IDEAS home Printed from https://ideas.repec.org/a/nat/natcom/v15y2024i1d10.1038_s41467-024-54204-2.html
   My bibliography  Save this article

Selective electrosynthesis of hydroxylamine from aqueous nitrate/nitrite by suppressing further reduction

Author

Listed:
  • Yirong Tang

    (Southern University of Science and Technology)

  • Zhan Jiang

    (Southern University of Science and Technology
    Ministry of Ecology and Environment)

  • Yubo Yuan

    (Southern University of Science and Technology)

  • Li Xu

    (State Environmental Protection Center for Coal-Fired Air Pollution Control)

  • Chuyao Jin

    (State Environmental Protection Center for Coal-Fired Air Pollution Control)

  • Bulin Chen

    (Southern University of Science and Technology)

  • Zhichao Lin

    (Southern University of Science and Technology)

  • Jie Zao

    (Southern University of Science and Technology)

  • Jianwei Du

    (Ministry of Ecology and Environment)

  • Xiao Zhang

    (State Environmental Protection Center for Coal-Fired Air Pollution Control)

  • Xiang Gao

    (State Environmental Protection Center for Coal-Fired Air Pollution Control)

  • Yongye Liang

    (Southern University of Science and Technology)

Abstract

The electrocatalytic reduction of nitrogenous waste offers a sustainable approach to producing nitrogen-containing chemicals. The selective synthesis of high-value hydroxylamine (NH2OH) is challenging due to the instability of NH2OH as an intermediate. Here, we present a rational electrocatalyst design strategy for promoting NH2OH electrosynthesis by suppressing the competing pathways of further reduction. We screen zinc phthalocyanines (ZnPc) with a high energy barrier for NH2OH reduction by regulating their intrinsic activity. Additionally, we discover that carbon nanotube substrates exhibit significant NH3-producing activity, which can be effectively inhibited by the high coverage of ZnPc molecules. In-situ characterizations reveal that NH2OH and HNO are generated as intermediates in nitrate reduction to NH3, and NH2OH can be enriched in the ZnPc electrode. In the H-cell, the optimized ZnPc catalyst demonstrates a Faradaic efficiency (FE) of 53 ± 1.7% for NH2OH with a partial current density exceeding 270 mA cm−2 and a turnover frequency of 7.5 ± 0.2 s−1. It also enables the rapid electrosynthesis of cyclohexanone oxime from nitrite with a FE of 64 ± 1.0%.

Suggested Citation

  • Yirong Tang & Zhan Jiang & Yubo Yuan & Li Xu & Chuyao Jin & Bulin Chen & Zhichao Lin & Jie Zao & Jianwei Du & Xiao Zhang & Xiang Gao & Yongye Liang, 2024. "Selective electrosynthesis of hydroxylamine from aqueous nitrate/nitrite by suppressing further reduction," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
  • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-54204-2
    DOI: 10.1038/s41467-024-54204-2
    as

    Download full text from publisher

    File URL: https://www.nature.com/articles/s41467-024-54204-2
    File Function: Abstract
    Download Restriction: no

    File URL: https://libkey.io/10.1038/s41467-024-54204-2?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. Jia-Yi Fang & Qi-Zheng Zheng & Yao-Yin Lou & Kuang-Min Zhao & Sheng-Nan Hu & Guang Li & Ouardia Akdim & Xiao-Yang Huang & Shi-Gang Sun, 2022. "Ampere-level current density ammonia electrochemical synthesis using CuCo nanosheets simulating nitrite reductase bifunctional nature," Nature Communications, Nature, vol. 13(1), pages 1-13, December.
    2. Yueshen Wu & Zhan Jiang & Xu Lu & Yongye Liang & Hailiang Wang, 2019. "Domino electroreduction of CO2 to methanol on a molecular catalyst," Nature, Nature, vol. 575(7784), pages 639-642, November.
    3. Yueshen Wu & Zhan Jiang & Zhichao Lin & Yongye Liang & Hailiang Wang, 2021. "Direct electrosynthesis of methylamine from carbon dioxide and nitrate," Nature Sustainability, Nature, vol. 4(8), pages 725-730, August.
    4. Yongmeng Wu & Jinghui Zhao & Changhong Wang & Tieliang Li & Bo-Hang Zhao & Ziyang Song & Cuibo Liu & Bin Zhang, 2023. "Electrosynthesis of a nylon-6 precursor from cyclohexanone and nitrite under ambient conditions," Nature Communications, Nature, vol. 14(1), pages 1-7, 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. Meng He & Yongmeng Wu & Rui Li & Yuting Wang & Cuibo Liu & Bin Zhang, 2023. "Aqueous pulsed electrochemistry promotes C−N bond formation via a one-pot cascade approach," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    2. Nannan Meng & Jiang Shao & Hongjiao Li & Yuting Wang & Xiaoli Fu & Cuibo Liu & Yifu Yu & Bin Zhang, 2022. "Electrosynthesis of formamide from methanol and ammonia under ambient conditions," Nature Communications, Nature, vol. 13(1), pages 1-8, December.
    3. Yan Liu & Jie Wei & Zhengwu Yang & Lirong Zheng & Jiankang Zhao & Zhimin Song & Yuhan Zhou & Jiajie Cheng & Junyang Meng & Zhigang Geng & Jie Zeng, 2024. "Efficient tandem electroreduction of nitrate into ammonia through coupling Cu single atoms with adjacent Co3O4," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    4. 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.
    5. Haozhou Yang & Na Guo & Shibo Xi & Yao Wu & Bingqing Yao & Qian He & Chun Zhang & Lei Wang, 2024. "Potential-driven structural distortion in cobalt phthalocyanine for electrocatalytic CO2/CO reduction towards methanol," Nature Communications, Nature, vol. 15(1), pages 1-14, December.
    6. Yilong Zhao & Yunxuan Ding & Wenlong Li & Chang Liu & Yingzheng Li & Ziqi Zhao & Yu Shan & Fei Li & Licheng Sun & Fusheng Li, 2023. "Efficient urea electrosynthesis from carbon dioxide and nitrate via alternating Cu–W bimetallic C–N coupling sites," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    7. Xinyi Ren & Jian Zhao & Xuning Li & Junming Shao & Binbin Pan & Aude Salamé & Etienne Boutin & Thomas Groizard & Shifu Wang & Jie Ding & Xiong Zhang & Wen-Yang Huang & Wen-Jing Zeng & Chengyu Liu & Ya, 2023. "In-situ spectroscopic probe of the intrinsic structure feature of single-atom center in electrochemical CO/CO2 reduction to methanol," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    8. Xianlong Li & Zhiliang Wang & Alireza Sasani & Ardeshir Baktash & Kai Wang & Haijiao Lu & Jiakang You & Peng Chen & Ping Chen & Yifan Bao & Shujun Zhang & Gang Liu & Lianzhou Wang, 2024. "Oxygen vacancy induced defect dipoles in BiVO4 for photoelectrocatalytic partial oxidation of methane," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
    9. Kui Fan & Wenfu Xie & Jinze Li & Yining Sun & Pengcheng Xu & Yang Tang & Zhenhua Li & Mingfei Shao, 2022. "Active hydrogen boosts electrochemical nitrate reduction to ammonia," Nature Communications, Nature, vol. 13(1), pages 1-13, December.
    10. Jiace Hao & Tongde Wang & Ruohan Yu & Jian Cai & Guohua Gao & Zechao Zhuang & Qi Kang & Shuanglong Lu & Zhenhui Liu & Jinsong Wu & Guangming Wu & Mingliang Du & Dingsheng Wang & Han Zhu, 2024. "Integrating few-atom layer metal on high-entropy alloys to catalyze nitrate reduction in tandem," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    11. Yizhou Dai & Huan Li & Chuanhao Wang & Weiqing Xue & Menglu Zhang & Donghao Zhao & Jing Xue & Jiawei Li & Laihao Luo & Chunxiao Liu & Xu Li & Peixin Cui & Qiu Jiang & Tingting Zheng & Songqi Gu & Yao , 2023. "Manipulating local coordination of copper single atom catalyst enables efficient CO2-to-CH4 conversion," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    12. Han Li & Leitao Xu & Shuowen Bo & Yujie Wang & Han Xu & Chen Chen & Ruping Miao & Dawei Chen & Kefan Zhang & Qinghua Liu & Jingjun Shen & Huaiyu Shao & Jianfeng Jia & Shuangyin Wang, 2024. "Ligand engineering towards electrocatalytic urea synthesis on a molecular catalyst," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    13. Wenjun Fan & Zhiyao Duan & Wei Liu & Rashid Mehmood & Jiating Qu & Yucheng Cao & Xiangyang Guo & Jun Zhong & Fuxiang Zhang, 2023. "Rational design of heterogenized molecular phthalocyanine hybrid single-atom electrocatalyst towards two-electron oxygen reduction," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    14. Yu Yang & Cheng Zhang & Chengyi Zhang & Yaohui Shi & Jun Li & Bernt Johannessen & Yongxiang Liang & Shuzhen Zhang & Qiang Song & Haowei Zhang & Jialei Huang & Jingwen Ke & Lei Zhang & Qingqing Song & , 2024. "Ligand-tuning copper in coordination polymers for efficient electrochemical C–C coupling," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    15. Ying Wang & Vinod K. Paidi & Weizhen Wang & Yong Wang & Guangri Jia & Tingyu Yan & Xiaoqiang Cui & Songhua Cai & Jingxiang Zhao & Kug-Seung Lee & Lawrence Yoon Suk Lee & Kwok-Yin Wong, 2024. "Spatial engineering of single-atom Fe adjacent to Cu-assisted nanozymes for biomimetic O2 activation," Nature Communications, Nature, vol. 15(1), pages 1-13, December.
    16. Sishuang Tang & Minghao Xie & Saerom Yu & Xun Zhan & Ruilin Wei & Maoyu Wang & Weixin Guan & Bowen Zhang & Yuyang Wang & Hua Zhou & Gengfeng Zheng & Yuanyue Liu & Jamie H. Warner & Guihua Yu, 2024. "General synthesis of high-entropy single-atom nanocages for electrosynthesis of ammonia from nitrate," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    17. Jiao Lan & Zengxi Wei & Ying-Rui Lu & DeChao Chen & Shuangliang Zhao & Ting-Shan Chan & Yongwen Tan, 2023. "Efficient electrosynthesis of formamide from carbon monoxide and nitrite on a Ru-dispersed Cu nanocluster catalyst," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    18. Philipp Keller & Michael A. Reiter & Patrick Kiefer & Thomas Gassler & Lucas Hemmerle & Philipp Christen & Elad Noor & Julia A. Vorholt, 2022. "Generation of an Escherichia coli strain growing on methanol via the ribulose monophosphate cycle," Nature Communications, Nature, vol. 13(1), pages 1-13, December.
    19. Ji Wei Sun & Xuefeng Wu & Peng Fei Liu & Jiacheng Chen & Yuanwei Liu & Zhen Xin Lou & Jia Yue Zhao & Hai Yang Yuan & Aiping Chen & Xue Lu Wang & Minghui Zhu & Sheng Dai & Hua Gui Yang, 2023. "Scalable synthesis of coordinatively unsaturated metal-nitrogen sites for large-scale CO2 electrolysis," Nature Communications, Nature, vol. 14(1), pages 1-13, December.
    20. Jun Bu & Siyu Chang & Jinjin Li & Sanyin Yang & Wenxiu Ma & Zhenpeng Liu & Siying An & Yanan Wang & Zhen Li & Jian Zhang, 2023. "Highly selective electrocatalytic alkynol semi-hydrogenation for continuous production of alkenols," Nature Communications, Nature, vol. 14(1), pages 1-9, 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_s41467-024-54204-2. 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.