乙酰丙酸
还原胺化
催化作用
贵金属
纳米颗粒
材料科学
苄胺
金属有机骨架
协同催化
化学
有机化学
纳米技术
吸附
作者
Yun Wang,Mengting Chen,Kaiyue Zhang,Haiyuan Wu,Jiale Wang,Yuran Cheng,Yingxin Liu,Zuojun Wei
标识
DOI:10.1021/acscatal.3c03854
摘要
Highly efficient transformation of renewable biomass and its derivatives into high-value-added chemicals and biofuels over non-noble-metal catalysts is attractive but challenging. Herein, we developed non-noble CoNi alloy nanoparticles confined in N-doped porous carbon (CoNi@NC) via simple pyrolysis of the metal–organic framework (MOF) precursor at 900 °C under an inert atmosphere. The as-obtained CoNi@NC catalyst exhibited higher performance than monometallic Co@NC and Ni@NC catalysts in the reductive amination of levulinic acid (LA) with benzylamine to N-benzyl-5-methyl-2-pyrrolidinone (BMP) under mild conditions of 130 °C and 3 MPa H2 for 6 h, achieving a full conversion of LA and a ≥ 99% yield of BMP. Detailed characterizations substantiated that multifunctional support and the significant synergistic effect between Co and Ni markedly enhanced the catalytic performance. Furthermore, CoNi@NC manifested outstanding recyclability (reusable 20 cycles without loss of activity), which was attributed to the well-dispersed CoNi alloy nanoparticles confined in the N-doped porous carbon and the anchoring of N species to metal nanoparticles. Additionally, the resultant CoNi@NC catalyst can be successfully applied in the one-pot transformation of LA/esters with amines/nitroarenes/nitriles to the corresponding N-substituted pyrrolidones, as well as the reductive amination of other carbonyl compounds with benzylamine to form N-heterocyclic compounds. Moreover, CoNi@NC enabled us to catalyze the continuous reductive amination of LA with amines in a trickle-bed reactor, which is a more promising, efficient, highly atomically economic, and green synthetic methodology, and exhibited excellent stability during the reaction over 36 h.
科研通智能强力驱动
Strongly Powered by AbleSci AI