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Nitrogen Fixation by Ru Single-Atom Electrocatalytic Reduction
Open accessAbstract
Summary Nitrogen fixation under ambient conditions remains a significant challenge. Here, we report nitrogen fixation by Ru single-atom electrocatalytic reduction at room temperature and pressure. In contrast to Ru nanoparticles, single Ru sites supported on N-doped porous carbon greatly promoted electroreduction of aqueous N2 selectively to NH3, affording an NH3 formation rate of 3.665 m g N H 3 h − 1 m g Ru − 1 at −0.21 V versus the reversible hydrogen electrode. Importantly, the addition of ZrO2 was found to significantly suppress the competitive hydrogen evolution reaction. An NH3 faradic efficiency of about 21% was achieved at a low overpotential (0.17 V), surpassing many other reported catalysts. Experiments combined with density functional theory calculations showed that the Ru sites with oxygen vacancies were major active centers that permitted stabilization of *NNH, destabilization of *H, and enhanced N2 adsorption. We envision that optimization of ZrO2 loading could further facilitate electroreduction of N2 at both high NH3 synthesis rate and faradic efficiency.
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Montoya, J. H., Tsai, C., Vojvodic, A., & Nørskov, J. K. (2015) · ChemSusChem · doi:10.1002/cssc.201500322 · Cited by 1,384
Fan, L., Liu, P. F., Yan, X., Gu, L., Yang, Z. Z., Yang, H. G., Qiu, S., & Yao, X. (2016) · Nature Communications · doi:10.1038/ncomms10667 · Cited by 748
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Fang, S., Zhu, X., Liu, X., Gu, J., Liu, W., Wang, D., Zhang, W., Lin, Y., Lu, J., Wei, S., et al. (2020) · Nature Communications · doi:10.1038/s41467-020-14848-2 · Cited by 585
Recent Advances in MOF‐Derived Single Atom Catalysts for Electrochemical Applications
Song, Z., Zhang, L., Doyle‐Davis, K., Fu, X., Luo, J., & Sun, X. (2020) · Advanced Energy Materials · doi:10.1002/aenm.202001561 · Cited by 412
Electrocatalysis of Single-Atom Sites: Impacts of Atomic Coordination
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Wu, Y., Li, X., Wei, Y., Fu, Z., Wei, W., Wu, X., Zhu, Q., & Xu, Q. (2021) · Advanced Materials · doi:10.1002/adma.202006965 · Cited by 378
Metadata
- Authors
- Tao, H., Choi, C., Ding, L.-X., Jiang, Z., Han, Z., Jia, M., Fan, Q., Gao, Y., Wang, H., Robertson, A. W., Hong, S., Jung, Y., Liu, S., & Sun, Z.
- Venue
- Chem
- Publisher
- Elsevier BV
- Published
- 2019-01
- Volume
- 5
- Issue
- 1
- Pages
- 204-214
- ISSN
- 2451-9294 (ISSN-L)
- OpenAlex
- W2899933645
- Cited by
- 944
- References
- 2
- FWCI
- 26.28
- Type
- journal article
- Language
- en
- Open access
- bronze
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- Tao, H., Choi, C., Ding, L.-X., Jiang, Z., Han, Z., Jia, M., Fan, Q., Gao, Y., Wang, H., Robertson, A. W., Hong, S., Jung, Y., Liu, S., & Sun, Z. (2019). Nitrogen Fixation by Ru Single-Atom Electrocatalytic Reduction. Chem. https://doi.org/10.1016/j.chempr.2018.10.007
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