IDEAS home Printed from https://ideas.repec.org/a/nat/natcom/v12y2021i1d10.1038_s41467-021-27240-5.html
   My bibliography  Save this article

Dihydroxyacetone valorization with high atom efficiency via controlling radical oxidation pathways over natural mineral-inspired catalyst

Author

Listed:
  • Jinling Wang

    (East China University of Science and Technology (ECUST)
    State Key Laboratory of Chemical Engineering, ECUST)

  • Xingchao Dai

    (Leibniz-Institut für Katalyse e.V. an der Universität Rostock (LIKAT)
    Chinese Academy of Sciences)

  • Hualin Wang

    (East China University of Science and Technology (ECUST))

  • Honglai Liu

    (State Key Laboratory of Chemical Engineering, ECUST)

  • Jabor Rabeah

    (Leibniz-Institut für Katalyse e.V. an der Universität Rostock (LIKAT))

  • Angelika Brückner

    (Leibniz-Institut für Katalyse e.V. an der Universität Rostock (LIKAT))

  • Feng Shi

    (Chinese Academy of Sciences)

  • Ming Gong

    (Fudan University)

  • Xuejing Yang

    (East China University of Science and Technology (ECUST))

Abstract

Diminishing fossil fuel resources and calls for sustainability are driving the urgent need for efficient valorization of renewable resources with high atom efficiency. Inspired from the natural goethite mineral with Mn paragenesis, we develop cost-effective MnO2/goethite catalysts for the efficient valorization of dihydroxyacetone, an important biomass-based platform molecule, into value-added glycolic acid and formic acid with 83.2% and 93.4% yields. The DHA substrates first undergo C−C cleavage to selectively form glycolic acid and hydroxymethyl (·CH2OH) radicals, which are further oxidized into formic acid. The kinetic and isotopic labeling experiments reveal that the catalase-like activity of MnO2 turns the oxidative radicals into oxygen, which then switches towards a hydroxymethyl peroxide (HMOO) pathway for formic acid generation and prevents formic acid over-oxidation. This nature-inspired catalyst design not only significantly improves the carbon efficiency to 86.6%, but also enhances the oxygen atom utilization efficiency from 11.2% to 46.6%, indicating a promising biomass valorization process.

Suggested Citation

  • Jinling Wang & Xingchao Dai & Hualin Wang & Honglai Liu & Jabor Rabeah & Angelika Brückner & Feng Shi & Ming Gong & Xuejing Yang, 2021. "Dihydroxyacetone valorization with high atom efficiency via controlling radical oxidation pathways over natural mineral-inspired catalyst," Nature Communications, Nature, vol. 12(1), pages 1-11, December.
    • Handle: RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-021-27240-5
    DOI: 10.1038/s41467-021-27240-5
    as

    Download full text from publisher

    File URL: https://www.nature.com/articles/s41467-021-27240-5
    File Function: Abstract
    Download Restriction: no
    File URL: https://libkey.io/10.1038/s41467-021-27240-5?utm_source=ideas
    LibKey link: if access is restricted and if your library uses this service, LibKey will redirect you to where you can use your library subscription to access this item
    ---><---

    References listed on IDEAS

    as
    1. Yan Li & Xinfa Wei & Lisong Chen & Jianlin Shi & Mingyuan He, 2019. "Nickel-molybdenum nitride nanoplate electrocatalysts for concurrent electrolytic hydrogen and formate productions," Nature Communications, Nature, vol. 10(1), pages 1-12, December.
    2. Gholami, Zahra & Abdullah, Ahmad Zuhairi & Lee, Keat-Teong, 2014. "Dealing with the surplus of glycerol production from biodiesel industry through catalytic upgrading to polyglycerols and other value-added products," Renewable and Sustainable Energy Reviews, Elsevier, vol. 39(C), pages 327-341.
    3. Yuanyi Zhou & Ling Zhang & Wenzhong Wang, 2019. "Direct functionalization of methane into ethanol over copper modified polymeric carbon nitride via photocatalysis," Nature Communications, Nature, vol. 10(1), pages 1-8, December.
    4. Min Wang & Meijiang Liu & Jianmin Lu & Feng Wang, 2020. "Photo splitting of bio-polyols and sugars to methanol and syngas," Nature Communications, Nature, vol. 11(1), pages 1-9, December.
    Full references (including those not matched with items on IDEAS)

    Citations

    Citations are extracted by the CitEc Project, subscribe to its RSS feed for this item.
    as


    Cited by:

    1. He, Zhuosen & Hou, Yucui & Li, He & Wei, Jian & Ren, Shuhang & Wu, Weize, 2023. "Novel chemical looping oxidation of biomass-derived carbohydrates to super-high-yield formic acid using heteropolyacids as oxygen carrier," Renewable Energy, Elsevier, vol. 207(C), pages 461-470.
    2. Yang Liu & Huishan Shang & Bing Zhang & Dongpeng Yan & Xu Xiang, 2024. "Surface fluorination of BiVO4 for the photoelectrochemical oxidation of glycerol to formic acid," Nature Communications, Nature, vol. 15(1), pages 1-12, December.

    Most related items

    These are the items that most often cite the same works as this one and are cited by the same works as this one.
    1. Ana L. Santos & Maria-João Cebola & Diogo M. F. Santos, 2021. "Towards the Hydrogen Economy—A Review of the Parameters That Influence the Efficiency of Alkaline Water Electrolyzers," Energies, MDPI, vol. 14(11), pages 1-35, May.
    2. Okoye, Patrick U. & Wang, Song & Khanday, Waheed Ahmad & Li, Sanxi & Tang, Tao & Zhang, Linnan, 2020. "Box-Behnken optimization of glycerol transesterification reaction to glycerol carbonate over calcined oil palm fuel ash derived catalyst," Renewable Energy, Elsevier, vol. 146(C), pages 2676-2687.
    3. Yang, Le & Lin, Hongju & Fang, Zhihao & Yang, Yanhui & Liu, Xiaohao & Ouyang, Gangfeng, 2023. "Recent advances on methane partial oxidation toward oxygenates under mild conditions," Renewable and Sustainable Energy Reviews, Elsevier, vol. 184(C).
    4. Lei, Yuanting & Zhang, Lili & Zhou, Danni & Xiong, Chengli & Zhao, Yafei & Chen, Wenxing & Xiang, Xu & Shang, Huishan & Zhang, Bing, 2022. "Construction of interconnected NiO/CoFe alloy nanosheets for overall water splitting," Renewable Energy, Elsevier, vol. 194(C), pages 459-468.
    5. He, Quan (Sophia) & McNutt, Josiah & Yang, Jie, 2017. "Utilization of the residual glycerol from biodiesel production for renewable energy generation," Renewable and Sustainable Energy Reviews, Elsevier, vol. 71(C), pages 63-76.
    6. Okoye, P.U. & Hameed, B.H., 2016. "Review on recent progress in catalytic carboxylation and acetylation of glycerol as a byproduct of biodiesel production," Renewable and Sustainable Energy Reviews, Elsevier, vol. 53(C), pages 558-574.
    7. Moreira, Rui & Bimbela, Fernando & Gandía, Luis M. & Ferreira, Abel & Sánchez, Jose Luis & Portugal, António, 2021. "Oxidative steam reforming of glycerol. A review," Renewable and Sustainable Energy Reviews, Elsevier, vol. 148(C).
    8. McKenna K. Goetz & Michael T. Bender & Kyoung-Shin Choi, 2022. "Predictive control of selective secondary alcohol oxidation of glycerol on NiOOH," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    9. Kai Shi & Di Si & Xue Teng & Lisong Chen & Jianlin Shi, 2024. "Pd/NiMoO4/NF electrocatalysts for the efficient and ultra-stable synthesis and electrolyte-assisted extraction of glycolate," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    10. Jun Qi & Yadong Du & Qi Yang & Na Jiang & Jiachun Li & Yi Ma & Yangjun Ma & Xin Zhao & Jieshan Qiu, 2023. "Energy-saving and product-oriented hydrogen peroxide electrosynthesis enabled by electrochemistry pairing and product engineering," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    11. Zuyun He & Jinwoo Hwang & Zhiheng Gong & Mengzhen Zhou & Nian Zhang & Xiongwu Kang & Jeong Woo Han & Yan Chen, 2022. "Promoting biomass electrooxidation via modulating proton and oxygen anion deintercalation in hydroxide," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    12. Hua Zhou & Yue Ren & Bingxin Yao & Zhenhua Li & Ming Xu & Lina Ma & Xianggui Kong & Lirong Zheng & Mingfei Shao & Haohong Duan, 2023. "Scalable electrosynthesis of commodity chemicals from biomass by suppressing non-Faradaic transformations," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    13. Ming Yang & Yimin Jiang & Chung-Li Dong & Leitao Xu & Yutong Huang & Shifan Leng & Yandong Wu & Yongxiang Luo & Wei Chen & Ta Thi Thuy Nga & Shuangyin Wang & Yuqin Zou, 2024. "A self-reactivated PdCu catalyst for aldehyde electro-oxidation with anodic hydrogen production," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    14. Lei Luo & Lei Fu & Huifen Liu & Youxun Xu & Jialiang Xing & Chun-Ran Chang & Dong-Yuan Yang & Junwang Tang, 2022. "Synergy of Pd atoms and oxygen vacancies on In2O3 for methane conversion under visible light," Nature Communications, Nature, vol. 13(1), pages 1-12, December.
    15. Yuyang Pan & Huiyan Zhang & Bowen Zhang & Feng Gong & Jianyong Feng & Huiting Huang & Srinivas Vanka & Ronglei Fan & Qi Cao & Mingrong Shen & Zhaosheng Li & Zhigang Zou & Rui Xiao & Sheng Chu, 2023. "Renewable formate from sunlight, biomass and carbon dioxide in a photoelectrochemical cell," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    16. Jia, Guangxin & He, Beibei & Ma, Wenlin & Sun, Yifan, 2019. "Thermodynamic analysis based on simultaneous chemical and phase equilibrium for dehydration of glycerol with methanol," Energy, Elsevier, vol. 188(C).
    17. Hejna, Aleksander & Kosmela, Paulina & Formela, Krzysztof & Piszczyk, Łukasz & Haponiuk, Józef T., 2016. "Potential applications of crude glycerol in polymer technology–Current state and perspectives," Renewable and Sustainable Energy Reviews, Elsevier, vol. 66(C), pages 449-475.
    18. Lam, Su Shiung & Liew, Rock Keey & Jusoh, Ahmad & Chong, Cheng Tung & Ani, Farid Nasir & Chase, Howard A., 2016. "Progress in waste oil to sustainable energy, with emphasis on pyrolysis techniques," Renewable and Sustainable Energy Reviews, Elsevier, vol. 53(C), pages 741-753.
    19. Qing Hong & Hong Yang & Yanfeng Fang & Wang Li & Caixia Zhu & Zhuang Wang & Sicheng Liang & Xuwen Cao & Zhixin Zhou & Yanfei Shen & Songqin Liu & Yuanjian Zhang, 2023. "Adaptable graphitic C6N6-based copper single-atom catalyst for intelligent biosensing," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    20. Budzianowski, Wojciech M., 2017. "High-value low-volume bioproducts coupled to bioenergies with potential to enhance business development of sustainable biorefineries," Renewable and Sustainable Energy Reviews, Elsevier, vol. 70(C), pages 793-804.

    More about this item

    Statistics

    Access and download statistics

    Corrections

    All material on this site has been provided by the respective publishers and authors. You can help correct errors and omissions. When requesting a correction, please mention this item's handle: RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-021-27240-5. See general information about how to correct material in RePEc.

    If you have authored this item and are not yet registered with RePEc, we encourage you to do it here. This allows to link your profile to this item. It also allows you to accept potential citations to this item that we are uncertain about.

    If CitEc recognized a bibliographic reference but did not link an item in RePEc to it, you can help with this form .

    If you know of missing items citing this one, you can help us creating those links by adding the relevant references in the same way as above, for each refering item. If you are a registered author of this item, you may also want to check the "citations" tab in your RePEc Author Service profile, as there may be some citations waiting for confirmation.

    For technical questions regarding this item, or to correct its authors, title, abstract, bibliographic or download information, contact: Sonal Shukla or Springer Nature Abstracting and Indexing (email available below). General contact details of provider: http://www.nature.com .

    Please note that corrections may take a couple of weeks to filter through the various RePEc services.

    IDEAS is a RePEc service. RePEc uses bibliographic data supplied by the respective publishers.