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Advancing oxygen separation:insights from experimental and computational analysis of La_(0.7)Ca_(0.3)Co_(0.3)Fe_(0.6)M_(0.1)O_(3-δ)(M=Cu,Zn)oxygen transport membranes

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Frontiers of Chemical Science and Engineering 2024年第6期18卷 17-29页

作者： Guoxing Chen Wenmei Liu Marc Widenmeyer Xiao Yu Zhijun Zhao songhak yoon Ruijuan Yan Wenjie Xie Armin Feldhoff Gert Homm Emanuel Ionescu Maria Fyta Anke Weidenkaff Fraunhofer Research Institution for Materials Recycling and Resource Strategies IWKS Alzenau 63755Germany Electrochemistry Laboratory Paul Scherrer InstituteVilligen PSI 5232Switzerland Department of Materials and Earth Sciences Materials and ResourcesTechnical University of DarmstadtDarmstadt 64287Germany Institute of Physical Chemistry and Electrochemistry Leibniz University HannoverHannover 30167Germany Institute for Computational Physics University of StuttgartStuttgart 70569Germany Computational Biotechnology RWTH AachenAachen 52074Germany

In this study,perovskite-type La_(0.7)Ca_(0.3)Co_(0.3)Fe_(0.6)M_(0.1)O_(3-δ)(M=Cu,Zn)powders were synthesized using a scalable reverse co-precipitation method,presenting them as novel materials for oxygen transport *** comprehensive study covered various aspects including oxygen permeability,crystal structure,conductivity,morphology,CO_(2) tolerance,and long-term regenerative durability with a focus on phase structure and *** membrane La_(0.7)Ca_(0.3)Co_(0.3)Fe_(0.6)M_(0.1)O_(3-δ)exhibited high oxygen permeation fluxes,reaching up to 0.88 and 0.64 mL·min^(−1)·cm^(−2) under air/He and air/CO_(2) gradients at 1173 K,*** 1600 h of CO_(2) exposure,the perovskite structure remained intact,showcasing superior CO_(2) resistance.A combination of first principles simulations and experimental measurements was employed to deepen the understanding of Cu/Zn substitution effects on the structure,oxygen vacancy formation,and transport behavior of the *** findings underscore the potential of this highly CO_(2)-tolerant membrane for applications in high-temperature oxygen *** enhanced insights into the oxygen transport mechanism contribute to the advancement of next-generation membrane materials.

关键词： perovskite oxygen permeation membrane oxygennionsdiffusiono xygen vacancy formation energy energy barrier

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Tailoring thermoelectric properties of Zr(0.43)Hf(0.57)NiSn half-Heusler compound by defect engineering

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Rare Metals 2020年第6期39卷 659-670页

作者： Krzysztof Galazka Wenjie Xie Sascha Populoh Myriam H.Aguirre songhak yoon Gesine Büttner Anke Weidenkaff Institute of Plasma Physics and Laser Microfusion Warsaw 01-497Poland Department of Materials Science Technische Universitat DarmstadtDarmstadt 64287Germany Laboratory for Solid State Chemistry and Catalysis EmpaDlibendorf 8600Switzerland Instituto de Nanociencia de Aragon Universidad de ZaragozaSaragossa 50018Spain Departamento de Fisica de la Materia Condensada Universidad de ZaragozaSaragossa 50009Spain Laboratorio de Microscopias Avanzadas Universidad de ZaragozaSaragossa 50018Spain Fraunhofer Research Institution for Materials Recycling and Resource Strategies IWKS Hanau 63457Germany

The thermoelectric transport properties of Zr0.43Hf0.57 NiSn half-Heusler compounds were investigated for samples sintered with different spark plasma sintering(SPS)periods:8,32 and 72 *** means of scanning transmission electron microscopy with a highangular annular dark-field detector(STEM-HAADF),it was found that sintering time affected the defect concentration,namely the amount of Ni interstitial atoms,and created locally ordered inclusions of full-Heusler *** structural information,phase composition and electrical transport properties could be consistently explained by the assumption that Ni interstitials give rise to an impurity band situated about 100 meV below the bottom of the conduction band via a self-doping *** impurity band was found to merge with the conduction band for the sample with intermediate SPS *** effect was ascribed to the gradual dissolution of full-Heusler phase inclusions and production of interstitial Ni defects,which eventually vanished for the sample with the longest sintering *** was demonstrated that the modification of the density of states near the edge of the conduction band and enhanced overall charge carrier concentration provided by defect engineering led to overall 26%increase in the thermoelectric figure of merit(ZT)with respect to the other samples.

关键词： Thermoelectric Half-Heusler Interstitial Defect engineering

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