首页|Synergy of heterogeneous Co/Ni dual atoms enabling selective C-O bond scission of lignin coupling with in-situ N-functionalization

Synergy of heterogeneous Co/Ni dual atoms enabling selective C-O bond scission of lignin coupling with in-situ N-functionalization

扫码查看
原文链接
  • NETL
  • NSTL
  • 万方数据
Selective cleavage of Csp2—OCH3 bond in lignin without breaking other types of C—O bonds followed by N-functionalization is fascinating for on-purpose valorization of biomass.Here,a Co/Ni-based dual-atom catalyst CoNiDA@NC prepared by in-situ evaporation and acid-etching of metal species from tailor-made metal-organic frameworks was efficient for reductive upgrading of various lignin-derived phenols to cyclohexanols(88.5％-99.9％yields),which had ca.4 times higher reaction rate than the single-atom cat-alyst and was superior to state-of-the-art heterogeneous catalysts.The synergistic catalysis of Co/Ni dual atoms facilitated both hydrogen dissociation and hydrogenolysis steps,and could optimize adsorption configuration of lignin-derived methoxylated phenols to further favor the Csp2-OCH3 cleavage,as elabo-rated by theoretical calculations.Notably,the CoNiDA@NC catalyst was highly recyclable,and exhibited excellent demethoxylation performance(77.1％yield)in real lignin monomer mixtures.Via in-situ cas-cade conversion processes assisted by dual-atom catalysis,various high-value N-containing chemicals,including caprolactams and cyclohexylamines,could be produced from lignin.

Biomass conversionHeterogeneous catalysisLigninDual-atom catalystSelective C-O cleavage

Baoyu Wang、Jinshu Huang、Hongguo Wu、Ximing Yan、Yuhe Liao、Hu Li

展开 >

National Key Laboratory of Green Pesticide,Key Laboratory of Green Pesticide & Agricultural Bioengineering,Ministry of Education,State-Local Joint Laboratory for Comprehensive Utilization of Biomass,College of Pharmacy & Center for R&D of Fine Chemicals,Guizhou University,Guiyang 550025,Guizhou,China

Guangxi Key Laboratory of Green Chemical Materials and Safety Technology,Beibu Gulf University,Qinzhou 535011,Guangxi,China

Guangzhou Institute of Energy Conversion,Chinese Academy of Sciences,Guangzhou 510640,Guangdong,China

National Natural Science Foundation of ChinaGuizhou Provincial S&T ProjectGuizhou Provincial S&T ProjectNatural Science Foundation of Guangxi Zhuang Autonomous RegionGuangxi Key Laboratory of Green Chemical Materials and Safety TechnologyBeibu Gulf UniversityBeibu Gulf UniversityGuizhou Provincial Higher Education Institution Program

22368014ZK[2022]011GCC[2023]0112023JJA1200982022SYSZZ022022ZZKT04Qianjiaoji[2023]082

2024

10.1016/j.jechem.2024.01.003

能源化学
中国科学院大连化学物理研究所 中国科学院成都有机化学研究所

能源化学

CSTPCDEI
影响因子：0.654
ISSN：2095-4956
年,卷(期)：2024.92(5)