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富缺陷Pd纳米粒子的制备及催化甲醇电催化氧化性能

Preparation of Pd nanoparticles with rich defects and its electrocatalytic oxidation of methanol
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摘要 在V(无水乙醇)∶V(水)=1∶4混合溶剂中构建了十二烷基硫酸钠(SDS)胶束模板,以Pd(NO3)2•2H2O为原料,采用超声辐射技术制备了富缺陷Pd纳米粒子(Pd-NPs)。采用TEM、HRTEM、XRD、XPS和UV-Vis吸收光谱对其进行了表征。将Pd-NPs作为电催化剂,探究了其在碱性介质(KOH)中对甲醇氧化反应(MOR)的电催化性能。结果表明,Pd-NPs粒径为(21.7±3.6)nm,其具备晶界、晶格错位、晶格膨胀、晶格扭曲等晶格缺陷,可以为MOR提供丰富的活性位点;Pd-NPs的电化学活性表面积为62.42 m^(2)/g,在浓度均为1.0 mol/L的KOH和CH_(3)OH混合溶液中的质量活度高达2474 A/g,是商业Pd/C(153 A/g)的16倍,经500圈循环伏安测试后,其质量活度保持率为82%;Pd-NPs在MOR计时电流测试3600 s时,其比活度为0.11 mA/cm^(2)。Pd的d波段中心向上移动,提高了吸附物对Pd的吸附能力,从而激活Pd-NPs表面,增强了其催化能力。 Sodium dodecyl sulfate(SDS)micellar templates were constructed in a solvent mixture of V(anhydrous ethanol)∶V(water)=1∶4.Defect rich Pd nanoparticles(Pd-NPs)were then prepared by ultrasonic irradiation technology using Pd(NO3)2•2H2O as raw material,characterized by TEM,HRTEM,XRD,XPS,and UV-Vis adsorption spectrum,and utilized as electrocatalysts for methanol oxidation reaction(MOR)in alkaline media(KOH)to evaluate their electrochemical behavior.The results indicated that the Pd-NPs,with a particle size of(21.7±3.6)nm,exhibited lattice defects such as grain boundary,lattice dislocation,lattice expansion,and lattice distortion,which could provide abundant active sites for MOR.The electrochemical active surface area of the Pd-NPs was 62.42 m^(2)/g,and their mass activity reached 2474 A/g in a mixed solution of 1.0 mol/L KOH and 1.0 mol/L CH_(3)OH,16 times higher than that of commercial Pd/C(153 A/g).After 500 cycles of cyclic voltammetry,the mass activity retention rate of the Pd-NPs was 82%.During the chronoamperometry test for MOR over 3600 s,the specific activity of the Pd-NPs was 0.11 mA/cm^(2).The upward shift of the d band center of Pd enhanced the adsorption capacity of adsorbates towards Pd,activating the surface of the Pd-NPs and augmenting their catalytic ability.
作者 王艳丽 卢小川 罗小丽 凌雯莹 陈建宏 谭德新 WANG Yanli;LU Xiaochuan;LUO Xiaoli;LING Wenying;CHEN Jianhong;TAN Dexin(School of Chemistry and Chemical Engineering,Lingnan Normal University,Zhanjiang 524048,Guangdong,China)
出处 《精细化工》 北大核心 2025年第10期2198-2207,共10页 Fine Chemicals
基金 广东省基础与应用基础研究基金项目(2022A1515011970) 岭南师范学院科研团队项目(LT2409)。
关键词 超声辐射 模板 PD 甲醇 电催化 催化技术 ultrasonic irradiation template Pd methanol electrocatalysis catalysis technology
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