Turn off MathJax
Article Contents
Article Navigation >  Green Energy&Environment  > 2026  > Accepted Manuscript
Zhiyang Tang, Xianyuan Wu, Jie Qu, Xinjun He, Fukun Li, Jinxing Long, Qiang Zeng, Haixia Su, Hongyan He, Xuehui Li. Syngas-Promoted Selective Catalytic Hydrogenolysis of Cellulose into C6-Ketones. Green Energy&Environment. doi: 10.1016/j.gee.2026.02.003
Citation: Zhiyang Tang, Xianyuan Wu, Jie Qu, Xinjun He, Fukun Li, Jinxing Long, Qiang Zeng, Haixia Su, Hongyan He, Xuehui Li. Syngas-Promoted Selective Catalytic Hydrogenolysis of Cellulose into C6-Ketones. Green Energy&Environment. doi: 10.1016/j.gee.2026.02.003
shu

Syngas-Promoted Selective Catalytic Hydrogenolysis of Cellulose into C6-Ketones

doi: 10.1016/j.gee.2026.02.003

  • a. School of Chemistry and Chemical Engineering, State Key Laboratory of Advanced Papermaking and Paper-based Materials, South China University of Technology, Guangzhou, Guangdong, 510640, China;

  • b. College of Environment and Resources, Chongqing Technology and Business University, Chongqing, 400067, China;

  • c. Institute of Engineering Technology, Sinopec Catalyst Co., Ltd, Beijing, 101100, China;

  • d. Beijing 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, China

Funds:

The authors gratefully acknowledge financial support from the National Natural Science Foundation of China (22338007, 22178130 and 22425806).

  • Received date 03 December 2025, Accepted date 24 February 2026, RevRecd date 22 January 2026, Available online 06 March 2026
    Abstract
  • Selective hydrogenolysis of cellulose into C6-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 H2. Herein, we report an alternative syngas-promoted hydrogenolysis method that eliminates these dual dependencies while enabling the selective transformation of cellulose into value-added C6-ketones. Under optimal conditions, using a commercial Pd/C catalyst at 230 °C and 3.0 MPa total pressure (H2/CO = 1.5/1.5 MPa) for 2 h, the yield of C6-ketones reached 37.8 C-mol%, representing a 6.8-fold enhancement compared to that obtained under pure H2. Mechanistic studies demonstrated a dual promotional effect of CO in directing cellulose to C6-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 + H2O ⇌ CO2 + H2), generating carbonic acid (H2CO3) in-situ via CO2 + H2O ⇌ H2CO3, which provides a controllable acidic environment that promotes key intermediate transformations associated with C6-ketone precursor formation.

     

    • FullText(HTML)
  • loading
    • References(58)
  • [1]
    L.T. Mika; E. Csefalvay; A. Nemeth, Chem. Rev. 118 (2018) 505-613.
    [2]
    E.M. Rubin, Nature 454 (2008) 841-845.
    [3]
    M. Yabushita; H. Kobayashi; A. Fukuoka, Appl. Catal. B: Environ. 145 (2014) 1-9.
    [4]
    J.S. Luterbacher; J.M. Rand; D.M. Alonso; J. Han; J.T. Youngquist; C.T. Maravelias; B.F. Pfleger; J.A. Dumesic, Science 343 (2014) 277-280.
    [5]
    Z. Sun; G. Bottari; A. Afanasenko; M.C.A. Stuart; P.J. Deuss; B. Fridrich; K. Barta, Nat. Catal. 1 (2018) 82-92.
    [6]
    W. Deng; Y. Feng; J. Fu; H. Guo; Y. Guo; B. Han; Z. Jiang; L. Kong; C. Li; H. Liu; P.T.T. Nguyen; P. Ren; F. Wang; S. Wang; Y. Wang; Y. Wang; S.S. Wong; K. Yan; N. Yan; X. Yang; Y. Zhang; Z. Zhang; X. Zeng; H. Zhou, Green Energy Environ. 8 (2023) 10-114.
    [7]
    M. Gao; Y. Tian; S. Liu; W. He; X. He; K. Wu; J. Long; Q. Zeng; X. Li, Green Chem. 27 (2025) 5210-5223.
    [8]
    C. Song; S. Liu; X. Peng; J. Long; W. Lou; X. Li, ChemSusChem 9 (2016) 3307-3316.
    [9]
    L. Hu; L. Lin; Z. Wu; S. Zhou; S. Liu, Appl. Catal. B: Environ. 174-175 (2015) 225-243.
    [10]
    N.S. Hassan; A.A. Jalil; C.N.C. Hitam; D.V.N. Vo; W. Nabgan, Environ. Chem. Lett. 18 (2020) 1625-1648.
    [11]
    A. Shrotri; H. Kobayashi; A. Fukuoka, Acc. Chem. Res. 51 (2018) 761-768.
    [12]
    Z. Cai; J. Long; Y. Li; L. Ye; B. Yin; L.J. France; J. Dong; L. Zheng; H. He; S. Liu; S.C.E. Tsang; X. Li, Chem 5 (2019) 2365-2377.
    [13]
    H. Su; Z. Bi; Y. Ni; L. Yan, Green Energy Environ. 4 (2019) 391-399.
    [14]
    J.N. Chheda; G.W. Huber; J.A. Dumesic, Angew. Chem. Int. Ed. 46 (2007) 7164-7183.
    [15]
    M. Yang; H. Qi; F. Liu; Y. Ren; X. Pan; L. Zhang; X. Liu; H. Wang; J. Pang; M. Zheng; A. Wang; T. Zhang, Joule 3 (2019) 1937-1948.
    [16]
    Y. Liu; R. Wang; H. Qi; X.Y. Liu; G. Li; A. Wang; X. Wang; Y. Cong; T. Zhang; N. Li, Nat. Commun. 12 (2021) 46.
    [17]
    G.W. Huber; J.N. Chheda; C.J. Barrett; J.A. Dumesic, Science 308 (2005) 1446-1450.
    [18]
    Y. Jing; Y. Guo; Q. Xia; X. Liu; Y. Wang, Chem 5 (2019) 2520-2546.
    [19]
    Y. Roman-Leshkov; C.J. Barrett; Z.Y. Liu; J.A. Dumesic, Nature 447 (2007) 982-985.
    [20]
    A. Fukuoka; P.L. Dhepe, Angew. Chem. Int. Ed. 45 (2006) 5161-5163.
    [21]
    N. Yan; C. Zhao; C. Luo; P.J. Dyson; H. Liu; Y. Kou, Journal of the American Chemical Society 128 (2006) 8714-8715.
    [22]
    C. Luo; S. Wang; H. Liu, Angew. Chem. Int. Ed. 46 (2007) 7636-7639.
    [23]
    N. Ji; T. Zhang; M. Zheng; A. Wang; H. Wang; X. Wang; J.G. Chen, Angew. Chem. Int. Ed. Engl. 47 (2008) 8510-8513.
    [24]
    H. Wang; H. Xin; C. Cai; C. Zhu; Z. Xiu; Q. Liu; Y. Weng; C. Wang; X. Zhang; S. Liu; Z. Peng; L. Ma, ACS Catal. 10 (2020) 10646-10660.
    [25]
    Y. Liu; C. Luo; H. Liu, Angew. Chem. Int. Ed. 51 (2012) 3249-3253.
    [26]
    Y. Liang; H. Wang; H. Xin; X. Hu; L. Yan; Q. Zhang; C. Wang; Q. Liu; L. Ma, ACS Sustainable Chem. Eng. 9 (2021) 15394-15405.
    [27]
    D. Ren; Z. Song; L. Li; Y. Liu; F. Jin; Z. Huo, Green Chem. 18 (2016) 3075-3081.
    [28]
    G.T. Jaya; R. Insyani; J. Park; A.F. Barus; M.G. Sibi; V. Ranaware; D. Verma; J. Kim, Appl. Catal. B: Environ. 312 (2022) 121368.
    [29]
    S. Xu; Q. Zhang; G. Dong; Z. Liu; J. Fu; S. Shi, Renew. Sust. Energ. Rev. 208 (2025) 115038.
    [30]
    C.-H. Kim; S.-Y. Lee; K.Y. Rhee; S.-J. Park, Adv. Compos. Hybrid Mater. 7 (2024) 55.
    [31]
    P. Puchalska; P.A. Crawford, Annu. Rev. Nutr. 41 (2021) 49-77.
    [32]
    J. Magano; J.R. Dunetz, Org. Process Res. Dev. 16 (2012) 1156-1184.
    [33]
    Q. Meng; M. Hou; H. Liu; J. Song; B. Han, Nat. Commun. 8 (2017) 14190.
    [34]
    V. Rajeshkumar; S. Chandrasekar; G. Sekar, Org. Biomol. Chem. 12 (2014) 8512-8518.
    [35]
    M.T. Musser, Ullmann's Encycl. Ind. Chem. 11 (2011) 49-60.
    [36]
    N. Clauser; C.D. Scown; J. Pett-Ridge; W.J. Sagues, Renew. Sust. Energ. Rev. 216 (2025) 115714.
    [37]
    S. Wang; G. Dai; H. Yang; Z. Luo, Prog. Energy Combust. Sci. 62 (2017) 33-86.
    [38]
    T. Li; K. Miao; Z. Zhao; Y. Li; H. Wang; A. Watanabe; N. Teramae; K. Wang, Energy Convers. Manage. 254 (2022) 115195.
    [39]
    A.J. Borchert; A.N. Wilson; W.E. Michener; J. Roback; W.R. Henson; K.J. Ramirez; G.T. Beckham, Green Chem. 25 (2023) 3278-3291.
    [40]
    J. Song; H. Fan; J. Ma; B. Han, Green Chem. 15 (2013) 2619-2635.
    [41]
    A. Wang; T. Zhang, Acc. Chem. Res. 46 (2013) 1377-1386.
    [42]
    A. Al-Rumaihi; M. Shahbaz; G. Mckay; H. Mackey; T. Al-Ansari, Renew. Sust. Energ. Rev. 167 (2022) 112715.
    [43]
    E.L. Kunkes; D.A. Simonetti; R.M. West; J.C. Serrano-Ruiz; C.A. Gartner; J.A. Dumesic, Science 322 (2008) 417-421.
    [44]
    Y. Liu; G. Li; Y. Hu; A. Wang; F. Lu; J.-J. Zou; Y. Cong; N. Li; T. Zhang, Joule 3 (2019) 1028-1036.
    [45]
    R.G.D. Santos; A.C. Alencar, Int. J. Hydrogen Energy 45 (2020) 18114-18132.
    [46]
    X. Chen; L.P. Granda-Marulanda; I.T. Mccrum; M.T.M. Koper, Nat. Commun. 13 (2022) 38.
    [47]
    C. Jin; Y. Liao; A. Zhang; S. Zhao; R. Wang; J. Li; H. Tang, Nano Energy 122 (2024) 109305.
    [48]
    K. Shirayama; X. Jin; K. Nozaki, Journal of the American Chemical Society 146 (2024) 14086-14094.
    [49]
    N. Lopez; B. Bridier; J. Perez-Ramirez, The Journal of Physical Chemistry C 112 (2008) 9346-9350.
    [50]
    R. Hou; T. Wang; X. Lan, Industrial & Engineering Chemistry Research 52 (2013) 13305-13312.
    [51]
    X. He; M. Gao; F. Li; Z. Tang; J. Qu; J. Long; Q. Zeng; X. Li, Green Chem. 27 (2025) 9746-9755.
    [52]
    R.J. Van Putten; J.C. Van Der Waal; E. De Jong; C.B. Rasrendra; H.J. Heeres; J.G. De Vries, Chem Rev 113 (2013) 1499-1597.
    [53]
    G. Tsilomelekis; M.J. Orella; Z. Lin; Z. Cheng; W. Zheng; V. Nikolakis; D.G. Vlachos, Green Chem. 18 (2016) 1983-1993.
    [54]
    M. Crespo-Quesada; A. Yarulin; M. Jin; Y. Xia; L. Kiwi-Minsker, Journal of the American Chemical Society 133 (2011) 12787-12794.
    [55]
    F. Tari; S. Hertle; H. Wang; J. Fischer; P.A. Van Aken; T. Sottmann; E. Klemm; Y. Traa. Investigating the Long-Term Kinetics of Pd Nanoparticles Prepared from Microemulsions and the Lindlar Catalyst for Selective Hydrogenation of 3-Hexyn-1-ol Catalysts [Online], 2024, p. 271.
    [56]
    N. Van Hieu; J.H. Craig, Surf. Sci. 160 (1985) L483-L487.
    [57]
    J.H. Yang; S.Y. Hwang; J.Y. Maeng; G.E. Park; S.Y. Yang; C.K. Rhee; Y. Sohn, ACS Appl. Mater. Interfaces 16 (2024) 3368-3387.
    [58]
    A.M. Ruppert; K. Weinberg; R. Palkovits, Angew. Chem. Int. Ed. 51 (2012) 2564-2601.
    • Relative Articles
    • Supplements(0)
    • Cited By
  • 加载中

Catalog

    通讯作者: 陈斌, bchen63@163.com
    • 1. 

      沈阳化工大学材料科学与工程学院 沈阳 110142

    1. 本站搜索
    2. 百度学术搜索
    3. 万方数据库搜索
    4. CNKI搜索
    Get Citation
    PDF
    XML

    Article Metrics

    Article views (10) PDF downloads(0) Cited by()
    Proportional views

    Publish With GEE

    Contact

    • Email：gee@ipe.ac.cn
    • Tel：010-82627075
    • Address：North 2nd street, Zhongguancun, Haidian District, Beijing, China

    Links

    京ICP备10002620号-1京公网安备 11010802039050号

    Supported by: Beijing Renhe Information Technology Co. Ltd    

    /

    DownLoad:  Full-Size Img  PowerPoint
    Return
    Return