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Volcano-type relationship between oxidation states and catalytic activity of single-atom catalysts towards hydrogen evolution

Author

Listed:
  • Dong Cao

    (Beijing University of Chemical Technology)

  • Haoxiang Xu

    (Beijing University of Chemical Technology)

  • Hongliang Li

    (University of Science and Technology of China)

  • Chen Feng

    (University of Science and Technology of China)

  • Jie Zeng

    (University of Science and Technology of China)

  • Daojian Cheng

    (Beijing University of Chemical Technology)

Abstract

To date, the effect of oxidation state on activity remains controversial in whether higher or lower oxidation states benefit the enhancement of catalytic activity. Herein, we discover a volcanic relationship between oxidation state and hydrogen evolution reaction activity based on Os single-atom catalysts. Firstly, a series of Os SACs with oxidation states ranging from + 0.9 to + 2.9 are synthesized via modifying the coordination environments, including Os-N3S1, Os-N4, Os-S6, Os-C3, and Os-C4S2. A volcano-type relation between oxidation states and hydrogen evolution activity emerge with a summit at a moderate experimental oxidation state of + 1.3 (Os-N3S1). Mechanism studies illustrate that with increasing oxidation states, the adsorption of H atoms on Os is strengthened due to increased energy level and decreased occupancy of anti-bonding states of Os-H bond until the anti-bonding states become empty. Further increasing the oxidation states weakens hydrogen adsorption because of the decreased occupancy of Os-H bonding states. In this work, we emphasize the essential role of oxidation state in manipulating activity, which offers insightful guidance for the rational design of single-atom catalysts.

Suggested Citation

  • Dong Cao & Haoxiang Xu & Hongliang Li & Chen Feng & Jie Zeng & Daojian Cheng, 2022. "Volcano-type relationship between oxidation states and catalytic activity of single-atom catalysts towards hydrogen evolution," Nature Communications, Nature, vol. 13(1), pages 1-11, December.
    • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-33589-y
    DOI: 10.1038/s41467-022-33589-y
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    as
    1. Lei Zhang & Rutong Si & Hanshuo Liu & Ning Chen & Qi Wang & Keegan Adair & Zhiqiang Wang & Jiatang Chen & Zhongxin Song & Junjie Li & Mohammad Norouzi Banis & Ruying Li & Tsun-Kong Sham & Meng Gu & Li, 2019. "Author Correction: Atomic layer deposited Pt-Ru dual-metal dimers and identifying their active sites for hydrogen evolution reaction," Nature Communications, Nature, vol. 10(1), pages 1-1, December.
    2. Hongzhou Yang & Lu Shang & Qinghua Zhang & Run Shi & Geoffrey I. N. Waterhouse & Lin Gu & Tierui Zhang, 2019. "A universal ligand mediated method for large scale synthesis of transition metal single atom catalysts," Nature Communications, Nature, vol. 10(1), pages 1-9, December.
    3. Kang Jiang & Min Luo & Zhixiao Liu & Ming Peng & Dechao Chen & Ying-Rui Lu & Ting-Shan Chan & Frank M. F. Groot & Yongwen Tan, 2021. "Rational strain engineering of single-atom ruthenium on nanoporous MoS2 for highly efficient hydrogen evolution," Nature Communications, Nature, vol. 12(1), pages 1-10, December.
    4. Yi Shi & Zhi-Rui Ma & Yi-Ying Xiao & Yun-Chao Yin & Wen-Mao Huang & Zhi-Chao Huang & Yun-Zhe Zheng & Fang-Ya Mu & Rong Huang & Guo-Yue Shi & Yi-Yang Sun & Xing-Hua Xia & Wei Chen, 2021. "Electronic metal–support interaction modulates single-atom platinum catalysis for hydrogen evolution reaction," Nature Communications, Nature, vol. 12(1), pages 1-11, December.
    5. Haihong Bao & Yuan Qiu & Xianyun Peng & Jia-ao Wang & Yuying Mi & Shunzheng Zhao & Xijun Liu & Yifan Liu & Rui Cao & Longchao Zhuo & Junqiang Ren & Jiaqiang Sun & Jun Luo & Xuping Sun, 2021. "Isolated copper single sites for high-performance electroreduction of carbon monoxide to multicarbon products," Nature Communications, Nature, vol. 12(1), pages 1-9, December.
    6. Lei Zhang & Rutong Si & Hanshuo Liu & Ning Chen & Qi Wang & Keegan Adair & Zhiqiang Wang & Jiatang Chen & Zhongxin Song & Junjie Li & Mohammad Norouzi Banis & Ruying Li & Tsun-Kong Sham & Meng Gu & Li, 2019. "Atomic layer deposited Pt-Ru dual-metal dimers and identifying their active sites for hydrogen evolution reaction," Nature Communications, Nature, vol. 10(1), pages 1-11, December.
    7. Ruijie Gao & Jian Wang & Zhen-Feng Huang & Rongrong Zhang & Wei Wang & Lun Pan & Junfeng Zhang & Weikang Zhu & Xiangwen Zhang & Chengxiang Shi & Jongwoo Lim & Ji-Jun Zou, 2021. "Pt/Fe2O3 with Pt–Fe pair sites as a catalyst for oxygen reduction with ultralow Pt loading," Nature Energy, Nature, vol. 6(6), pages 614-623, June.
    8. Yuan Pan & Yinjuan Chen & Konglin Wu & Zheng Chen & Shoujie Liu & Xing Cao & Weng-Chon Cheong & Tao Meng & Jun Luo & Lirong Zheng & Chenguang Liu & Dingsheng Wang & Qing Peng & Jun Li & Chen Chen, 2019. "Regulating the coordination structure of single-atom Fe-NxCy catalytic sites for benzene oxidation," Nature Communications, Nature, vol. 10(1), pages 1-11, December.
    9. Xijun Liu & Jia He & Shunzheng Zhao & Yunpeng Liu & Zhe Zhao & Jun Luo & Guangzhi Hu & Xiaoming Sun & Yi Ding, 2018. "Self-powered H2 production with bifunctional hydrazine as sole consumable," Nature Communications, Nature, vol. 9(1), pages 1-10, December.
    10. Yujing Ren & Yan Tang & Leilei Zhang & Xiaoyan Liu & Lin Li & Shu Miao & Dang Sheng Su & Aiqin Wang & Jun Li & Tao Zhang, 2019. "Unraveling the coordination structure-performance relationship in Pt1/Fe2O3 single-atom catalyst," Nature Communications, Nature, vol. 10(1), pages 1-9, December.
    11. Haifeng Qi & Ji Yang & Fei Liu & LeiLei Zhang & Jingyi Yang & Xiaoyan Liu & Lin Li & Yang Su & Yuefeng Liu & Rui Hao & Aiqin Wang & Tao Zhang, 2021. "Highly selective and robust single-atom catalyst Ru1/NC for reductive amination of aldehydes/ketones," Nature Communications, Nature, vol. 12(1), pages 1-11, December.
    12. Zhirong Zhang & Chen Feng & Chunxiao Liu & Ming Zuo & Lang Qin & Xupeng Yan & Yulin Xing & Hongliang Li & Rui Si & Shiming Zhou & Jie Zeng, 2020. "Electrochemical deposition as a universal route for fabricating single-atom catalysts," Nature Communications, Nature, vol. 11(1), pages 1-8, December.
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    1. 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.
    2. Sheng Qian & Feng Xu & Yu Fan & Ningyan Cheng & Huaiguo Xue & Ye Yuan & Romain Gautier & Tengfei Jiang & Jingqi Tian, 2024. "Tailoring coordination environments of single-atom electrocatalysts for hydrogen evolution by topological heteroatom transfer," Nature Communications, Nature, vol. 15(1), pages 1-11, December.

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