Conjugated Coordination Polymer as a New Platform for Efficient and Selective Electroreduction of Nitrate into Ammonia

Electroreduction of nitrate into ammonia (NRA) provides a sustainable route to convert the widespread nitrate pollutants into high‐value‐added products under ambient conditions, which unfortunately suffers from unsatisfactory selectivity due to the competitive hydrogen evolution reaction (HER). Prev...

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Vydáno v:Advanced materials (Weinheim) Ročník 35; číslo 10; s. e2209855 - n/a
Hlavní autoři: Zhang, Yizhe, Zheng, Hui, Zhou, Kangjie, Ye, Jinyu, Chu, Kaibin, Zhou, Zhiyou, Zhang, Longsheng, Liu, Tianxi
Médium: Journal Article
Jazyk:angličtina
Vydáno: Germany Wiley Subscription Services, Inc 01.03.2023
Témata:
Ammonia
ammonia synthesis
Business competition
conjugated coordination polymers
Coordination polymers
electrocatalysis
Electrowinning
Hydrogen evolution reactions
Materials science
Modulation
nitrate electroreduction
Nitrates
Protons
Selectivity
Single atom catalysts
Strategy
conjugated coordination polymers
electrocatalysis
ammonia synthesis
nitrate electroreduction
ISSN:0935-9648, 1521-4095, 1521-4095
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Shrnutí:Electroreduction of nitrate into ammonia (NRA) provides a sustainable route to convert the widespread nitrate pollutants into high‐value‐added products under ambient conditions, which unfortunately suffers from unsatisfactory selectivity due to the competitive hydrogen evolution reaction (HER). Previous strategies of modifying the metal sites of catalysts often met a dilemma for simultaneously promoting activity and selectivity toward NRA. Here, a general strategy is reported to enable an efficient and selective NRA process through coordination modulation of single‐atom catalysts to tailor the local proton concentration at the catalyst surface. By contrast, two analogous Ni‐single‐atom enriched conjugated coordination polymers (NiO4‐CCP and NiN4‐CCP) with different coordination motifs are investigated for the proof‐of‐concept study. The NiO4‐CCP catalyst exhibits an ammonia yield rate as high as 1.83 mmol h−1 mg−1 with a Faradaic efficiency of 94.7% under a current density of 125 mA cm−2, outperforming the NiN4‐CCP catalyst. These experimental and theoretical studies both suggest that the strategy of coordination modulation can not only accelerate the NRA by adjusting the adsorption energies of NRA intermediates on the metal sites but also inhibit the HER through regulating the proton migration with contributions from the metal‐hydrated cations adsorbed at the catalyst surface, thus achieving simultaneous enhancement of NRA selectivity and activity. A general strategy for simultaneous enhancement of activity and selectivity toward nitrate electroreduction into ammonia (NRA) is demonstrated by utilizing Ni‐based conjugated coordination polymer catalysts for the proof‐of‐concept study. Coordination modulation can tailor their electrostatic attractions with the metal‐hydrated cations that can regulate proton migration at the catalyst surface, promoting the NRA and inhibiting the competitive hydrogen evolution reaction (HER).
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ISSN:0935-9648
1521-4095
1521-4095
DOI:10.1002/adma.202209855