Palladium-Ceria Catalysts with Enhanced Alkaline Hydrogen Oxidation Activity for Anion Exchange Membrane Fuel Cells

被引:70
作者
Bellini, Marco [1 ]
Pagliaro, Maria V. [1 ]
Lenarda, Anna [2 ]
Fornasiero, Paolo [2 ]
Marelli, Marcello [3 ]
Evangelisti, Claudio [3 ]
Innocenti, Massimo [4 ]
Jia, Qingying [5 ]
Mukerjee, Sanjeev [5 ]
Jankovic, Jasna [6 ]
Wang, Lianqin [7 ]
Varcoe, John R. [7 ]
Krishnamurthy, Chethana B. [8 ]
Grinberg, Ilya [8 ]
Davydova, Elena [9 ]
Dekel, Dario R. [9 ,10 ]
Miller, Hamish A. [1 ]
Vizza, Francesco [1 ]
机构
[1] CNR ICCOM, Ist Chim Composti Organometall, Via Madonna del Piano 10, I-50019 Sesto Fiorentino, Italy
[2] Univ Trieste, INSTM, Dept Chem & Pharmaceut Sci, Via L Giorgieri 1, I-34127 Trieste, Italy
[3] CNR, ISTM, Via Camillo Golgi 19, I-20133 Milan, Italy
[4] Univ Firenze, Dipartimento Chim Ugo Schiff, Via Lastruccia 3-13, I-50019 Sesto Fiorentino, Italy
[5] Northeastern Univ, Dept Chem & Chem Biol, Boston, MA 02115 USA
[6] Univ Connecticut, Mat Sci & Engn Dept, Storrs, CT 06269 USA
[7] Univ Surrey, Dept Chem, Guildford GU2 7XH, Surrey, England
[8] Bar Ilan Univ, Dept Chem, IL-52900 Ramat Gan, Israel
[9] Technion Israel Inst Technol, Wolfson Dept Chem Engn, IL-3200003 Haifa, Israel
[10] Technion Israel Inst Technol, Nancy & Stephan Grand Technion Energy Program GTE, IL-3200003 Haifa, Israel
基金
以色列科学基金会; 欧盟地平线“2020”; 英国工程与自然科学研究理事会;
关键词
fuel cells; platinum free; anion exchange membrane; palladium; ceria; W CM(-2); BINDING-ENERGY; ELECTROCATALYSTS; MEDIA; PERFORMANCE; STABILITY; MECHANISM; PLATINUM; ADSORPTION; CARBON;
D O I
10.1021/acsaem.9b00657
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
Anion exchange membrane fuel cells (AEMFCs) offer several important advantages with respect to proton exchange membrane fuel cells, including the possibility of avoiding the use of platinum catalysts to help overcome the high cost of fuel cell systems. Despite such potential benefits, the slow kinetics of the hydrogen oxidation reaction (HOR) in alkaline media and limitations in performance stability (because of the degradation of the anion conducting polymer electrolyte components) have generally impeded AEMFC development. Replacing Pt with an active but more sustainable HOR catalyst is a key objective. Herein, we report the synthesis of a Pd-CeO2/C catalyst with engineered Pd-to-CeO2 interfacial contact. The optimized Pd-CeO2 interfacial contact affords an increased HOR activity leading to >1.4 W cm(-2) peak power densities in AEMFC tests. This is the only Pt-free HOR catalyst yet reported that matches state-of-the-art AEMFC power performances (>1 W cm(-2)). Density functional theory calculations suggest that the exceptional HOR activity is attributable to a weakening of the hydrogen binding energy through the interaction of Pd atoms with the oxygen atoms of CeO2. This interaction is facilitated by a structure that consists of oxidized Pd atoms coordinated by four CeO2 oxygen atoms, confirmed by X-ray absorption spectroscopy.
引用
收藏
页码:4999 / 5008
页数:19
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