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US 2011 0217623A1 (19) United States (12) Patent Application Publication (10) Pub. No.: US 2011/0217623 A1 Jiang et al. (43) Pub. Date: Sep. 8, 2011 (54) PROTON EXCHANGEMEMBRANE FOR Related U.S. Application Data FUEL CELL APPLICATIONS (60) Provisional application No. 61/050,368, filed on May (75) Inventors: San Ping Jiang, Singapore (SG); 5, 2008. Haolin Tang, Singapore (SG); Ee O O Ho Tang, Singapore (SG); Shanfu Publication Classification Lu, Singapore (SG) (51) Int. Cl. HOLM 8/2 (2006.01) DEFENCE SCIENCE & BOSD 5/12 (2006.01) TECHNOLOGY AGENCY, Singapore (SG) (52) U.S. Cl. ............................ 429/495; 521/27; 427/115 (21) Appl. No.: 12/991,377 (57) ABSTRACT (22) PCT Filed: May 5, 2009 The present invention refers to an inorganic proton conduct ing electrolyte consisting of a mesoporous crystalline metal (86). PCT No.: PCT/SG2O09/OOO160 oxide matrix and a heteropolyacid bound within the mesopo rous matrix. The present invention also refers to a fuel cell S371 (c)(1), including Such an electrolyte and methods for manufacturing (2), (4) Date: May 24, 2011 Such inorganic electrolytes. b are: er sai. ss. Silica - HPw - a H' transfer through HPW (E~13.02) -----> H transfer through Silica (E-54.88) Patent Application Publication Sep. 8, 2011 Sheet 1 of 17 US 2011/0217623 A1 F.G. 1 FG. 2 A1 With 35% HPW - with 15% HPW wo- with 20% HPW on with 25% HPW - with 35% HPW with 15% HPW With 20% HPW With 15% HPW O 1 2 3 4 5 6 7 8 2 theta / degree Patent Application Publication Sep. 8, 2011 Sheet 2 of 17 US 2011/0217623 A1 FG. 3 -- with 15% HAP -- with 20% HAP was we with 25%HAP i . .2 0.4 0.6 0.8 Relative Pressure PIP, 0.5 O 5 10 15 20 25 30 35 40 Pore diameter / nm FG. 4 0.2O O.15 i O.10 O.05 OOO O 50 1 OO 150 2OO Immersing time ?h Patent Application Publication Sep. 8, 2011 Sheet 3 of 17 US 2011/0217623 A1 F.G. 5 Temperature f 'C 50 1OO 150 200 3OO 350 E 9 E. S 0.01 O.O1 O O humidified G 100°C O.OO1 O.OO1 3.5 3.O 2.5 2.O 15 1000 | T 1 K Patent Application Publication Sep. 8, 2011 Sheet 4 of 17 US 2011/0217623 A1 F.G. 6 Preterated Siiga "HO-SiOS-OH, Multiphase self-asserably . to : Patent Application Publication Sep. 8, 2011 Sheet 5 of 17 US 2011/0217623 A1 FIG. 7 Temperature I'C 100 75 50 25 E= 13.02 kJ mol 1E3 N o E=36.27 kJ mol 1E-61 2.6 2.7 2.8 2.9 3.0 3.1 3.2 3.3 3.4 1000 T 1 K FG. 8 E E s b age Silica - HPW - N H transfer through HPW (E-13.02) -----> H transfer through Silica (E-54.88) Patent Application Publication Sep. 8, 2011 Sheet 6 of 17 US 2011/0217623 A1 FG. 9 1079, re-O 889.W-o-W 1400 120 1000 OC 60 400 200 Wavenumber 1 cm FIG 10 r" Before site c. 4 3 2 5 2.0 Q 1 nm' Patent Application Publication Sep. 8, 2011 Sheet 7 of 17 US 2011/0217623 A1 FIG 11 2D hexagonal Body-centered 3D Face-centered 3D Bicontinues 3D P6mm Im3m Fm3m a3d i . r a 100 oo oz o.4 os os 10 Relative pressure / P/Po Pore size / nm Patent Application Publication Sep. 8, 2011 Sheet 8 of 17 US 2011/0217623 A1 Patent Application Publication Sep. 8, 2011 Sheet 9 of 17 US 2011/0217623 A1 F.G. 15 Temperature IC 125 100 75 50 25 8 2D hexagonal HPWilsilica # 3D face-centered HPWIsilica 3D body-centered HPWisitica 2.4 2.6 2.8 3.0 3.2 3.4 1000 T 1 K Patent Application Publication Sep. 8, 2011 Sheet 10 of 17 US 2011/0217623 A1 FG 16 O.O.30 0.025A. : 0. O 1 O F.G. 17 AA AAA AA AA AAA A100-c. o O oio O 9 Pie o O o O soc 0.06................... 0.04 on 40 cc 0.02 O.OO : : : : O 10 2O 30 40 50 60 th Patent Application Publication Sep. 8, 2011 Sheet 11 of 17 US 2011/0217623 A1 F.G. 18 Keggin HPW also isosos, oror 'g o3. osos. s 3. structure odoo ascasioso, TEos Eto-S-oet acter c torsstroy Porous N O Meso-silica/HPW -Thin Porous Ni O Eyle Patent Application Publication Sep. 8, 2011 Sheet 12 of 17 US 2011/0217623 A1 F.G. 19 0.20 0.15 y E D 0.12 st s s 9. e y 0.08 O D f s 0.04 a f too o1 o2 o3 o os os 0.00 Current Density I Acm Patent Application Publication Sep. 8, 2011 Sheet 13 of 17 US 2011/0217623 A1 FIG. 20 O.7 (a)a) cell pperformance O.6 9 Y Y - 120 t O.5 s 2 - 100 9. 0.4 s S 8O O C 03 ExxKC - 60 5 O9 0.2 tax SXXi? 40 h -O- 10 Methanol, 80°C O.1 -- 16 M methanol, 80°C al - - 10 Methanol, 300°C - 20 &: -C)- 16M methanol, 300°C O.O O O 1OO 2OO 300 400 500 6OO Current density mA cm b) cell stabili O.50 (b) ty 16M methanol fuel, 300°C v 1.OMethanol fuel, 300°C D N. O.4O ()g O.35 O D is 0.30 O O.25 O.2O O 1O 2O 3O 4.O 50 6O 7O Time I min Patent Application Publication Sep. 8, 2011 Sheet 14 of 17 US 2011/0217623 A1 FG. 21 s O 2OO 400 6OO Current density fmA cm FIG. 22 Patent Application Publication Sep. 8, 2011 Sheet 15 of 17 US 2011/0217623 A1 FG, 23 FG. 24 Á Vacuum Patent Application Publication Sep. 8, 2011 Sheet 16 of 17 US 2011/0217623 A1 FG. 25 CC. -- Polarization curve 140 - Power densi 120 OO 3. S al 9, 8O i s 2. 9 60 3 P S O s 40 B. su 2O O O.O 0.1 0.2 0.3 O.4 0.5 Current density(A cm) a HPW/silica disc b. MEA Patent Application Publication Sep. 8, 2011 Sheet 17 of 17 US 2011/0217623 A1 US 2011/0217623 A1 Sep. 8, 2011 PROTON EXCHANGEMEMBRANE FOR surface of the catalyst is reduced. At high temperatures CO FUEL CELL APPLICATIONS does not constitute a poison for the fuel cell but can instead be used directly as fuel for the high temperature fuel cell. CROSS-REFERENCE TO RELATED 0008 Direct methanol fuel cells also benefit from APPLICATIONS improved oxidation kinetics at elevated temperatures, and 0001. This application claims benefit of priority of U.S. direct ethanol becomes a viable fuel in the range of 150 to provisional application No. 61/050,368, filed May 5, 2008, 300°C. In addition, the thermal enhancement for redox activ the contents of it being hereby incorporated by reference in its ity allows for the exploration of alternative catalysts which do entirety for all purposes. not function well at lower temperatures. 0009. The development of alternative electrocatalysts, FIELD OF THE INVENTION particularly those based on non-precious metal catalysts is 0002 The present invention relates generally to fuel cell critical for the commercial viability of PEMFC technologies. technology, in particular to the field of proton exchange mem Operating at high temperatures has also the advantage of branes for fuel cells operating at elevated temperatures. creating a greater driving force for more efficient cooling. This is particularly important for transport applications to BACKGROUND OF THE INVENTION reduce balance of plant equipment. Furthermore, high grade 0003 Polymer electrolyte fuel cells (PEMFCs), which exhaust heat can be integrated into fuel processing stages. employ proton exchange membranes (PEMs), are considered Operation of a fuel cell at ambient pressure and elevated to be promising Sources of electrical energy. An advantage of temperatures strongly indicates that an optimal high tempera a PEMFC is its high-energy conversion efficiency and sim ture membrane would be one whose proton conductivity is plicity in design, resulting in reliability and convenience. not or less dependent on the presence of water. PEMFCs 0004 APEMFC consists of a proton-conducting polymer based on perfluorosulfonic acid polymer (PFSA) electrolyte membrane, such as Nafion(R), sandwiched between two elec Such as Nafion(R) cannot be operated at temperatures higher trodes. In general, fuel cells generate electricity from a simple than 100°C. Owing to the dehydration or volatility of water at electrochemical reaction in which an oxidizer, typically oxy an elevated temperature. The hydration of the membrane is gen from air, and a fuel, typically hydrogen, combine to form crucial for the PEMFC performance since proton conductiv a product, which is water for the typical fuel cell. Oxygen (air) ity of the sulfonic polymer PEMs decreases drastically under continuously passes over the cathode and hydrogen passes dehydration. over the anode to generate electricity, by-product heat and 0010 Several approaches have been proposed to develop water. The electrolyte that separates the anode and cathode is high-temperature membranes for fuel cell application. One of an ion-conducting material. At the anode, hydrogen and its the approaches is to imbibitions the PFSA membranes with electrons are separated so that the hydrogen ions (protons) hygroscopic inorganic particles such as silica, TiO, or Zeolite pass through the electrolyte while the electrons pass through that could retain wateratelevated temperatures above 100° C.
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  • Experimental Studies on the Dynamic Memcapacitance Modulation of the Reo3@Res2 Composite Material-Based Diode

    Experimental Studies on the Dynamic Memcapacitance Modulation of the Reo3@Res2 Composite Material-Based Diode

    nanomaterials Article Experimental Studies on the Dynamic Memcapacitance Modulation of the ReO3@ReS2 Composite Material-Based Diode Joanna Borowiec 1,2,* , Mengren Liu 3 , Weizheng Liang 4, Theo Kreouzis 2 , Adrian J. Bevan 2 , Yi He 1, Yao Ma 1 and William P. Gillin 1,2 1 College of Physics, Sichuan University, Chengdu 610064, China; [email protected] (Y.H.); [email protected] (Y.M.); [email protected] (W.P.G.) 2 Materials Research Institute and School of Physics and Astronomy, Queen Mary University of London, Mile End Road, London E1 4NS, UK; [email protected] (T.K.); [email protected] (A.J.B.) 3 Sichuan University—Pittsburgh Institute, Chengdu 610207, China; [email protected] 4 The Peac Institute of Multiscale Sciences, Chengdu 610031, China; [email protected] * Correspondence: [email protected]; Tel.: +86-028-854-12323 Received: 4 October 2020; Accepted: 19 October 2020; Published: 23 October 2020 Abstract: In this study, both memcapacitive and memristive characteristics in the composite material based on the rhenium disulfide (ReS2) rich in rhenium (VI) oxide (ReO3) surface overlayer (ReO3@ReS2) and in the indium tin oxide (ITO)/ReO3@ReS2/aluminum (Al) device configuration is presented. Comprehensive experimental analysis of the ReO3@ReS2 material properties’ dependence on the memcapacitor electrical characteristics was carried out by standard as well as frequency-dependent current–voltage, capacitance–voltage, and conductance–voltage studies. Furthermore, determination of the charge carrier conduction model, charge carrier mobility, density of the trap states, density of the available charge carrier, free-carrier concentration, effective density of states in the conduction band, activation energy of the carrier transport, as well as ion hopping was successfully conducted for the ReO3@ReS2 based on the experimental data.