The operational efficiency of membrane electrode assemblies in direct liquid fuel cells is critically dependent on the fuel purity in the anode compartment.To address the inherent challenge of fuel mixing problem in a...The operational efficiency of membrane electrode assemblies in direct liquid fuel cells is critically dependent on the fuel purity in the anode compartment.To address the inherent challenge of fuel mixing problem in alcohol systems,we propose a rational catalyst design strategy focusing on morphological and compositional optimization.Sodium borohydride-derived PtCuMo alloy aerogels(AA)exhibit abundant grain boundary defects,while solvothermally prepared nanowire arrays(NA)maintain excellent single-crystalline characteristics.Density functional theory calculations demonstrate that engineered grain boundaries can effectively broaden the adsorption energy window for key reaction intermediates,enabling superior adaptability to diverse catalytic pathways.By precisely controlling Cu content,we identified Pt_(3)Cu_(3)Mo_(0.5)AA as the optimal catalyst configuration,demonstrating 150% enhancement in methanol oxidation reaction activity compared to Pt_(3)Cu_(6)Mo_(0.5)NA(1.5 vs.0.6 A·mg_(Pt)^(-1))and 17% improvement in ethanol oxidation reaction performance versus Pt_(3)Cu_(1)Mo_(0.5)NA(0.82 vs.0.70 A·mg_(Pt)^(-1)).Practical application testing using gas diffusion electrodes(anode loading:0.85 mg_(Pt)·cm^(-2))achieved a mass-specific power density of 14.14 W·g_(Pt)^(-1)in 1:1 methanol/ethanol blends,representing a 3.5-fold improvement over commercial Pt/C benchmarks.This work establishes a fundamental framework for developing highperformance,broad-spectrum electrocatalysts in advanced fuel cell systems.展开更多
基金financially supported by the National Natural Science Foundation of China(No.52073214)Guangxi Natural Science Fund for Distinguished Young Scholars(No.2024GXNSFFA010008).
文摘The operational efficiency of membrane electrode assemblies in direct liquid fuel cells is critically dependent on the fuel purity in the anode compartment.To address the inherent challenge of fuel mixing problem in alcohol systems,we propose a rational catalyst design strategy focusing on morphological and compositional optimization.Sodium borohydride-derived PtCuMo alloy aerogels(AA)exhibit abundant grain boundary defects,while solvothermally prepared nanowire arrays(NA)maintain excellent single-crystalline characteristics.Density functional theory calculations demonstrate that engineered grain boundaries can effectively broaden the adsorption energy window for key reaction intermediates,enabling superior adaptability to diverse catalytic pathways.By precisely controlling Cu content,we identified Pt_(3)Cu_(3)Mo_(0.5)AA as the optimal catalyst configuration,demonstrating 150% enhancement in methanol oxidation reaction activity compared to Pt_(3)Cu_(6)Mo_(0.5)NA(1.5 vs.0.6 A·mg_(Pt)^(-1))and 17% improvement in ethanol oxidation reaction performance versus Pt_(3)Cu_(1)Mo_(0.5)NA(0.82 vs.0.70 A·mg_(Pt)^(-1)).Practical application testing using gas diffusion electrodes(anode loading:0.85 mg_(Pt)·cm^(-2))achieved a mass-specific power density of 14.14 W·g_(Pt)^(-1)in 1:1 methanol/ethanol blends,representing a 3.5-fold improvement over commercial Pt/C benchmarks.This work establishes a fundamental framework for developing highperformance,broad-spectrum electrocatalysts in advanced fuel cell systems.
