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A Durable Nickel Single‐Atom Catalyst for Hydrogenation Reactions and Cellulose Valorization under Harsh Conditions
Author(s) -
Liu Wengang,
Chen Yinjuan,
Qi Haifeng,
Zhang Leilei,
Yan Wensheng,
Liu Xiaoyan,
Yang Xiaofeng,
Miao Shu,
Wang Wentao,
Liu Chenguang,
Wang Aiqin,
Li Jun,
Zhang Tao
Publication year - 2018
Publication title -
angewandte chemie
Language(s) - English
Resource type - Journals
eISSN - 1521-3757
pISSN - 0044-8249
DOI - 10.1002/ange.201802231
Subject(s) - nickel , catalysis , heterolysis , cellulose , chemistry , dissociation (chemistry) , polymer chemistry , organic chemistry
Hydrothermally stable, acid‐resistant nickel catalysts are highly desired in hydrogenation reactions, but such a catalyst remains absent owing to the inherent vulnerability of nickel under acidic conditions. An ultra‐durable Ni‐N‐C single‐atom catalyst (SAC) has now been developed that possesses a remarkable Ni content (7.5 wt %) required for practical usage. This SAC shows not only high activities for hydrogenation of various unsaturated substrates but also unprecedented durability for the one‐pot conversion of cellulose under very harsh conditions (245 °C, 60 bar H 2 , presence of tungstic acid in hot water). Using integrated spectroscopy characterization and computational modeling, the active site structure is identified as (Ni‐N4)⋅⋅⋅N, where significantly distorted octahedral coordination and pyridinic N constitute a frustrated Lewis pair for the heterolytic dissociation of dihydrogen, and the robust covalent chemical bonding between Ni and N atoms accounts for its ultrastability.