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Interfacial active sites on Co-Co2C@carbon heterostructure for enhanced catalytic hydrogen generation

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Abstract

Designing catalysts with capable dual-active sites to drive catalytic hydrogen generation is necessary for the future hydrogen economy. Herein, the interfacial active sites consisting of Co and Co-C on Co-Co2C@carbon heterostructure are designed through annealing and high-pressure carbonization. The operating temperature during the high-pressure carbonization under a CO-reducing environment is responsible for the construction and regulation of Co-Co2C@C heterostructure. The optimal catalyst has a high turnover frequency (TOF) of 33.1 min−1 and low activation energy (Ea) of 27.3 kJ·mol–1 during the hydrolysis of NH3BH3. The catalytic stability of Co-Co2C@C has no dramatic deterioration even after 5 cyclic usages. The interfacial active sites and the carbon on the catalyst surface enhance hydrogen generation kinetics and catalytic stability. The construction of interfacial active sites in Co-Co2C@C prompts the dissociation of reactants (NH3BH3 and H2O molecules), leading to an enhanced catalytic hydrogen generation from NH3BH3 hydrolysis (Co activates NH3BH3 and Co-C activates H2O). The construction of hetero-structural catalysts provides theoretical direction for the rational design of advanced transition metal carbide materials in the field of energy catalysis and conversion.

Graphical abstract

摘要

设计具有双活性位点的催化剂驱动催化制氢对未来的“氢经济”发展至关重要。基于此，通过煅烧和高压碳化的策略设计了具有Co和Co–C界面活性位点的Co-Co2C@Carbon异质结构催化剂。高压碳化是在CO还原气体存在的情况下进行的，其中不同的高压碳化温度在构建Co-Co2C@carbon异质结构的过程中有着重要的作用。设计的最佳催化剂在NH3BH3水解制氢过程中表现出优异的催化活性 (TOF = 33.1 min−1) 和较低的活化能 (Ea = 27.3 kJ mol−1)。而且Co-Co2C@C的催化活性在经过5圈循环之后没有剧烈的下降。催化剂中界面活性位点和碳的存在增强了催化产氢动力学和稳定性。Co-Co2C@C中界面活性位点的构建加快了NH3BH3和H2O分子的吸附和解离，进而促进NH3BH3催化制氢活性，其中Co活化NH3BH3，Co–C活化H2O。该异质结构的构建为能源催化转化领域合理设计高效的过渡金属碳化物催化剂提供了理论指导。

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Acknowledgements

This study was financially supported by the National Natural Science Foundation of China (Nos. 52071135, 51871090 and U1804135), the Fundamental Research Funds for the Universities of Henan Province (Nos. NSFRF220201 and NSFRF200402).

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Authors and Affiliations

  1. College of Chemistry and Chemical Engineering, Henan Polytechnic University, Jiaozuo, 454003, China

    Huan-Huan Zhang, Yang-Bin Ren, Zhen-Luo Yuan, Xian-Yun Liu, Yan-Ping Fan & Bao-Zhong Liu

  2. ISM, UMR CNRS No 5255, Univ. Bordeaux, Talence Cedex, 33405, France

    Nai-Xin Kang

  3. Department of Chemistry, The Women University Multan, Kutchery Campus, Multan, 66000, Pakistan

    Sehrish Mehdi

  4. Department of Materials Science and Engineering, Pennsylvania State University, University Park, PA, 16802, USA

    Cong-Cong Xing

  5. Research Center of Green Catalysis, College of Chemistry, Zhengzhou University, Zhengzhou, 450001, China

    Bao-Jun Li

  6. Henan Key Laboratory of Coal Green Conversion, Henan Polytechnic University, Jiaozuo, 454003, China

    Bao-Zhong Liu

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Zhang, HH., Ren, YB., Yuan, ZL. et al. Interfacial active sites on Co-Co2C@carbon heterostructure for enhanced catalytic hydrogen generation. Rare Met. 42, 1935–1945 (2023). https://doi.org/10.1007/s12598-022-02224-6

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