Microanalysis of Brain Angiotensin Peptides Using Ultrasensitive Capillary Electrophoresis Trapped Ion Mobility Mass Spectrometry.

While the role of the renin-angiotensin system (RAS) in peripheral circulation is well characterized, we still lack an in-depth understanding of its role within the brain. This knowledge gap is sustained by lacking technologies for trace-level angiotensin detection throughout tissues, such as the brain. To provide a bridging solution, we enhanced capillary electrophoresis (CE) nanoflow electrospray ionization (ESI) with large-volume sample stacking and employed trapped ion mobility time-of-flight (timsTOF) tandem HRMS detection. A dynamic pH junction helped stack approximately 10 times more of the sample than optimal using the field-amplified reference. In conjunction, the efficiency of ion generation was maximized by a cone-jet nanospray on a low sheath-flow tapered-tip nano-electrospray emitter. The platform provided additional peptide-dependent information, the collision cross section, to filter chemical noise and improve sequence identification and detection limits. The lower limit of detection reached sub-picomolar or ∼30 zmol (∼18,000 copies) level. All nine targeted angiotensin peptides in mouse tissue samples were detectable and quantifiable from the paraventricular nucleus (PVN) of the hypothalamus even after removal of circulatory blood components (perfusion). We anticipate CE-ESI with timsTOF HRMS to be broadly applicable for the ultrasensitive detection of brain peptidomes in pursuit of a better understanding of the brain.

N, P, and S Codoped Graphene-Like Carbon Nanosheets for Ultrafast Uranium (VI) Capture with High Capacity.

The development of functional materials for the highly efficient capture of radionuclides, such as uranium from nuclear waste solutions, is an important and challenging topic. Here, few-layered N, P, and S codoped graphene-like carbon nanosheets (NPS-GLCs) that are fabricated in the 2D confined spacing of silicate RUB-15 and applied as sorbents to remove U(VI)ions from aqueous solutions are presented. The NPS-GLCs exhibit a large capacity, wide pH suitability, an ultrafast removal rate, stability at high ionic strengths, and excellent selectivity for U(VI) as compared to multiple competing metal ions. The 2D ultrathin structure of NPS-GLCs with large spacing of 1 nm not only assures the rapid mass diffusion, but also exposes a sufficient active site for the adsorption. Strong covalent bonds such as P-O-U and S-O-U are generated between the heteroatom (N, P, S) with UO2 2+ according to X-ray photoelectron spectroscopy analysis and density functional theory theoretical calculations. This work highlights the interaction mechanism of low oxidation state heteroatoms with UO2 2+, thereby shedding light on the material design of uranium immobilization in the pollution cleanup of radionuclides.