Acta Chim. Sinica ›› 2016, Vol. 74 ›› Issue (7): 587-592.DOI: 10.6023/A16040196 Previous Articles     Next Articles

Article

介观结构氮掺杂碳纳米笼负载铂-钌合金催化剂的优异甲醇电氧化性能

黎聃勤a,b, 张志琦a,b, 臧鹏远a,b, 马延文a,b, 吴强a,b, 杨立军a,b, 陈强a,b, 王喜章a,b, 胡征a,b   

  1. a. 江苏省纳米技术重点实验室 介观化学教育部重点实验室 南京大学化学化工学院 南京 210023;
    b. 南京大学(苏州) 高新技术研究院 苏州 215123
  • 收稿日期:2016-04-20 出版日期:2016-07-15 发布日期:2016-06-07
  • 通讯作者: 王喜章 E-mail:wangxzh@nju.edu.cn
  • 基金资助:

    项目受国家重大科学研究计划纳米专项(No.2013CB932902)、国家自然科学基金(Nos.21473089,51232003,21373108,51571110,21573107)、苏州市科技计划(ZXG2013025)、常州市科技计划(CE20130032)和江苏高校优势学科建设工程资助.

Alloyed Pt–Ru Nanoparticles Immobilized on Mesostructured Nitrogen-Doped Carbon Nanocages for Efficient Methanol Electrooxidation

Li Danqina,b, Zhang Zhiqia,b, Zang Pengyuana,b, Ma Yanwena,b, Wu Qianga,b, Yang Lijuna,b, Chen Qianga,b, Wang Xizhanga,b, Hu Zhenga,b   

  1. a. Jiangsu Provincial Lab for Nanotechnology, Key Laboratory of Mesoscopic Chemistry of MOE, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210023, China;
    b. High-Tech Research Institute of Nanjing University (Suzhou), Suzhou, Jiangsu 215123
  • Received:2016-04-20 Online:2016-07-15 Published:2016-06-07
  • Supported by:

    Project supported by the National Basic Research Program of China (973 Program, No. 2013CB932902), National Natural Science Foundation of China (Nos. 21473089, 51232003, 21373108, 51571110, 21573107), Suzhou Science and Technology Project (ZXG2013025) and Changzhou Technology Support Program (CE20130032). This work was also supported by a Project Funded by the Priority Academic Program Development of Jiangsu Higher Education Institutions.

Direct methanol fuel cells (DMFC) have attracted extensive attention as ideal candidates for automotive and portable applications owing to the fascinating advantages such as high conversion efficiency, environmental friendliness, safety, wide sources of methanol, and simple cell structure. Electrocatalysts are one of crucial factors limiting the performance of DMFC. Nowadays, precious Pt-based catalyst, in spite of costliness and scarcity, is the most popular catalyst for methanol oxidation reaction (MOR) at anode due to the much better performances than those of the non-Pt catalysts. But there exists some shortcomings such as poor CO-tolerance and durability. Pt alloying with other metals, e.g. Ru, is an effective strategy to improve the catalytic performance. In addition, the support with a large specific surface area (SSA), high conductivity and suitable porous structure, such as sp2 carbon, could lead to high dispersion, high utilization and stability of Pt-based nanoparticles, also favorable for MOR. Recently, by in situ MgO template method, we reported the unique 3D hierarchical carbon-based nanocages featured with ultrahigh SSA, micro-meso-macro-pore coexistence, good conductivity and easy doping, which exhibited excellent electrochemical performances. Herein, taking the advantages of nitrogen-dopant anchoring function and unique mesostructures of hierarchical N-doped carbon nanocages (hNCNC), we report the Pt-Ru electrocatalysts immobilized on hNCNC (Pt-Ru/hNCNC) prepared via modified microwave-assisted ethylene glycol (EG) reduction method. The so-constructed Pt-Ru/hNCNC catalysts with ca. 30 wt% loading and tunable atomic ratio of Pt to Ru have a highly homogeneous dispersion of metal nanoparticles with the average size of ca. 3 nm. The alloying Pt-Ru/hNCNC catalysts demonstrate good CO-tolerance, high MOR activity and durability, superior to those of the counterparts of Pt/hNCNC and commercial PtRu/C. The good electrochemical performance can be ascribed to the synergistic effects of the bifunctional effect due to introduction of Ru, small size and high dispersion of metal nanoparticles induced by the large SSA and nitrogen participation of hNCNC, and multi-scaled hierarchical pore structures beneficial to the mass transportation. These results proposed a potential strategy to develop the high-performance Pt-based MOR catalysts based on the novel mesostructured hNCNC.

Key words: direct methanol fuel cell, electrocatalyst, mesostructured, nitrogen-doped carbon nanocages, Pt-Ru alloy nano-particles, methanol oxidation