新型核壳AuTi@PtNi纳米催化剂: 增强氧还原催化活性及稳定性

doi:10.1016/S1872-2067(23)64568-1

催化学报 ›› 2024, Vol. 56: 81-87.DOI: 10.1016/S1872-2067(23)64568-1

新型核壳AuTi@PtNi纳米催化剂: 增强氧还原催化活性及稳定性

于亚楠^a^,^b^,¹, 鲁少杰^a, 胡一平^a, 周雨^a, 岳秦^a^,^*()

^a电子科技大学, 基础与前沿研究院, 四川成都610000
^b清华四川能源互联网研究院, 四川成都610000

收稿日期:2023-10-09 接受日期:2023-11-16 出版日期:2024-01-18 发布日期:2024-01-10
通讯作者: *电子信箱: qinyue@uestc.edu.cn (岳秦).
作者简介:¹共同第一作者.
基金资助:
国家青年拔尖人才支持计划和四川省科技计划(2020YJ0243);煤炭高效利用与绿色化工国家重点实验室基金(2022-K28)

A novel core-shell nanostructure of Ti-Au nanocrystal with PtNi alloy skin: Enhancing the durability for oxygen reduction reaction

Giday Fisseha^a^,¹, Ya’nan Yu^a^,^b^,¹, Shaojie Lu^a, Yiping Hu^a, Yu Zhou^a, Qin Yue^a^,^*()

^aInstitute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 610000, Sichuan, China
^bSichuan Energy Internet Research Institute Tsinghua University, Chengdu 610000, Sichuan, China

Received:2023-10-09 Accepted:2023-11-16 Online:2024-01-18 Published:2024-01-10
Contact: *E-mail: qinyue@uestc.edu.cn (Q. Yue).
About author:¹Contributed equally to this work.
Supported by:
National Youth Top-notch Talent Support Program of China, and the Sichuan Science and Technology Program(2020YJ0243);Foundation of State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering(2022-K28)

摘要/Abstract

摘要：

质子交换膜燃料电池(PEMFCs)将化学燃料转化为电能, 具有能量转换效率高、清洁、零排放等特点, 被认为是未来重要的能源利用装置. 与阳极发生的氢氧化反应相比, 阴极发生的氧还原反应(ORR)是动力学缓慢的过程, 严重阻碍了燃料电池的广泛应用, 因此迫切需要开发高活性的电催化剂来降低其电化学过电位, 提高反应动力学. 铂基纳米晶是氧还原反应有效的电催化剂, 但存在成本高、储量少且耐用性差等问题. 将铂(Pt)与过渡金属(Fe, Co, Ni等)合金化可以提升催化活性, 且最外层有序的Pt原子层可以有效地避免过渡金属的腐蚀溶解, 同时, 利用金(Au)与Pt基合金形成核壳结构可以有效地降低催化剂成本, 同时增强稳定性. 然而, 在以Au作为核时, 很难通过退火处理获得富含Pt层的核壳催化剂.

本文利用钛(Ti)原子与Au原子合金化后的协同作用, 成功地制备了核壳AuTi@PtNi氧还原催化剂. 由于Ti与Au的强相互作用, 使得该催化剂即使经高温退火处理, 依旧可以使Au保持在内部, 同时可以获得富Pt壳层. 利用配备有电子能量损失谱的透射电子显微镜及X射线电子能谱对催化剂进行表征, 结果表明, Ti的引入可大大提升催化剂的热稳定性. 由于具有核壳结构及富Pt的PtNi壳层, 退火后的AuTi@PtNi-400催化剂在0.9 V(RHE)时的质量比活性(5.26 A mg_Pt^‒1)和面积比活性(2.72 mA cm^‒2)分别是商业化Pt/C催化剂的19.26倍和9.84倍. 另外, AuTi@PtNi-400催化剂在20000圈循环测试后质量活性衰减不到10%, 稳定性好于商业化Pt/C催化剂和未经过退火的AuTi@PtNi催化剂. 进一步对AuTi@PtNi-400进行电催化测试, 结果表明, 在功率密度达到0.61 W cm^‒2的同时可产生1.31 A cm^‒2的电流密度, 该结果优于商业化Pt(1.05 A cm^‒2和0.34 W cm^‒2)以及Ti-Au@PtNi/C (1.25 A cm^‒2和0.62 W cm^‒2), 峰值功率密度高达0.80 W cm^‒2, 这表明所制备的Ti-Au@PtNi/C-400催化剂不仅在三电极体系中具有较好的性能, 在电堆测试中也展现出高性能, 可以较大地满足和促进燃料电池的发展和应用.

综上所述, 对于燃料电池阴极催化剂, 可结合形貌工程及协调作用, 制备出低成本高性能的ORR催化剂, 为燃料电池的进一步应用提供新思路.

关键词: 钛掺杂, 富铂层, 热处理, 氧化还原反应, 核壳结构

Abstract:

The sluggish oxygen reduction reaction (ORR) at the cathode largely hinders the practical application of the proton-exchange membrane fuel cells (PEMFCs). Pt-based nanocrystals are the most effective electrocatalysts for the oxygen reduction reaction, however, suffer high cost, scarcity and unsatisfied durability. Herein, we report a new category of annealed multimetallic core-shell catalyst of gold core doped with titanium and platinum-nickel (PtNi) shell with Pt-rich surface as a highly active and robust electrocatalyst for ORR. The introduction of titanium can effectively stabilize the gold core, avoiding the outward migration of Au atoms and ensuring the exposure of Pt-Ni active sites. The experimental findings revealed that the annealed Ti-Au@PtNi NPs catalyst provides 19.26 and 9.84 times higher mass and specific activities than commercial Pt/C catalysts for the oxygen reduction reaction. Moreover, durability tests of annealed Ti-Au@PtNi NPs show no noticeable activity loss even after 20000 potential cycles between 0.6 and 1.0 V vs. RHE, demonstrating a promising catalyst for the oxygen reduction reaction.

Key words: Titanium doping, Pt-rich surface, Thermal annealing, Oxygen reduction reaction, Core-shell nanostructure

于亚楠, 鲁少杰, 胡一平, 周雨, 岳秦. 新型核壳AuTi@PtNi纳米催化剂: 增强氧还原催化活性及稳定性[J]. 催化学报, 2024, 56: 81-87.

Giday Fisseha, Ya’nan Yu, Shaojie Lu, Yiping Hu, Yu Zhou, Qin Yue. A novel core-shell nanostructure of Ti-Au nanocrystal with PtNi alloy skin: Enhancing the durability for oxygen reduction reaction[J]. Chinese Journal of Catalysis, 2024, 56: 81-87.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(23)64568-1

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Fig. 1. Structural and compositional characterizations of Au@PtNi nanoparticles and Ti-Au@PtNi nanoparticles (Before and after annealing): TEM images of 4.56 nm Ti NPs (a), 5.20 nm Ti-Au NPs (b), 7.64 nm Ti-Au@PtNi NPs (c). (d) STEM-EDX images of Pt, Au and Ni of Au@PtNi/C NPs. (e) STEM-EDX images of Pt, Au and Ni of Au@PtNi/C NPs-400. (f) STEM-EDX images of Pt, Au, Ni and Ti of Ti-Au@PtNi/C NPs. (g) STEM-EDX images of Pt, Au, Ni and Ti of Ti-Au@PtNi/C NPs-400.

Fig. 2. (a) Comparison of XRD patterns of as-prepared Ti-Au@PtNi/C and Ti-Au@PtNi/C-400, (b) Comparison of XPS patterns of as-prepared Ti-Au@PtNi/C and Ti-Au@PtNi/C-400 (c) Pt 4f XPS spectra of as-prepared Ti-Au@PtNi/C and Ti-Au@PtNi/C-400, (d) Ni 2p XPS spectra of as-prepared Ti-Au@PtNi/C and Ti-Au@PtNi/C-400, (e) Ti 2p XPS spectra of as-prepared Ti-Au@PtNi/C and Ti-Au@PtNi/C-400, (f) Au 4f XPS spectra of as-prepared Ti-Au@PtNi/C and Ti-Au@PtNi/C-400.

Fig. 3. Electrochemical performance of catalysts. (a) CV curves of Pt/C, Au@PtNi/C, Ti-Au@PtNi/C and Ti-Au@PtNi/C-400. (b) LSV curves of Pt/C, Au@PtNi/C, Ti-Au@PtNi/C and Ti-Au@PtNi/C-400. (c) Histogram of ECSA of Pt/C, Au@PtNi/C, as-prepared Ti-Au@PtNi/C and Ti-Au@PtNi/C-400. (d) Summary of specific activities and mass activities for the ORR @0.9 V vs. RHE with 1600 r min?1 at a sweep rate of 20 mV s?1 of Pt/C, Au@PtNi/C, as-prepared Ti-Au@PtNi/C and Ti-Au@PtNi/C-400.

Fig. 4. Durability performance of catalysts. (a) ORR polarization curves before and after different potential cycles for Ti-Au@PtNi/C. (b) Specific and mass activity evolutions for various potential cycles. (c) ORR polarization curves before and after different potential cycles for Ti-Au@PtNi/C-400. (d) Specific and mass activity evolutions for various potential cycles.

Fig. 5. Fuel-cell performance of various catalysts. Air-H2 fuel cell polarization plots with the Ti-Au@PtNi/C-400, Ti-Au@PtNi/C and Pt/C as cathode catalysts. Test conditions: 80 °C, 100% relative humidity, atmospheric backpressure. Air and H2 flow rates were fixed at 0.2 and 0.1 L min?1.

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新型核壳AuTi@PtNi纳米催化剂: 增强氧还原催化活性及稳定性

A novel core-shell nanostructure of Ti-Au nanocrystal with PtNi alloy skin: Enhancing the durability for oxygen reduction reaction

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