IDEAS home Printed from https://ideas.repec.org/a/nat/natcom/v15y2024i1d10.1038_s41467-024-49544-y.html
   My bibliography  Save this article

Microenvironment regulation breaks the Faradaic efficiency-current density trade-off for electrocatalytic deuteration using D2O

Author

Listed:
  • Meng He

    (Tianjin University)

  • Rui Li

    (Tianjin University)

  • Chuanqi Cheng

    (Tianjin University)

  • Cuibo Liu

    (Tianjin University
    Tianjin University)

  • Bin Zhang

    (Tianjin University
    Tianjin University)

Abstract

The high Faradaic efficiency (FE) of the electrocatalytic deuteration of organics with D2O at a large current density is significant for deuterated electrosynthesis. However, the FE and current density are the two ends of a seesaw because of the severe D2 evolution side reaction at nearly industrial current densities. Herein, we report a combined scenario of a nanotip-enhanced electric field and surfactant-modified interface microenvironment to enable the electrocatalytic deuteration of arylacetonitrile in D2O with an 80% FE at −100 mA cm−2. The increased concentration with low activation energy of arylacetonitrile due to the large electric field along the tips and the accelerated arylacetonitrile transfer and suppressed D2 evolution by the surfactant-created deuterophobic microenvironment contribute to breaking the trade-off between a high FE and large current density. Furthermore, the application of our strategy in other deuteration reactions with improved Faradaic efficiencies at −100 mA cm−2 rationalizes the design concept.

Suggested Citation

  • Meng He & Rui Li & Chuanqi Cheng & Cuibo Liu & Bin Zhang, 2024. "Microenvironment regulation breaks the Faradaic efficiency-current density trade-off for electrocatalytic deuteration using D2O," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
  • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-49544-y
    DOI: 10.1038/s41467-024-49544-y
    as

    Download full text from publisher

    File URL: https://www.nature.com/articles/s41467-024-49544-y
    File Function: Abstract
    Download Restriction: no

    File URL: https://libkey.io/10.1038/s41467-024-49544-y?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. Bo-Hang Zhao & Fanpeng Chen & Mengke Wang & Chuanqi Cheng & Yongmeng Wu & Cuibo Liu & Yifu Yu & Bin Zhang, 2023. "Economically viable electrocatalytic ethylene production with high yield and selectivity," Nature Sustainability, Nature, vol. 6(7), pages 827-837, July.
    2. Jiaxin Guo & Yao Zheng & Zhenpeng Hu & Caiyan Zheng & Jing Mao & Kun Du & Mietek Jaroniec & Shi-Zhang Qiao & Tao Ling, 2023. "Direct seawater electrolysis by adjusting the local reaction environment of a catalyst," Nature Energy, Nature, vol. 8(3), pages 264-272, March.
    3. Mohammadreza Esmaeilirad & Zhen Jiang & Ahmad M. Harzandi & Alireza Kondori & Mahmoud Tamadoni Saray & Carlo U. Segre & Reza Shahbazian-Yassar & Andrew M. Rappe & Mohammad Asadi, 2023. "Imidazolium-functionalized Mo3P nanoparticles with an ionomer coating for electrocatalytic reduction of CO2 to propane," Nature Energy, Nature, vol. 8(8), pages 891-900, August.
    4. Rui Li & Yongmeng Wu & Changhong Wang & Meng He & Cuibo Liu & Bin Zhang, 2022. "One-pot H/D exchange and low-coordinated iron electrocatalyzed deuteration of nitriles in D2O to α,β-deuterio aryl ethylamines," Nature Communications, Nature, vol. 13(1), pages 1-12, December.
    5. Pengfei Li & Chengcheng Guo & Siyi Wang & Dengke Ma & Tian Feng & Yanwei Wang & Youai Qiu, 2022. "Facile and general electrochemical deuteration of unactivated alkyl halides," Nature Communications, Nature, vol. 13(1), pages 1-8, December.
    6. Ala Bunescu & Yusra Abdelhamid & Matthew J. Gaunt, 2021. "Multicomponent alkene azidoarylation by anion-mediated dual catalysis," Nature, Nature, vol. 598(7882), pages 597-603, October.
    7. Min Liu & Yuanjie Pang & Bo Zhang & Phil De Luna & Oleksandr Voznyy & Jixian Xu & Xueli Zheng & Cao Thang Dinh & Fengjia Fan & Changhong Cao & F. Pelayo García de Arquer & Tina Saberi Safaei & Adam Me, 2016. "Enhanced electrocatalytic CO2 reduction via field-induced reagent concentration," Nature, Nature, vol. 537(7620), pages 382-386, September.
    8. Zhenhua Li & Xiaofan Li & Hua Zhou & Yan Xu & Si-Min Xu & Yue Ren & Yifan Yan & Jiangrong Yang & Kaiyue Ji & Li Li & Ming Xu & Mingfei Shao & Xianggui Kong & Xiaoming Sun & Haohong Duan, 2022. "Electrocatalytic synthesis of adipic acid coupled with H2 production enhanced by a ligand modification strategy," Nature Communications, Nature, vol. 13(1), pages 1-12, December.
    Full references (including those not matched with items on IDEAS)

    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. Kejian Kong & An-Zhen Li & Ye Wang & Qiujin Shi & Jing Li & Kaiyue Ji & Haohong Duan, 2023. "Electrochemical carbon–carbon coupling with enhanced activity and racemate stereoselectivity by microenvironment regulation," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    2. Yu Shen & Xiao-Long Zhang & Ming-Rong Qu & Jie Ma & Sheng Zhu & Yu-Lin Min & Min-Rui Gao & Shu-Hong Yu, 2024. "Cr dopant mediates hydroxyl spillover on RuO2 for high-efficiency proton exchange membrane electrolysis," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    3. Kang Yang & Ming Li & Tianqi Gao & Guoliang Xu & Di Li & Yao Zheng & Qiang Li & Jingjing Duan, 2024. "An acid-tolerant metal-organic framework for industrial CO2 electrolysis using a proton exchange membrane," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    4. Pan Ran & Aoqian Qiu & Tianshu Liu & Fangyuan Wang & Bailin Tian & Beiyao Xiang & Jun Li & Yang Lv & Mengning Ding, 2024. "Universal high-efficiency electrocatalytic olefin epoxidation via a surface-confined radical promotion," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    5. Ruixin Yang & Yanming Cai & Yongbing Qi & Zhuodong Tang & Jun-Jie Zhu & Jinxiang Li & Wenlei Zhu & Zixuan Chen, 2024. "How local electric field regulates C–C coupling at a single nanocavity in electrocatalytic CO2 reduction," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    6. Yicui Kang & Simão M. João & Rui Lin & Kang Liu & Li Zhu & Junwei Fu & Weng-Chon (Max) Cheong & Seunghoon Lee & Kilian Frank & Bert Nickel & Min Liu & Johannes Lischner & Emiliano Cortés, 2024. "Effect of crystal facets in plasmonic catalysis," Nature Communications, Nature, vol. 15(1), pages 1-13, December.
    7. Xiaowei Shi & Chao Dai & Xin Wang & Jiayue Hu & Junying Zhang & Lingxia Zheng & Liang Mao & Huajun Zheng & Mingshan Zhu, 2022. "Protruding Pt single-sites on hexagonal ZnIn2S4 to accelerate photocatalytic hydrogen evolution," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    8. Jie Xu & Xiong-Xiong Xue & Gonglei Shao & Changfei Jing & Sheng Dai & Kun He & Peipei Jia & Shun Wang & Yifei Yuan & Jun Luo & Jun Lu, 2023. "Atomic-level polarization in electric fields of defects for electrocatalysis," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
    9. Mengjie Jiao & Jie Zhang & Minyan Wang & Hongjian Lu & Zhuangzhi Shi, 2024. "Metallaphotoredox deuteroalkylation utilizing thianthrenium salts," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    10. 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.
    11. Ye Tian & Botao Huang & Yizhi Song & Yirui Zhang & Dong Guan & Jiani Hong & Duanyun Cao & Enge Wang & Limei Xu & Yang Shao-Horn & Ying Jiang, 2024. "Effect of ion-specific water structures at metal surfaces on hydrogen production," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    12. Qiyou Wang & Kang Liu & Kangman Hu & Chao Cai & Huangjingwei Li & Hongmei Li & Matias Herran & Ying-Rui Lu & Ting-Shan Chan & Chao Ma & Junwei Fu & Shiguo Zhang & Ying Liang & Emiliano Cortés & Min Li, 2022. "Attenuating metal-substrate conjugation in atomically dispersed nickel catalysts for electroreduction of CO2 to CO," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    13. Chenhui Zhou & Jia Shi & Zhaoqi Dong & Lingyou Zeng & Yan Chen & Ying Han & Lu Li & Wenyu Zhang & Qinghua Zhang & Lin Gu & Fan Lv & Mingchuan Luo & Shaojun Guo, 2024. "Oxophilic gallium single atoms bridged ruthenium clusters for practical anion-exchange membrane electrolyzer," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    14. Zhiwei Zhao & Ranran Zhang & Yaowen Liu & Zile Zhu & Qiuyan Wang & Youai Qiu, 2024. "Electrochemical C−H deuteration of pyridine derivatives with D2O," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
    15. 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.
    16. Shixuan Zhao & Bin Liu & Kailang Li & Shujie Wang & Gong Zhang & Zhi-Jian Zhao & Tuo Wang & Jinlong Gong, 2024. "A silicon photoanode protected with TiO2/stainless steel bilayer stack for solar seawater splitting," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    17. Pengcheng Ye & Keqing Fang & Haiyan Wang & Yahao Wang & Hao Huang & Chenbin Mo & Jiqiang Ning & Yong Hu, 2024. "Lattice oxygen activation and local electric field enhancement by co-doping Fe and F in CoO nanoneedle arrays for industrial electrocatalytic water oxidation," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    18. Min Liu & Tian Feng & Yanwei Wang & Guangsheng Kou & Qiuyan Wang & Qian Wang & Youai Qiu, 2023. "Metal-free electrochemical dihydroxylation of unactivated alkenes," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
    19. Mengjun Xiao & Qianbao Wu & Ruiqi Ku & Liujiang Zhou & Chang Long & Junwu Liang & Andraž Mavrič & Lei Li & Jing Zhu & Matjaz Valant & Jiong Li & Zhenhua Zeng & Chunhua Cui, 2023. "Self-adaptive amorphous CoOxCly electrocatalyst for sustainable chlorine evolution in acidic brine," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    20. Mengfan Li & Xu Cheng, 2024. "Aggregation-induced C–C bond formation on an electrode driven by the surface tension of water," Nature Communications, Nature, vol. 15(1), pages 1-8, December.

    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:15:y:2024:i:1:d:10.1038_s41467-024-49544-y. 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.