Promotion of mixed protonic-electronic transport in La5.4WO11.1-δ membranes under H2S atmospheres

被引：3

作者：

Escolastico, S. ^{[1
,4
]}

Balaguer, M. ^{[1
]}

Solis, C. ^{[2
]}

Toldra-Reig, F. ^{[1
]}

Somacescu, S. ^{[3
]}

Gerhards, U. ^{[4
]}

Aguadero, A. ^{[5
]}

Haas-Santo, K. ^{[4
]}

Dittmeyer, R. ^{[4
]}

Serra, J. M. ^{[1
]}

机构：

[1] Univ Politecn Valencia, Consejo Super Invest Cient, Inst Tecnol Quim, Avda Los Naranjos S-N, Valencia 46022, Spain

[2] Helmholtz Zentrum Hereon, German Engn Mat Sci Ctr GEMS, Heinz Maier Leibnitz Zentrum MLZ, D-85748 Garching, Germany

[3] Romanian Acad, Ilie Murgulescu Inst Phys Chem, Spl Independentei 202, Bucharest 060021, Romania

[4] Karlsruhe Inst Technol, IMVT, D-76344 Eggenstein Leopoldshafen, Germany

[5] Imperial Coll, Dept Mat, London SW7 2AZ, England

来源：

JOURNAL OF MATERIALS CHEMISTRY A | 2023年 / 11卷 / 32期

关键词：

HYDROGEN PERMEATION; SEPARATION PERFORMANCE; H-2; SEPARATION; SULFUR; PEROVSKITES; SULFIDATION; TOLERANCE; STABILITY; CONDUCTOR; METHANE;

D O I：

10.1039/d3ta01827j

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

Catalytic membrane reactors (CMR) based on H-2-separation membranes can improve the performance of thermodynamically-limited reactions such as high-pressure steam methane reforming, ammonia cracking, non-oxidative aromatics production, and water gas shift reaction (WGS). In these industrial processes, the membrane surfaces are typically exposed to steam, CO2, CO, H2S, and hydrocarbons in combination with high temperatures. Therefore, the membrane materials require long-term thermo-chemical stability under the mentioned conditions. Stability in H2S is of outstanding importance since its presence, even at ppm level, gives rise to substantial surface poisoning and decomposition of most materials. Here we characterize the influence of H2S on the crystalline structure, lattice composition, and hydrogen-transport properties of La5.4WO11.1-& delta;, one of the reference protonic membrane materials. The incorporation of sulfide ions in the crystal lattice is ascertained from XRD, XPS, FESEM, WDS, EDS, and FIB-SIMS analyses. UV-vis spectroscopy and EIS measurements illustrate the effect of the incorporated sulfur in the transport properties, i.e., vigorously promoting the electronic conductivity mediated by the concurrent partial reduction of tungsten cations (W6+). The rise in electronic conductivity allowed an H-2 flux of 0.042 mL cm(-2) min(-1) to be reached at 700 & DEG;C for a & SIM;700 & mu;m-thick membrane, in contrast with negligible H-2 permeation in H2S-free conditions.

引用

页码：17246 / 17256

页数：11