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Fe-Modified Pd as an Effective Multifunctional Electrocatalyst for Catalytic Oxygen Reduction and Glycerol Oxidation Reactions in Alkaline Media
ACS Applied Energy Materials ( IF 6.4 ) Pub Date : 2021-09-17 , DOI: 10.1021/acsaem.1c01920
Andrea Cassani 1 , Nazym Tuleushova 1 , Qing Wang 2 , Hazar Guesmi 2 , Valerie Bonniol 1 , Julien Cambedouzou 1 , Sophie Tingry 1 , Mikhael Bechelany 1 , David Cornu 1 , Yaovi Holade 1
Affiliation  

The development of high-performance catalytic nanomaterials is important to implement sustainable and electrochemical energy devices of alkaline fuel cells, metal–air batteries, and electrolyzers in the envisaged energy-transition scenarios. Synthesizing effective nanocatalysts as both anode materials for oxidation of glycerol (byproduct of the biodiesel industry) and cathode materials for the oxygen reduction reaction (ORR) is still a bottleneck. Herein, we report palladium-based nanomaterials whose physicochemical and electrochemical properties are tuned by the judicious choice of the support (rGO, Vulcan XC72R), the addition of a coelement (Fe), and the structure (alloy/core–shell). The bimetallic-based electrode shows a drastically enhanced electrocatalytic performance with a beneficial shifting of the onset potential, production of high currents, and good durability for both the ORR (kinetic current density jk = 2 mA cmPd–2 or 1 A mgPd–1) and glycerol oxidation (jp = 2.3 mA cmPd–2 or 1.11 A mgPd–1 at the peak), higher than those of commercial catalysts and existing literature values. The present results also provide new fundamental insights about the accurate measurement of the kinetic metrics of the ORR by employing a rotating-disk (-ring) electrode setup in alkaline electrolytes with metallic catalysts. Indeed, the anodic scanning of the electrode from a low potential to a higher one results in an ultrafast electrochemical kinetics with a positive shift of the half-wave potential of ΔE1/2,anodic/cathodic = 60 mV from the cathodic direction to the anodic one. The kinetic current density dramatically increases, jk,anodic = 19.0×, 6.9×, 3.4×, and 2.4× jk,cathodic at 950, 900, 870, and 850 mVRHE, respectively. The advantage of the synthesis methodology relies on the nonuse of organic molecules as capping agents and surfactants in order to produce bare (ligand-free) bimetallic PdFe electrocatalysts with a clean catalytic surface in a facile and straightforward way.

中文翻译:

Fe修饰的Pd作为碱性介质中催化氧还原和甘油氧化反应的有效多功能电催化剂

高性能催化纳米材料的开发对于在设想的能量转换场景中实现碱性燃料电池、金属-空气电池和电解槽的可持续和电化学能源设备非常重要。合成有效的纳米催化剂作为甘油氧化的阳极材料(生物柴油工业的副产品)和氧还原反应(ORR)的阴极材料仍然是一个瓶颈。在此,我们报告了钯基纳米材料,其物理化学和电化学性能通过载体(rGO、Vulcan XC72R)的明智选择、辅元素(Fe)的添加和结构(合金/核-壳)进行调节。基于双金属的电极显示出显着增强的电催化性能,并且起始电位的有利转移,j k = 2 mA cm Pd –2或 1 A mg Pd –1)和甘油氧化(峰值处j p = 2.3 mA cm Pd –2或 1.11 A mg Pd –1),高于商业催化剂和现有催化剂文学价值。目前的结果还提供了关于通过在具有金属催化剂的碱性电解质中使用旋转盘(-环)电极装置准确测量 ORR 动力学指标的新的基本见解。事实上,电极从低电位到高电位的阳极扫描导致超快电化学动力学,Δ E的半波电位正移1/2,anodic/cathodic = 60 mV 从阴极方向到阳极方向。动电流密度显着增加,j k,anodic = 19.0×, 6.9×, 3.4×, 和 2.4× j k,cathodic在 950, 900, 870, 和 850 mV RHE,分别。该合成方法的优势在于不使用有机分子作为封端剂和表面活性剂,以便以一种简便直接的方式生产具有清洁催化表面的裸露(无配体)双金属 PdFe 电催化剂。
更新日期:2021-09-27
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