Syngas-promoted selective catalytic hydrogenolysis of cellulose into C_(6)-ketonesOA
Selective hydrogenolysis of cellulose into C_(6)-ketones offers a promising route for the production of high-value carbonyl compounds.However,conventional metal-catalyzed hydrogenolysis methods typically rely on externally added acids and require high-purity H_(2).Herein,we report an alternative syngas-promoted hydrogenolysis method that eliminates these dual dependencies while enabling the selective transformation of cellulose into value-added C_(6)-ketones.Under optimal conditions,using a commercial Pd/C catalyst at 230℃and 3.0 MPa total pressure(H_(2)/CO=1.5/1.5 MPa)for 2 h,the yield of C_(6)-ketones reached 37.8%,representing a 6.8-fold enhancement compared to that obtained under pure H_(2).Mechanistic studies demonstrated a dual promotional effect of CO in directing cellulose to C_(6)-ketones.First,competitive adsorption of CO on Pd active sites suppresses excessive hydrogenation and undesired hydrogenolysis of cellulose-derived intermediates.Second,CO participates in the water-gas shift(WGS)reaction(CO+H_(2)O⇌CO_(2)+H_(2)),generating carbonic acid(H_(2)CO_(3))in-situ via CO_(2)+H_(2)O⇌H_(2)CO_(3),which provides a controllable acidic environment that promotes key intermediate transformations associated with C_(6)-ketone precursor formation.
Zhiyang Tang;Xianyuan Wu;Jie Qu;Xinjun He;Fukun Li;Jinxing Long;Qiang Zeng;Haixia Su;Hongyan He;Xuehui Li
School of Chemistry and Chemical Engineering,State Key Laboratory of Advanced Papermaking and Paper-based Materials,South China University of Technology,Guangzhou,510640,ChinaSchool of Chemistry and Chemical Engineering,State Key Laboratory of Advanced Papermaking and Paper-based Materials,South China University of Technology,Guangzhou,510640,ChinaSchool of Chemistry and Chemical Engineering,State Key Laboratory of Advanced Papermaking and Paper-based Materials,South China University of Technology,Guangzhou,510640,ChinaSchool of Chemistry and Chemical Engineering,State Key Laboratory of Advanced Papermaking and Paper-based Materials,South China University of Technology,Guangzhou,510640,ChinaCollege of Environment and Resources,Chongqing Technology and Business University,Chongqing,400067,ChinaSchool of Chemistry and Chemical Engineering,State Key Laboratory of Advanced Papermaking and Paper-based Materials,South China University of Technology,Guangzhou,510640,ChinaSchool of Chemistry and Chemical Engineering,State Key Laboratory of Advanced Papermaking and Paper-based Materials,South China University of Technology,Guangzhou,510640,ChinaInstitute of Engineering Technology,Sinopec Catalyst Co.,Ltd.,Beijing,101100,ChinaBeijing Key Laboratory of Solid State Battery and Energy Storage Process,State Key Laboratory of Mesoscience and Engineering,CAS Key Laboratory of Green Process and Engineering,Institute of Process Engineering,Chinese Academy of Sciences,Beijing,100190,ChinaSchool of Chemistry and Chemical Engineering,State Key Laboratory of Advanced Papermaking and Paper-based Materials,South China University of Technology,Guangzhou,510640,China
化学化工
CelluloseHydrogenolysisC_(6)-ketonesPd/C catalystSyngas(H_(2)/CO)
《Green Energy & Environment》 2026 (5)
P.1393-1401,9
financial support from the National Natural Science Foundation of China(22338007,22178130 and 22425806).
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