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MOF-derived Cu embedded into N-doped mesoporous carbon as a robust support of PdAu nanocatalysts for ethanol electrooxidation

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Abstract

Metal–organic frameworks (MOFs) have attracted widespread attention due to their large surface area and porous structure. Rationally designing the nanostructures of MOFs to promote their application in ethanol electrooxidation is still a challenge. Here, a novel Cu-NCNs (Cu-nitrogen-doped carbon nanotubes) support was synthesized by pyrolysis of melamine (MEL) and Cu-ZIF-8 together, and then, Pd–Au nanoalloys were loaded by sodium borohydride reduction method to prepare PdAu@Cu-NCNs catalysts. The generating mesoporous carbon with high specific surface area and favorable electron and mass transport can be used as a potential excellent carrier for PdAu nanoparticles. In addition, the balance of catalyst composition and surface structure was tuned by controlling the content of Pd and Au. Thus, the best-performed Pd2Au2@Cu-NCN-1000–2 (where 1000 means the carrier calcination temperature, and 2 means the calcination constant temperature time) catalyst exhibits better long-term stability and electrochemical activity for ethanol oxidation in alkaline media (4.80 A·mg−1), which is 5.05 times higher than that of commercial Pd/C (0.95 A· mg−1). Therefore, this work is beneficial to further promoting the application of MOFs in direct ethanol fuel cells (DEFCs) and can be used as inspiration for the design of more efficient catalyst support structures.

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摘要

金属有机骨架 (MOFs) 因其较大的表面积和多孔结构而受到广泛关注。合理设计MOF结构以促进其在乙醇电氧化中的应用仍然是一个挑战。本文通过热解三聚氰胺和Cu-ZIF-8的复合材料来制备新型Cu-NCNs载体, 再通过硼氢化钠还原法负载Pd–Au纳米合金制备PdAu@Cu-NCNs催化剂。生成的介孔碳Cu-NCNs具有高比表面积和良好的电子和质量传输, 可作为PdAu纳米颗粒的潜在优良载体。此外, 通过控制Pd和Au的含量来调节催化剂成分和表面结构的平衡。性能最佳的Pd2Au2@Cu-NCN-1000–2催化剂在碱性介质中的乙醇氧化具有更好的长期稳定性和电化学活性 (4.80 A/mg), 是商业Pd/C(0.95 A/mg) 的5.05倍。因此, 本工作有利于进一步促进MOF在直接乙醇燃料电池中的应用, 可为设计更高效的催化剂载体提供启示。

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Acknowledgements

This work is financially supported by the Program for Professor of Special Appointment (Eastern Scholar) at SIHL, Project of Shanghai Municipal Science and Technology Commission (No. 22DZ2291100), Open Fund of Anhui International Joint Research Center for Nano Carbon-based Materials and Environmental Health (No. NCMEH2022Y02), Gaoyuan Discipline of Shanghai-Materials Science and Engineering, and Shanghai Polytechnic University-Drexel University Joint Research Center for Optoelectronics and Sensing. This work is also supported by the Science Fund for Distinguished Young Scholars of Fujian Province (No. 2019J06027), the Open Project of Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices (Soochow University) (No. KS2022), Collaborative Innovation Center of Suzhou Nano Science & Technology, the 111 Project, Joint International Research Laboratory of Carbon-Based Functional Materials and Devices.

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  1. School of Energy and Materials, Shanghai Engineering Research Center of Advanced Thermal Functional Materials, Shanghai Key Laboratory of Engineering Materials Application and Evaluation, Shanghai Polytechnic University, Shanghai, 201209, China

    Yu-Fu Huang, Peng Wu, Jun-Ping Tang, Jing Li, Shuai Chen, Xue-Ling Zhao, Cheng Chen & Dong-Hai Lin

  2. State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, 361005, China

    Jian Yang & Shi-Gang Sun

  3. School of Chemistry and Chemical Engineering, Chongqing University, Chongqing, 401331, China

    Bin-Wei Zhang

  4. Center of Advanced Energy Technology and Electrochemistry, Institute of Advanced Interdisciplinary Studies, Chongqing University, Chongqing, 400044, China

    Bin-Wei Zhang & Shi-Gang Sun

  5. Institute of Functional Nano & Soft Materials (FUNSOM), Jiangsu Key Laboratory for Carbon-Based Functional Materials & Devices, Soochow University, Suzhou, 215123, China

    Yan-Yun Ma

  6. Department of Materials Science and Engineering, Drexel University, Philadelphia, PA, 19104, USA

    Wei-Heng Shi

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Huang, YF., Wu, P., Tang, JP. et al. MOF-derived Cu embedded into N-doped mesoporous carbon as a robust support of PdAu nanocatalysts for ethanol electrooxidation. Rare Met. 43, 1083–1094 (2024). https://doi.org/10.1007/s12598-023-02512-9

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