The DOI matches its Crossref record; 52 of the 52 references it cites were found in a registry or an index.
Electrocatalytic Hydrogenation Boosts Reduction of Nitrate to Ammonia over Single-Atom Cu with Cu(I)-N3C1 Sites
Abstract
The conversion of nitrate to ammonia can serve two important functions: mitigating nitrate pollution and offering a low energy intensity pathway for ammonia synthesis. Conventional ammonia synthesis from electrocatalytic nitrate reduction reactions (NO 3 RR) is often impeded by incomplete nitrate conversion, sluggish kinetics, and the competition of hydrogen evolution reactions. Herein, atomic Cu sites anchored on micro-/mesoporous nitrogen-doped carbon (Cu MNC) with fine-tuned hydrophilicity, micro-/mesoporous channels, and abundant Cu(I) sites were synthesized for selective nitrate reduction to ammonia, achieving ambient temperature and pressure hydrogenation of nitrate. Laboratory experiments demonstrated that the catalyst has an ammonia yield rate per active site of 5466 mmol g Cu –1 h –1 and transformed 94.8% nitrate in wastewater containing 100 mg-N L –1 to near drinking water standard (MCL of 5 mg-N L –1 ) at −0.64 V vs RHE. Extended X-ray absorption fine structure (EXAFS) and theoretical calculations showed that the coordination environment of Cu(I) sites (Cu(I)-N 3 C 1 ) localizes the charge around the central Cu atoms and adsorbs *NO 3 and *H onto neighboring Cu and C sites with balanced adsorption energy. The Cu(I)-N 3 C 1 moieties reduce the activation energy of rate-limiting steps (*HNO 3 → *NO 2, *NH 2 → *NH 3 ) compared with conventional Cu(II)-N 4 and lead to a thermodynamically favorable process to NH 3 . The as-prepared electrocatalytic cell can run continuously for 84 h (14 cycles) and produce 21.7 mg NH 3 with only 5.64 × 10 –3 kWh energy consumption, suitable for decentralized nitrate removal and ammonia synthesis from nitrate-containing wastewater.
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Cites
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Electrocatalytic Nitrate Reduction for Sustainable Ammonia Production
van Langevelde, P. H., Katsounaros, I., & Koper, M. T. M. (2021) · Joule · doi:10.1016/j.joule.2020.12.025 · Cited by 1,378
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Efficient Ammonia Electrosynthesis from Nitrate on Strained Ruthenium Nanoclusters
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Cited by
Pulsed Nitrate-to-Ammonia Electroreduction Facilitated by Tandem Catalysis of Nitrite Intermediates
Li, P., Li, R., Liu, Y., Xie, M., Jin, Z., & Yu, G. (2023) · Journal of the American Chemical Society · doi:10.1021/jacs.3c00334 · Cited by 466
Recent Advances in Electrocatalysts for Efficient Nitrate Reduction to Ammonia
Liu, D., Qiao, L., Peng, S., Bai, H., Liu, C., Ip, W. F., Lo, K. H., Liu, H., Ng, K. W., Wang, S., et al. (2023) · Advanced Functional Materials · doi:10.1002/adfm.202303480 · Cited by 336
Advances in iron-based electrocatalysts for nitrate reduction
Yuan, S., Xue, Y., Ma, R., Ma, Q., Chen, Y., & Fan, J. (2023) · Science of The Total Environment · doi:10.1016/j.scitotenv.2023.161444 · Cited by 117
Self-citationPhu, T. K. C., Pham, T. N., Nguyen, A.-G., Tran, T. N., Tran, T. M.-A., Le, N. N., Nguyen, P. L., & Phung, T. V. B. (2025) · iScience · doi:10.1016/j.isci.2025.112729 · Cited by 16
Metadata
- Authors
- Xue, Y., Yu, Q., Ma, Q., Chen, Y., Zhang, C., Teng, W., Fan, J., & Zhang, W.-X.
- Venue
- Environmental Science & Technology
- Publisher
- American Chemical Society (ACS)
- Published
- 2022-09-29
- Volume
- 56
- Issue
- 20
- Pages
- 14797-14807
- ISSN
- 0013-936X (ISSN-L)
- 1520-5851
- OpenAlex
- W4297973771
- Cited by
- 268
- References
- 52
- FWCI
- 9.61
- Type
- journal article
- Language
- en
- Open access
- closed
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- Xue, Y., Yu, Q., Ma, Q., Chen, Y., Zhang, C., Teng, W., Fan, J., & Zhang, W.-X. (2022). Electrocatalytic Hydrogenation Boosts Reduction of Nitrate to Ammonia over Single-Atom Cu with Cu(I)-N3C1 Sites. Environmental Science & Technology. https://doi.org/10.1021/acs.est.2c04456
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