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Interfacial engineering of metallic rhodium by thiol modification approach for ambient electrosynthesis of ammonia

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Abstract

Here we report a vapor-phase reaction approach to fabricate rhodium(I)-dodecanethiol complex coated on carbon fiber cloth (Rh(I)-SC12H25/CFC), followed by low-temperature pyrolysis to achieve dodecanethiol modified Rh (Rh@SC12H25/CFC) for electrocatalytic nitrogen reduction reaction (NRR). The results demonstrate that after pyrolysis for 0.5 h at 150 °C, the obtained Rh@SC12H25/CFC-0.5 exhibits excellent NRR activity with an NH3 yield rate of 121.2 ± 6.6 µg·h−1·cm−2 (or 137.7 ± 7.5 µg·h−1·mgRh−1) and a faradaic efficiency (FE) of 51.6 ± 3.8% at −0.2 V (vs. RHE) in 0.1 M Na2SO4. The theoretical calculations unveil that the adsorption of dodecanethiol on the hollow sites of Rh(111) plane is thermodynamically favorable, effectively regulating the electronic structure and surface wettability of metallic Rh. Importantly, the dodecanethiol modification on Rh(111) obviously decreases the surface H⋆ coverage, thus inhibiting the competitive hydrogen evolution reaction and concurrently reducing the electrocatalytic NRR energy barrier.

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Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (No. 51872292), the young project of Anhui Provincial Natural Science Foundation (No. 1908085QB83).

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Authors and Affiliations

  1. Laboratory of Materials Physics, Centre for Environmental and Energy Nanomaterials, Anhui Key Laboratory of Nanomaterials and Nanotechnology, CAS Center for Excellence in Nanoscience, Institute of Solid State Physics, HFIPS, Chinese Academy of Sciences, Hefei, 230031, China

    Meng Jin, Xinyuan Zhang, Xian Zhang, Hongjian Zhou, Yunxia Zhang, Guozhong Wang & Haimin Zhang

  2. University of Science and Technology of China, Hefei, 230026, China

    Meng Jin, Xinyuan Zhang, Xian Zhang, Hongjian Zhou, Yunxia Zhang, Guozhong Wang & Haimin Zhang

  3. School of Science, Huzhou University, Huzhou, 313000, China

    Miaomiao Han

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Jin, M., Zhang, X., Zhang, X. et al. Interfacial engineering of metallic rhodium by thiol modification approach for ambient electrosynthesis of ammonia. Nano Res. 15, 8826–8835 (2022). https://doi.org/10.1007/s12274-022-4585-y

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