Katharina Hermainski, Alexander Yakushev, Dominik Dietzel, Christoph Emanuel Düllmann, Jochen Ballof, Pavol Mošat’, Felix Sprunk, Pavel Bartl, Jan John, Jörg Krier, Mojmír Němec, Jon Petter Omtvedt and Jan Štursa
{"title":"钋对石英表面的反应性。","authors":"Katharina Hermainski, Alexander Yakushev, Dominik Dietzel, Christoph Emanuel Düllmann, Jochen Ballof, Pavol Mošat’, Felix Sprunk, Pavel Bartl, Jan John, Jörg Krier, Mojmír Němec, Jon Petter Omtvedt and Jan Štursa","doi":"10.1039/D5CP02381E","DOIUrl":null,"url":null,"abstract":"<p >Beyond the (quasi)stable and abundant elements lead and bismuth, all elements are radioactive, with polonium being the first of a series of radioelements up to primordial uranium. Interest in understanding its chemical behavior is increasing, not least due to its co-production in accelerator-driven systems and high radiotoxicity. Polonium is also the lighter homologue of the superheavy element livermorium, which has not been studied chemically to date. Polonium therefore acts as a benchmark to verify the structure of the periodic table at the heavy-element frontier. Here, we report on gas–solid thermochromatography studies of polonium in the atom-at-a-time regime under helium and hydrogen gas atmospheres. Quartz surfaces with different degrees of hydroxylation were used as a stationary phase. On quartz glass with low OH-concentrations, a volatile species interacting with an adsorption enthalpy of −85<small><sup>+3</sup></small><small><sub>−2</sub></small> kJ mol<small><sup>−1</sup></small> was found and assigned to elemental polonium. On more highly hydroxylated quartz glass, an additional deposition zone due to a species with an adsorption enthalpy of −139<small><sup>+6</sup></small><small><sub>−5</sub></small> kJ mol<small><sup>−1</sup></small> was observed and attributed to a polonium species formed by chemical reactions with the surface. Under our experimental conditions, chemical reactions of polonium in the solid phase dominate over reactions in the gas phase. Thus, the nature of the surface should be considered as an important parameter in future gas chromatography studies.</p>","PeriodicalId":99,"journal":{"name":"Physical Chemistry Chemical Physics","volume":" 40","pages":" 21414-21423"},"PeriodicalIF":2.9000,"publicationDate":"2025-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.rsc.org/en/content/articlepdf/2025/cp/d5cp02381e?page=search","citationCount":"0","resultStr":"{\"title\":\"Reactivity of polonium towards quartz surfaces\",\"authors\":\"Katharina Hermainski, Alexander Yakushev, Dominik Dietzel, Christoph Emanuel Düllmann, Jochen Ballof, Pavol Mošat’, Felix Sprunk, Pavel Bartl, Jan John, Jörg Krier, Mojmír Němec, Jon Petter Omtvedt and Jan Štursa\",\"doi\":\"10.1039/D5CP02381E\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >Beyond the (quasi)stable and abundant elements lead and bismuth, all elements are radioactive, with polonium being the first of a series of radioelements up to primordial uranium. Interest in understanding its chemical behavior is increasing, not least due to its co-production in accelerator-driven systems and high radiotoxicity. Polonium is also the lighter homologue of the superheavy element livermorium, which has not been studied chemically to date. Polonium therefore acts as a benchmark to verify the structure of the periodic table at the heavy-element frontier. Here, we report on gas–solid thermochromatography studies of polonium in the atom-at-a-time regime under helium and hydrogen gas atmospheres. Quartz surfaces with different degrees of hydroxylation were used as a stationary phase. On quartz glass with low OH-concentrations, a volatile species interacting with an adsorption enthalpy of −85<small><sup>+3</sup></small><small><sub>−2</sub></small> kJ mol<small><sup>−1</sup></small> was found and assigned to elemental polonium. On more highly hydroxylated quartz glass, an additional deposition zone due to a species with an adsorption enthalpy of −139<small><sup>+6</sup></small><small><sub>−5</sub></small> kJ mol<small><sup>−1</sup></small> was observed and attributed to a polonium species formed by chemical reactions with the surface. Under our experimental conditions, chemical reactions of polonium in the solid phase dominate over reactions in the gas phase. 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Beyond the (quasi)stable and abundant elements lead and bismuth, all elements are radioactive, with polonium being the first of a series of radioelements up to primordial uranium. Interest in understanding its chemical behavior is increasing, not least due to its co-production in accelerator-driven systems and high radiotoxicity. Polonium is also the lighter homologue of the superheavy element livermorium, which has not been studied chemically to date. Polonium therefore acts as a benchmark to verify the structure of the periodic table at the heavy-element frontier. Here, we report on gas–solid thermochromatography studies of polonium in the atom-at-a-time regime under helium and hydrogen gas atmospheres. Quartz surfaces with different degrees of hydroxylation were used as a stationary phase. On quartz glass with low OH-concentrations, a volatile species interacting with an adsorption enthalpy of −85+3−2 kJ mol−1 was found and assigned to elemental polonium. On more highly hydroxylated quartz glass, an additional deposition zone due to a species with an adsorption enthalpy of −139+6−5 kJ mol−1 was observed and attributed to a polonium species formed by chemical reactions with the surface. Under our experimental conditions, chemical reactions of polonium in the solid phase dominate over reactions in the gas phase. Thus, the nature of the surface should be considered as an important parameter in future gas chromatography studies.
期刊介绍:
Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions.
The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.