Plasma‐Enhanced Chemical‐Vapor‐Deposition Synthesis of Photoredox‐Active Nitrogen‐Doped Carbon from NH3 and CH4 Gases

• Published in: Angewandte Chemie International Edition Vol. 62; no. 33; pp. e202307236 - n/a
• Main Authors: Wang, Yan, Fang, Yuanxing, Wang, Yankun, Wu, Haisu, Anpo, Masakazu, Yu, Jimmy C., Wang, Xinchen
• Format: Journal Article
• Language: English
• Published: Weinheim Wiley Subscription Services, Inc 14.08.2023
• Edition: International ed. in English
• Subjects: Active Sites; Amines; Ammonia; Atmosphere; Atmospheric chemistry; Carbon; Chemical evolution; Chemical synthesis; Chemical Vapor Deposition; Gases; Hydrogen peroxide; Imines; Infrared Spectroscopy; Methane; Nitrogen; Nitrogen-Doped Carbon; Photocatalysts; Photochemical reactions; Photoreduction
• ISSN: 1433-7851; 1521-3773
• DOI: 10.1002/anie.202307236

Earth's primordial atmosphere was rich in ammonia and methane. To understand the evolution of the atmosphere, these two gases were used to make photoredox‐active nitrogen‐doped carbon (NDC). Photocatalysts such as NDC might play an important role in the development of geological and atmospheric chemistry during the Archean era. This study describes the synthesis of NDC directly from NH3 and CH4 gases. The photocatalyst product can be used to selectively synthesize imines by photo‐oxidization of amines, producing H2O2 simultaneously in the photoreduction reaction. Our findings shed light on the chemical evolution of the Earth. NH3 and CH4 gases were applied as precursors to synthesize nitrogen‐doped carbon (NDC) photocatalysts. Without any co‐catalysts, the NDC was demonstrated to drive photoredox reactions, and active sites on the NDC have been investigated. Because in the Archean era, the atmosphere of Earth was filled with NH3 and CH4 gases, this study is important to understand the evolution of biomolecules in the Earth by photochemistry.