Investigation of the Ionization Mechanism of NAD/NADH-Modified Gold Electrodes in ToF-SIMS Analysis

Overview

Journal J Am Soc Mass Spectrom

Specialty Chemistry

Date 2018 Jun 6

PMID 29869326

Authors

Xin Hua

Li-Jun Zhao

Yi-Tao Long

Affiliations

Soon will be listed here.

Abstract

Analysis of nicotinamide adenine dinucleotide (NAD/NADH)-modified electrodes is important for in vitro monitoring of key biological processes. In this work, time-of-flight secondary ion mass spectrometry (ToF-SIMS) was used to analyze NAD/NADH-modified gold electrodes. Interestingly, no obvious characteristic peaks of nicotinamide fragment could be observed in the mass spectra of NAD/NADH in their neutral sodium pyrophosphate form. However, after acidification, the characteristic peaks for both NAD and NADH were detected. This was due to the suppression effect of inner pyrophosphoric salts in both neutral molecules. Besides, it was proved that the suppression by inner salt was intramolecular. No obvious suppression was found between neighboring molecules. These results demonstrated the suppression effect of inner salts in ToF-SIMS analysis, providing useful evidence for the study of ToF-SIMS ionization mechanism of organic molecule-modified electrodes. Graphical Abstract ᅟ.

References

Sacci R, Dudney N, More K, Parent L, Arslan I, Browning N . Direct visualization of initial SEI morphology and growth kinetics during lithium deposition by in situ electrochemical transmission electron microscopy. Chem Commun (Camb). 2014; 50(17):2104-7. DOI: 10.1039/c3cc49029g. View

Lacey S, Wan J, von Wald Cresce A, Russell S, Dai J, Bao W . Atomic force microscopy studies on molybdenum disulfide flakes as sodium-ion anodes. Nano Lett. 2014; 15(2):1018-24. DOI: 10.1021/nl503871s. View

Piwowar A, Lockyer N, Vickerman J . Salt effects on ion formation in desorption mass spectrometry: an investigation into the role of alkali chlorides on peak suppression in time-of-flight-secondary ion mass spectrometry. Anal Chem. 2009; 81(3):1040-8. DOI: 10.1021/ac8020888. View

Yao H, Zheng G, Hsu P, Kong D, Cha J, Li W . Improving lithium-sulphur batteries through spatial control of sulphur species deposition on a hybrid electrode surface. Nat Commun. 2014; 5:3943. DOI: 10.1038/ncomms4943. View

Steuber J, Vohl G, Casutt M, Vorburger T, Diederichs K, Fritz G . Structure of the V. cholerae Na+-pumping NADH:quinone oxidoreductase. Nature. 2014; 516(7529):62-7. DOI: 10.1038/nature14003. View

Quah T, Milton R, Abdellaoui S, Minteer S . Bioelectrocatalytic NAD/NADH inter-conversion: transformation of an enzymatic fuel cell into an enzymatic redox flow battery. Chem Commun (Camb). 2017; 53(60):8411-8414. DOI: 10.1039/c7cc03842a. View

Kang C, Kang J, Lee N, Yoon Y, Yang H . DT-Diaphorase as a Bifunctional Enzyme Label That Allows Rapid Enzymatic Amplification and Electrochemical Redox Cycling. Anal Chem. 2017; 89(15):7974-7980. DOI: 10.1021/acs.analchem.7b01223. View

Wang S, Cazelles R, Liao W, Vazquez-Gonzalez M, Zoabi A, Abu-Reziq R . Mimicking Horseradish Peroxidase and NADH Peroxidase by Heterogeneous Cu-Modified Graphene Oxide Nanoparticles. Nano Lett. 2017; 17(3):2043-2048. DOI: 10.1021/acs.nanolett.7b00093. View

Lee J, Ninomiya S, Matsuo J, Gilmore I, Seah M, Shard A . Organic depth profiling of a nanostructured delta layer reference material using large argon cluster ions. Anal Chem. 2009; 82(1):98-105. DOI: 10.1021/ac901045q. View

10.

Sheraz Nee Rabbani S, Barber A, Fletcher J, Lockyer N, Vickerman J . Enhancing secondary ion yields in time of flight-secondary ion mass spectrometry using water cluster primary beams. Anal Chem. 2013; 85(12):5654-8. PMC: 3686110. DOI: 10.1021/ac4013732. View

11.

Passarelli M, Newman C, Marshall P, West A, Gilmore I, Bunch J . Single-Cell Analysis: Visualizing Pharmaceutical and Metabolite Uptake in Cells with Label-Free 3D Mass Spectrometry Imaging. Anal Chem. 2015; 87(13):6696-702. DOI: 10.1021/acs.analchem.5b00842. View

12.

Vorng J, Kotowska A, Passarelli M, West A, Marshall P, Havelund R . Semiempirical Rules To Determine Drug Sensitivity and Ionization Efficiency in Secondary Ion Mass Spectrometry Using a Model Tissue Sample. Anal Chem. 2016; 88(22):11028-11036. DOI: 10.1021/acs.analchem.6b02894. View

13.

Zhu X, Lu M, Lee B, Ugurbil K, Chen W . In vivo NAD assay reveals the intracellular NAD contents and redox state in healthy human brain and their age dependences. Proc Natl Acad Sci U S A. 2015; 112(9):2876-81. PMC: 4352772. DOI: 10.1073/pnas.1417921112. View

14.

Ma W, Li D, Sutherland T, Li Y, Long Y, Chen H . Reversible redox of NADH and NAD+ at a hybrid lipid bilayer membrane using ubiquinone. J Am Chem Soc. 2011; 133(32):12366-9. DOI: 10.1021/ja204014s. View

15.

Lu J, Hua X, Long Y . Recent advances in real-time and in situ analysis of an electrode-electrolyte interface by mass spectrometry. Analyst. 2017; 142(5):691-699. DOI: 10.1039/c6an02757a. View

16.

Tokranov A, Sheldon B, Li C, Minne S, Xiao X . In situ atomic force microscopy study of initial solid electrolyte interphase formation on silicon electrodes for Li-ion batteries. ACS Appl Mater Interfaces. 2014; 6(9):6672-86. DOI: 10.1021/am500363t. View

17.

Harry K, Hallinan D, Parkinson D, MacDowell A, Balsara N . Detection of subsurface structures underneath dendrites formed on cycled lithium metal electrodes. Nat Mater. 2013; 13(1):69-73. DOI: 10.1038/nmat3793. View

18.

Axnanda S, Crumlin E, Mao B, Rani S, Chang R, Karlsson P . Using "Tender" X-ray Ambient Pressure X-Ray Photoelectron Spectroscopy as A Direct Probe of Solid-Liquid Interface. Sci Rep. 2015; 5:9788. PMC: 4650780. DOI: 10.1038/srep09788. View