Dr. Anusree Sundar, Dr. Nataliya V. Maksimchuk, Dr. Irina D. Ivanchikova, Dr. Olga V. Zalomaeva, Dr. Danica Bajuk-Bogdanović, Prof. Oxana A. Kholdeeva, Prof. Gordana Ćirić-Marjanović, Dr. Bassem S. Bassil, Prof. Ulrich Kortz
{"title":"用于基于 H2O2 的均相、异相和双相氧化催化的含过氧 Zr/Hf Wells-Dawson 聚氧化金属酸盐","authors":"Dr. Anusree Sundar, Dr. Nataliya V. Maksimchuk, Dr. Irina D. Ivanchikova, Dr. Olga V. Zalomaeva, Dr. Danica Bajuk-Bogdanović, Prof. Oxana A. Kholdeeva, Prof. Gordana Ćirić-Marjanović, Dr. Bassem S. Bassil, Prof. Ulrich Kortz","doi":"10.1002/ceur.202300066","DOIUrl":null,"url":null,"abstract":"<p>Four peroxo-Zr and Hf containing polyanions, [M<sub>2</sub>(O<sub>2</sub>)<sub>2</sub>(X<sub>2</sub>W<sub>17</sub>O<sub>61</sub>)<sub>2</sub>]<sup>16−</sup> (X=P, M=Zr<sup>IV</sup> (<b>ZrP</b>), Hf<sup>IV</sup> (<b>HfP</b>); X=As, M=Zr<sup>IV</sup> (<b>ZrAs</b>), Hf<sup>IV</sup> (<b>HfAs</b>) were synthesized and structurally characterized. The structures consist of two monolacunary Wells-Dawson ions which are connected head-on <i>via</i> two side-on peroxo bridges. The four new polyanions are solution-stable as shown by <sup>31</sup>P NMR, Raman and FT-IR spectroscopic studies. Comparative studies on alcohol oxidation with a solvent- and phase-transfer catalyst-free biphasic oxidative system with homogeneous and supported-catalyst were performed and several noteworthy observations in reactivity and selectivity were observed, such as the highly selective ring-opening oxidation of cyclohexanol to adipic acid. Tetra-<i>n</i>-butylammonium salts of <b>ZrP</b> and <b>HfP</b> were also synthesized to study the catalytic activity of the compounds in the homogenous H<sub>2</sub>O<sub>2</sub>-based oxidation of olefins, <i>α</i>,<i>β</i>-unsaturated carbonyl compounds, and thioethers in organic solvent.</p>","PeriodicalId":100234,"journal":{"name":"ChemistryEurope","volume":"2 1","pages":""},"PeriodicalIF":0.0000,"publicationDate":"2023-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ceur.202300066","citationCount":"0","resultStr":"{\"title\":\"Peroxo-Zr/Hf-Containing Wells-Dawson Polyoxometalates for H2O2-based Homogeneous, Heterogeneous, and Biphasic Oxidation Catalysis\",\"authors\":\"Dr. Anusree Sundar, Dr. Nataliya V. Maksimchuk, Dr. Irina D. Ivanchikova, Dr. Olga V. Zalomaeva, Dr. Danica Bajuk-Bogdanović, Prof. Oxana A. Kholdeeva, Prof. Gordana Ćirić-Marjanović, Dr. Bassem S. Bassil, Prof. Ulrich Kortz\",\"doi\":\"10.1002/ceur.202300066\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p>Four peroxo-Zr and Hf containing polyanions, [M<sub>2</sub>(O<sub>2</sub>)<sub>2</sub>(X<sub>2</sub>W<sub>17</sub>O<sub>61</sub>)<sub>2</sub>]<sup>16−</sup> (X=P, M=Zr<sup>IV</sup> (<b>ZrP</b>), Hf<sup>IV</sup> (<b>HfP</b>); X=As, M=Zr<sup>IV</sup> (<b>ZrAs</b>), Hf<sup>IV</sup> (<b>HfAs</b>) were synthesized and structurally characterized. The structures consist of two monolacunary Wells-Dawson ions which are connected head-on <i>via</i> two side-on peroxo bridges. The four new polyanions are solution-stable as shown by <sup>31</sup>P NMR, Raman and FT-IR spectroscopic studies. Comparative studies on alcohol oxidation with a solvent- and phase-transfer catalyst-free biphasic oxidative system with homogeneous and supported-catalyst were performed and several noteworthy observations in reactivity and selectivity were observed, such as the highly selective ring-opening oxidation of cyclohexanol to adipic acid. Tetra-<i>n</i>-butylammonium salts of <b>ZrP</b> and <b>HfP</b> were also synthesized to study the catalytic activity of the compounds in the homogenous H<sub>2</sub>O<sub>2</sub>-based oxidation of olefins, <i>α</i>,<i>β</i>-unsaturated carbonyl compounds, and thioethers in organic solvent.</p>\",\"PeriodicalId\":100234,\"journal\":{\"name\":\"ChemistryEurope\",\"volume\":\"2 1\",\"pages\":\"\"},\"PeriodicalIF\":0.0000,\"publicationDate\":\"2023-12-20\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ceur.202300066\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ChemistryEurope\",\"FirstCategoryId\":\"1085\",\"ListUrlMain\":\"https://onlinelibrary.wiley.com/doi/10.1002/ceur.202300066\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"\",\"JCRName\":\"\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ChemistryEurope","FirstCategoryId":"1085","ListUrlMain":"https://onlinelibrary.wiley.com/doi/10.1002/ceur.202300066","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"","JCRName":"","Score":null,"Total":0}
Peroxo-Zr/Hf-Containing Wells-Dawson Polyoxometalates for H2O2-based Homogeneous, Heterogeneous, and Biphasic Oxidation Catalysis
Four peroxo-Zr and Hf containing polyanions, [M2(O2)2(X2W17O61)2]16− (X=P, M=ZrIV (ZrP), HfIV (HfP); X=As, M=ZrIV (ZrAs), HfIV (HfAs) were synthesized and structurally characterized. The structures consist of two monolacunary Wells-Dawson ions which are connected head-on via two side-on peroxo bridges. The four new polyanions are solution-stable as shown by 31P NMR, Raman and FT-IR spectroscopic studies. Comparative studies on alcohol oxidation with a solvent- and phase-transfer catalyst-free biphasic oxidative system with homogeneous and supported-catalyst were performed and several noteworthy observations in reactivity and selectivity were observed, such as the highly selective ring-opening oxidation of cyclohexanol to adipic acid. Tetra-n-butylammonium salts of ZrP and HfP were also synthesized to study the catalytic activity of the compounds in the homogenous H2O2-based oxidation of olefins, α,β-unsaturated carbonyl compounds, and thioethers in organic solvent.
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