Electrochemical reduction of nitrate to ammonia via direct eight-electron transfer using a copper–molecular solid catalyst

Chen, Gao‐Feng; Yuan, Yifei; Jiang, Haifeng; Ren, Shiyu; Ding, Liang‐Xin; Ma, Lu; Wu, Tianpin; Lü, Jun; Wang, Haihui

doi:10.1038/s41560-020-0654-1

Cited by 1,051 publications

(810 citation statements)

References 36 publications

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“…), similar yields of 14 NH4 + -14 N and 15 NH4 + -15 N were achieved. The quantitative results of 1 H NMR perfectly correspond to that of colorimetric methods using Nessler's reagent…”

supporting

confidence: 60%

“…13 However, a low yield rate and a low achievable selectivity at high current densities has plagued its future. 14 Among all the nitrogencontaining alternatives, nitrate (NO3 -) is undoubtedly the most promising. [15][16] The disintegration of NO3into the deoxygenated species only requires an energy of 204 kJ/mol, much lower than the cleavage energy of N≡N bond (941 kJ/mol).…”

Section: Introductionmentioning

confidence: 99%

“…[15][16] The disintegration of NO3into the deoxygenated species only requires an energy of 204 kJ/mol, much lower than the cleavage energy of N≡N bond (941 kJ/mol). [13][14] Meanwhile, higher reaction energy barrier for N2 reduction occurring at solid-gas-liquid interfaces is demanded compared to that of nitrate reduction reaction (NITRR) at solid-liquid interfaces. [15][16] In view of energy consumption, exploring the electrocatalytic NITRR makes perfect sense for low temperature NH3 synthesis.…”

Section: Introductionmentioning

confidence: 99%

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Alloying effect-induced electron polarization drives nitrate reduction to ammonia

Yin

Peng

Xiong

et al. 2020

Preprint

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Electrocatalytic conversion of nitrate (NO3-) to ammonia (NH3) holds significant potential in the control of nitrogen oxide (NOx) from stationary sources. However, previous studies on reaction intermediates remain unclear. Here we report that Pd/Cu2O hybrids with mesoporous hollow sphere structure show high selectivity (96.70%) and Faradaic efficiency (94.32%) for NH3 synthesis from NO3-. Detailed characterizations demonstrate that (1) Pd enables electrons transfer (Pd 3d → Cu 3d) and makes the polarization of Cu 3d orbitals by forming partial PdCu alloys, which makes Pd electron-deficiency but offers empty orbits to adsorb NO3-; (2) electron-rich Cu are more conducive to the occurrence of NO3- reduction. The mutual confirmation of online differential electrochemical mass spectrometry and density functional theory calculations demonstrates that PdCu alloys block the generation of *NOH intermediate and facilitate the formation of *N, finally leading to a higher catalytic performance.

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“…), similar yields of 14 NH4 + -14 N and 15 NH4 + -15 N were achieved. The quantitative results of 1 H NMR perfectly correspond to that of colorimetric methods using Nessler's reagent…”

supporting

confidence: 60%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

See 1 more Smart Citation

Alloying effect-induced electron polarization drives nitrate reduction to ammonia

Yin

Peng

Xiong

et al. 2020

Preprint

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“…The FE of PTCDA reached a maximum value of 85.9%, and the rate of NH 3 generation was 436 ± 85 μg/hr/cm 2 at −0.4 V versus RHE. 160 The outstanding performance of this catalyst can be attributed to two aspects. On the one hand, suppressed HER and enhanced H-N bonding, which originates from Cu electronic structure.…”

Section: Direct Reduction Of Nitrate To Ammoniamentioning

confidence: 99%

Rational design on photo(electro)catalysts for artificial nitrogen looping

Liu

Wang

et al. 2021

EcoMat

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Nitrogen, one of most important elements on the Earth, plays an essential role in shaping the modern society. The natural nitrogen looping, however, is insufficient to satisfy the high demand of the large-scale human activities. To achieve a more sustainable and efficient utilization of nitrogen, artificial nitrogen looping by photo(electro)catalytic processes has been considered as a feasible strategy. In this context, the rational design on the high-performance catalysts for nitrogen looping becomes increasingly important and urgent. On this basis, herein, we provide a timely review on the recent progress, achievements, and essential challenges for the artificial nitrogen looping process, mainly including photo(electro)catalytic transformations among dinitrogen, ammonia, gaseous nitrogen oxides, nitrate, and so on. Especially, the photo(electro)catalysts used in various reactions involved in nitrogen looping, including nitrogen reduction reaction, nitrogen oxidation reaction, ammonia oxidation reaction, ammonia decomposition reaction, etc., are systematically introduced. Finally, we hope that this review will help us deepen the understanding of nitrogen looping-related photo(electro)catalysts, and further pave a way toward the sustainable development on energy and environment. K E Y W O R D Senvironmental protection, nitrogen looping, photo(electro)catalysis, sustainable energy Mengying Li and Xiaoqing Liu contributed equally to this study.

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“…[ 1b ] Therefore, it is very urgent to search a clean and sustainable process for the production of ammonia. Many methods have been proposed for the purpose, such as, electroreduction of nitrate to ammonia, [ 6 ] electrochemical nitrogen reduction reaction (e‐NRR), [ 7 ] photocatalytic NRR, [ 8 ] plasma‐chemical NRR, [ 9 ] biochemical photocatalytic NRR, [ 10 ] and chemical looping NRR. [ 11 ]…”

Section: Introductionmentioning

confidence: 99%

Development of Electrocatalysts for Efficient Nitrogen Reduction Reaction under Ambient Condition

Liu

Chen

et al. 2020

Adv Funct Materials

165

120

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As one of the most important chemicals and an energy carrier, synthetic ammonia has been widely studied to meet the increasing demand. Among various strategies, electrochemical nitrogen reduction reaction (e‐NRR) is a promising way because of its green nature and easy set‐up on large‐scale. However, its practical application is extremely limited because of the very‐low production rate, which is strongly dependent on the electrocatalysts used. Therefore, searching novel efficient electrocatalysts for e‐NRR is essential to promote the technology. In this review, it highlights the insights on the mechanism for the NH3 electrochemical synthesis, recommend a reliable protocol for the ammonia detection, and systematically summarize the recent development on novel electrocatalysts, including noble metal‐based materials, single‐metal‐atom catalysts, non‐noble metal, and their compounds, and metal‐free materials, for efficient e‐NRR in both experimental and theoretical studies. Various strategies to improve the catalytic performance by increasing exposed active sites or tuning electronic structures, including surface control, defect engineering, and hybridization, are carefully discussed. Finally, perspectives and challenges are outlined. It can be expected that this review provides insightful guidance on the development of advanced catalytic systems to produce ammonia through N2 reduction.

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Electrochemical reduction of nitrate to ammonia via direct eight-electron transfer using a copper–molecular solid catalyst

Cited by 1,051 publications

References 36 publications

Alloying effect-induced electron polarization drives nitrate reduction to ammonia

Alloying effect-induced electron polarization drives nitrate reduction to ammonia

Rational design on photo(electro)catalysts for artificial nitrogen looping

Development of Electrocatalysts for Efficient Nitrogen Reduction Reaction under Ambient Condition

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