物理化学学报 >> 2023, Vol. 39 >> Issue (3): 2209004.doi: 10.3866/PKU.WHXB202209004

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基于微流控技术平台的Pt基三元电催化剂高通量合成和筛选

胡洋1, 刘斌2, 徐路遥3, 董自强4, 仵亚婷1, 刘杰2,*(), 钟澄2,5,6,*(), 胡文彬2,5,6,*()   

  1. 1 上海交通大学材料科学与工程学院, 金属基复合材料国家重点实验室, 上海 200240
    2 天津大学材料科学与工程学院, 先进陶瓷与加工技术教育部重点实验室, 天津 300072
    3 深圳市中物科技有限公司, 广东 深圳 518052
    4 上海大学材料基因组研究所, 上海 200444
    5 天津大学材料科学与工程学院, 天津市复合与功能材料重点实验室, 天津 300072
    6 天津大学-新加坡国立大学福州联合学院, 天津大学国际校区, 福州 350207
  • 收稿日期:2022-09-05 录用日期:2022-10-04 发布日期:2022-10-11
  • 通讯作者: 刘杰,钟澄,胡文彬 E-mail:jieliu0109@tju.edu.cn;cheng.zhong@tju.edu.cn;wbhu@tju.edu.cn
  • 基金资助:
    国家重点研发计划(2016YFB0700205);天津市自然科学杰出青年基金(18JCJQJC46500);天津市“131”创新型人才培养工程;国家“万人计划”青年拔尖人才项目及国家自然科学基金(51722403)

High-Throughput Synthesis and Screening of Pt-Based Ternary Electrocatalysts Using a Microfluidic-Based Platform

Yang Hu1, Bin Liu2, Luyao Xu3, Ziqiang Dong4, Yating Wu1, Jie Liu2,*(), Cheng Zhong2,5,6,*(), Wenbin Hu2,5,6,*()   

  1. 1 State Key Laboratory of Metal Matrix Composites, School of Materials Science and Engineering, Shanghai Jiao Tong University, Shanghai 200240, China
    2 Key Laboratory of Advanced Ceramics and Machining Technology (Ministry of Education), School of Materials Science and Engineering, Tianjin University, Tianjin 300072, China
    3 Shenzhen Zhongwu Technology Co., Ltd, Shenzhen 518052, Guangdong Province, China
    4 Materials Genome Institute, Shanghai University, Shanghai 200444, China
    5 Tianjin Key Laboratory of Composite and Functional Materials, School of Materials Science and Engineering, Tianjin University, Tianjin 300072, China
    6 Joint School of National University of Singapore and Tianjin University, International Campus of Tianjin University, Fuzhou 350207, China
  • Received:2022-09-05 Accepted:2022-10-04 Published:2022-10-11
  • Contact: Jie Liu,Cheng Zhong,Wenbin Hu E-mail:jieliu0109@tju.edu.cn;cheng.zhong@tju.edu.cn;wbhu@tju.edu.cn
  • About author:Email: wbhu@tju.edu.cn (W.H.)
    Email: cheng.zhong@tju.edu.cn (C.Z.)
    Email: jieliu0109@tju.edu.cn (J.L.)
  • Supported by:
    the National Key Research and Development Program(2016YFB0700205);the Tianjin Natural Science Foundation for Distinguished Young Scholar(18JCJQJC46500);the "131" First Level Innovative Talents Training Project in Tianjin;the National Youth Talent Support Program, and the National Science Foundation for Excellent Young Scholar(51722403)

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摘要：

高性能铂基电催化剂的高效合成和筛选对于加速其在各个领域的进一步发展和应用具有重要意义。微流控高通量技术在铂基电催化剂的合成参数优化应用方面具有巨大的潜力。然而，缺少性能评估的微流控高通量合成无法最大限度地发挥其优势。在这项工作中，我们构建了将材料的高通量合成与高通量筛选相结合的多功能平台。该平台的微流控芯片可以生成三种不同前驱体金属离子的20级浓度梯度。微反应器阵列具有100个微通道，用于材料合成和电化学表征。利用该平台我们合成了5组铂基三元电催化剂(共计100种不同的组分)，并进行了电化学表征，直接确定了Pt基三元电催化剂对析氧反应的最佳组成。这表明我们所构建微流控高通量平台具有高效性和灵活性，可大大缩短了新材料开发和材料性能优化的周期。

关键词: 高通量方法, 电催化剂, 微流控技术, 电化学表征, 析氧反应

Abstract:

Pt-based electrocatalysts have received extensive attention owing to their wide applications in various fields, including fuel cells, hydrogen production, degradation of organic pollutants, electrochemical sensors, and oxidation of small molecules. Therefore, the efficient synthesis and screening of high-performance Pt-based electrocatalysts is necessary for accelerating their further development and application in these fields. The conventional method for developing the advanced materials and optimizing their synthesis parameters is time-consuming, inefficient, and costly. Microfluidic high-throughput techniques have the great potential for optimizing the synthesis parameters of Pt-based electrocatalysts. However, microfluidic high-throughput synthesis without performance evaluation cannot maximize its advantages. Therefore, it is highly desirable to develop a platform that combines the high-throughput synthesis of materials and the evaluation of their properties in a high-throughput fashion to improve the overall screening efficiency of the novel materials. In this study, a versatile microfluidic high-throughput platform, combining the high-throughput synthesis and screening of materials, was constructed. The microfluidic chip generated 20-level concentration gradients of the three different precursors. Microreactor arrays with 100 microchannels were used for the material synthesis and electrochemical characterization. A wide range of concentration combinations of the three different precursor solutions was achieved using the microfluidic chip. Five groups of Pt-based ternary electrocatalysts (100 different components in total) were synthesized and electrochemically characterized using the designed platform. The obtained Pt-based electrocatalysts exhibited a loose particle morphology, and were composed of small nanoparticles. The efficient preparation of Pt-based electrocatalysts with controllable compositions was also achieved through the high-throughput synthesis platform. The catalytic performance of the Pt-based catalysts towards oxygen evolution reaction (OER) was characterized by chronoamperometry. The optimal composition of Pt-based ternary electrocatalysts for OER was directly determined using the designed platform. For NiPtCu, the samples with a relatively high atomic percentage (approximately 50%) of Pt (i.e., Ni0.30Pt0.56Cu0.14, Ni0.17Pt0.52Cu0.31 and Ni0.12Pt0.48Cu0.40) exhibited higher electrocatalytic activity and stability, whereas the samples with a relatively high atomic percentage (> 50%) of Cu possessed lower activity and stability. For AuPtNi and AuPtCu, the samples wherein Au and Pt accounted for a large proportion of the sample (i.e., Ni or Cu < 10%) and the atomic ratios of Au : Pt were (3–4) : 1, e.g., Au0.71Pt0.25Ni0.04 and Au0.77Pt0.18Cu0.05, displayed high electrocatalytic activity and stability. As the atomic fraction of Au decreased, the atomic ratio of Pt and Ni in AuPtNi approached 3 : 1 or that of Pt and Cu in AuPtCu reached to 1 : 1, the samples (Au0.54Pt0.35Ni0.11, Au0.35Pt0.42Cu0.23, Au0.27Pt0.41Cu0.32 and Au0.12Pt0.32Cu0.56) all demonstrated high electrocatalytic activity and stability. The samples (Pt0.06Cu0.94) wherein the atomic percentages of Au and Pt were all less than 10%, exhibited poor electrocatalytic activity and stability. For RhPtNi and RhPtCu, when the atomic percentage of Rh in RhPtNi and RhPtCu was high (50%–90%) and almost no Ni or Cu was present, the samples (Rh0.91Pt0.09 and Rh0.82Pt0.18 for RhPtNi, as well as Rh0.88Pt0.12 and Rh0.75Pt0.21Cu0.04 for RhPtCu) all had high electrocatalytic activity and stability. As the atomic percentage of Rh decreased and that of Pt increased, the atomic percentages of Rh and Pt were relatively close, Rh0.54Pt0.32Ni0.14 and Rh0.51Pt0.36Cu0.14 showing high electrocatalytic activity and stability. When the atomic percentages of Ni and Cu were high (> 50%), the RhPtNi and RhPtCu samples all showed the relatively poor electrocatalytic activity and stability. These results demonstrate the high efficiency and flexibility of the constructed microfluidic high-throughput platform, which significantly shortens the cycle for the development cycle of new materials and the optimization of their properties.

Key words: High-throughput method, Electrocatalyst, Microfluidic technique, Electrochemical evaluation, Oxygen evolution reaction