Molecular-level Degradation Pathways of Black Phosphorus Revealed by Mass Spectrometry Fingerprinting

Overview

Journal Chem Sci

Publisher Royal Society of Chemistry

Specialty Chemistry

Date 2023 Jun 23

PMID 37350838

Authors

Xiu Huang

Yong Li

Guangbo Qu

Xue-Feng Yu

Dong Cao

Qian Liu

Guibin Jiang

Affiliations

Soon will be listed here.

Abstract

Understanding the molecular mechanism of material transformation raises a great challenge for material characterization techniques. As a promising 2D material, the application potential of black phosphorus (BP) is seriously compromised by its environmental instability. However, until now, the degradation mechanism of BP remains ambiguous. Here we show that by using laser desorption ionization mass spectrometry (LDI-MS) fingerprinting it is possible to unravel the degradation pathways of BP at the molecular level without any chemical labeling. We found that BP-based materials can generate intrinsic phosphorus cluster (P or P) fingerprint peaks in LDI-MS in both positive-ion and negative-ion modes, which allows the degradation processes of BP materials to be monitored by providing abundant mass information about intermediates and products with the sample-to-sample RSDs in the range of 1.0-28.4%. The stability of BP or cerium-encapsulated BP was monitored under ambient and increased temperature conditions for up to 20 or 180 days. Notably, by using LDI-MS fingerprinting, we reveal an unreported BP degradation pathway, , nitrogen (N)-addition oxidation, in addition to the direct oxidation pathway. Our results not only enable an in-depth understanding of the chemical instability of BP, but also, importantly, demonstrate a new powerful platform for monitoring and characterization of material transformation.

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