Ghosh Srabanti, Bysakh Sandip, Basu Rajendra Nath
Fuel Cell and Battery Division, CSIR - Central Glass and Ceramic Research Institute 196, Raja S. C. Mullick Road Kolkata-700032 India
Materials Characterization Division, CSIR - Central Glass and Ceramic Research Institute 196, Raja S. C. Mullick Road Kolkata-700032 India.
Nanoscale Adv. 2019 Aug 19;1(10):3929-3940. doi: 10.1039/c9na00317g. eCollection 2019 Oct 9.
A facile route to anchor a nanoalloy catalyst on graphitic carbon nanosheets (GCNs) has been developed for preparing high-performance electrode materials for application in direct alcohol fuel cells (DAFCs). Uniformly dispersed bimetallic Pd-Fe nanoparticles (NPs) with tunable composition have been immobilized on GCNs derived from mesocarbon microbeads (MCMBs) by a one-pot radiolytic reduction method. The Pd-Fe/GCN hybrid shows promising electrocatalytic activity for the methanol, ethanol, ethylene glycol, tri-ethylene glycol and glycerol oxidation reactions in alkaline medium. The as-prepared flower-shape PdFe/GCN nanohybrids have high mass activity for the ethanol oxidation reaction (EOR), which is ∼36 times (11 A per mg Pd) higher than that of their monometallic counterparts. Moreover, the onset oxidation potential for the EOR on the PdFe/GCN nanohybrids negatively shifts 780 mV compared to that on commercial Pd/C electrocatalysts, suggesting fast kinetics and superior electrocatalytic activity. Additionally, chronoamperometry measurements display good long-term cycling stability of the PdFe/GCN nanohybrids for the EOR and also demonstrate only ∼7% loss in forward current density after 1000 cycles. The superior catalytic activity and stability may have originated from the modified electronic structure of the Pd-Fe nanoalloys and excellent physicochemical properties of the graphitic nanosheets. The present synthetic route using GCNs as the supporting material will contribute to further design of multimetallic nanoarchitectures with controlled composition and desired functions for fuel cell applications.
已开发出一种将纳米合金催化剂锚定在石墨碳纳米片(GCNs)上的简便方法,用于制备应用于直接醇类燃料电池(DAFCs)的高性能电极材料。通过一锅法辐射还原法,将具有可调组成的均匀分散的双金属钯铁纳米颗粒(NPs)固定在由中间相碳微球(MCMBs)衍生的GCNs上。钯铁/GCN杂化物在碱性介质中对甲醇、乙醇、乙二醇、三乙二醇和甘油氧化反应显示出有前景的电催化活性。所制备的花状钯铁/GCN纳米杂化物对乙醇氧化反应(EOR)具有高质量活性,比其单金属对应物高约36倍(每毫克钯11 A)。此外,与商业钯/碳电催化剂相比,钯铁/GCN纳米杂化物上EOR的起始氧化电位负移780 mV,表明其动力学快且电催化活性优异。此外,计时电流法测量显示钯铁/GCN纳米杂化物对EOR具有良好的长期循环稳定性,并且在1000次循环后正向电流密度仅损失约7%。优异的催化活性和稳定性可能源于钯铁纳米合金的改性电子结构以及石墨纳米片优异的物理化学性质。使用GCNs作为支撑材料的当前合成路线将有助于进一步设计具有可控组成和所需功能的多金属纳米结构,用于燃料电池应用。