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Metallic Co Nanoarray Catalyzes Selective NH₃ Production from Electrochemical Nitrate Reduction at Current Densities Exceeding 2 A cm^-2.

ABSTRACT: Electrochemical nitrate reduction (NITRR) offers a promising alternative toward nitrogen recycling and ammonia production under ambient conditions, for which highly active and selective electrocatalyst is desired. In this study, metallic cobalt nanoarrays as facilely prepared from the electrochemical reduction of Co(OH)₂ nanoarrays (NAs) are demonstrated to exhibit unprecedented NH₃ producing capability from catalyzing NITRR. Benefitting from the high intrinsic activity of Co⁰, intimate contact between active species and conductive substrate and the nanostructure which exposes large number of active sites, the Co-NAs electrode exhibits current density of -2.2 A cm^-2 and NH₃ production rate of 10.4 mmol h^-1 cm^-2 at -0.24 V versus RHE under alkaline condition and significantly surpasses reported counterparts. Moreover, the close-to-unity (≥96%) Faradaic efficiency (FE) toward NH₃ is achieved over wide application range (potential, NO₃ ^- concentration and pH). Density function theory calculation reveals the optimized adsorption energy of NITRR intermediates on Co surface over Co(OH)₂. Furthermore, it is proposed that despite the sluggish kinetics of Volmer step (H₂O → *H + *OH) which provides protons in conventional hydrogenation mechanism, the proton-supplying water dissociation process on Co surface is drastically facilitated following a concerted water dissociation-hydrogenation pathway.

SUBMITTER: Deng X

PROVIDER: S-EPMC8025016 | biostudies-literature |

REPOSITORIES: biostudies-literature

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Project description:BackgroundIn northwest of China, mini Chinese cabbage (Brassica pekinensis) is highly valued by consumers, and is widely cultivated during winter in solar-greenhouses where low light (LL) fluence (between 85 and 150 μmol m-2 s-1 in day) is a major abiotic stress factor limiting plant growth and crop productivity. The mechanisms with which various NH4+: NO3- ratios affected growth and photosynthesis of mini Chinese cabbage under normal (200 μmol m-2 s-1) and low (100 μmol m-2 s-1) light conditions was investigated. The four solutions with different ratios of NH4+: NO3- applied were 0:100, 10:90, 15:85 and 25:75 with the set up in a glasshouse in hydroponic culture. The most appropriate NH4+: NO3- ratio that improved the tolerance of mini Chinese cabbage seedlings to LL was found in our current study.ResultsUnder low light, the application of NH4+: NO3- (10:90) significantly stimulated growth compared to only NO3- by increasing leaf area, canopy spread, biomass accumulation, and net photosynthetic rate. The increase in net photosynthetic rate was associated with an increase in: 1) maximum and effective quantum yield of PSII; 2) activities of Calvin cycle enzymes; and 3) levels of mRNA relative expression of several genes involved in Calvin cycle. In addition, glucose, fructose, sucrose, starch and total carbohydrate, which are the products of CO2 assimilation, accumulated most in the cabbage leaves that were supplied with NH4+: NO3- (10:90) under LL condition. Low light reduced the carbohydrate: nitrogen (C: N) ratio while the application of NH4+: NO3- (10:90) alleviated the negative effect of LL on C: N ratio mainly by increasing total carbohydrate contents.ConclusionsThe application of NH4+:NO3- (10:90) increased rbcL, rbcS, FBA, FBPase and TK expression and/or activities, enhanced photosynthesis, carbohydrate accumulation and improved the tolerance of mini Chinese cabbage seedlings to LL. The results of this study would provide theoretical basis and technical guidance for mini Chinese cabbage production. In practical production, the ratio of NH4+:NO3- should be adjusted with respect to light fluence for successful growing of mini Chinese cabbage.

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Metallic Co Nanoarray Catalyzes Selective NH₃ Production from Electrochemical Nitrate Reduction at Current Densities Exceeding 2 A cm^-2.

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Metallic Co Nanoarray Catalyzes Selective NH3 Production from Electrochemical Nitrate Reduction at Current Densities Exceeding 2 A cm-2.

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Metallic Co Nanoarray Catalyzes Selective NH₃ Production from Electrochemical Nitrate Reduction at Current Densities Exceeding 2 A cm^-2.