Результаты исследований: Научные публикации в периодических изданиях › статья › Рецензирование
Refining Universal Procedures for Ammonium Quantification via Rapid 1H NMR Analysis for Dinitrogen Reduction Studies. / Hodgetts, Rebecca Y.; Kiryutin, Alexey S.; Nichols, Peter и др.
в: ACS Energy Letters, Том 5, № 3, 13.03.2020, стр. 736-741.Результаты исследований: Научные публикации в периодических изданиях › статья › Рецензирование
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TY - JOUR
T1 - Refining Universal Procedures for Ammonium Quantification via Rapid 1H NMR Analysis for Dinitrogen Reduction Studies
AU - Hodgetts, Rebecca Y.
AU - Kiryutin, Alexey S.
AU - Nichols, Peter
AU - Du, Hoang Long
AU - Bakker, Jacinta M.
AU - MacFarlane, Douglas R.
AU - Simonov, Alexandr N.
N1 - Publisher Copyright: © 2020 American Chemical Society.
PY - 2020/3/13
Y1 - 2020/3/13
N2 - As research on sustainable ammonia synthesis via electrochemical and photochemical N2 reduction progresses to include a wider variety of aqueous and aprotic electrolytes, 1H NMR spectroscopy is increasingly adopted as a means for ammonium quantification. However, this method is highly sensitive to experimental parameters, as demonstrated herein using a highly versatile and robust NMR pulse program. We demonstrate the sensitivity of the measurement to the final pH of the analyzed solution and identify a [H+] concentration range enabling robust quantification. We compare direct quantification versus calibration approaches to show that the former is highly sensitive to spin relaxation effects and identify the latter as the most reliable approach. This method, when optimized, enables direct, rapid quantification of both 14NH4 + and 15NH4 + within 12-22 min. The limit of detection of 5-10 μM, depending on the solvent, which meets the needs of current electrochemical and photochemical N2 reduction research.
AB - As research on sustainable ammonia synthesis via electrochemical and photochemical N2 reduction progresses to include a wider variety of aqueous and aprotic electrolytes, 1H NMR spectroscopy is increasingly adopted as a means for ammonium quantification. However, this method is highly sensitive to experimental parameters, as demonstrated herein using a highly versatile and robust NMR pulse program. We demonstrate the sensitivity of the measurement to the final pH of the analyzed solution and identify a [H+] concentration range enabling robust quantification. We compare direct quantification versus calibration approaches to show that the former is highly sensitive to spin relaxation effects and identify the latter as the most reliable approach. This method, when optimized, enables direct, rapid quantification of both 14NH4 + and 15NH4 + within 12-22 min. The limit of detection of 5-10 μM, depending on the solvent, which meets the needs of current electrochemical and photochemical N2 reduction research.
KW - NITROGEN REDUCTION
KW - BERTHELOT REACTION
KW - SALICYLATE
KW - CATALYSTS
KW - ELECTROREDUCTION
KW - TEMPERATURE
KW - CHEMISTRY
KW - PRESSURE
KW - SODIUM
KW - N-15
UR - http://www.scopus.com/inward/record.url?scp=85082394087&partnerID=8YFLogxK
U2 - 10.1021/acsenergylett.9b02812
DO - 10.1021/acsenergylett.9b02812
M3 - Article
AN - SCOPUS:85082394087
VL - 5
SP - 736
EP - 741
JO - ACS Energy Letters
JF - ACS Energy Letters
SN - 2380-8195
IS - 3
ER -
ID: 23892590