In Vitro Diagnostic Examination and Prognosis Surveillance by Hierarchical Heterojunction-Assisted Metabolic Analysis

Abstract

High-throughput metabolic analysis based on laser desorption/ionization mass spectrometry exhibits broad prospects in the field of large-scale precise medicine, for which the assisted ionization ability of the matrix becomes a determining step. In this work, the gold-decorated hierarchical metal oxide heterojunctions (dubbed Au/HMOHs) are proposed as a matrix for extracting urine metabolic fingerprints (UMFs) of primary nephrotic syndrome (PNS). The hierarchical heterojunctions are simply derived from metal–organic framework (MOF)-on-MOF hybrids, and the native built-in electric field from heterojunctions plus the extra Au decoration provides remarkable ionization efficiency, attaining high-quality UMFs. These UMFs are employed to realize precise diagnosis, subtype classification, and effective prognosis evaluation of PNS by appropriate machine learning, all with 100% accurate ratios. Moreover, a high-confidence marker panel for PNS diagnosis is constructed. Interestingly, all panel metabolite markers present obviously uniform downregulation in PNS compared to healthy controls, shedding light on mechanism exploration and pathway analysis. This work drives the application of metabolomics toward precision medicine.

Designed Directional Growth of Ti-Metal–Organic Frameworks for Decoding Alzheimer’s Disease-Specific Exosome Metabolites

“…The UV–visible spectra in Figure f show that mTi-MOFs exhibit stronger absorption at 355 nm than Ti-MOFs, indicating the synergistic effect of PDA-functionalized magnetic particles and Ti-MOFs. This could facilitate energy absorption, electronic transfer, and the ionization of metabolites. , According to reports, the appropriate charge on the matrix surface could facilitate the formation of cation adducts . As a result, we monitored the charge change during the synthesis of mTi-MOFs by measuring the zeta potential.…”

Hollow Core–Shell Metal Oxide Heterojunctions for the Urinary Metabolic Fingerprint-Based Noninvasive Diagnostic Strategy

“…22−24 Various inorganic materials, especially hybrid metal oxides, show unique attraction in LDI analysis, namely avoiding background interference in the low mass range (<1000 Da) compared with traditional organic matrices. 12,25−27 The heat dissipation and charge transfer properties of hybrid metal oxide matrices are considered the great forces behind thermally driven desorption and photoionization during LDI-MS. 22,23,28 However, the deficient design of the structure and composition may have an insufficiently positive affection on the selective ionization of small metabolites, leading the results to not be ideal enough for precise disease screening. Our group has confirmed that p−n metal oxide heterojunctions (MOHs) can greatly improve the transfer of holes from n-type to p-type one, thereby enhancing the separation efficiency of electron−hole pairs at the heterojunction under laser irradiation 23 and facilitating charge transfer of analytes to improve ionization.…”

“…12,25−27 The heat dissipation and charge transfer properties of hybrid metal oxide matrices are considered the great forces behind thermally driven desorption and photoionization during LDI-MS. 22,23,28 However, the deficient design of the structure and composition may have an insufficiently positive affection on the selective ionization of small metabolites, leading the results to not be ideal enough for precise disease screening. Our group has confirmed that p−n metal oxide heterojunctions (MOHs) can greatly improve the transfer of holes from n-type to p-type one, thereby enhancing the separation efficiency of electron−hole pairs at the heterojunction under laser irradiation 23 and facilitating charge transfer of analytes to improve ionization. 29 Moreover, the hollow core−shell structure has been demonstrated to have the ability to enhance the light absorption of metal oxides and electron−hole separation.…”

“…Mass spectrometry (MS), surface-enhanced Raman spectroscopy, and nuclear magnetic resonance are the most versatile analytical avenues for complex biological samples in metabolic research. In particular, MS-based techniques have high sensitivity and low sample consumption, which is especially meaningful for clinically valuable samples. , Recently, laser desorption/ionization MS (LDI-MS) has attracted much attention in metabolic analysis due to its high throughput, fast detection speed, and simple sample preparation. − Various inorganic materials, especially hybrid metal oxides, show unique attraction in LDI analysis, namely avoiding background interference in the low mass range (<1000 Da) compared with traditional organic matrices. ,− The heat dissipation and charge transfer properties of hybrid metal oxide matrices are considered the great forces behind thermally driven desorption and photoionization during LDI-MS. ,, However, the deficient design of the structure and composition may have an insufficiently positive affection on the selective ionization of small metabolites, leading the results to not be ideal enough for precise disease screening. Our group has confirmed that p–n metal oxide heterojunctions (MOHs) can greatly improve the transfer of holes from n-type to p-type one, thereby enhancing the separation efficiency of electron–hole pairs at the heterojunction under laser irradiation and facilitating charge transfer of analytes to improve ionization .…”

Multiscale Element-Doped Nanowire Array-Coupled Machine Learning Reveals Metabolic Fingerprints of Nonreversible Liver Diseases

“…26 Among much else the former can effectively transfer laser energy to analytes, and the latter two can promote efficient desorption and ionization of analytes. 27,28 Previously, we have confirmed metal/semiconductor composites are promising matrix candidates, since their thermal dissipation and charge transfer properties contribute a lot to thermal-driven desorption and photoinduced ionization during LDI MS. 29,30 In addition, structural morphology, which has an important impact on the thermal/photon-driven desorption process, is another key factor affecting the detection sensitivity of LDI-MS. Highly ordered nanoarrays and pores are two widely used structures, 27 which can expose more active sites for analyte adsorption apart from the above-mentioned advantages.…”