Unveiling the Activity Origin of a Copper‐based Electrocatalyst for Selective Nitrate Reduction to Ammonia

Wang, Yuting; Zhou, Wei; Jia, Ranran; Yu, Yifu; Zhang, Bin

doi:10.1002/ange.201915992

Cited by 143 publications

(134 citation statements)

References 50 publications

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“…The direct reduction of nitrate to ammonia could provide a more promising strategy for ammonia industry in the future due to higher solubility and activity of nitrate in aqueous solution than that of nitrogen gas. 165 etc. ), and so on.…”

Section: Direct Reduction Of Nitrate To Ammoniamentioning

confidence: 98%

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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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Section: Direct Reduction Of Nitrate To Ammoniamentioning

confidence: 98%

“…In this field, the main catalysts include metals (eg, Al, 159 Cu, 160 Cu‐Ni, 161 etc. ), metal compounds (Co 3 O 4 , 162,163 ), metal composites (eg, Ni/TiO 2 , 164 Cu/Cu 2 O, 165 etc. ), and so on.…”

Section: Conversion Between Ammonia and Nitric Acid/nitratementioning

confidence: 99%

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

Liu

Wang

et al. 2021

EcoMat

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“…Therefore, the (111) surface of Cu2O, as the most stable surface, was chosen to be reconstructed as the slab model, featuring a [3×3] supercell and three Cu2O layers. 13 The slab model of PdCu was constructed by loading a triatomic cluster of Pd on the Cu2O…”

Section: Dft Calculation Detailmentioning

confidence: 99%

“…[10][11][12] As an alternative, electrocatalytic N2 reduction at ambient conditions with proton derived from decomposition of H2O has recently attracted research interest. 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.…”

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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Theoretical Insights into the Mechanism of Selective Nitrate‐to‐Ammonia Electroreduction on Single‐Atom Catalysts

Niu

Zhang

Wang

et al. 2020

Adv Funct Materials

343

287

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Selective nitrate‐to‐ammonia electrochemical conversion is an efficient pathway to solve the pollution of nitrate and an attractive strategy for low‐temperature ammonia synthesis. However, current studies for nitrate electroreduction (NO3RR) mainly focus on metal‐based catalysts, which remains challenging because of the poor understanding of the catalytic mechanism. Herein, taking single transition metal atom supported on graphitic carbon nitrides (g‐CN) as an example, the NO3RR feasibility of single‐atom catalysts (SACs) is first demonstrated by using density functional theory calculations. The results reveal that highly efficient NO3RR toward NH3 can be achieved on Ti/g‐CN and Zr/g‐CN with low limiting potentials of −0.39 and −0.41 V, respectively. Furthermore, the considerable energy barriers are observed during the formation of byproducts NO2, NO, N2O, and N2 on Ti/g‐CN and Zr/g‐CN, guaranteeing their high selectivity. This work provides a new route for the application of SACs and paves the way to the development of NO3RR.

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Unveiling the Activity Origin of a Copper‐based Electrocatalyst for Selective Nitrate Reduction to Ammonia

Cited by 143 publications

References 50 publications

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

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

Alloying effect-induced electron polarization drives nitrate reduction to ammonia

Theoretical Insights into the Mechanism of Selective Nitrate‐to‐Ammonia Electroreduction on Single‐Atom Catalysts

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