Polyurea‐Modified Magnetic Particles with Versatile Probes for Chemoselective Capture of Carbonyl Metabolites and Biomarker Discovery

Abstract

Playing a great role in human physiologies and pathologies, carbonyl metabolites are intimately associated with a variety of diseases, though the effective analysis method of them remains a challenge. A hydrazide‐terminated polyurea‐modified magnetic particle (HPMP) with versatile probes is developed to address this issue. The capture ability of HPMPs for carbonyl metabolite is more than 1200 µmol g−1, which is increased by 4 orders of magnitude via the introduction of polyurea. With a broad linear range of over 4 orders of magnitude, remarkably improved sensitivity, and limit of detection at attomole quantities, HPMPs are applied in relative quantification of more than 1500 carbonyl metabolites in 113 human serum samples with high throughput and high coverage. The combined indicators of these metabolites demonstrates a great diagnostic accuracy for distinguishing between health and disease subjects as well as differentiating the patients with benign lung disease and lung cancer. Combining powerful capture ability, low‐cost preparation, and convenient operation, the HPMPs demonstrate extensive application in biomarker discovery and the detailed study of the biochemical landscape.

Profiling of Amino Metabolites in Biological Samples without Protein Precipitation Using a Solid-Phase-Supported Phenyl Isothiocyanate-Based Chemoselective Probe

“…In addition, the cleavage condition requires the addition of Pd­(OAc) 2 , PPh 3 , and dimethylbarbituric acid, which introduce new impurities. On the basis of these works, our group introduces polymers onto the surface of magnetic beads, which has greatly increased the loading of probes and the coverage of metabolites. ,, For example, HPMP can detect over 1500 carbonyls. However, of all these probes, protein needs to be removed in advance to remove their impact on the coupling.…”

“…19−21 Hydroxylamine and hydrazide groups modified on magnetic particles were applied to capture carbonyl metabolites with improved coverage and sensitivity. 22,23 The emergence of these probes provides models for future research. However, in the above probes, the efficiency is not satisfied for the reduced reactivity between the solid and liquid phases.…”

“…The introduction of magnetic materials further facilitates the purification process. Active ester and squaric acid were linked to magnetic beads for analysis of amino compounds in biological samples. − Hydroxylamine and hydrazide groups modified on magnetic particles were applied to capture carbonyl metabolites with improved coverage and sensitivity. , The emergence of these probes provides models for future research. However, in the above probes, the efficiency is not satisfied for the reduced reactivity between the solid and liquid phases.…”

Polyurea-magnetic hierarchical porous composites for profiling of anionic metabolites

“…S1 †). 27 As shown in the scanning electron microscopy (SEM) images (Fig. 1A and S2 †) the polyurea shells account for most of the PMC-DAP, PMC-DAB and PMC-HMDA, but have little PMC-MPDA.…”

“…The bands at around 1616 cm −1 are attributed to the stretching vibration of the C]O. [27][28][29] And the bands at 2939 and 2861 cm −1 are assigned to the C-H stretching vibration. The bands at around 3338 and 1575 cm −1 are assigned to the N-H stretching and bending vibrations.…”