Шляхи ЕСI-MС фрагментації деяких 1,2,4-триазол-3-тіонів, проміжних продуктів при синтезі активних фармацевтичних інгредієнтів

Aim. To determine the fragmentation pathways of eight 1,2,4-triazole-3-thiones, which are intermediate products in the synthesis of active pharmaceutical ingredients of potential and registered pharmaceutical formulations.Results and discussion. HPLC-MS analysis of eight 1,2,4-triazole-3-thiones, wh...

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Veröffentlicht in:Журнал органічної та фармацевтичної хімії
Datum:2020
Jahrgang:18
Heft:1(69)
Сторінки:22-33
ISSN:2518-1548
Автори та афіліації:
  • Borys O. Varynskyi — Zaporizhzhia State Medical University
  • Andriy G. Kaplaushenko — Zaporizhzhia State Medical University — ORCID: 0000-0003-3704-5539
Hauptverfasser: Varynskyi, Borys O., Kaplaushenko, Andriy G.
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Sprache:Englisch
Veröffentlicht: National University of Pharmacy 2020
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Journal of Organic and Pharmaceutical Chemistry
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author Varynskyi, Borys O.
Kaplaushenko, Andriy G.
author_facet Varynskyi, Borys O.
Kaplaushenko, Andriy G.
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author_orcid_str_mv 0000-0003-3704-5539
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container_title Журнал органічної та фармацевтичної хімії
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description Aim. To determine the fragmentation pathways of eight 1,2,4-triazole-3-thiones, which are intermediate products in the synthesis of active pharmaceutical ingredients of potential and registered pharmaceutical formulations.Results and discussion. HPLC-MS analysis of eight 1,2,4-triazole-3-thiones, which are intermediate products in the synthesis of salts of 1,2,4-triazolylthioacetate acids, has been carried out; the mass spectra of the compounds to be analyzed have been registered in ESI-mode with different fragmentor voltage (0, 100, 200 V). The fragmentation pathways and patterns of ion decay for compounds to be analyzed have been proposed.Experimental part. Agilent 1260 Infinity HPLC System with Agilent 6120 mass spectrometer were used. HPLC-MS conditions: column – 4,6 × 30 mm, reversible phase Zorbax SB C18, 1.8 μm, 40 oC; mobile phase – 0.1 % HCOOH in H2O and 0.1 % HCOOH in СH3CN in isocratic mode (50:50, v/v); the flow rate – 0.4 mL/min; ion source – API-ES; positive polarity; drying gas – nitrogen (rate – 10 L/min); the capillary voltage – 4000 V; scanning in the range of m/z 100 – 1000.Conclusions. For the first time it has been interpreted the mass spectra of 1,2,4-triazole-3-thiones series, the intermediate compounds in the synthesis of active pharmaceutical ingredients of pharmaceutical formulations. The fragmentation pathways and patterns of eight 1,2,4-triazole-3-thiones have been shown. Received: 06.09.2019Revised: 20.01.2020Accepted: 27.02.2020
doi_str_mv 10.24959/ophcj.20.177613
first_indexed 2025-07-17T13:00:26Z
format Article
fulltext Journal of Organic and Pharmaceutical Chemistry. – 2020. – Vol. 18, Iss. 1 (69) 22 ISSN 2308-8303 (Print) ISSN 2518-1548 (Online) UDC 547.792: 543.51 https://doi.org/10.24959/ophcj.20.177613 B. O. Varynskyi, А. G. Kaplaushenko Zaporizhzhia State Medical University, Ukraine 26, Mayakovsky Ave., Zaporizhzhia, 69035, Ukraine. E-mail: varinsky@zsmu.zp.ua ESI-MS fragmentation pathways of some 1,2,4-triazole- 3-thiones, the intermediate compounds in the synthesis of active pharmaceutical ingredients Aim. To determine the fragmentation pathways of eight 1,2,4-triazole-3-thiones, which are intermediate products in the synthesis of active pharmaceutical ingredients of potential and registered pharmaceutical formulations. Results and discussion. HPLC-MS analysis of eight 1,2,4-triazole-3-thiones, which are intermediate products in the synthesis of salts of 1,2,4-triazolylthioacetate acids, has been carried out; the mass spectra of the com- pounds to be analyzed have been registered in ESI-mode with different fragmentor voltage (0, 100, 200 V). The fragmentation pathways and patterns of ion decay for compounds to be analyzed have been proposed. Experimental part. Agilent 1260 Infinity HPLC System with Agilent 6120 mass spectrometer were used. HPLC-MS conditions: column – ∅4,6 × 30 mm, reversible phase Zorbax SB C18, 1.8 μm, 40 oC; mobile phase – 0.1 % HCOOH in H2O and 0.1 % HCOOH in СH3CN in isocratic mode (50:50, v/v); the flow rate – 0.4 mL/min; ion source – API-ES; positive polarity; drying gas – nitrogen (rate – 10 L/min); the capillary voltage – 4000 V; scan- ning in the range of m/z 100 – 1000. Conclusions. For the first time it has been interpreted the mass spectra of 1,2,4-triazole-3-thiones series, the intermediate compounds in the synthesis of active pharmaceutical ingredients of pharmaceutical formula- tions. The fragmentation pathways and patterns of eight 1,2,4-triazole-3-thiones have been shown. Key words: mass spectrometry; high performance liquid chromatography; 1,2,4-triazole-3-thiones Б. О. Варинський, А. Г. Каплаушенко Запорізький державний медичний університет, Україна Шляхи ЕСI-MС фрагментації деяких 1,2,4-триазол-3-тіонів, проміжних продуктів при синтезі активних фармацевтичних інгредієнтів Мета. Визначити шляхи фрагментації восьми 1,2,4-триазол-3-тіонів, які є проміжними продуктами в син- тезі активних фармацевтичних інгредієнтів потенційних та зареєстрованих фармацевтичних препаратів. Результати та їх обговорення. Проведено ВЕРХ-МС аналіз восьми 1,2,4-триазол-3-тіонів, які є про- міжними продуктами при синтезі солей 1,2,4-триазолілтіоацетатних кислот; мас-спектри досліджуваних сполук зареєстровано в ЕСІ-режимі з різною напругою фрагментатора (0, 100, 200 В). Запропоновано шля- хи фрагментації та закономірності розпаду іонів для аналізованих сполук. Експериментальна частина. Для досліджень використано систему HPLC Agilent 1260 Infinity з мас- спектрометром Agilent 6120. ВЕРХ-МС умови: колонка – ∅4,6 × 30 мм, обернена фаза Zorbax SB C18, 1,8 μm, 40 oC; рухома фаза – 0,1 % HCOOH в H2O та 0,1 % HCOOH в СH3CN в ізократичному режимі (50:50, v/v); швидкість потоку – 0,4 мл/хв; джерело іонів – API-ES; позитивна полярність; газ-осушувач – азот (швид- кість – 10 л/хв); напруга капіляра – 4000 V; сканування в діапазоні m/z 100 – 1000. Висновки. Вперше інтерпретовано мас-спектри серії 1,2,4-триазол-3-тіонів, проміжних сполук при син- тезі активних фармацевтичних інгредієнтів фармацевтичних препаратів. Показано шляхи фрагментації та розпаду восьми 1,2,4-триазол-3-тіонів. Ключові слова: мас-спектрометрія; високоефективна рідинна хроматографія; 1,2,4-триазол-3-тіони Б. А. Варинский, А. Г. Каплаушенко Запорожский государственный медицинский университет, Украина Пути ЭСИ-MС фрагментации некоторых 1,2,4-триазол-3-тионов, промежуточных продуктов при синтезе активных фармацевтических ингредиентов Цель. Определить пути фрагментации восьми 1,2,4-триазол-3-тионов, являющихся промежуточными продуктами в синтезе активных фармацевтических ингредиентов потенциальных и зарегистрированных фармацевтических препаратов. Результаты и их обсуждение. Проведен ВЭЖХ-МС анализ восьми 1,2,4-триазол-3-тионов, являю- щихся промежуточными продуктами при синтезе солей 1,2,4-триазолилтиоацетатних кислот; масс-спектры исследуемых соединений зарегистрированы в ЭСИ-режиме с различным напряжением фрагментатора (0, 100, 200 В). Предложены пути фрагментации и закономерности распада ионов для исследуемых соеди- нений. Экспериментальная часть. Для исследований использована система HPLC Agilent 1260 Infinity с масс- спектрометром Agilent 6120. ВЭЖХ-МС условия: колонка – ∅4,6 × 30 мм, обращенная фаза Zorbax SB C18, 1,8 μm, 40 oC; подвижная фаза – 0,1 % HCOOH в H2O и 0,1 % HCOOH в СH3CN в изократическом режиме (50:50, v/v); скорость потока – 0,4 мл/мин; источник ионов – API-ES; позитивная полярность; газ-осушитель – азот (скорость – 10 л/мин); напряжение капилляра – 4000 V; сканирование в диапазоне m/z 100 – 1000. Выводы. Впервые интерпретированы масс-спектры серии 1,2,4-триазол-3-тионов, промежуточных про- дуктов при синтезе активных фармацевтических ингредиентов фармацевтических препаратов. Показаны пути фрагментации и распада восьми 1,2,4-триазол-3-тионов. Ключевые слова: масс-спектрометрия; высокоэффективная жидкостная хроматография; 1,2,4-триазол-3-тионы Журнал органічної та фармацевтичної хімії. – 2020. – Т. 18, вип. 1 (69) 23 ISSN 2518-1548 (Online) ISSN 2308-8303 (Print) Heterocyclic systems based on 1,2,4-triazole are the subject of interest for the present-day medicinal chemistry. They have the antioxidative, hepatopro- tective and other activities; moreover, some of them have been already registered and used in the present- day veterinary (tryfusol, avesstym) [1, 2], and one of them is on the stage of registration for human use and manufacturing application (thiometrizol) [3]. In this way, the study of the preparation methods and the quality control of all stages of the develop- ment and production of the abovementioned com- pounds and their initial products in the synthesis is the urgent task for the present-day pharmaceutical science and of a scientific interest and practical im- portance. One of the main methods, which may be used for the effective and reliable identification and the quan- titative determination of the target products of the or- ganic synthesis and impurities is chromatography with mass spectrometric detection. The most appro- priate for the analytical goals is a combination of high performance liquid chromatography and mass spectro- metry with ionization under atmospheric pressure, in electrospray (ESI), chemical ionization under at- mospheric pressure (APCI), photochemical ionization under atmospheric pressure (APPI). The current work is devoted to ionization in electrospray, which is the best choice for the analysis of polar non-volatile com- pounds, such as the analytes under research. At the first stage, there was the optimization of the mass spectrometry detection conditions [4], at the second stage the behavior of analytes to be chro- matographed was studied [5]. Patterns of hydrazide of definite organic acids and their corresponding hydrazinecarbothioamides mass spectrometric decay were showed [6]. The mass frag- mentation patterns of 1,2,4-triazole derivatives were reported in different articles [7 – 10]. The aim of the present work is to study mass- spectra and offer plausible fragmentation pathways of eight 1,2,4-triazole-3-thiones, the intermediate pro- ducts in the synthesis of active pharmaceutical ingre- dients. The elucidation of fragmentation pathways was based on the electrospray ionization single quadru- pole mass spectrometry. Results and discussion The mass spectra are presented in graphical and tabular form, providing the most intensive peaks star- ting about 1 %. The maximal peak was shown from isotope group peaks. All compounds can exist as a thiol and thione forms. We analyzed the mass spectra and suggested the possible fragmentation pathways of the compounds. 4-(2-Methoxyphenyl)-5-(pyridin-4-yl)-2,4- dihydro-3H-1,2,4-triazole-3-thione. The ion with m/z 285.0 is observed at 0 V, 100 V, and 200 V of colli- sion voltages (Fig. 1). This ion corresponds to the quasi- molecular ion (protonated molecule) of the current sub- stance. The isotope peaks are also present in the mass spectrum. The ion with m/z 253.1 at 100 V and 200 V is detected (Fig. 2 – 3, Table 1); it is formed by heterolytic cleavage of bonds between a phenyl carbon and oxygen of the methoxy group. It is also possible that this ion cor- responds to the structure created as a result of the sulf- hydryl group cleavage from the quasimolecular ion. Fig. 1. Mass-spectra of 4-(2-methoxyphenyl)-5-(pyridin-4-yl)-2,4-dihydro-3H-1,2,4-triazole-3-thione at different fragmentor voltage (0, 100, 200 V) N N H N SH N N N H2 N S N O Me O Me N N H N S CN HN N N SH N OH N N H N N O Me N N N S N OMe N N HN S N O Me 285.080457 Da 253.054243 Da 275.096108 Da 253.108387 Da 567.137988 Da H2 Fig. 2. The pathways proposed for the dissociation of 4-(2-methoxyphenyl)-5-(pyridin-4-yl)-2,4-dihydro-3H-1,2,4-triazole- 3-thione and theoretical monoisotopic masses of ions at 100 V Journal of Organic and Pharmaceutical Chemistry. – 2020. – Vol. 18, Iss. 1 (69) 24 ISSN 2308-8303 (Print) ISSN 2518-1548 (Online) A pattern for the cation with m/z 275.1 appearing in the mass spectrum at 100 V has been offered (Fig. 2). The methoxy group elimination and the reduction of the triazol cycle are observed. The cation with Table 1 The values of ions m/z of 4-(2-methoxyphenyl)-5- (pyridin-4-yl)-2,4-dihydro-3H-1,2,4-triazole-3-thione ions and the relative abundance at 100 V and 200 V No m/z Relative abundance, % 100 V 1 253.1 14.7 2 275.1 0.9 3 285.0 100.0 4 567.0 1.5 200 V 1 169.2 1.0 2 184.0 1.2 3 197.1 29.6 4 212.1 6.7 5 221.0 4.8 6 237.1 6.6 7 253.1 16.1 8 269.9 4.8 9 271.0 1.1 10 285.0 100.0 11 567.1 3.4 Table 2 The values of ions m/z of 5-(furan-2-yl)-4-phenyl- 2,4-dihydro-3H-1,2,4-triazole-3-thione and the relative abundance at 100 V and 200 V No m/z Relative abundance, % 100 V 1 212.0 2.0 2 244.1 100.0 3 485.0 1.7 200 V 1 105.1 27.6 2 109.1 7.9 3 115.1 1.4 4 118.1 5.8 5 130.0 3.1 6 151.0 1.5 7 157.0 7.2 8 170.1 12.1 9 185.1 10.6 10 212.1 2.3 11 216.0 3.0 12 244.1 100.0 13 265.0 1.0 14 485.0 3.6 15 485.0 1.7 N NH2 N N O Me S N NH N N C S NN N N O Me SS N H N N O Me N N NH N N O Me N N N N C N NH2 N N OH S N NH N N O Me SH 253.054243 Da 285.080457 Da 567.137988 Da 253.108387 Da 221.082173 Da 271.064807 Da N C Me 212.094414 Da N C 197.070939 Da N NH2 NH2C O Me S 221.061733 Da N NH2 N N S Me 221.085543 Da N NH2 N N S O Me 237.080457 Da H N O N OH Fig. 3. The pathways proposed for the dissociation of 4-(2-methoxyphenyl)-5-(pyridin-4-yl)-2,4-dihydro-3H-1,2,4-triazole- 3-thione and theoretical monoisotopic masses of ions at 200 V Журнал органічної та фармацевтичної хімії. – 2020. – Т. 18, вип. 1 (69) 25 ISSN 2518-1548 (Online) ISSN 2308-8303 (Print) m/z 567.1 is the quasimolecular ion (a protonated dimer) of the compound at 0 V, 100 V and 200 V. 200 V of collision voltage cause the appearance of the cation with m/z 237.1. (Fig. 3). It is formed due to partial destruction of the methoxyphenyl cycle. Several structures of the cation with m/z 221.0 have been offered. The first one is splitting off sulfur and the methoxyl group, it leads to formation of the phe- nylium carbocation. The second one is due to the de- struction of the pyridin cycle, the corresponding cat- ion radicals are formed, the third structure is due to the destruction of the metoxyphenyl cycle. The ion with m/z 271.0 appears during сleavage of the me- thyl group from a quasimolecular ion. The destruc- tion of the triazole cycle is also possible with the for- mation of the following ions: the radical cation with m/z 212.1 and the cation with m/z 197.1 are formed. 5-(Furan-2-yl)-4-phenyl-2,4-dihydro-3H-1,2,4- triazole-3-thione. At fragmentor voltage of 100 V the quasimolecular (protonated molecule) ion with m/z 244.1 and the dimer cation with m/z 485.0 are formed (Fig. 4, Table 2). Fig. 4. Mass-spectra of 5-(furan-2-yl)-4-phenyl-2,4-dihydro-3H-1,2,4-triazole-3-thione at different fragmentor voltage (100, 200 V) N N H N SH O N N H N O N N N Me N N N HC HN N H H N SH N N N S O N N N S Me N NH N S Me HN NH N Me S N NH H N Me S N N H N S O N N N S O N N C N H2C N N C N N Me Me NH3 HN Me 170.071274 Da 485.08489 Da 109.088601 Da151.122975 Da 157.063449 Da170.071274 Da 212.081838 Da 185.094749 Da 244.053908 Da 105.035519 Da 216.058994 Da130.043344 Da 118.043344 Da 115.019869 Da H2 H2 H2 H2 H2C Fig. 5. The pathways proposed for the dissociation of 5-(furan-2-yl)-4-phenyl-2,4-dihydro-3H-1,2,4-triazole-3-thione and theoretical monoisotopic masses of ions at 200 V Journal of Organic and Pharmaceutical Chemistry. – 2020. – Vol. 18, Iss. 1 (69) 26 ISSN 2308-8303 (Print) ISSN 2518-1548 (Online) There is also the ion with m/z 212.1, which ap- pears as a result of splitting off sulfur from a quasimo- lecular ion (Fig. 4). When the fragmentor voltage is increased from 100 to 200 V, more than 10 new ions appear (Table 2, Fig. 5). The ion with m/z 212.1 is also present at voltage of 200 V. The radical cation with m/z 185.1 appears during cleavage of CO from the ion with m/z 212.1. In the case of additional splitting of the methyl group, the cation with m/z 170.1 appears. The alternative structure of the cation with m/z 170.1 may appear from a quasimolecular ion during the destruction of the furan cycle and elimination of the SH-group. With further cleavage of the methylene group the radical cation with m/z 157.0 appears. During disintegra- tion of the triazole cycle the cation with m/z 151.0 appears at first, then the radical cation with m/z 109.1. A direct elimination of the furan and ben- zene ring from thiol forms of a quasimolecular ion with the reduction of the triazole cycle; in this case, the appearance of the radical cation with m/z 105.1 is possible. If CO is cleaved from the quasimolecu- lar ion, the cation with m/z 216.1 may be formed. This cation turns into the ion with m/z 130.0 after eliminating the methylene group and benzene ring. In the case of the triazole сycle reduction, the forma- tion of the ion with m/z 118.0 is possible. The radi- cal cation with m/z 115.1 may appear after cleavage of CH2 from the ion with m/z 130.0. 5-(Pyridin-4-yl)-1,2-dihydro-3H-1,2,4-tria- zole-3-thione. At voltage of 0, 100, 200, and 300 V the quasimolecular cation of the protonated substan- ce with m/z 179.0 is observed in mass spectra, as well as the dimeric cation with m/z 355.0 and a partially hydrogenized dimeric cation with m/z 357.0 are for- med (Fig. 6 – 7, Table 3). At 0 V the adduct of the quazimolecular ion of the protonated ion exists with dimethyl sulfoxide with m/z 257.0. The substance studied is solved in dime- thyl sulfoxide. The scan range of 160 – 1000 m/z is used for maximal exclusion of ions, which are the products of transformation of dimethyl sulfoxide in the ion source, it has not entirely obtained yet. The ions of product fragmentation of the compound studied have low in- tensity (less than 1 % of the basic peak intensity); therefore, the interpretation of them is considered to be inappropriate. 5-(Morpholin-4-ylmethyl)-4-phenyl-2,4-di- hydro-3H-1,2,4-triazole-3-thione. At voltage of 100 V the quasimolecular ion MH+ with m/z 277.1, as well as the ion with m/z 245.1 are present (Fig. 8, Table 4). The ion with m/z 245.1 appears after cleavage of sulfur from a quasimolecular ion. The cation with Fig. 6. Mass-spectra of 5-(pyridin-4-yl)-1,2-dihydro-3H-1,2,4-triazole-3-thione at different fragmentor voltage (0, 100, 200 V) N N H H N SH N N N H N S N N N H NH S N N HN N S N N N H NH S N N HN H N S N 179.031316 Da 355.054259 Da 357.069909 Da H2 Fig. 7. The pathways proposed for the dissociation of 5-(pyridin-4-yl)-1,2-dihydro-3H-1,2,4-triazole-3-thione and monoisotopic masses of ions Table 3 The values of ions m/z of 5-(pyridin-4-yl)-1,2-dihydro- 3H-1,2,4-triazole-3-thione and the relative abundance at 0 V, 100 V, 200 V No m/z Relative abundance, % 0 V 1 172.0 0.8 2 179.0 100.0 3 257.0 71.9 4 355.1 5.0 5 357.0 10.2 100 V 1 179.0 100.0 2 355.0 0.6 3 357.0 0.5 200 V 1 179.0 100.0 2 354.8 1.1 Журнал органічної та фармацевтичної хімії. – 2020. – Т. 18, вип. 1 (69) 27 ISSN 2518-1548 (Online) ISSN 2308-8303 (Print) m/z 173.1 is formed during forthcoming elimination of the phenyl radical and reduction of the triazole cycle. After cleavage of triazole, cations with m/z 102.1 and 100.1 appear (Fig. 9) [6]. At voltage of 200 V (Table 4, Fig. 10) the quasimo- lecular ion may be disintegrated in few ways. Firstly, after elimination of sulfur, the triazole cycle reduction and the morpholine fragment separation, the radical cation with m/z 163.0 is formed, and then after clea- vage of the methylene radical the cation with m/z 148.0 is observed. The structure of the ion with m/z 148.0 is also possible; it corresponds to the cation, which appears during elimination of sulfur, the morpholine- methylene fragment and partial reduction of the tria- zole cycle. The cation with m/z 136.0 is formed after cleavage of sulfur, the morpholinemethylene fragment and partial destruction of the triazole cycle. During elimination of the morpholine fragment from the quasimolecular ion the ion with m/z 190.0 appears. The alternative structure of the radical ca- tion with m/z 163.0 may be obtained by destruction of the triazole cycle. Elimination of sulfur and the mor- pholine methylene fragment, the triazole cycle destruc- tion lead to the appearance of the radical cation with m/z 105.1. During cleavage of sulfur, the phenyl ra- dical and the triazole cycle destruction the radical ca- tion with m/z 157.1 is formed, it is successively trans- formed into the cation with m/z 143.0, 131.1 and 100.1 (we suggested two structures; one of them was de- monstrated in the previous research paper [6]). After elimination of the phenyl fragment and the morpho- line cycle destruction the formation of the alternative Table 4 The values of ions m/z of 5-(morpholin-4-ylmethyl)- 4-phenyl-2,4-dihydro-3H-1,2,4-triazole-3-thione and the relative abundance at 100 V and 200 V No m/z Relative abundance, % 100 V 1 100.15 3.3 2 102.15 1.1 3 173.1 1.1 4 245.05 2.2 5 277.1 100.0 6 551.15 3.5 200 V 1 100.1 100.0 2 105.1 52.8 3 117.1 12.1 4 131.10 89.5 5 136.0 9.5 6 143.0 1.0 7 148.0 4.0 8 157.1 5.5 9 163.0 7.3 10 190.0 83.4 11 277.1 8.1 12 551.2 30.7 Fig. 8. Mass-spectra of 5-(morpholin-4-ylmethyl)-4-phenyl-2,4-dihydro-3H-1,2,4-triazole-3-thione (100, 200 V) Table 5 The values of ions m/z of 4-methyl-5-(morpholin- 4-ylmethyl)-2,4-dihydro-3H-1,2,4-triazole-3-thione and the relative abundance at 100 V and 200 V No m/z Relative abundance, % 100 V 1 100.1 1.6 2 183.1 1.0 3 215.1 100.0 4 429.1 4.9 200 V 1 100.1 100.0 2 128.1 15.7 3 215.1 9.5 4 427.1 1.9 Journal of Organic and Pharmaceutical Chemistry. – 2020. – Vol. 18, Iss. 1 (69) 28 ISSN 2308-8303 (Print) ISSN 2518-1548 (Online) N N H N N SHO N N H N N S O N N N NS O N N H N N O N N N N SO HN N H N N O N O H2C NH O Me N O 277.111758 Da 551.200589 Da 245.139688 Da 173.139688 Da 100.07569 Da 102.09134 Da 100.07569 Da H2 H2 Fig. 9. The pathways proposed for the dissociation of 5-(morpholin-4-ylmethyl)-4-phenyl-2,4-dihydro-3H-1,2,4-triazole-3-thione and theoretical monoisotopic masses of ions at 100 V N N H N N SHO N N H N N S O N N N NS O N N N N SO N O H2C N O 277.111758 Da 551.200589 Da 100.07569 Da 100.07569 Da HN N H N HN N H N Me HN N CH H N NH NH3N N N H N H2C S NS N N N H N S H2N HN N H H N S Me HN Me N N O H2N N N O H3N N O 105.057301 Da 148.086924 Da 136.086924 Da 163.110399 Da 148.086924 Da 157.120964 Da 143.105313 Da 131.11789 Da 131.038593 Da 117.035519 Da 190.043344 Da 163.045021 Da H2 H2 Fig. 10. The pathways proposed for the dissociation of 5-(morpholin-4-ylmethyl)-4-phenyl-2,4-dihydro-3H-1,2,4-triazole-3-thione and theoretical monoisotopic masses of ions at 200 V Журнал органічної та фармацевтичної хімії. – 2020. – Т. 18, вип. 1 (69) 29 ISSN 2518-1548 (Online) ISSN 2308-8303 (Print) Fig. 11. Mass-spectra of 4-methyl-5-(morpholin-4-ylmethyl)-2,4-dihydro-3H-1,2,4-triazole-3-thione at different fragmentor voltage (100, 200 V) N N H N N Me SHO N N N N Me S O N N N N Me S O N N N N Me SO N O H2C N O 215.096108 Da 429.184939 Da 100.07569 Da 100.07569 Da N N H N N Me O 183.124038 Da H2 H2 Fig. 12. The pathways proposed for the dissociation of 4-methyl- 5-(morpholin-4-ylmethyl)-2,4-dihydro-3H-1,2,4-triazole-3-thione and theoretical monoisotopic masses of ions at 100 V N N H N N Me SHO N N H N N Me S O N N N N Me S O N N N N Me SO N O H2C N O 215.096108 Da 427.169289 Da 100.07569 Da 100.07569 Da HN N N H N Me 128.105678 Da Me H2 Fig. 13. The pathways proposed for the dissociation of 4-methyl- 5-(morpholin-4-ylmethyl)-2,4-dihydro-3H-1,2,4-triazole-3-thione and theoretical monoisotopic masses of ions at 200 V Fig. 14. Mass-spectra of 4-ethyl-5-(morpholin-4-ylmethyl)-2,4-dihydro-3H-1,2,4-triazole-3-thione at different fragmentor voltage (100, 200 V) Journal of Organic and Pharmaceutical Chemistry. – 2020. – Vol. 18, Iss. 1 (69) 30 ISSN 2308-8303 (Print) ISSN 2518-1548 (Online) structure of the cation with m/z 131.1 becomes pos- sible, then it creates the cation with m/z 117.1. At both voltages of 100 V and 200 V the protonated cation of the dimer of the compound with m/z 551.2 mentio- ned appears (Fig. 9 – 10). 4-Methyl-5-(morpholin-4-ylmethyl)-2,4-di- hydro-3H-1,2,4-triazole-3-thione. At the fragmen- tor voltage of 100 V the quasimolecular ion with m/z 215.1 of the compound itself can be observed. We can also mark the ion of the dimer of the sub- stance with the reduction of one of the triazole cycle. The cation with m/z 183.1 appears as a result of eli- mination of sulfur from a quasimolecular ion. The for- mation of the cation with m/z 100.1 is possible after the destruction of the triazole cycle corresponding to the above-described morpholine methylene deri- vatives (Fig. 11 – 12, Table 5). Voltage of 200 V initiates the formation of the qua- simolecular ion with m/z 215.1 and the dimeric ion with m/z 427.1. After elimination of sulfur and par- tial destruction of the morpholine cycle the radical cation with m/z 128.1 is observed. In the case of de- struction of the triazole cycle morpholine methylene the cation with m/z 100.1 appears (Fig. 13, Table 5). N N H N N SHO N N N N S O N N N NS O N N N N SO 229.111758 Da 457.216239 Da Me Me Me Me N N H N N O 197.139688 Da Me H2 H2 Fig. 15. The pathways proposed for the dissociation of 4-ethyl-5- (morpholin-4-ylmethyl)-2,4-dihydro-3H-1,2,4-triazole-3-thione and theoretical monoisotopic masses of ions at 100 V Table 6 The values of ions m/z of 4-ethyl-5-(morpholin- 4-ylmethyl)-2,4-dihydro-3H-1,2,4-triazole-3-thione and the relative abundance at 100 V and 200 V No m/z Relative abundance, % 100 V 1 197.1 1.5 2 229.1 100.0 3 457.2 10.6 200 V 1 100.1 100.0 2 114.0 3.0 3 142.0 20.9 4 229.1 17.7 5 455.0 1.2 6 457.1 1.4 N N H N N SHO N N N N S O N N N NS O N N N N SO 229.111758 Da 457.216239 Da Me Me Me Me HN N N H N 142.121298 Da Me N N H N N S O N N N NS O 455.200589 Da Me Me Me H2N N N Me Me N O H2C N O 114.102574 Da 100.07569 Da H2 H2 Fig. 16. The pathways proposed for the dissociation of 4-ethyl-5-(morpholin-4-ylmethyl)-2,4-dihydro-3H-1,2,4-triazole-3-thione and theoretical monoisotopic masses of ions at 200 V Журнал органічної та фармацевтичної хімії. – 2020. – Т. 18, вип. 1 (69) 31 ISSN 2518-1548 (Online) ISSN 2308-8303 (Print) 4-Ethyl-5-(morpholin-4-ylmethyl)-2,4-dihy- dro-3H-1,2,4-triazole-3-thione. At voltage of 100 V we can observe the quasimolecular ion with m/z 229.1 and the dimeric ion m/z 457.1 with partial reduction of one of the triazole cycles. The elimination of sul- fur leads to formation of the cation with m/z 197.1 (Fig. 14 – 15, Table 6). Voltage of 200 V initiates the appearance of a qu- asimolecular ion of the substance. The formation of the dimeric cation with m/z 455.0 and the cation with m/z 457.2 is observed. The percentage of the ca- tion with m/z 457.2 decreases in almost eight ti- mes comparing with the voltage of 100 V (Fig. 16, Table 6). After cleavage of sulfur, the partial destruction of the morpholine cycle and the fractional reduction of the triazole cycle the radical cation with m/z 142.0 is formed. This cation after elimination of the methyl- amine group can be transformed into the cation with m/z 114.0. The appearance of the cation with m/z 100.1 is observed as a result of the triazole cycle destruc- tion as described above. Fig. 17. Mass-spectra of 5-(morpholin-4-ylmethyl)-2,4-dihydro-3H-1,2,4-triazole-3-thione at different fragmentor voltage (100, 200 V) N N H H N N SHO N N H N N SO 201.080457 Da N NH H N N S O N N H N NS O 399.137988 Da N O H2C N O 100.07569 Da 100.07569 Da H2 Fig. 18. The pathways proposed for the dissociation of 5-(morpholin-4-ylmethyl)-2,4-dihydro-3H-1,2,4-triazole-3-thione and theoretical monoisotopic masses of ions at 100 V N N H H N N SHO N N H N N SO 201.080457 Da N NH H N N S O N N H N NS O 399.137988 Da N O N O 100.07569 Da 100.07569 Da N N H N H2C SH NH N H MeN O 114.012044 Da 157.120964 Da H2C H2 Fig. 19. The pathways proposed for the dissociation of 5-(morpholin- 4-ylmethyl)-2,4-dihydro-3H-1,2,4-triazole-3-thione and theoretical monoisotopic masses of ions at 200 V Table 7 The values of ions m/z of 5-(morpholin-4-ylmethyl)- 2,4-dihydro-3H-1,2,4-triazole-3-thione and the relative abundance at 100 V and 200 V No m/z Relative abundance, % 100 V 1 100.2 2.2 2 201.0 100.0 3 399.1 7.2 200 V 1 100.1 100.0 2 114.1 4.6 3 157.1 1.0 4 201.1 16.8 5 284.1 6.6 6 312.1 1.0 7 399.1 19.9 Journal of Organic and Pharmaceutical Chemistry. – 2020. – Vol. 18, Iss. 1 (69) 32 ISSN 2308-8303 (Print) ISSN 2518-1548 (Online) 5-(Morpholin-4-ylmethyl)-2,4-dihydro-3H- 1,2,4-triazole-3-thione. The quasimolecular ion MH+ with m/z 201.0 and the dimer ion with m/z 399.1 are formed at 100 V (Fig. 17 – 18, Table 7). Splitting off the triazole cycle causes the forma- tion of the methylene morpholinium cation with m/z 100.1. The quasimolecular ion of disintegration products appears at 200 V. At the triazole cycle de- cay the cation with m/z 157.1 is formed. The cleavage of the morpholine radical causes the formation of the cation with m/z 114.1 (Fig. 19, Table 7). 5-(2-Methoxyphenyl)-2,4-dihydro-3H-1,2,4- triazole-3-thione. The quasimolecular ion MH+ with m/z 208.0 exists at 100 V. It creates the dimeric ion of the compound with m/z 413.0 (Fig. 20 – 21, Table 8). Voltage of 200 V causes fragmentation of these ions. The cation with m/z 176.0 appears after cleavage of sulfur. The further elimination of the methyl group and the triazole cycle reduction cause the radical ca- tion with m/z 165.1. The cleavage of the methyl radi- cal from the quasimolecular ion causes the forma- tion of the radical cation with m/z 193.0. Removing of an oxygen atom and proton is a possible cause of the alternative structures of the ion with m/z 176.0 (Fig. 22, Table 8). Experimental part 4-(2-Methoxyphenyl)-5-(pyridin-4-yl)-2,4-di- hydro-3H-1,2,4-triazole-3-thione 1; 5-(furan-2-yl)- 4-phenyl-2,4-dihydro-3H-1,2,4-triazole-3-thione 2; 5-(pyridin-4-yl)-1,2-dihydro-3H-1,2,4-triazole- 3-thione 3; 5-(morpholin-4-ylmethyl)-4-phenyl-2,4- dihydro-3H-1,2,4-triazole-3-thione 4; 4-methyl-5-(mor- pholin-4-ylmethyl)-2,4-dihydro-3H-1,2,4-triazole- 3-thione 5; 4-ethyl-5-(morpholin-4-ylmethyl)-2,4-di- hydro-3H-1,2,4-triazole-3-thione 6; 5-(morpholin-4- ylmethyl)-2,4-dihydro-3H-1,2,4-triazole-3-thione 7; 5-(2-methoxyphenyl)-2,4-dihydro-3H-1,2,4-triazole- 3-thione 8 were synthesized in the Zaporizhzhia State Medical University at the Department of Natural Sci- ences for Foreign Students and Toxicological Che- mistry, Physical and Colloid Chemistry Department. The composition of compounds was confirmed by elemental analysis and IR, UV, 1H NMR spectroscopy, chromatography with mass spectrometric detection. Fig. 20. Mass-spectra of 5-(2-methoxyphenyl)-2,4-dihydro-3H-1,2,4-triazole-3-thione at different fragmentor voltage (100, 200 V) N N H H N SH N N H N S 208.053908 Da N NH H N S N N H N S 413.08489 Da OMe OMe OMe O Me H2 Fig. 21. The pathways proposed for the dissociation of 5-(2-methoxyphenyl)-2,4-dihydro-3H-1,2,4-triazole-3-thione and theoretical monoisotopic masses of ions at 100 V Table 8 The values of ions m/z of 5-(2-methoxyphenyl)- 2,4-dihydro-3H-1,2,4-triazole-3-thione and the relative abundance at 100 V and 200 V No m/z Relative abundance, % 100 V 1 208.0 100.0 2 413.0 6.2 200 V 1 165.1 5.2 2 176.0 1.1 3 193.0 55.6 4 208.1 41.2 5 413.0 23.2 Журнал органічної та фармацевтичної хімії. – 2020. – Т. 18, вип. 1 (69) 33 ISSN 2518-1548 (Online) ISSN 2308-8303 (Print) Acetonitrile (HPLC gradient grade), formic acid (100 %) were purchased from Merck KGaA (Darmstadt, Germany). Highly purified water (18 MΩ under 25°C) was produced using the Direct Q 3UV Millipore sys- tem (Molsheim, France). Sample solutions. Solutions of compounds 2, 4 – 7 in 50 % acetonitrile and compounds 1, 3, 8 in dime- thyl sulfoxide were prepared by dissolving to the fi- nal concentration of 1 mg/mL. Agilent 1260 Infinity HPLC System (degasser, bi- nary pump, autosampler) with Agilent 6120 single- quadrupole mass-spectrometer and software Open- LAB CDS were used. HPLC-MS conditions: 1) column – ∅4,6 × 30 mm, reversible phase Zorbax SB C18, 1.8 μm; 2) column temperature – 40 oC; 3) eluent А – 0.1% HCOOH in H2O; eluent B – 0.1% HCOOH in СH3CN; isocratic mode (50:50, v/v); 4) the flow rate – 0.4 mL/min; 5) ion source – API-ES; 6) positive polarity; 7) drying gas – nitrogen (rate – 10 L/min); 8) the capillary voltage – 4000 V; 9) scanning in the range of m/z 100 – 1000 and 160 – 1000 for compounds 2, 4 – 7 and 1, 3, 8, respectively. Conclusions 1. The ESI mass spectra of eight 1,2,4-triazolethi- ones at different fragmentor voltage have been shown. 2. For the first time mass spectra of ESI 1,2,4-tria- zolethiones series, the intermediate materials in the syn- thesis of active pharmaceutical ingredients of phar- maceutical formulations has been interpreted. 3. The fragmentation pathways and patterns of eight 1,2,4-triazolethiones have been proposed. Conflict of interests: authors have no conflict of interests to declare. References 1. Pruglo, Ye. S.; Pohorlyuk, A. Yu.; Parchenko, V. V.; Panasenko, O. I.; Knysh, Ye. G. Antiviral activity of trifuzol for the broiler at poultry farm. Zaporozhye Medical Journal 2016, (1(94)), 77 – 80. https://doi.org/10.14739/2310-1210.2016.1.64062. 2. Бушуєва, І. В.; Березовський, А. В.; Книш, Є. Г.; Панасенко, О. І. Застосування препарату «Авесстим» для підвищення ефективності вакцинопро- філактики та вплив препарату на резистентність курчат. ScienceRise 2014, 4 (1(4)), 94 – 97. https://doi.org/10.15587/2313-8416.2014.29279. 3. Каплаушенко, А. Г. Дослідження зі створення нового оригінального вітчизняного лікарського засобу на основі 1,2,4-тріазолу. Науко- вий журнал МОЗ України 2013, 2(3), 115 – 121. 4. Varynskyi, B. O.; Kaplaushenko, A. G. Optimization of the detection conditions for the series of 1,2,4-triazole-3-thiones for FIA-ESI-MS and HPLC- ESI-MS. News of Pharmacy 2016, (1(85)), 7 – 11. https://doi.org/10.24959/nphj.16.2063. 5. Варинський, Б. О. Вивчення методом ВЕРХ-ДМД-МС закономірностей утримування ряду 1,2,4-тріазол-3-тіонів – напівпродуктів у син- тезі активних фармацевтичних інгредієнтів. Фармаком 2016, (1), 32 – 40. 6. Варинський, Б. О.; Каплаушенко, А. Г.; Малецький, М. М.; Тімошик, Ю. В. Вивчення закономірностей мас-спектрометричного розпаду гідра- зидів деяких органічних кислот та їх відповідних гідразинокарботіоамідів. Український біофармацевтичний журнал 2015, (6(41)), 60 – 71. 7. Eswaran, S.; Adhikari, A. V.; Shetty, N. S. Synthesis and antimicrobial activities of novel quinoline derivatives carrying 1,2,4-triazole moiety. Eur. J. Med. Chem. 2009, 44 (11), 4637 – 4647. https://doi.org/10.1016/j.ejmech.2009.06.031. 8. Economou, A.; Botitsi, H.; Antoniou, S.; Tsipi, D. Determination of multi-class pesticides in wines by solid-phase extraction and liquid chromatog- raphy-tandem mass spectrometry. J. Chromatogr. A 2009, 1216 (31), 5856 – 5867. https://doi.org/10.1016/j.chroma.2009.06.031. 9. Salionov, V. A.; Varynskyi, B. A.; Parchenko, V. V. Mass-spectrometric fragmentation of sodium 2-(4-methyl-5-(thiophene-2-yl)-4H-1,2,4-triazole- 3-ylthio)acetate. Zaporozhye Medical Journal 2015, (5(92)), 93 – 96. https://doi.org/10.14739/2310-1210.2015.5.53774. 10. Gonsalves, A. R.; Pineiro, M.; Martins, J. M.; Barata, P. A.; Menezes, J. C. Identification of Alprazolam and its degradation products using LC-MS-MS. ARKIVOC 2010, 2010 (5), 128 – 141. https://doi.org/10.3998/ark.5550190.0011.513. Received: 06. 09. 2019 Revised: 20. 01. 2020 Accepted: 27. 02. 2020 N N H H N SH N N H N S 208.053908 Da N NH H N S N N H N S 413.08489 Da OMe OMe OMe O Me N N H H N 176.081838 Da OMe HN N H N 165.089663 Da O HN N N 193.030433 Da O S HN N H N 176.027694 Da C S H2 H2 H2 Fig. 22. The pathways proposed for the dissociation of 5-(2-methoxyphenyl)-2,4-dihydro-3H-1,2,4-triazole-3-thione and theoretical monoisotopic masses of ions at 200 V The research was carried out according to the budget theme of the Ministry of Public Health of Ukraine “Development, validation of analysis procedures for API – 1,2,4-triazole derivatives using chromatography and mass-spectrometry” (the state registration No. 011611005829; the research period 2016 – 2020).
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spelling oai:ojs.journals.uran.ua:article-1776132026-08-24T18:04:29Z ESI-MS fragmentation pathways of some 1,2,4-triazole-3-thiones, the intermediate compounds in the synthesis of active pharmaceutical ingredients Пути ЭСИ-MС фрагментации некоторых 1,2,4-триазол-3-тионов, промежуточных продуктов при синтезе активных фармацевтических ингредиентов Шляхи ЕСI-MС фрагментації деяких 1,2,4-триазол-3-тіонів, проміжних продуктів при синтезі активних фармацевтичних інгредієнтів Varynskyi, Borys O. Kaplaushenko, Andriy G. mass spectrometry high performance liquid chromatography 1 2 4-triazole-3-thiones UDC 547.792 543.51 мас-спектрометрія високоефективна рідинна хроматографія 1 2 4-триазол-3-тіони УДК 547.792 543.51 масс-спектрометрия высокоэффективная жидкостная хроматография 1 2 4-триазол-3-тионы УДК 547.792 543.51 Aim. To determine the fragmentation pathways of eight 1,2,4-triazole-3-thiones, which are intermediate products in the synthesis of active pharmaceutical ingredients of potential and registered pharmaceutical formulations.Results and discussion. HPLC-MS analysis of eight 1,2,4-triazole-3-thiones, which are intermediate products in the synthesis of salts of 1,2,4-triazolylthioacetate acids, has been carried out; the mass spectra of the compounds to be analyzed have been registered in ESI-mode with different fragmentor voltage (0, 100, 200 V). The fragmentation pathways and patterns of ion decay for compounds to be analyzed have been proposed.Experimental part. Agilent 1260 Infinity HPLC System with Agilent 6120 mass spectrometer were used. HPLC-MS conditions: column – 4,6 × 30 mm, reversible phase Zorbax SB C18, 1.8 μm, 40 oC; mobile phase – 0.1 % HCOOH in H2O and 0.1 % HCOOH in СH3CN in isocratic mode (50:50, v/v); the flow rate – 0.4 mL/min; ion source – API-ES; positive polarity; drying gas – nitrogen (rate – 10 L/min); the capillary voltage – 4000 V; scanning in the range of m/z 100 – 1000.Conclusions. For the first time it has been interpreted the mass spectra of 1,2,4-triazole-3-thiones series, the intermediate compounds in the synthesis of active pharmaceutical ingredients of pharmaceutical formulations. The fragmentation pathways and patterns of eight 1,2,4-triazole-3-thiones have been shown. Received: 06.09.2019Revised: 20.01.2020Accepted: 27.02.2020 Цель. Определить пути фрагментации восьми 1,2,4-триазол-3-тионов, являющихся промежуточными продуктами в синтезе активных фармацевтических ингредиентов потенциальных и зарегистрированных фармацевтических препаратов.Результаты и их обсуждение. Проведен ВЭЖХ-МС анализ восьми 1,2,4-триазол-3-тионов, являющихся промежуточными продуктами при синтезе солей 1,2,4-триазолилтиоацетатних кислот; масс-спектры исследуемых соединений зарегистрированы в ЭСИ-режиме с различным напряжением фрагментатора (0, 100, 200 В). Предложены пути фрагментации и закономерности распада ионов для исследуемых соединений.Экспериментальная часть. Для исследований использована система HPLC Agilent 1260 Infinity с масс-спектрометром Agilent 6120. ВЭЖХ-МС условия: колонка – ∅ 4,6 × 30 мм, обращенная фаза Zorbax SB C18, 1,8 μm, 40 oC; подвижная фаза – 0,1 % HCOOH в H2O и 0,1 % HCOOH в СH3CN в изократическом режиме (50:50, v/v); скорость потока – 0,4 мл/мин; источник ионов – API-ES; позитивная полярность; газ-осушитель – азот (скорость – 10 л/мин); напряжение капилляра – 4000 V; сканирование в диапазоне m/z 100 – 1000.Выводы. Впервые интерпретированы масс-спектры серии 1,2,4-триазол-3-тионов, промежуточных продуктов при синтезе активных фармацевтических ингредиентов фармацевтических препаратов. Показаны пути фрагментации и распада восьми 1,2,4-триазол-3-тионов. Received: 06.09.2019Revised: 20.01.2020Accepted: 27.02.2020 Мета. Визначити шляхи фрагментації восьми 1,2,4-триазол-3-тіонів, які є проміжними продуктами в синтезі активних фармацевтичних інгредієнтів потенційних та зареєстрованих фармацевтичних препаратів.Результати та їх обговорення. Проведено ВЕРХ-МС аналіз восьми 1,2,4-триазол-3-тіонів, які є проміжними продуктами при синтезі солей 1,2,4-триазолілтіоацетатних кислот; мас-спектри досліджуваних сполук зареєстровано в ЕСІ-режимі з різною напругою фрагментатора (0, 100, 200 В). Запропоновано шляхи фрагментації та закономірності розпаду іонів для аналізованих сполук.Експериментальна частина. Для досліджень використано систему HPLC Agilent 1260 Infinity з мас-спектрометром Agilent 6120. ВЕРХ-МС умови: колонка –∅ 4,6 × 30 мм, обернена фаза Zorbax SB C18, 1,8 μm, 40 oC; рухома фаза – 0,1 % HCOOH в H2O та 0,1 % HCOOH в СH3CN в ізократичному режимі (50:50, v/v); швидкість потоку – 0,4 мл/хв; джерело іонів – API-ES; позитивна полярність; газ-осушувач – азот (швидкість – 10 л/хв); напруга капіляра – 4000 V; сканування в діапазоні m/z 100 – 1000.Висновки. Вперше інтерпретовано мас-спектри серії 1,2,4-триазол-3-тіонів, проміжних сполук при синтезі активних фармацевтичних інгредієнтів фармацевтичних препаратів. Показано шляхи фрагментації та розпаду восьми 1,2,4-триазол-3-тіонів. Received: 06.09.2019Revised: 20.01.2020Accepted: 27.02.2020 National University of Pharmacy 2020-03-05 Article Article application/pdf https://ophcj.nuph.edu.ua/article/view/ophcj.20.177613 10.24959/ophcj.20.177613 Journal of Organic and Pharmaceutical Chemistry; Vol. 18 No. 1(69) (2020); 22-33 Журнал органической и фармацевтической химии; Том 18 № 1(69) (2020); 22-33 Журнал органічної та фармацевтичної хімії; Том 18 № 1(69) (2020); 22-33 2518-1548 2308-8303 en https://ophcj.nuph.edu.ua/article/view/ophcj.20.177613/198315 Copyright (c) 2020 Borys O. Varynskyi, Andriy G. Kaplaushenko https://creativecommons.org/licenses/by/4.0
spellingShingle мас-спектрометрія
високоефективна рідинна хроматографія
1
2
4-триазол-3-тіони
УДК 547.792
543.51
Varynskyi, Borys O.
Kaplaushenko, Andriy G.
Шляхи ЕСI-MС фрагментації деяких 1,2,4-триазол-3-тіонів, проміжних продуктів при синтезі активних фармацевтичних інгредієнтів
title Шляхи ЕСI-MС фрагментації деяких 1,2,4-триазол-3-тіонів, проміжних продуктів при синтезі активних фармацевтичних інгредієнтів
title_alt ESI-MS fragmentation pathways of some 1,2,4-triazole-3-thiones, the intermediate compounds in the synthesis of active pharmaceutical ingredients
Пути ЭСИ-MС фрагментации некоторых 1,2,4-триазол-3-тионов, промежуточных продуктов при синтезе активных фармацевтических ингредиентов
title_full Шляхи ЕСI-MС фрагментації деяких 1,2,4-триазол-3-тіонів, проміжних продуктів при синтезі активних фармацевтичних інгредієнтів
title_fullStr Шляхи ЕСI-MС фрагментації деяких 1,2,4-триазол-3-тіонів, проміжних продуктів при синтезі активних фармацевтичних інгредієнтів
title_full_unstemmed Шляхи ЕСI-MС фрагментації деяких 1,2,4-триазол-3-тіонів, проміжних продуктів при синтезі активних фармацевтичних інгредієнтів
title_short Шляхи ЕСI-MС фрагментації деяких 1,2,4-триазол-3-тіонів, проміжних продуктів при синтезі активних фармацевтичних інгредієнтів
title_sort шляхи есi-mс фрагментації деяких 1,2,4-триазол-3-тіонів, проміжних продуктів при синтезі активних фармацевтичних інгредієнтів
topic мас-спектрометрія
високоефективна рідинна хроматографія
1
2
4-триазол-3-тіони
УДК 547.792
543.51
topic_facet mass spectrometry
high performance liquid chromatography
1
2
4-triazole-3-thiones
UDC 547.792
543.51
мас-спектрометрія
високоефективна рідинна хроматографія
1
2
4-триазол-3-тіони
УДК 547.792
543.51
масс-спектрометрия
высокоэффективная жидкостная хроматография
1
2
4-триазол-3-тионы
УДК 547.792
543.51
url https://ophcj.nuph.edu.ua/article/view/ophcj.20.177613
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