Details

Autor(en) / Beteiligte

• Su, Hui
• Gao, Peng
• Wang, Meng‐Ying
• Zhai, Guang‐Yao
• Zhang, Jun‐Jun
• Zhao, Tian‐Jian
• Su, Juan
• Antonietti, Markus
• Li, Xin‐Hao
• Chen, Jie‐Sheng

Titel

Grouping Effect of Single Nickel−N4 Sites in Nitrogen‐Doped Carbon Boosts Hydrogen Transfer Coupling of Alcohols and Amines

Ist Teil von

• Angewandte Chemie International Edition, 2018-11, Vol.57 (46), p.15194-15198

Auflage

International ed. in English

Ort / Verlag

Weinheim: Wiley Subscription Services, Inc

Erscheinungsjahr

2018

Quelle

Alma/SFX Local Collection

Beschreibungen/Notizen

• As a new type of heterogeneous catalyst with “homogeneous‐like” activity, single‐site transition‐metal materials are usually treated as integrated but separate active centers. A novel grouping effect is reported for single Ni−N4 sites in nitrogen‐doped carbon (Ni/NC), where an effective ligand‐stabilized polycondensation method endows Ni/NC nanocatalysts with a high content of single‐site Ni up to 9.5 wt %. The enhanced electron density at each single Ni−N4 site promotes a highly efficient hydrogen transfer, which is exemplified by the coupling of benzyl alcohol and aniline into N‐benzylaniline with a turnover frequency (TOF) value of 7.0 molN‐benzylaniline molmetal−1 h−1; this TOF outpaces that of reported stable non‐noble‐metal‐based catalysts by a factor of 2. Herd instinct: A grouping effect is observed for single Ni−N4 sites in a Ni catalyst supported by nitrogen‐doped carbon (NC). A high 9.5 wt % Ni content was achieved with a ligand‐stabilized polycondensation method. An enhanced electron density effect manifests at each single Ni−N4 site, which decreases the binding energy of H radicals to Ni and promotes efficient coupling of benzyl alcohol and aniline to form N‐benzylaniline.