催化作用
材料科学
生物量(生态学)
木质纤维素生物量
可再生能源
原子经济
纳米技术
碳纤维
选择性
超分子化学
金属有机骨架
Atom(片上系统)
化学工程
有机化学
化学
分子
复合数
吸附
海洋学
工程类
发酵
计算机科学
电气工程
复合材料
嵌入式系统
地质学
作者
Wu‐Jun Liu,Xiao Zhou,Min Yuan,Jiawei Huang,Jie‐Jie Chen,Yuen Wu,Han‐Qing Yu
标识
DOI:10.1002/adma.202305924
摘要
Utilizing renewable biomass as a substitute for fossil resources to produce high-value chemicals with a low carbon footprint is an effective strategy for achieving a carbon-neutral society. Production of chemicals via single-atom catalysis is an attractive proposition due to its remarkable selectivity and high atomic efficiency. In this work, a supramolecular-controlled pyrolysis strategy is employed to fabricate a palladium single-atom (Pd1 /BNC) catalyst with B-doped Pd-Nx atomic configuration. Owing to the meticulously tailored local coordination microenvironment, the as-synthesized Pd1 /BNC catalyst exhibits remarkable conversion capability for a wide range of biomass-derived aldehydes/ketones. Thorough characterizations and density functional theory calculations reveal that the highly polar metal-N-B site, formed between the central Pd single atom and its adjacent N and B atoms, promotes hydrogen activation from the donor (reductants) and hydrogen transfer to the acceptor (C═O group), consequently leading to exceptional selectivity. This system can be further extended to directly synthesize various aromatic and furonic amines from renewable lignocellulosic biomass, with their greenhouse gas emission potentials being negative in comparison to those of fossil-fuel resource-based amines. This research presents a highly effective and sustainable methodology for constructing C─N bonds, enabling the production of a diverse array of amines from carbon-neutral biomass resources.
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