多孔碳纳米纤维负载Pd纳米颗粒用于增强电催化氧还原性能
Pd Nanoparticles Anchored on Porous Carbon Nanofibers for Enhanced Electrocatalytic Oxygen Reduction Reaction
作者单位E-mail
莫志勇 南通大学化学化工学院, 南通 226019  
宋诗竹 南通大学化学化工学院, 南通 226019  
力文玉 南通大学化学化工学院, 南通 226019  
何学龙 南通大学化学化工学院, 南通 226019  
谌璐 南通大学化学化工学院, 南通 226019  
高晓红 南通大学化学化工学院, 南通 226019 gao.xh@ntu.edu.cn 
李奇 南通大学化学化工学院, 南通 226019 zhuiqiuzhizhuo@163.com 
摘要: 采用溶剂热法合成了以锆为金属核心、2-氨基为配体的锆基金属有机骨架(UiO-66)纳米材料,通过静电纺丝技术制备出UiO-66自由分散的聚丙烯腈(PAN/UiO-66)纤维,可控热解得到多孔碳纳米纤维(porous carbon nanofibers,PCNFs),结合湿化学还原法在PCNFs表面沉积Pd纳米颗粒,得到PCNFs@Pd复合材料。通过扫描电子显微镜、透射电子显微镜、X射线衍射技术对其形貌、组成、结构进行表征;采用电化学工作站分别测试了PCNFs@Pd在0.1 mol·L-1 KOH和0.1 mol·L-1 HClO4电解质中氧还原性能(oxygen reduction reaction,ORR)。结果表明,在PAN纤维中添加UiO-66显著提高了PCNFs@Pd(Pd负载量为0.34%)复合材料的ORR性能。相比40% Pt/C,在碱性电解质中,PCNFs@Pd复合材料展示出更低的Tafel斜率、更优异的循环稳定性和耐甲醇中毒性。在酸性电解质中也表现出类似20% Pt/C的催化活性和循环稳定性。
关键词: UIO-66  静电纺丝  多孔碳纳米纤维  Pd纳米颗粒  氧还原反应
基金项目: 江苏省自然科学基金(No.BK20210834)、江苏省高等学校自然科学面上项目(No.20KJB430046)和南通市科技项目(No.JC2021098)资助
Abstract: Zirconium-based metal-organic frameworks (UiO-66) nanomaterials with 2-amino terephthalic acid as a ligand was synthesized by the solvothermal method. PAN/UiO-66 fibers with free-dispersed UiO-66 nanoparticles were prepared by electrospinning. Porous carbon nanofibers (PCNFs) were prepared by controllable pyrolysis. Pd nanoparticles were deposited on the surface of PCNFs by the wet-chemistry reduction method to obtain PCNFs@Pd composites. The morphologies, compositions, and structures of PCNFs@Pd were characterized by scanning electron microscope, transmission electron microscope, and X-ray diffraction. The performances of oxygen reduction reaction (ORR) of PCNFs@Pd were tested by electrochemical workstations in 0.1 mol·L-1 KOH and 0.1 mol·L-1 HClO4 electrolytes, respectively. It was found that adding UiO-66 into PAN fibers significantly improved the ORR performance of PCNFs@Pd (0.34% of Pd loading) composites. Compared with 40%Pt/C, PCNFs@Pd composites in alkaline electrolytes showed lower Tafel slope, better cycle stability, and methanol toxicity resistance. Moreover, the catalytic activity and cycle stability of PCNFs@Pd were comparable to that of 20%Pt/C in acidic electrolytes.
Keywords: UIO-66  electrospinning  porous carbon nanofibers  Pd nanoparticles  oxygen reduction reaction
投稿时间:2021-12-03 修订日期:2022-04-14
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莫志勇,宋诗竹,力文玉,何学龙,谌璐,高晓红,李奇.多孔碳纳米纤维负载Pd纳米颗粒用于增强电催化氧还原性能[J].无机化学学报,2022,38(6):1037-1048.
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