance the active sites and overcome the sluggish kinetics of metal sulfides, the creation of an amorphous RuS 2 (a-RuS 2 ) biocatalytic system is reported, which can dramatically boost the peroxidase-mimetic activity of RuS 2 for the enzymatic detection of diverse biomolecules. Due to the existence of abundant accessible active sites and mildly surface oxidation, the a-RuS 2 biocatalyst displays a twofold V max value and much higher reaction kinetics/turnover number (1.63 × 10 −2 s −1 ) compared to that of the crystallized RuS 2 . Noticeably, the a-RuS 2 -based biosensor shows an extremely low detection limit of H 2 O 2 (3.25 × 10 −6 m), l-cysteine (3.39 × 10 −6 m), and glucose (9.84 × 10 −6 m), respectively, thus showing superior detection sensitivity to many currently reported peroxidase-mimetic nanomaterials. This work offers a new path to create highly sensitive and specific colorimetric biosensors in detecting biomolecules and also provides valuable insights for engineering robust enzyme-like biocatalysts via amorphization-modulated design.

Reactive oxygen nanobiocatalysts: activity-mechanism disclosures, catalytic center evolutions, and changing states

“…( In addition, novel target-oriented characterisation techniques, especially in situ methods, such as in situ XAS, in situ XRD, and also in situ Raman, have emerged as frontier techniques to perform real-time monitors for a better understanding of the catalytic mechanisms, thus facilitating the DFT calculation, and guiding the future design of catalysts also deserves more attention to clearly detect the complex catalytic conversion chemistry and to reveal the catalytic mechanisms of RONBCs. [303][304][305] (4) Exploring diverse enzyme-like catalytic activities other than redox enzymes to broaden the application fields of RONBCs Compared with natural enzymes, the catalytic types of RONBCs are still too narrow to satisfy diverse application fields. So far, Fig.…”

“…In addition, novel target-oriented characterisation techniques, especially in situ methods, such as in situ XAS, in situ XRD, and also in situ Raman, have emerged as frontier techniques to perform real-time monitors for a better understanding of the catalytic mechanisms, thus facilitating the DFT calculation, and guiding the future design of catalysts also deserves more attention to clearly detect the complex catalytic conversion chemistry and to reveal the catalytic mechanisms of RONBCs. 303–305…”