IDEAS home Printed from https://ideas.repec.org/a/nat/natcom/v15y2024i1d10.1038_s41467-024-53179-4.html
   My bibliography  Save this article

Electrical monitoring of single-event protonation dynamics at the solid-liquid interface and its regulation by external mechanical forces

Author

Listed:
  • Cong Zhao

    (Nankai University)

  • Jiazheng Diao

    (University of Science and Technology of China)

  • Zhao Liu

    (Nankai University)

  • Jie Hao

    (Nankai University)

  • Suhang He

    (Nankai University)

  • Shaojia Li

    (Nankai University)

  • Xingxing Li

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

  • Guangwu Li

    (Nankai University
    Institute of Nankai University, 16th Floor, Yantian Science & Technology Building)

  • Qiang Fu

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

  • Chuancheng Jia

    (Nankai University)

  • Xuefeng Guo

    (Nankai University
    Peking University)

Abstract

Detecting chemical reaction dynamics at solid-liquid interfaces is important for understanding heterogeneous reactions. However, there is a lack of exploration of interface reaction dynamics from the single-molecule perspective, which can reveal the intrinsic reaction mechanism underlying ensemble experiments. Here, single-event protonation reaction dynamics at a solid-liquid interface are studied in-situ using single-molecule junctions. Molecules with amino terminal groups are used to construct single-molecule junctions. An interfacial cationic state present after protonation is discovered. Real-time electrical measurements are used to monitor the reversible reaction between protonated and deprotonated states, thereby revealing the interfacial reaction mechanism through dynamic analysis. The protonation reaction rate constant has a linear positive correlation with proton concentration, whereas the deprotonation reaction rate constant has a linear negative correlation. In addition, external mechanical forces can effectively regulate the protonation reaction process. This work provides a single-molecule perspective for exploring interface science, which will contribute to the development of heterogeneous catalysis and electrochemistry.

Suggested Citation

  • Cong Zhao & Jiazheng Diao & Zhao Liu & Jie Hao & Suhang He & Shaojia Li & Xingxing Li & Guangwu Li & Qiang Fu & Chuancheng Jia & Xuefeng Guo, 2024. "Electrical monitoring of single-event protonation dynamics at the solid-liquid interface and its regulation by external mechanical forces," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
  • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-53179-4
    DOI: 10.1038/s41467-024-53179-4
    as

    Download full text from publisher

    File URL: https://www.nature.com/articles/s41467-024-53179-4
    File Function: Abstract
    Download Restriction: no

    File URL: https://libkey.io/10.1038/s41467-024-53179-4?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. Insoo Ro & Ji Qi & Seungyeon Lee & Mingjie Xu & Xingxu Yan & Zhenhua Xie & Gregory Zakem & Austin Morales & Jingguang G. Chen & Xiaoqing Pan & Dionisios G. Vlachos & Stavros Caratzoulas & Phillip Chri, 2022. "Bifunctional hydroformylation on heterogeneous Rh-WOx pair site catalysts," Nature, Nature, vol. 609(7926), pages 287-292, September.
    2. Robert Wild & Markus Nötzold & Malcolm Simpson & Thuy Dung Tran & Roland Wester, 2023. "Tunnelling measured in a very slow ion–molecule reaction," Nature, Nature, vol. 615(7952), pages 425-429, March.
    3. Yao-Hui Wang & Shisheng Zheng & Wei-Min Yang & Ru-Yu Zhou & Quan-Feng He & Petar Radjenovic & Jin-Chao Dong & Shunning Li & Jiaxin Zheng & Zhi-Lin Yang & Gary Attard & Feng Pan & Zhong-Qun Tian & Jian, 2021. "In situ Raman spectroscopy reveals the structure and dissociation of interfacial water," Nature, Nature, vol. 600(7887), pages 81-85, December.
    4. Lei Zhang & Chen Yang & Chenxi Lu & Xingxing Li & Yilin Guo & Jianning Zhang & Jinglong Lin & Zhizhou Li & Chuancheng Jia & Jinlong Yang & K. N. Houk & Fanyang Mo & Xuefeng Guo, 2022. "Precise electrical gating of the single-molecule Mizoroki-Heck reaction," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
    5. Gao-Feng Chen & Yifei Yuan & Haifeng Jiang & Shi-Yu Ren & Liang-Xin Ding & Lu Ma & Tianpin Wu & Jun Lu & Haihui Wang, 2020. "Electrochemical reduction of nitrate to ammonia via direct eight-electron transfer using a copper–molecular solid catalyst," Nature Energy, Nature, vol. 5(8), pages 605-613, August.
    6. Marco Favaro & Beomgyun Jeong & Philip N. Ross & Junko Yano & Zahid Hussain & Zhi Liu & Ethan J. Crumlin, 2016. "Unravelling the electrochemical double layer by direct probing of the solid/liquid interface," Nature Communications, Nature, vol. 7(1), pages 1-8, November.
    7. Jie Dai & Yinlong Zhu & Yu Chen & Xue Wen & Mingce Long & Xinhao Wu & Zhiwei Hu & Daqin Guan & Xixi Wang & Chuan Zhou & Qian Lin & Yifei Sun & Shih-Chang Weng & Huanting Wang & Wei Zhou & Zongping Sha, 2022. "Hydrogen spillover in complex oxide multifunctional sites improves acidic hydrogen evolution electrocatalysis," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    8. Latha Venkataraman & Jennifer E. Klare & Colin Nuckolls & Mark S. Hybertsen & Michael L. Steigerwald, 2006. "Dependence of single-molecule junction conductance on molecular conformation," Nature, Nature, vol. 442(7105), pages 904-907, August.
    9. Jinshi Li & Pingchuan Shen & Shijie Zhen & Chun Tang & Yiling Ye & Dahai Zhou & Wenjing Hong & Zujin Zhao & Ben Zhong Tang, 2021. "Mechanical single-molecule potentiometers with large switching factors from ortho-pentaphenylene foldamers," Nature Communications, Nature, vol. 12(1), pages 1-11, December.
    10. A. I. Yanson & G. Rubio Bollinger & H. E. van den Brom & N. Agraït & J. M. van Ruitenbeek, 1998. "Formation and manipulation of a metallic wire of single gold atoms," Nature, Nature, vol. 395(6704), pages 783-785, October.
    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. Woojung Lee & Liang Li & María Camarasa-Gómez & Daniel Hernangómez-Pérez & Xavier Roy & Ferdinand Evers & Michael S. Inkpen & Latha Venkataraman, 2024. "Photooxidation driven formation of Fe-Au linked ferrocene-based single-molecule junctions," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
    2. Jinshi Li & Pingchuan Shen & Zeyan Zhuang & Junqi Wu & Ben Zhong Tang & Zujin Zhao, 2023. "In-situ electro-responsive through-space coupling enabling foldamers as volatile memory elements," Nature Communications, Nature, vol. 14(1), pages 1-13, December.
    3. Jie Dai & Yawen Tong & Long Zhao & Zhiwei Hu & Chien-Te Chen & Chang-Yang Kuo & Guangming Zhan & Jiaxian Wang & Xingyue Zou & Qian Zheng & Wei Hou & Ruizhao Wang & Kaiyuan Wang & Rui Zhao & Xiang-Kui , 2024. "Spin polarized Fe1−Ti pairs for highly efficient electroreduction nitrate to ammonia," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    4. Wanru Liao & Jun Wang & Ganghai Ni & Kang Liu & Changxu Liu & Shanyong Chen & Qiyou Wang & Yingkang Chen & Tao Luo & Xiqing Wang & Yanqiu Wang & Wenzhang Li & Ting-Shan Chan & Chao Ma & Hongmei Li & Y, 2024. "Sustainable conversion of alkaline nitrate to ammonia at activities greater than 2 A cm−2," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    5. Tao Zhang & Qitong Ye & Zengyu Han & Qingyi Liu & Yipu Liu & Dongshuang Wu & Hong Jin Fan, 2024. "Biaxial strain induced OH engineer for accelerating alkaline hydrogen evolution," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    6. Hao Shi & Tanyuan Wang & Jianyun Liu & Weiwei Chen & Shenzhou Li & Jiashun Liang & Shuxia Liu & Xuan Liu & Zhao Cai & Chao Wang & Dong Su & Yunhui Huang & Lior Elbaz & Qing Li, 2023. "A sodium-ion-conducted asymmetric electrolyzer to lower the operation voltage for direct seawater electrolysis," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    7. Xin Liu & Yan Jiao & Yao Zheng & Mietek Jaroniec & Shi-Zhang Qiao, 2022. "Mechanism of C-N bonds formation in electrocatalytic urea production revealed by ab initio molecular dynamics simulation," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    8. Ziang Xu & Lei Wan & Yiwen Liao & Maobin Pang & Qin Xu & Peican Wang & Baoguo Wang, 2023. "Continuous ammonia electrosynthesis using physically interlocked bipolar membrane at 1000 mA cm−2," Nature Communications, Nature, vol. 14(1), pages 1-13, December.
    9. Jian Zhang & Thomas Quast & Bashir Eid & Yen-Ting Chen & Ridha Zerdoumi & Stefan Dieckhöfer & João R. C. Junqueira & Sabine Seisel & Wolfgang Schuhmann, 2024. "In-situ electrochemical reconstruction and modulation of adsorbed hydrogen coverage in cobalt/ruthenium-based catalyst boost electroreduction of nitrate to ammonia," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    10. Leopoldo Mejía & Pilar Cossio & Ignacio Franco, 2023. "Microscopic theory, analysis, and interpretation of conductance histograms in molecular junctions," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    11. 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.
    12. Eamonn Murphy & Yuanchao Liu & Ivana Matanovic & Martina Rüscher & Ying Huang & Alvin Ly & Shengyuan Guo & Wenjie Zang & Xingxu Yan & Andrea Martini & Janis Timoshenko & Beatriz Roldán Cuenya & Iryna , 2023. "Elucidating electrochemical nitrate and nitrite reduction over atomically-dispersed transition metal sites," Nature Communications, Nature, vol. 14(1), pages 1-15, December.
    13. Ananta Dey & Amal Mendalz & Anna Wach & Robert Bericat Vadell & Vitor R. Silveira & Paul Maurice Leidinger & Thomas Huthwelker & Vitalii Shtender & Zbynek Novotny & Luca Artiglia & Jacinto Sá, 2024. "Hydrogen evolution with hot electrons on a plasmonic-molecular catalyst hybrid system," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    14. Zhiyuan Han & An Chen & Zejian Li & Mengtian Zhang & Zhilong Wang & Lixue Yang & Runhua Gao & Yeyang Jia & Guanjun Ji & Zhoujie Lao & Xiao Xiao & Kehao Tao & Jing Gao & Wei Lv & Tianshuai Wang & Jinji, 2024. "Machine learning-based design of electrocatalytic materials towards high-energy lithium||sulfur batteries development," Nature Communications, Nature, vol. 15(1), pages 1-13, December.
    15. Michael L. Whittaker & David Ren & Colin Ophus & Yugang Zhang & Laura Waller & Benjamin Gilbert & Jillian F. Banfield, 2022. "Ion complexation waves emerge at the curved interfaces of layered minerals," Nature Communications, Nature, vol. 13(1), pages 1-8, December.
    16. Xiao-Ting Yin & En-Ming You & Ru-Yu Zhou & Li-Hong Zhu & Wei-Wei Wang & Kai-Xuan Li & De-Yin Wu & Yu Gu & Jian-Feng Li & Bing-Wei Mao & Jia-Wei Yan, 2024. "Unraveling the energy storage mechanism in graphene-based nonaqueous electrochemical capacitors by gap-enhanced Raman spectroscopy," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    17. Xiaoqi Lang & Lixue Shi & Zhilun Zhao & Wei Min, 2024. "Probing the structure of water in individual living cells," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    18. Bocheng Zhang & Zechuan Dai & Yanxu Chen & Mingyu Cheng & Huaikun Zhang & Pingyi Feng & Buqi Ke & Yangyang Zhang & Genqiang Zhang, 2024. "Defect-induced triple synergistic modulation in copper for superior electrochemical ammonia production across broad nitrate concentrations," Nature Communications, Nature, vol. 15(1), pages 1-14, December.
    19. 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.
    20. Jieyuan Li & Ruimin Chen & Jielin Wang & Ying Zhou & Guidong Yang & Fan Dong, 2022. "Subnanometric alkaline-earth oxide clusters for sustainable nitrate to ammonia photosynthesis," Nature Communications, Nature, vol. 13(1), pages 1-11, 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_s41467-024-53179-4. 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.