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含氧空位TiO2-CNT负载Pt单原子电催化剂的电化学性能

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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进行了表征,采用标准的三口电解池对其电化学性能进行了评价.结果表明,TiO2-CNT上成功引入了氧空位缺陷,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,形成了共价配位键,具有金属载体强相互作用.Pt SA/TiO2(OV)-CNT的半波电位为0.804 V,0.90 V时的质量活性(MA)451.24 A/g(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.
Electrochemical performance of oxygen-containing vacancy TiO2-CNT support Pt single-atom electrocatalyst
In order to reduce the Pt loading and atom utilization of Pt-supported catalysts,TiO2-CNT composite support was prepared from carboxylated multi-walled carbon nanotubes(MWCNT)and tetrabutyl titanate via sol-gel method,and its surface was introduced a large number of oxygen vacancy(OV)defects by high temperature heat treatment.An electrocatalyst Pt SA/TiO2(OV)-CNT anchored by a composite support with oxygen vacancy defects was then prepared by deposition-precipitation of Pt single-atom(Pt SA)on TiO2(OV)-CNT,characterized by XRD,electron paramagnetic resonance spectroscopy(EPR),HAADF-STEM and XPS,and evaluated by standard three-port electrolytic cell for its electrochemical performance.The results showed that oxygen vacancy defects were successfully introduced onto TiO2-CNT and Pt SA was anchered in the TiO2(OV)-CNT lattice,with charge transfer between the two forming strong metal-support interactions.Pt SA/TiO2(OV)-CNT exhibited a half-wave potential of 0.804 V,a mass activity(MA)of 451.24 A/g(Pt),and a Tafel slope of 63.75 mV/dec at 0.90 V.During oxygen reduction(ORR)operation for 10000 s,the normalized current decreased by 17%,showing better ORR dynamics.Pt SA/TiO2(OV)-CNT showed high catalytic activity with lower Pt loading(mass fraction 1.13%),due to the strong anchoring effect of oxygen vacancy on Pt SA and the protective effect of TiO2 film on CNT.

oxygen vacancycomposite supportssingle-atomhalf-wave potentialmass activityatomic utilization

王肖博、闫岸如、朱玲、兰天、刘学胜、马淑芳、王智勇

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陕西科技大学 材料科学与工程学院,陕西 西安 710021

北京工业大学 物理与光电工程学院,北京 100124

氧空位 复合载体 单原子 半波电位 质量活度 原子利用率

2024

精细化工
大连化工研究院设计院 中国化工学会精细化工专业委员会 辽宁省化工研究院

精细化工

CSTPCD北大核心
影响因子:0.557
ISSN:1003-5214
年,卷(期):2024.41(12)