4.6 Article

Photocatalytic N2 Reduction: Uncertainties in the Determination of Ammonia Production

期刊

ACS SUSTAINABLE CHEMISTRY & ENGINEERING
卷 9, 期 1, 页码 560-568

出版社

AMER CHEMICAL SOC
DOI: 10.1021/acssuschemeng.0c08064

关键词

N-2 reduction; uncertainties; NH4+ determination; photocatalysis

资金

  1. National Natural Science Foundation of China [21671153]
  2. Application Foundation Frontier Project of Wuhan Science and Technology Bureau [2019020701011493]
  3. Hubei Superior and Distinctive Discipline Group of Mechatronics and Automobiles

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The study aimed to enhance the photocatalytic N-2 reduction activity, but the uncertainties in NH4+ determination methods made the assessment of actual yield unreliable. Residual alcohols, amines, and other N-containing surfactants in the reaction system could significantly interfere with NH4+ determination, therefore, caution is advised in interpreting the results of photocatalytic N-2 reduction experiments.
Photocatalytic N-2 reduction is a thermodynamically and kinetically challenging reaction. Many research works have focused on the construction of oxygen vacancy with abundant localized electrons in the photocatalyst to activate N-2 and weaken the N N triple bond. In this work, we initially intended to construct oxygen vacancy on Bi2MO6 (M = W, Mo) nanomaterials to achieve improved photocatalytic N-2 reduction activity. However, NH4+ determination by Nessler's reagent method and the ion chromatography method showed completely opposite results, indicating that there were many uncertainties in the determination of the actual NH4+ yield in the photocatalytic N-2 reduction experiment. To further systematically clarify the uncertainties in NH4+ determination, different bismuth-related photocatalysts and P25 were also used to investigate the influence factors on photocatalytic N-2 reduction. It demonstrated that the residual alcohols, amines, and other N-containing surfactants in the reaction system could significantly interfere with the determination of the actual NH4+ yield. Therefore, we should be cautious of the results of the photocatalytic N-2 reduction experiment. It is quite essential to select an appropriate NH4+ determination method and design fully reasonable control experiments to obtain accurate data of photocatalytic N-2 reduction.

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