含氧空位TiO2-CNT载体负载Pt单原子电催化剂的电化学性能
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1.陕西科技大学 材料科学与工程学院;2.北京工业大学 材料与制造学部激光工程研究院

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中图分类号:TM911.42 文献标识码:A

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军科委重点项目


Electrochemical performance of Pt single-atom electrocatalysts loaded with oxygen-containing vacancy TiO2-CNT carriers
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1.School of Materials Science and Engineering,Shaanxi University of Science and Technology,Xi''an;2.Institute of Laser Engineering,Department of Materials and Manufacturing,Beijing University of Technology

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Key projects of the Military Science and Technology Commission

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    摘要:

    为降低Pt负载型催化剂的Pt负载量和原子利用率,以羧基化多壁碳纳米管(MWCNT)和钛酸四丁酯为原料,通过溶胶凝胶法制备了TiO2-CNT复合载体,采用高温热处理在其表面引入大量氧空位(OV)缺陷,最后通过沉积沉淀法使Pt单原子(Pt SA)负载在TiO2(OV)-CNT上,制备了一种含氧空位缺陷的复合载体锚定Pt SA的电催化剂Pt SA/TiO2(OV)-CNT。采用XRD、电子顺磁共振波谱仪(EPR)、HAADF-STEM、XPS对Pt SA/TiO2(OV)-CNT的结构组成和微观形貌进行了表征,采用标准的三口电解池对其电化学性能进行评价。结果表明,TiO2-CNT上成功引入氧空位缺陷,并将Pt SA锚定在TiO2(OV)-CNT晶格中,Pt SA和TiO2(OV)-CNT之间存在电荷转移,形成共价配位键,具有金属载体强相互作用(SMSI);电化学评价中,Pt SA/TiO2(OV)-CNT的半波电位0.804 V,0.9 V时的质量活性(MA)451.24 mg/mg(Pt),Tafel斜率63.75 mV/dec,在10000 s的氧还原(ORR)运行过程中,归一化电流下降17%,展现了较优的ORR的动力学。Pt SA/TiO2(OV)-CNT以较低的Pt负载量(质量分数1.13%)表现出较高的催化活性,得益于氧空位对Pt SA的强锚定作用和TiO2薄膜对CNT的保护作用。 关键词:氧空位;复合载体;单原子;半波电位;质量活度;原子利用率

    Abstract:

    We designed a composite carrier containing oxygen vacancy defects for anchoring Pt single-atom electrocatalyst Pt SA/TiO2(OV)-CNT. The TiO2-CNT composite carrier was synthesized by solgel method, a large number of oxygen vacancy defects were introduced on its surface by high temperature heat treatment, and finally Pt SA was loaded on TiO2(OV)-CNT by the deposition-precipitation method. The structure and microscopic morphology of the composites were characterized by XRD, EPR, HAADF-STEM and XPS. The results showed that oxygen vacancy defects were successfully introduced on TiO2-CNT and Pt SA existed in the TiO2(OV)-CNT lattice, with charge transfer between the two to form Strong metal-support interactions (SMSI). Further oxygen reduction results showed that Pt SA/TiO2(OV)-CNT had a half-wave potential of 0.804 V, a mass activity MA of 451.24 mg/mgPt, and a Tafel slope of 63.75 mV/dec. The ICP results show that the Pt loading is only 1.13 % of the mass of Pt SA/TiO2(OV)-CNT, which indicated that Pt SA /TiO2(OV)-CNT catalyst can still exhibit excellent catalytic activity with low Pt loading and high atom utilization compared with commercial Pt/C catalysts. Key words: oxygen reduction; composite carrier; single atom; half-wave potential; mass activity; atomic

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王肖博,闫岸如,朱玲,兰天,刘学胜,马淑芳,王智勇.含氧空位TiO2-CNT载体负载Pt单原子电催化剂的电化学性能[J].精细化工,2024,41(12):

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  • 收稿日期:2023-11-05
  • 最后修改日期:2024-01-15
  • 录用日期:2023-12-25
  • 在线发布日期: 2024-12-10
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