IDEAS home Printed from https://ideas.repec.org/a/nat/natcom/v16y2025i1d10.1038_s41467-025-55885-z.html
   My bibliography  Save this article

Photocatalytic asymmetric C-C coupling for CO2 reduction on dynamically reconstructed Ruδ+-O/Ru0-O sites

Author

Listed:
  • Hongguang Zhang
  • Asfaw Yohannes

    (2500 University Drive NW)

  • Heng Zhao
  • Zheng Li
  • Yejun Xiao

    (Chinese Academy of Sciences)

  • Xi Cheng
  • Hui Wang
  • Zhangkang Li
  • Samira Siahrostami

    (8888 University Drive)

  • Md Golam Kibria
  • Jinguang Hu

Abstract

Solar-driven CO2 reduction to value-added C2 chemicals is thermodynamically challenging due to multiple complicated steps. The design of active sites and structures for photocatalysts is necessary to improve solar energy efficiency. In this work, atomically dispersed Ru-O sites in RuxIn2-xO3 are constructed by interior lattice anchoring of Ru. This results in the dynamic reconstruction of Ruδ+-O/Ru0-O sites upon photoexcitation, which facilitates the CO2 activation, *CO intermediates adsorption, and C-C coupling as demonstrated by varied in situ techniques. A SiO2 core in RuxIn2-xO3/SiO2 construction further enhances the solar energy utilization and individual RuxIn2-xO3 nanocrystals dispersion for photocatalytic CO2 reduction reaction. It results in the maximum ethanol production rate up to 31.6 μmol/g/h with over 90% selectivity. DFT simulation reveals that the C2 dimer formation primarily underwent an asymmetric *CO-*CHO coupling route via a low-energy precedence ladder of *CHO. This work provides an insightful understanding of active sites with dynamic reconstruction towards asymmetric C-C coupling for CO2RR at the atomic scale.

Suggested Citation

  • Hongguang Zhang & Asfaw Yohannes & Heng Zhao & Zheng Li & Yejun Xiao & Xi Cheng & Hui Wang & Zhangkang Li & Samira Siahrostami & Md Golam Kibria & Jinguang Hu, 2025. "Photocatalytic asymmetric C-C coupling for CO2 reduction on dynamically reconstructed Ruδ+-O/Ru0-O sites," Nature Communications, Nature, vol. 16(1), pages 1-14, December.
    • Handle: RePEc:nat:natcom:v:16:y:2025:i:1:d:10.1038_s41467-025-55885-z
    DOI: 10.1038/s41467-025-55885-z
    as

    Download full text from publisher

    File URL: https://www.nature.com/articles/s41467-025-55885-z
    File Function: Abstract
    Download Restriction: no
    File URL: https://libkey.io/10.1038/s41467-025-55885-z?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. Xianyu Deng & Jianjun Zhang & Kezhen Qi & Guijie Liang & Feiyan Xu & Jiaguo Yu, 2024. "Ultrafast electron transfer at the In2O3/Nb2O5 S-scheme interface for CO2 photoreduction," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    2. Yixuan Wang & Yang Liu & Lingling Wang & Silambarasan Perumal & Hongdan Wang & Hyun Ko & Chung-Li Dong & Panpan Zhang & Shuaijun Wang & Ta Thi Thuy Nga & Young Dok Kim & Yujing Ji & Shufang Zhao & Ji-, 2024. "Coupling photocatalytic CO2 reduction and CH3OH oxidation for selective dimethoxymethane production," Nature Communications, Nature, vol. 15(1), pages 1-15, December.
    3. Xiaoxia Chang & Sudarshan Vijay & Yaran Zhao & Nicholas J. Oliveira & Karen Chan & Bingjun Xu, 2022. "Understanding the complementarities of surface-enhanced infrared and Raman spectroscopies in CO adsorption and electrochemical reduction," Nature Communications, Nature, vol. 13(1), pages 1-12, December.
    4. Tingjiang Yan & Na Li & Linlin Wang & Weiguang Ran & Paul N. Duchesne & Lili Wan & Nhat Truong Nguyen & Lu Wang & Meikun Xia & Geoffrey A. Ozin, 2020. "Bismuth atom tailoring of indium oxide surface frustrated Lewis pairs boosts heterogeneous CO2 photocatalytic hydrogenation," Nature Communications, Nature, vol. 11(1), pages 1-10, December.
    5. Zheng Chen & Zhangyun Liu & Xin Xu, 2023. "Dynamic evolution of the active center driven by hemilabile coordination in Cu/CeO2 single-atom catalyst," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    6. Sheng-Chih Lin & Chun-Chih Chang & Shih-Yun Chiu & Hsiao-Tien Pai & Tzu-Yu Liao & Chia-Shuo Hsu & Wei-Hung Chiang & Ming-Kang Tsai & Hao Ming Chen, 2020. "Operando time-resolved X-ray absorption spectroscopy reveals the chemical nature enabling highly selective CO2 reduction," Nature Communications, Nature, vol. 11(1), pages 1-12, December.
    7. Joseph V. Ryan & Alan D. Berry & Michele L. Anderson & Jeffrey W. Long & Rhonda M. Stroud & Veronica M. Cepak & Valerie M. Browning & Debra R. Rolison & Celia I. Merzbacher, 2000. "Electronic connection to the interior of a mesoporous insulator with nanowires of crystalline RuO2," Nature, Nature, vol. 406(6792), pages 169-172, July.
    8. Siqi Zhao & Oliver Christensen & Zhaozong Sun & Hongqing Liang & Alexander Bagger & Kristian Torbensen & Pegah Nazari & Jeppe Vang Lauritsen & Steen Uttrup Pedersen & Jan Rossmeisl & Kim Daasbjerg, 2023. "Steering carbon dioxide reduction toward C–C coupling using copper electrodes modified with porous molecular films," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    9. Shenghua Wang & Dake Zhang & Wu Wang & Jun Zhong & Kai Feng & Zhiyi Wu & Boyu Du & Jiaqing He & Zhengwen Li & Le He & Wei Sun & Deren Yang & Geoffrey A. Ozin, 2022. "Grave-to-cradle upcycling of Ni from electroplating wastewater to photothermal CO2 catalysis," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
    10. Ruotian Chen & Zefeng Ren & Yu Liang & Guanhua Zhang & Thomas Dittrich & Runze Liu & Yang Liu & Yue Zhao & Shan Pang & Hongyu An & Chenwei Ni & Panwang Zhou & Keli Han & Fengtao Fan & Can Li, 2022. "Spatiotemporal imaging of charge transfer in photocatalyst particles," Nature, Nature, vol. 610(7931), pages 296-301, October.
    11. Jian Jin & Joshua Wicks & Qiuhong Min & Jun Li & Yongfeng Hu & Jingyuan Ma & Yu Wang & Zheng Jiang & Yi Xu & Ruihu Lu & Gangzheng Si & Panagiotis Papangelakis & Mohsen Shakouri & Qunfeng Xiao & Pengfe, 2023. "Constrained C2 adsorbate orientation enables CO-to-acetate electroreduction," Nature, Nature, vol. 617(7962), pages 724-729, May.
    12. Yaguang Li & Jianchao Hao & Hui Song & Fengyu Zhang & Xianhua Bai & Xianguang Meng & Hongyuan Zhang & Shufang Wang & Yong Hu & Jinhua Ye, 2019. "Selective light absorber-assisted single nickel atom catalysts for ambient sunlight-driven CO2 methanation," Nature Communications, Nature, vol. 10(1), pages 1-9, December.
    13. Yuvraj Y. Birdja & Elena Pérez-Gallent & Marta C. Figueiredo & Adrien J. Göttle & Federico Calle-Vallejo & Marc T. M. Koper, 2019. "Advances and challenges in understanding the electrocatalytic conversion of carbon dioxide to fuels," Nature Energy, Nature, vol. 4(9), pages 732-745, September.
    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. Yufei Cao & Zhu Chen & Peihao Li & Adnan Ozden & Pengfei Ou & Weiyan Ni & Jehad Abed & Erfan Shirzadi & Jinqiang Zhang & David Sinton & Jun Ge & Edward H. Sargent, 2023. "Surface hydroxide promotes CO2 electrolysis to ethylene in acidic conditions," Nature Communications, Nature, vol. 14(1), pages 1-8, December.
    2. Xiaoyang He & Li Lin & Xiangying Li & Minzhi Zhu & Qinghong Zhang & Shunji Xie & Bingbao Mei & Fanfei Sun & Zheng Jiang & Jun Cheng & Ye Wang, 2024. "Roles of copper(I) in water-promoted CO2 electrolysis to multi-carbon compounds," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    3. Zhiwen Jiang & Carine Clavaguéra & Changjiang Hu & Sergey A. Denisov & Shuning Shen & Feng Hu & Jun Ma & Mehran Mostafavi, 2023. "Direct time-resolved observation of surface-bound carbon dioxide radical anions on metallic nanocatalysts," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    4. Yunjie Zou & Chengliang Mao & Mingkai Xu & Chao Xing & Ruizhao Wang & Geoffrey A. Ozin & Lan Ling, 2024. "Surface frustrated Lewis pairs in titanium nitride enable gas phase heterogeneous CO2 photocatalysis," Nature Communications, Nature, vol. 15(1), pages 1-13, December.
    5. Shifu Wang & Fuhua Li & Jian Zhao & Yaqiong Zeng & Yifan Li & Zih-Yi Lin & Tsung-Ju Lee & Shuhui Liu & Xinyi Ren & Weijue Wang & Yusen Chen & Sung-Fu Hung & Ying-Rui Lu & Yi Cui & Xiaofeng Yang & Xuni, 2024. "Manipulating C-C coupling pathway in electrochemical CO2 reduction for selective ethylene and ethanol production over single-atom alloy catalyst," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    6. Philipp Grosse & Aram Yoon & Clara Rettenmaier & Antonia Herzog & See Wee Chee & Beatriz Roldan Cuenya, 2021. "Dynamic transformation of cubic copper catalysts during CO2 electroreduction and its impact on catalytic selectivity," Nature Communications, Nature, vol. 12(1), pages 1-11, December.
    7. Junyuan Duan & Tianyang Liu & Yinghe Zhao & Ruoou Yang & Yang Zhao & Wenbin Wang & Youwen Liu & Huiqiao Li & Yafei Li & Tianyou Zhai, 2022. "Active and conductive layer stacked superlattices for highly selective CO2 electroreduction," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
    8. Cheng Du & Joel P. Mills & Asfaw G. Yohannes & Wei Wei & Lei Wang & Siyan Lu & Jian-Xiang Lian & Maoyu Wang & Tao Guo & Xiyang Wang & Hua Zhou & Cheng-Jun Sun & John Z. Wen & Brian Kendall & Martin Co, 2023. "Cascade electrocatalysis via AgCu single-atom alloy and Ag nanoparticles in CO2 electroreduction toward multicarbon products," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    9. Sung-Fu Hung & Aoni Xu & Xue Wang & Fengwang Li & Shao-Hui Hsu & Yuhang Li & Joshua Wicks & Eduardo González Cervantes & Armin Sedighian Rasouli & Yuguang C. Li & Mingchuan Luo & Dae-Hyun Nam & Ning W, 2022. "A metal-supported single-atom catalytic site enables carbon dioxide hydrogenation," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    10. Peng, Wanxi & Chuong Nguyen, Thi Hong & Nguyen, Dang Le Tri & Wang, Ting & Van Thi Tran, Thi & Le, Trung Hieu & Le, Hai Khoa & Grace, Andrews Nirmala & Singh, Pardeep & Raizadaa, Pankaj & Nguyen Dinh,, 2021. "A roadmap towards the development of superior photocatalysts for solar- driven CO2-to-fuels production," Renewable and Sustainable Energy Reviews, Elsevier, vol. 148(C).
    11. Khandelwal, Akshat & Maarisetty, Dileep & Baral, Saroj Sundar, 2022. "Fundamentals and application of single-atom photocatalyst in sustainable energy and environmental applications," Renewable and Sustainable Energy Reviews, Elsevier, vol. 167(C).
    12. Kaili Yao & Jun Li & Adnan Ozden & Haibin Wang & Ning Sun & Pengyu Liu & Wen Zhong & Wei Zhou & Jieshu Zhou & Xi Wang & Hanqi Liu & Yongchang Liu & Songhua Chen & Yongfeng Hu & Ziyun Wang & David Sint, 2024. "In situ copper faceting enables efficient CO2/CO electrolysis," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    13. Pengtang Wang & Hao Yang & Cheng Tang & Yu Wu & Yao Zheng & Tao Cheng & Kenneth Davey & Xiaoqing Huang & Shi-Zhang Qiao, 2022. "Boosting electrocatalytic CO2–to–ethanol production via asymmetric C–C coupling," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
    14. Zhengwei Yang & Zhen-Yu Wu & Zhexing Lin & Tianji Liu & Liping Ding & Wenbo Zhai & Zipeng Chen & Yi Jiang & Jinlei Li & Siyun Ren & Zhenhui Lin & Wangxi Liu & Jianyong Feng & Xing Zhang & Wei Li & Yi , 2024. "Optically selective catalyst design with minimized thermal emission for facilitating photothermal catalysis," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    15. Jiaqi Feng & Libing Zhang & Shoujie Liu & Liang Xu & Xiaodong Ma & Xingxing Tan & Limin Wu & Qingli Qian & Tianbin Wu & Jianling Zhang & Xiaofu Sun & Buxing Han, 2023. "Modulating adsorbed hydrogen drives electrochemical CO2-to-C2 products," Nature Communications, Nature, vol. 14(1), pages 1-11, December.
    16. Qitao Chen & Baodong Mao & Yanhong Liu & Yunjie Zhou & Hui Huang & Song Wang & Longhua Li & Wei-Cheng Yan & Weidong Shi & Zhenhui Kang, 2024. "Designing 2D carbon dot nanoreactors for alcohol oxidation coupled with hydrogen evolution," Nature Communications, Nature, vol. 15(1), pages 1-14, December.
    17. Subrato Acharjya & Jiacheng Chen & Minghui Zhu & Chong Peng, 2021. "Elucidating the reactivity and nature of active sites for tin phthalocyanine during CO2 reduction," Greenhouse Gases: Science and Technology, Blackwell Publishing, vol. 11(6), pages 1191-1197, December.
    18. Jiajie Hou & Bingjun Xu & Qi Lu, 2024. "Influence of electric double layer rigidity on CO adsorption and electroreduction rate," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    19. Xinyang Gao & Yongjun Jiang & Jiyuan Liu & Guoshuai Shi & Chunlei Yang & Qinshang Xu & Yuanqing Yun & Yuluo Shen & Mingwei Chang & Chenyuan Zhu & Tingyu Lu & Yin Wang & Guanchen Du & Shuzhou Li & Shen, 2024. "Intermediate-regulated dynamic restructuring at Ag-Cu biphasic interface enables selective CO2 electroreduction to C2+ fuels," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    20. Hongnan Jia & Na Yao & Yiming Jin & Liqing Wu & Juan Zhu & Wei Luo, 2024. "Stabilizing atomic Ru species in conjugated sp2 carbon-linked covalent organic framework for acidic water oxidation," Nature Communications, Nature, vol. 15(1), pages 1-13, 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:16:y:2025:i:1:d:10.1038_s41467-025-55885-z. 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.