A Surface Matrix of Au NPs Decorated Graphdiyne for Multifunctional Laser Desorption/Ionization Mass Spectrometry

Abstract

The development of the valid strategy to enhance laser desorption/ ionization efficiency gives rise to widespread concern in surface-assisted laser desorption/ ionization mass spectrometry (SALDI-MS) technology. Herein, a hybrid of Au NPdecorated graphdiyne (Au/GDY) was fabricated and employed as the SALDI-MS matrix for the first time, and a mechanism based on photothermal and photochemical energy conversions was proposed to understand LDI processes. Given theoretical simulations and microstructure characterizations, it was revealed that the formation of a coupled thermal field and internal electric field endow the as-prepared Au/GDY matrix with superior desorption and ionization efficiency, respectively. Moreover, laser-induced matrix ablation introduced strain and defect level into the Au/GDY hybrid, suppressing the recombination of charge carriers and thereby facilitating analyte ionization. The optimized Au/GDY matrix allowed for reliable detection of trace sulfacetamide and visualization of exogenous/ endogenous components in biological tissues. This work offers an integrated solution to promote LDI efficiency based on collaborative photothermal conversion and internal electric field, and may inspire the design of novel semiconductor-based surface matrices.

Role of Chalcogenides in Sensitive Therapeutic Drug Monitoring Using Laser Desorption and Ionization

“…Furthermore, the generation of holes can lead to the transfer of excited electrons to surface adsorbents (e.g., residual H 2 O, O 2 , and AED molecules) or to their thermal dissipation. − These can lead to LDI-favorable processes other than Coulomb repulsion such as the generation of reactive hydroxyl radicals and local heat confinement. Therefore, we attribute the enhanced LDI efficiency of MoTe 2 and WTe 2 to the synergistic contribution of their electronic and thermal properties, which facilitates both thermal and charge-driven desorption (Scheme ).…”

“…As an analytical tool widely used in pharmaceutical and biomedical analyses, LDI-MS is an easy-to-use technique that provides timeliness, high analytical throughput, and high sensitivity. Since the photocatalytic effect and the photothermal conversion induced by laser irradiation are critical aspects of the LDI process, the overall analytical performance can be strongly influenced by the properties of the ionization assistant reagent, commonly known as the matrix. − In this context, TMDCs such as MoS 2 and WS 2 , which are known for their efficiency in photocatalysis and photothermal conversion, have been widely investigated in biomolecule analysis, demonstrating feasibility comparable to that of other extensively studied materials, such as metal nanoparticles and carbon-based nanomaterials.…”

Application of Graphdiyne Confined Gold Nanoparticles Modified Electrode as A Robust Sensing Platform for The Detection of 7-Hydroxy-6-Methoxy-Hydrocoumarin

“…30 Pei et al fabricated a hybrid of AuNPs decorated GDY and employed as the SALDI-MS matrix, which could reliably detect trace sulfacetamide. 31 Tao et al encapsulated GDY on the surface of AuNPs, which was applied to Raman imaging of living cells. 32 Gao et al used GDY as substrate for the electroless deposition of AuNPs, which exhibited higher catalytic performance for the reduction of 4-nitrophenol.…”