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Surveying the electrocatalytic CO2-to-CO activity of heterogenized metallomacrocycles via accurate clipping at the molecular level

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Abstract

Heterogenized phthalocyanine-based molecular catalysts are the ideal electrocatalytic platforms for CO2 reduction reaction (CO2RR) because of their well-defined structures and potential properties. In addition to the pursuit of catalytic performances at industrial potentials, it is equally important to explore experimental rules and design considerations behind activity and selectivity. Herein, we successfully developed a series of nickel phthalocyanines (NiPcs) with different alkyl chains immobilized on multi-walled carbon nanotubes (CNT) to unveil the structure—performance relationship for electrocatalytic CO2RR in neutral electrolyte. Interestingly, a volcano-type trend was found between the activity for CO2-to-CO conversion and alkyl chain lengths of NiPcs on CNT. Experimental results further indicate that their electrocatalytic CO2RR activities are highly related to the molecular dispersion and the heterointerfacial charge transfer capability adjusted by the alkyl chains. Particularly, the optimized electrocatalyst via accurate clipping at the molecular level exhibits an ultrahigh activity with Faradaic efficiency of CO up to 99.52%.

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Acknowledgements

The authors are grateful for the financial supports of the National Key R&D Program of China (No. 2021YFA1500402), the National Natural Science Foundation of China (NSFC) (Nos. 21901246, 22105203, and 22175174), and the Natural Science Foundation of Fujian Province (Nos. 2020J01116 and 2021J06033).

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Authors and Affiliations

  1. State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences (CAS), Fuzhou, 350002, China

    Meng-Ke Hu, Ning Wang, Dong-Dong Ma & Qi-Long Zhu

  2. College of Chemistry, Fuzhou University, Fuzhou, 350002, China

    Meng-Ke Hu, Ning Wang & Qi-Long Zhu

  3. Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China, Fuzhou, 350108, China

    Qi-Long Zhu

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  1. Meng-Ke Hu
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  2. Ning Wang
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Correspondence to Dong-Dong Ma or Qi-Long Zhu.

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Surveying the electrocatalytic CO2-to-CO activity of heterogenized metallomacrocycles via accurate clipping at the molecular level

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Hu, MK., Wang, N., Ma, DD. et al. Surveying the electrocatalytic CO2-to-CO activity of heterogenized metallomacrocycles via accurate clipping at the molecular level. Nano Res. 15, 10070–10077 (2022). https://doi.org/10.1007/s12274-022-4444-x

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