Binary Iron-Manganese Cocatalyst for Simultaneous Activation of C-C and C-O Bonds to Maximally Utilize Lignin for Syngas Generation over InGaN.

Autor: Yu T; Key Laboratory for Power Machinery and Engineering of Ministry of Education, Research Center for Renewable Synthetic Fuel, School of Mechanical Engineering, Shanghai Jiao Tong University, 800 Dongchuan Road, Shanghai, 200240, China., Zhao Y; Department of Mining and Materials Engineering, McGill University, 3610 University Street, Montreal, QC H3A0C9, Canada., Li J; Key Laboratory for Power Machinery and Engineering of Ministry of Education, Research Center for Renewable Synthetic Fuel, School of Mechanical Engineering, Shanghai Jiao Tong University, 800 Dongchuan Road, Shanghai, 200240, China., Li Y; Key Laboratory for Power Machinery and Engineering of Ministry of Education, Research Center for Renewable Synthetic Fuel, School of Mechanical Engineering, Shanghai Jiao Tong University, 800 Dongchuan Road, Shanghai, 200240, China., Qiu L; Key Laboratory for Power Machinery and Engineering of Ministry of Education, Research Center for Renewable Synthetic Fuel, School of Mechanical Engineering, Shanghai Jiao Tong University, 800 Dongchuan Road, Shanghai, 200240, China., Pan H; Key Laboratory for Power Machinery and Engineering of Ministry of Education, Research Center for Renewable Synthetic Fuel, School of Mechanical Engineering, Shanghai Jiao Tong University, 800 Dongchuan Road, Shanghai, 200240, China., Salman Nasir M; Key Laboratory for Power Machinery and Engineering of Ministry of Education, Research Center for Renewable Synthetic Fuel, School of Mechanical Engineering, Shanghai Jiao Tong University, 800 Dongchuan Road, Shanghai, 200240, China., Song J; Department of Mining and Materials Engineering, McGill University, 3610 University Street, Montreal, QC H3A0C9, Canada., Huang Z; Key Laboratory for Power Machinery and Engineering of Ministry of Education, Research Center for Renewable Synthetic Fuel, School of Mechanical Engineering, Shanghai Jiao Tong University, 800 Dongchuan Road, Shanghai, 200240, China., Zhou B; Key Laboratory for Power Machinery and Engineering of Ministry of Education, Research Center for Renewable Synthetic Fuel, School of Mechanical Engineering, Shanghai Jiao Tong University, 800 Dongchuan Road, Shanghai, 200240, China.
Jazyk: angličtina
Zdroj: Angewandte Chemie (International ed. in English) [Angew Chem Int Ed Engl] 2024 Oct 30, pp. e202413528. Date of Electronic Publication: 2024 Oct 30.
DOI: 10.1002/anie.202413528
Abstrakt: Solar-powered lignin reforming offers a carbon-neutral route for syngas production. This study explores a dual non-precious iron-manganese cocatalyst to simultaneously activate both C-C and C-O bonds for maximizing the utilization of various substituents of native lignin to yield syngas. The cocatalyst, integrated with InGaN nanowires on a Si wafer, affords a measurable syngas evolution rate of 42.4 mol g cat -1  h -1 from native lignin in distilled water with a high selectivity of 93 % and tunable H 2 /CO ratios under concentrated light, leading to a considerable light-to-fuel efficiency of 11.8 %. The high FeMn atom efficiency arising from the 1-dimensional nanostructure of InGaN enables the achievement of a high turnover frequency (TOF) of 220896 mol syngas per mol FeMn per hour. Combined experimental and theoretical investigations reveal that the synergetic iron-manganese cocatalyst supported by InGaN nanowires enables simultaneous activation of C-C and C-O bonds with comparable minimized dissociation energies, thus promising to maximally utilize different substituents of -OCH 3 , and -CH 2 CH 2 CH 3 in lignin for syngas production. Moreover, the dual Fe-Mn cocatalyst demonstrates a most energetically favorable route for the consecutive release of hydrogen from •CH 3 and •OH by the oxidative holes while inhibiting the reversion of hydrogen and hydroxyl into water.
(© 2024 Wiley-VCH GmbH.)
Databáze: MEDLINE
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