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Atomic Pyridinic Nitrogen Sites Promoting Levulinic Acid Hydrogenations over Double-Shelled Hollow Ru/C Nanoreactors.
Liu, Xiaoyan; Ye, Sheng; Lan, Guojun; Su, Panpan; Zhang, Xiaoli; Price, Cameron Alexander Hurd; Li, Ying; Liu, Jian.
Afiliação
  • Liu X; State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Zhongshan Road 457, Dalian, 116023, China.
  • Ye S; Institute of Industrial Catalysis, Zhejiang University of Technology, Chaowang Road 18, Hangzhou, 310014, China.
  • Lan G; State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Zhongshan Road 457, Dalian, 116023, China.
  • Su P; DICP-Surrey Joint Centre for Future Materials, Department of Chemical and Process Engineering, and Advanced Technology Institute, University of Surrey, Guilford, Surrey, GU2 7XH, UK.
  • Zhang X; Institute of Industrial Catalysis, Zhejiang University of Technology, Chaowang Road 18, Hangzhou, 310014, China.
  • Price CAH; State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Zhongshan Road 457, Dalian, 116023, China.
  • Li Y; State Centre for International Cooperation on Designer Low-Carbon & Environmental Materials, School of Materials Science and Engineering, Zhengzhou University, Zhengzhou, 450001, China.
  • Liu J; DICP-Surrey Joint Centre for Future Materials, Department of Chemical and Process Engineering, and Advanced Technology Institute, University of Surrey, Guilford, Surrey, GU2 7XH, UK.
Small ; 17(33): e2101271, 2021 08.
Article em En | MEDLINE | ID: mdl-34254441
Nitrogen-doped nanocarbons are widely used as supports for metal-heterogeneous catalytic conversions. When nitrogen-doped nanocarbon supports are used to disperse metallic nanoparticles (MNPs), the nitrogen dopant can enhance MNPs electron density to reach higher catalytic activity and promote MNPs stability through anchoring effects. However, the precise identification of active nitrogen species between N-dopants and reactants is rarely reported. Herein, a proof-of-concept study on the active N species for levulinic acid hydrogenation is reported. A double-shell structured carbon catalyst (DSC) is designed with selectively locating ultrafine Ru NPs only on inner carbon shell, specifically, different N species on the external carbon shell. Through the design of such a nanostructure, it is demonstrated that the alkaline pyridinic N species on the outer shell serves as an anchor point for the spontaneous binding of the acidic reactant. The pyridinic N content can be modulated from 7.4 to 29.2 mg gcat-1 by selecting different precursors. Finally, the Ru-DSC-CTS (using chitosan as the precursor) catalyst achieves a 99% conversion of levulinic acid under 70 °C and 4 MPa hydrogen pressure for 1 h. This work sheds light on the design of nanoreactors at the atomic scale and investigates heterogeneous catalysis at the molecular level.
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Texto completo: 1 Base de dados: MEDLINE Assunto principal: Ácidos Levulínicos / Nitrogênio Idioma: En Revista: Small Assunto da revista: ENGENHARIA BIOMEDICA Ano de publicação: 2021 Tipo de documento: Article País de afiliação: China

Texto completo: 1 Base de dados: MEDLINE Assunto principal: Ácidos Levulínicos / Nitrogênio Idioma: En Revista: Small Assunto da revista: ENGENHARIA BIOMEDICA Ano de publicação: 2021 Tipo de documento: Article País de afiliação: China