IDEAS home Printed from https://ideas.repec.org/a/nat/natcom/v15y2024i1d10.1038_s41467-024-53427-7.html
   My bibliography  Save this article

Integrating few-atom layer metal on high-entropy alloys to catalyze nitrate reduction in tandem

Author

Listed:
  • Jiace Hao

    (Jiangnan University)

  • Tongde Wang

    (Tongji University)

  • Ruohan Yu

    (Wuhan University of Technology)

  • Jian Cai

    (Jiangnan University)

  • Guohua Gao

    (Tongji University)

  • Zechao Zhuang

    (Tsinghua University
    Columbia University)

  • Qi Kang

    (Tongji University)

  • Shuanglong Lu

    (Jiangnan University)

  • Zhenhui Liu

    (Nanjing University of Aeronautics and Astronautics)

  • Jinsong Wu

    (Wuhan University of Technology)

  • Guangming Wu

    (Tongji University)

  • Mingliang Du

    (Jiangnan University)

  • Dingsheng Wang

    (Tsinghua University)

  • Han Zhu

    (Jiangnan University)

Abstract

While high-entropy alloy (HEA) catalysts seem to have the potential to break linear scaling relationships (LSRs) due to their structural complexity, the weighted averaging of properties among multiple principal components actually makes it challenging to diverge from the symmetry dependencies imposed by the LSRs. Herein, we develop a ‘surface entropy reduction’ method to induce the exsolution of a component with weak affinity for others, resulting in the formation of few-atom-layer metal (FL-M) on the surface of HEAs. These exsolved FL-M surpass the confines of the original configurational space of conventional HEAs, and collaborate with the HEA substrate, serving as geometrically separated active sites for multiple intermediates in a complex reaction. This FL-M-covered HEA shows an outstanding performance for electrocatalytic reduction of nitrate to ammonia (NH3) with a Faradaic efficiency of 92.7%, an NH3 yield rate of 2.45 mmol h–1 mgcat.–1, and high long-term stability (>200 h). Our work achieves the precise manipulation of atomic arrangement, thereby expanding both the chemical space occupied by known HEA catalysts and their potential application scenarios.

Suggested Citation

  • 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.
  • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-53427-7
    DOI: 10.1038/s41467-024-53427-7
    as

    Download full text from publisher

    File URL: https://www.nature.com/articles/s41467-024-53427-7
    File Function: Abstract
    Download Restriction: no

    File URL: https://libkey.io/10.1038/s41467-024-53427-7?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. Matthew W. Glasscott & Andrew D. Pendergast & Sondrica Goines & Anthony R. Bishop & Andy T. Hoang & Christophe Renault & Jeffrey E. Dick, 2019. "Electrosynthesis of high-entropy metallic glass nanoparticles for designer, multi-functional electrocatalysis," Nature Communications, Nature, vol. 10(1), pages 1-8, December.
    3. 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.
    4. Qingqing Ding & Yin Zhang & Xiao Chen & Xiaoqian Fu & Dengke Chen & Sijing Chen & Lin Gu & Fei Wei & Hongbin Bei & Yanfei Gao & Minru Wen & Jixue Li & Ze Zhang & Ting Zhu & Robert O. Ritchie & Qian Yu, 2019. "Tuning element distribution, structure and properties by composition in high-entropy alloys," Nature, Nature, vol. 574(7777), pages 223-227, October.
    5. Jiace Hao & Zechao Zhuang & Kecheng Cao & Guohua Gao & Chan Wang & Feili Lai & Shuanglong Lu & Piming Ma & Weifu Dong & Tianxi Liu & Mingliang Du & Han Zhu, 2022. "Unraveling the electronegativity-dominated intermediate adsorption on high-entropy alloy electrocatalysts," Nature Communications, Nature, vol. 13(1), pages 1-13, December.
    6. Chade Lv & Lixiang Zhong & Hengjie Liu & Zhiwei Fang & Chunshuang Yan & Mengxin Chen & Yi Kong & Carmen Lee & Daobin Liu & Shuzhou Li & Jiawei Liu & Li Song & Gang Chen & Qingyu Yan & Guihua Yu, 2021. "Selective electrocatalytic synthesis of urea with nitrate and carbon dioxide," Nature Sustainability, Nature, vol. 4(10), pages 868-876, 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. 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.
    2. 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.
    3. Yang Li & Shisheng Zheng & Hao Liu & Qi Xiong & Haocong Yi & Haibin Yang & Zongwei Mei & Qinghe Zhao & Zu-Wei Yin & Ming Huang & Yuan Lin & Weihong Lai & Shi-Xue Dou & Feng Pan & Shunning Li, 2024. "Sequential co-reduction of nitrate and carbon dioxide enables selective urea electrosynthesis," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    4. 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.
    5. 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.
    6. 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.
    7. Xinhong Chen & Yumeng Cheng & Bo Zhang & Jia Zhou & Sisi He, 2024. "Gradient-concentration RuCo electrocatalyst for efficient and stable electroreduction of nitrate into ammonia," Nature Communications, Nature, vol. 15(1), pages 1-13, December.
    8. Lin He & Menggang Li & Longyu Qiu & Shuo Geng & Yequn Liu & Fenyang Tian & Mingchuan Luo & Hu Liu & Yongsheng Yu & Weiwei Yang & Shaojun Guo, 2024. "Single-atom Mo-tailored high-entropy-alloy ultrathin nanosheets with intrinsic tensile strain enhance electrocatalysis," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    9. Jae Bok Seol & Won-Seok Ko & Seok Su Sohn & Min Young Na & Hye Jung Chang & Yoon-Uk Heo & Jung Gi Kim & Hyokyung Sung & Zhiming Li & Elena Pereloma & Hyoung Seop Kim, 2022. "Mechanically derived short-range order and its impact on the multi-principal-element alloys," Nature Communications, Nature, vol. 13(1), pages 1-13, December.
    10. 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.
    11. 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.
    12. 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.
    13. Ying Han & Hangman Chen & Yongwen Sun & Jian Liu & Shaolou Wei & Bijun Xie & Zhiyu Zhang & Yingxin Zhu & Meng Li & Judith Yang & Wen Chen & Penghui Cao & Yang Yang, 2024. "Ubiquitous short-range order in multi-principal element alloys," Nature Communications, Nature, vol. 15(1), pages 1-13, December.
    14. 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.
    15. Xiaoran Zhang & Xiaorong Zhu & Shuowen Bo & Chen Chen & Mengyi Qiu & Xiaoxiao Wei & Nihan He & Chao Xie & Wei Chen & Jianyun Zheng & Pinsong Chen & San Ping Jiang & Yafei Li & Qinghua Liu & Shuangyin , 2022. "Identifying and tailoring C–N coupling site for efficient urea synthesis over diatomic Fe–Ni catalyst," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    16. 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.
    17. Keun Su Kim & Martin Couillard & Ziqi Tang & Homin Shin & Daniel Poitras & Changjun Cheng & Olga Naboka & Dean Ruth & Mark Plunkett & Lixin Chen & Liliana Gaburici & Thomas Lacelle & Michel Nganbe & Y, 2024. "Continuous synthesis of high-entropy alloy nanoparticles by in-flight alloying of elemental metals," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    18. Qian Wu & Chencheng Dai & Fanxu Meng & Yan Jiao & Zhichuan J. Xu, 2024. "Potential and electric double-layer effect in electrocatalytic urea synthesis," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    19. Yunqing Kang & Ovidiu Cretu & Jun Kikkawa & Koji Kimoto & Hiroki Nara & Asep Sugih Nugraha & Hiroki Kawamoto & Miharu Eguchi & Ting Liao & Ziqi Sun & Toru Asahi & Yusuke Yamauchi, 2023. "Mesoporous multimetallic nanospheres with exposed highly entropic alloy sites," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    20. Bharath, G. & Karthikeyan, G. & Kumar, Anuj & Prakash, J. & Venkatasubbu, Devanand & Kumar Nadda, Ashok & Kumar Gupta, Vijai & Abu Haija, Mohammad & Banat, Fawzi, 2022. "Surface engineering of Au nanostructures for plasmon-enhanced electrochemical reduction of N2 and CO2 into urea in the visible-NIR region," Applied Energy, Elsevier, vol. 318(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:15:y:2024:i:1:d:10.1038_s41467-024-53427-7. 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.