Construction of a ternary component chip with enhanced desorption efficiency for laser desorption/ionization mass spectrometry based metabolic fingerprinting

Abstract

Introduction:In vitro metabolic fingerprinting encodes diverse diseases for clinical practice, while tedious sample pretreatment in bio-samples has largely hindered its universal application. Designed materials are highly demanded to construct diagnostic tools for high-throughput metabolic information extraction.Results: Herein, a ternary component chip composed of mesoporous silica substrate, plasmonic matrix, and perfluoroalkyl initiator is constructed for direct metabolic fingerprinting of biofluids by laser desorption/ionization mass spectrometry.Method: The performance of the designed chip is optimized in terms of silica pore size, gold sputtering time, and initiator loading parameter. The optimized chip can be coupled with microarrays to realize fast, high-throughput (∼second/sample), and microscaled (∼1 μL) sample analysis in human urine without any enrichment or purification. On-chip urine fingerprints further allow for differentiation between kidney stone patients and healthy controls.Discussion: Given the fast, high throughput, and easy operation, our approach brings a new dimension to designing nano-material-based chips for high-performance metabolic analysis and large-scale diagnostic use.

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

“…As one of the critical factors determining LDI efficiency, which is associated with enhanced intensity of the MS signal, thermal-driven desorption has gained significant attention. − In detail, ionization assistant reagents with low thermal conductivity can induce local heat confinement upon laser irradiation more efficiently, leading to a higher ion-desorption efficiency. ,,, Recently, Cheng and Ng showed that the desorption process can also be highly influenced by the extent of hole generation. , Specifically, desorption can be facilitated by electrostatic repulsion between positively charged analytes and holes generated on the substrate surface upon laser irradiation (i.e., charge-driven desorption) …”

Vacancy‐Driven High‐Performance Metabolic Assay for Diagnosis and Therapeutic Evaluation of Depression

“…In addition, we conducted experiments to demonstrate the enhanced photothermal conversion in Vo‐Co‐2, using the chemical thermometer benzyl pyridinium ion (BP) as the indicator. [ 27 ] As shown in Figure S21 (Supporting Information), compared with Co 3 O 4 , Vo‐Co‐1, and Vo‐Co‐3, Vo‐Co‐2 displayed a higher desorption efficiency under the same laser intensity, and its thermal‐driven desorption was enhanced the most. The results suggested that an appropriate amount of oxygen vacancies induces enhanced thermal‐driven desorption, consistent with the higher photothermal conversion of Vo‐Co‐2 (Figure 2e).…”

“…Synthesis of Thermometer Molecules: The synthesis of BP followed a method reported in ref. [27] Typically, 100 μL of benzyl chloride was added to 2 mL pyridine. Then, the mixture was stirred at 60 °C for 5 h in a 25 mL round-bottomed flask.…”