In many aspects of the matrix-assisted laser desorption/ionization mass spectrometry imaging (MALDI MSI) technique, the discovery of new MALDI matrixes has been a major task for the improvement of ionization efficiency, signal intensity, and molecular coverage. In this work, five analog compounds, including phthalhydrazide, 3-aminophthalhydrazide (3-APH or luminol) and its sodium salt, 4-aminophthalhydrazide (4-APH), and 3-nitrophthalhydrazide (3-NPH) were evaluated as potential matrixes for MALDI Fourier-transform ion cyclotron resonance (FTICR) MSI of metabolites in mouse brain tissue. The five candidate MALDI matrixes were mainly evaluated according to the solid-state ultraviolet absorption, the ion yields and species, and the dual-polarity detection. Among the five candidate matrixes, 3-APH and its sodium salt enabled the detection of endogenous metabolites better than the three other candidates in dual polarities. The best results were observed with 3-APH. Compared with commonly used MALDI matrixes such as 2,5-dihydroxybenzoic acid, α-cyano-4-hydroxycinnamic acid, and 9-aminoacridine, 3-APH exhibited superior performance in dual polarity MALDI MSI, higher sensitivity, broader molecular coverage, and lower background noise. The use of 3-APH led to on-tissue MALDI FTICR MSI of 159 and 207 mouse brain metabolites in the positive and negative ion modes, respectively. Among these metabolites, nucleotides, fatty acids, glycerolipids, glycerophospholipids, sphingolipids, and saccharolipids are included. 3-APH was further used for MALDI FTICR MSI of metabolic responses to ischemia-induced disturbances in mouse brain subjected to middle cerebral artery occlusion (MCAO), thus revealing the alteration of 105 metabolites in the ipsilateral hemispheres. This further emphasizes the great potential of 3-APH as a matrix for the localization of biomarkers in brain diseases.
Photochemical processes generate mass-independent fractionation (MIF) of mercury (Hg) isotopes in the atmosphere-ocean system, and the subduction of marine sediments or hydrated oceanic crust may recycle the resultant Hg isotope signature into the volcanic-arc environment. This environment typically hosts epithermal gold deposits, which are characterized by a specific Hg-Sb-As metal association. We investigated the Hg isotopic composition of seven volcanic-arc–related epithermal gold deposits in northeast China and revisited the isotopic composition of Hg in hydrothermal ore deposits in circum-Pacific and Mediterranean volcanic arcs. The gold ore samples in northeast China mostly display positive Δ199Hg values (0.11‰ ± 0.07‰, 1σ, n = 48) similar to those observed in the Pacific Rim (0.07‰ ± 0.09‰, 1σ, n = 182) and the Mediterranean Cenozoic volcanic belt (0.09‰ ± 0.08‰, 1σ, n = 9). Because Hg in marine sediments and seawater has positive Δ199Hg, we infer that Hg-bearing epithermal deposits in active continental margin settings receive most Hg from recycled seawater in marine sediments, through the release of Hg by dehydration from the subducting oceanic slab. However, negative to near-zero Δ199Hg values were observed in Hg-bearing deposits in the South China craton (–0.09‰ ± 0.05‰, 1σ, n = 105) and in the intraplate magmatic-hydrothermal Almadén Hg deposit in Spain (–0.02‰ ± 0.06‰, 1σ, n = 26), which are considered to relate to basement and mantle sources, respectively. Hg isotopes have the potential to trace lithospheric Hg cycling.
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