Metal-facilitated, sustainable nitroarene hydrogenation under ambient conditions

Ruan, Chongyan; Yang, Kunran; Beckett, Caitlin; Martin, William; Walter, Eric D.; Hu, Wenda; Liu, Junchen; Zayan, Noha; Lessin, Benjamin; Faherty, Jacob Ken; Akutsu, Ryota; Hu, Jian Zhi; Li, Fanxing

doi:10.1016/j.jcat.2024.115428

Metal-facilitated, sustainable nitroarene hydrogenation under ambient conditions

Journal Article · Thu Mar 07 23:00:00 EST 2024 · Journal of Catalysis

DOI:https://doi.org/10.1016/j.jcat.2024.115428· OSTI ID:2350556

Ruan, Chongyan ^[1]; Yang, Kunran ^[1]; ^[1]; Martin, William ^[1]; Walter, Eric D. ^[2]; Hu, Wenda ^[2]; ^[1]; Zayan, Noha ^[1]; ^[1]; Faherty, Jacob Ken ^[1]; ^[3]; Hu, Jian Zhi ^[2]; ^[1]

North Carolina State University, Raleigh, NC (United States)
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Shinshu Univ., Ueda, Nagano (Japan)

Hydrogenation is a critical reaction in the chemical industry, yielding a range of important compounds such as fine chemicals, pharmachemicals and agrochemicals. However, conventional hydrogenation typically requires pressurized hydrogen, high temperatures and involves noble metal catalysts. Here, we proposed a two-step hydrogenation process, utilizing water as the hydrogen source for the industrially important reduction of nitroarenes to anilines. A metal or reduced metal oxide, which can be obtained from solar thermal or electrochemical reduction, acts as the active site for nitrobenzene adsorption, H₂O dissociation and in-situ hydrogen generation. Among the 15 metal and reduced metal oxides investigated, Zn and Sn emerged as highly efficient catalysts for the reduction of a broad range of organic nitro compounds under mild conditions, with H₂ utilization efficiency 1-2 orders of magnitude above the state-of-the-art. The presented protocol provides extra dimensions for designing and optimizing conventional hydrogenation process with an alternative pathway. The reactive hydrogen atoms generated in-situ effectively overcome the barriers associated with hydrogen gas dissolution and its subsequent dissociation on the catalyst surface, thereby greatly enhancing the overall effectiveness for the hydrogenation reaction. This research potentially establishes a sustainable, generally applicable alternative to conventional hydrogenation methods, simultaneously presenting a viable solution for renewable energy storage.

View Accepted Manuscript (DOE)

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE; National Science Foundation (NSF)

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 2350556

Report Number(s):: PNNL-SA--198311

Journal Information:: Journal of Catalysis, Journal Name: Journal of Catalysis Vol. 432; ISSN 0021-9517

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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