镍
催化作用
纤维素
化学
Atom(片上系统)
材料科学
化学工程
有机化学
计算机科学
工程类
嵌入式系统
作者
Wengang Liu,Yinjuan Chen,Haifeng Qi,Leilei Zhang,Wensheng Yan,Xiaoyan Liu,Xiaofeng Yang,Shu Miao,Wentao Wang,Chenguang Liu,Aiqin Wang,Jun Li,Tao Zhang
标识
DOI:10.1002/anie.201802231
摘要
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 H2 , 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.
科研通智能强力驱动
Strongly Powered by AbleSci AI