IDEAS home Printed from https://ideas.repec.org/a/nat/natcom/v14y2023i1d10.1038_s41467-023-43649-6.html
   My bibliography  Save this article

Nonredox trivalent nickel catalyzing nucleophilic electrooxidation of organics

Author

Listed:
  • Yuandong Yan

    (Nanjing University)

  • Ruyi Wang

    (Nanjing University)

  • Qian Zheng

    (Nanjing University)

  • Jiaying Zhong

    (Nanjing University)

  • Weichang Hao

    (Beihang University)

  • Shicheng Yan

    (Nanjing University
    Nanjing University)

  • Zhigang Zou

    (Nanjing University
    Nanjing University)

Abstract

A thorough comprehension of the mechanism behind organic electrooxidation is crucial for the development of efficient energy conversion technology. Here, we find that trivalent nickel is capable of oxidizing organics through a nucleophilic attack and electron transfer via a nonredox process. This nonredox trivalent nickel exhibits exceptional kinetic efficiency in oxidizing organics that possess the highest occupied molecular orbital energy levels ranging from −7.4 to −6 eV (vs. Vacuum level) and the dual local softness values of nucleophilic atoms in nucleophilic functional groups, such as hydroxyls (methanol, ethanol, benzyl alcohol), carbonyls (formamide, urea, formaldehyde, glucose, and N-acetyl glucosamine), and aminos (benzylamine), ranging from −0.65 to −0.15. The rapid electrooxidation kinetics can be attributed to the isoenergetic channels created by the nucleophilic attack and the nonredox electron transfer via the unoccupied eg orbitals of trivalent nickel (t2g6eg1). Our findings are valuable in identifying kinetically fast organic electrooxidation on nonredox catalysts for efficient energy conversions.

Suggested Citation

  • Yuandong Yan & Ruyi Wang & Qian Zheng & Jiaying Zhong & Weichang Hao & Shicheng Yan & Zhigang Zou, 2023. "Nonredox trivalent nickel catalyzing nucleophilic electrooxidation of organics," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
  • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-43649-6
    DOI: 10.1038/s41467-023-43649-6
    as

    Download full text from publisher

    File URL: https://www.nature.com/articles/s41467-023-43649-6
    File Function: Abstract
    Download Restriction: no

    File URL: https://libkey.io/10.1038/s41467-023-43649-6?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. Haoliang Huang & Yu-Chung Chang & Yu-Cheng Huang & Lili Li & Alexander C. Komarek & Liu Hao Tjeng & Yuki Orikasa & Chih-Wen Pao & Ting-Shan Chan & Jin-Ming Chen & Shu-Chih Haw & Jing Zhou & Yifeng Wan, 2023. "Unusual double ligand holes as catalytic active sites in LiNiO2," Nature Communications, Nature, vol. 14(1), pages 1-14, December.
    2. Hen Dotan & Avigail Landman & Stafford W. Sheehan & Kirtiman Deo Malviya & Gennady E. Shter & Daniel A. Grave & Ziv Arzi & Nachshon Yehudai & Manar Halabi & Netta Gal & Noam Hadari & Coral Cohen & Avn, 2019. "Decoupled hydrogen and oxygen evolution by a two-step electrochemical–chemical cycle for efficient overall water splitting," Nature Energy, Nature, vol. 4(9), pages 786-795, September.
    3. Xi Yang & Chris P. Nielsen & Shaojie Song & Michael B. McElroy, 2022. "Breaking the hard-to-abate bottleneck in China’s path to carbon neutrality with clean hydrogen," Nature Energy, Nature, vol. 7(10), pages 955-965, October.
    4. Shi-Kui Geng & Yao Zheng & Shan-Qing Li & Hui Su & Xu Zhao & Jun Hu & Hai-Bo Shu & Mietek Jaroniec & Ping Chen & Qing-Hua Liu & Shi-Zhang Qiao, 2021. "Nickel ferrocyanide as a high-performance urea oxidation electrocatalyst," Nature Energy, Nature, vol. 6(9), pages 904-912, September.
    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. Xiang Liu & Yu-Quan Zhu & Jing Li & Ye Wang & Qiujin Shi & An-Zhen Li & Kaiyue Ji & Xi Wang & Xikang Zhao & Jinyu Zheng & Haohong Duan, 2024. "Electrosynthesis of adipic acid with high faradaic efficiency within a wide potential window," Nature Communications, Nature, vol. 15(1), pages 1-16, 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. Lan, Yuncheng & Lu, Junhui & Wang, Suilin, 2023. "Study of the geometry and structure of a thermoelectric leg with variable material properties and side heat dissipation based on thermodynamic, economic, and environmental analysis," Energy, Elsevier, vol. 282(C).
    2. Zhao, Meng-Jie & He, Qian & Xiang, Ting & Ya, Hua-Qin & Luo, Hao & Wan, Shanhong & Ding, Jun & He, Jian-Bo, 2023. "Automatic operation of decoupled water electrolysis based on bipolar electrode," Renewable Energy, Elsevier, vol. 203(C), pages 583-591.
    3. Guo, Zhi & Mao, Xianqiang & Lu, Jianhong & Gao, Yubing & Chen, Xing & Zhang, Shining & Ma, Zhiyuan, 2024. "Can a new power system create more employment in China?," Energy, Elsevier, vol. 295(C).
    4. Liu, Haifeng & Ampah, Jeffrey Dankwa & Afrane, Sandylove & Adun, Humphrey & Jin, Chao & Yao, Mingfa, 2023. "Deployment of hydrogen in hard-to-abate transport sectors under limited carbon dioxide removal (CDR): Implications on global energy-land-water system," Renewable and Sustainable Energy Reviews, Elsevier, vol. 184(C).
    5. 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.
    6. Xintong Gao & Xiaowan Bai & Pengtang Wang & Yan Jiao & Kenneth Davey & Yao Zheng & Shi-Zhang Qiao, 2023. "Boosting urea electrooxidation on oxyanion-engineered nickel sites via inhibited water oxidation," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    7. Xin Kang & Fengning Yang & Zhiyuan Zhang & Heming Liu & Shiyu Ge & Shuqi Hu & Shaohai Li & Yuting Luo & Qiangmin Yu & Zhibo Liu & Qiang Wang & Wencai Ren & Chenghua Sun & Hui-Ming Cheng & Bilu Liu, 2023. "A corrosion-resistant RuMoNi catalyst for efficient and long-lasting seawater oxidation and anion exchange membrane electrolyzer," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    8. Liu-Chun Wang & Pei-Yu Chiou & Ya-Ping Hsu & Chin-Lai Lee & Chih-Hsuan Hung & Yi-Hsuan Wu & Wen-Jyun Wang & Gia-Ling Hsieh & Ying-Chi Chen & Li-Chan Chang & Wen-Pin Su & Divinah Manoharan & Min-Chiao , 2023. "Prussian blue analog with separated active sites to catalyze water driven enhanced catalytic treatments," Nature Communications, Nature, vol. 14(1), pages 1-16, December.
    9. Meng Niu & Xiangjun Li & Chen Sun & Xiaoqing Xiu & Yue Wang & Mingyue Hu & Haitao Dong, 2023. "Operation Optimization of Wind/Battery Storage/Alkaline Electrolyzer System Considering Dynamic Hydrogen Production Efficiency," Energies, MDPI, vol. 16(17), pages 1-20, August.
    10. Lin, Yuancheng & Ma, Linwei & Li, Zheng & Ni, Weidou, 2023. "The carbon reduction potential by improving technical efficiency from energy sources to final services in China: An extended Kaya identity analysis," Energy, Elsevier, vol. 263(PE).
    11. Qian Dang & Haiping Lin & Zhenglong Fan & Lu Ma & Qi Shao & Yujin Ji & Fangfang Zheng & Shize Geng & Shi-Ze Yang & Ningning Kong & Wenxiang Zhu & Youyong Li & Fan Liao & Xiaoqing Huang & Mingwang Shao, 2021. "Iridium metallene oxide for acidic oxygen evolution catalysis," Nature Communications, Nature, vol. 12(1), pages 1-10, December.
    12. Jiachen Li & Yuqiang Ma & Cong Zhang & Chi Zhang & Huijun Ma & Zhaoqi Guo & Ning Liu & Ming Xu & Haixia Ma & Jieshan Qiu, 2023. "Green electrosynthesis of 3,3’-diamino-4,4’-azofurazan energetic materials coupled with energy-efficient hydrogen production over Pt-based catalysts," Nature Communications, Nature, vol. 14(1), pages 1-15, December.
    13. Zhou, Bo & Zhang, Cheng, 2023. "When green finance meets banking competition: Evidence from hard-to-abate enterprises of China," Pacific-Basin Finance Journal, Elsevier, vol. 78(C).
    14. Chen, Huayu & Wang, Zehao & He, He & Chen, Jiadian & Yin, Hang & Yu, Dandan & Liang, Junhui & Qin, Laishun & Huang, Yuexiang & Chen, Da, 2024. "Few-layer MoAlB nanosheets with Al vacancies enhanced hydroxyl adsorption for improved water oxidation kinetics," Renewable Energy, Elsevier, vol. 225(C).
    15. Danlu Xu & Zhoubin Liu & Jiahui Zhu & Qin Fang & Rui Shan, 2023. "Linking Cost Decline and Demand Surge in the Hydrogen Market: A Case Study in China," Energies, MDPI, vol. 16(12), pages 1-13, June.
    16. Xiubei Yang & Qizheng An & Xuewen Li & Yubin Fu & Shuai Yang & Minghao Liu & Qing Xu & Gaofeng Zeng, 2024. "Charging modulation of the pyridine nitrogen of covalent organic frameworks for promoting oxygen reduction reaction," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    17. Fan Liao & Kui Yin & Yujin Ji & Wenxiang Zhu & Zhenglong Fan & Youyong Li & Jun Zhong & Mingwang Shao & Zhenhui Kang & Qi Shao, 2023. "Iridium oxide nanoribbons with metastable monoclinic phase for highly efficient electrocatalytic oxygen evolution," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    18. Fernando Rocha & Christos Georgiadis & Kevin Droogenbroek & Renaud Delmelle & Xavier Pinon & Grzegorz Pyka & Greet Kerckhofs & Franz Egert & Fatemeh Razmjooei & Syed-Asif Ansar & Shigenori Mitsushima , 2024. "Proton exchange membrane-like alkaline water electrolysis using flow-engineered three-dimensional electrodes," Nature Communications, Nature, vol. 15(1), pages 1-13, December.
    19. Yong Zuo & Sebastiano Bellani & Michele Ferri & Gabriele Saleh & Dipak V. Shinde & Marilena Isabella Zappia & Rosaria Brescia & Mirko Prato & Luca Trizio & Ivan Infante & Francesco Bonaccorso & Libera, 2023. "High-performance alkaline water electrolyzers based on Ru-perturbed Cu nanoplatelets cathode," Nature Communications, Nature, vol. 14(1), pages 1-15, December.
    20. Yang, Wei & Bao, Jingjing & Liu, Hongtao & Zhang, Jun & Guo, Lin, 2023. "Low-grade heat to hydrogen: Current technologies, challenges and prospective," Renewable and Sustainable Energy Reviews, Elsevier, vol. 188(C).

    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:14:y:2023:i:1:d:10.1038_s41467-023-43649-6. 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.