alternativeАльтернативная энергетика и экология (ISJAEE)Alternative Energy and Ecology (ISJAEE)1608-8298Международный издательский дом научной периодики "Спейс10.15518/isjaee.2017.31-36.024-035alternative-1242Research ArticleВОДОРОДНАЯ ЭКОНОМИКАHYDROGEN ECONOMYИССЛЕДОВАНИЕ ПРОТОННОЙ ПРОВОДИМОСТИ КОМПОЗИТНЫХ МЕТАЛЛОКЕРАМИЧЕСКИХ МАТЕРИАЛОВ НА ОСНОВЕ ВОЛЬФРАМАТОВ НЕОДИМА ЧЕТЫРЕХЭЛЕКТРОДНЫМ МЕТОДОМ С ИОННЫМИ ЗОНДАМИSTUDY OF TRANSPORT PROPERTIES OF COMPOSITE METAL-CERAMIC MEMBRANE MATERIALS FOR SELECTIVE SEPARATION OF HYDROGENhttps://orcid.org/0000-0002-8209-533УваровН. Ф.UvarovN. F.

д-р хим. наук, главный научный сотрудник, зав. лабораторией Института химии твердого тела и механохимии СО РАН (Новосибирск); профессор, зав. кафедрой Новосибирского государственного технического университета; профессор Ново- сибирского государственного университета

ResearcherID: A-5031-2014

SPIN-код: 8137-4513,

AuthorID: 33743

D.Sc. in Chemistry, Head Research Scientist, Head of the Laboratory at the Institute of Solid State Chemistry and Mechanochemistry, SB RAS; Professor, Head of Department of Novosibirsk State Technical University; Professor at Novosibirsk State University

ResearcherID: A-5031-2014

SPIN-код: 8137-4513,

AuthorID: 33743

uvarov@solid.nsc.ruУлихинА. С.UlihinA. S.

канд. хим. наук, старший научный сотрудник лаборатории неравновесных твердофазных систем Института химии твердого тела и меха- нохимии СО РАН (Новосибирск)

Researcher ID: P-1187-2017

SPIN-код: 2810-7309

Ph.D. in Chemistry, Senior Researcher at the Laboratory of Nonequilibrium Solid-Phase Systems of the Institute of Solid State Chemistry and Mechanochemistry of the SB RAS

Researcher ID: P-1187-2017

SPIN-код: 2810-7309

uvarov@solid.nsc.ruhttps://orcid.org/0000-0003-0995-1526БеспалкоЮ. Н.BespalkoYu. N.

канд. хим. наук, научный сотрудник Лаборатории катализаторов глубокого окисления Института катализа СО РАН (Новосибирск)

ResearcherID: D-2058-2014

SPIN-код: 4097-5494,

AuthorID: 180559

Ph.D. in Chemistry, Research Scientist of Laboratory of Catalysts of Deep Oxidation, Boreskov Institute of Catalysis SB RAS

ResearcherID: D-2058-2014

SPIN-код: 4097-5494,

AuthorID: 180559

uvarov@solid.nsc.ruЕремеевН. Ф.EremeevN. F.

канд. хим. наук, научный сотрудник Института катализа СО РАН

Researcher ID: D-7148-2012

РИНЦ: 642122

Scopus: 55645818400

Ph.D. in Chemistry, Researcher, Boreskov Institute of Catalysis SB RAS

Researcher ID: D-7148-2012

РИНЦ: 642122

Scopus: 55645818400

uvarov@solid.nsc.ruКрасновА. В.KrasnovA. V.

младший научный сотрудник Института катализа СО РАН

Junior Researcher at the Boreskov Institute of Catalysis SB RAS

 

uvarov@solid.nsc.ruhttps://orcid.org/0000-0003-0866-8788СкрябинП. И.SkriabinP. I.

аспирант, младший научный сотрудник Института катализа СО РАН

ResearcherID: O-5095-2016

SPIN-код: 2282-4707

Ph.D. Student, Junior Researcher at the Boreskov Institute of Сatalysis SB RAS

ResearcherID: O-5095-2016

SPIN-код: 2282-4707

uvarov@solid.nsc.ruhttps://orcid.org/0000-0003-2404-0325СадыковВ. А.SadykovV. A.

д-р хим. наук, главный научный сотрудник, зав. лабораторией Института катализа СО РАН (Новосибирск); зав. лаб., профессор Новосибирского государственного университета; член Американского химического общества и Общества по изучению свойств материалов

Researcher ID: F-9131-2012

D.Sc. in Chemistry, Chief Research Scientist, Head of the Laboratory at the Boreskov Institute of Catalysis SB RAS; Professor and Head of Laboratory of Novosibirsk State University; a Member of American Chemical Society and Materials Research Society

Researcher ID: F-9131-2012

uvarov@solid.nsc.ruИнститут химии твердого тела и механохимии СО РАН; Новосибирский государственный университет; Новосибирский государственный технический университетРоссияInstitute of Solid State Chemistry and Mechanochemistry SB RAS; Novosibirsk State University; Novosibirsk State Technical UniversityRussian FederationИнститут химии твердого тела и механохимии СО РАНРоссияInstitute of Solid State Chemistry and Mechanochemistry SB RASRussian FederationИнститут катализа им. Борескова СО РАНРоссияBoreskov Institute of Catalysis SB RASRussian FederationНовосибирский государственный университет; Институт катализа им. Борескова СО РАНРоссияNovosibirsk State University; Boreskov Institute of Catalysis SB RASRussian Federation201728012018031-362435Copyright © Международный издательский дом научной периодики "Спейс, 20182018Международный издательский дом научной периодики "СпейсМеждународный издательский дом научной периодики "Спейсhttps://www.isjaee.com/jour/about/submissions#copyrightNoticehttps://www.isjaee.com/jour/article/view/1242

Синтезированы керамические твердые протонные электролиты La0,99Ca0,01NbO4, Nd5,5WO11,25-δ и Nd5,5W0,5Mo0.5O11,25-δ , измерена протонная проводимость этих электролитов при температуре 300–650 оС в атмосфере сухого и влажного воздуха. Показано, что твердые электролиты обладают высокой протонной проводимостью ~ 10-4 См/см при 500 оC. Методом горячего прессования в атмосфере аргона изготовлены плотные металлокерамические материалы состава Ni0,5Cu0,5+Nd5,5WO11,25- δ и Ni0,5Cu0,5+Nd5,5W0,5Mo0,5O11,25-δ , которые обладают общей проводимостью, типичной для металлов. При исследовании свойств металлокерамических материалов возникает проблема экспериментального определения вклада ионной (в данном случае протонной) проводимости в общую проводимость материала. Значения протонной проводимости могут быть оценены по результатам изучения водородной проницаемости мембран и диффузии водорода, однако эти методы достаточно сложны в аппаратурном исполнении, поэтому наиболее актуальными в данном случае являются относительно простые и доступные электрофизические методы. Впервые проведены измерения парциальной протонной проводимости полученных композитных материалов в 4-электродной ячейке с помощью ионных зондов, изготовленных из керамического протонного проводника La0,99Ca0,01NbO4 в атмосфере влажного водорода при температуре 300–650 оС. В области низких температур значения парциальной протонной проводимости, измеренные в 4-электродной ячейке, хорошо согласуются с аналогичными значениями, полученными при стандартных измерениях комплексного импеданса исходных керамик, не содержащих металлов, в то время как в области высоких температур значения, полученные различными методами, расходятся. Это расхождение может быть объяснено вкладом электрохимической реакции, протекающей на границе раздела фаз ионный зонд/металл и сопровождающейся растворением атомарного водорода в металле. В общем случае измеряемое значение ионной проводимости может быть как занижено, так и завышено по сравнению с реальным значением в зависимости от скорости химических реакций, протекающих на электродах. Тем не менее в ограниченной области температур использование 4-х электродных измерений с протонными зондами позволяет получить корректные результаты.

 

Ceramic solid proton electrolytes La0,99Ca0,01NbO4, Nd5,5WO11,25-δ и Nd5,5W0,5Mo0.5O11,25-δ were synthesized and their proton conductivity was measured in the temperature range of 300-650 оС in an atmosphere of dry and humid air. Solid electrolytes are shown to have a high proton conductivity ~ 10-4 S/cm at 500 оС. Dense metal-ceramic composites containing phases of metal Ni0,5Cu0,5 and oxides Nd5.5WO11.25 or Nd5.5W0.5Mo0.5O11.25-δ with the typical total conductivity of metals were obtained using hot pressing technique an argon atmosphere. The problem arises with an experimental determination of the ionic (in this case proton) conductivity contribution to the overall conductivity of the material comprises when studying the metal-ceramic materials properties. The proton conductivity values can be estimated from the results of studying the hydrogen permeability of membranes and the diffusion of hydrogen; however, these methods are rather complicated in instrumentation. Therefore the use of relatively simple and accessible electrical measurement methods to solve this problem is very relevant. In this paper, the partial proton conductivity of the composite materials mentioned above was first measured using a 4-electrode cell with ion probes made of a ceramic proton conductor La0,99Ca0,01NbO4in an atmosphere of moist hydrogen and at the temperature range of 300-650 оC. In the low temperature region, the partial proton conductivity values measured in the 4-electrode cell are in good agreement with those obtained by standard complex impedance analysis for the pure ceramics not containing metal. In high temperature region, the values obtained by two independent techniques differ. This can be explained by the contribution of the electrochemical reaction proceeding at the interface between the ion probe and the metal phases and accompanied by the dissolution of atomic hydrogen in the metal. In general, the measured value of the ionic conductivity can be either underestimated or overestimated in comparison with the real one, depending on the rate of chemical reactions occurring at the electrodes. Nevertheless, in a limited temperature range, the use of four-electrode measurements with ionic (proton) probes allows one to obtain correct results.

 

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The authors declare that there are no conflicts of interest present.