Cobalt-N4 macrocyclic complexes for heterogeneous electrocatalysis of the CO2 reduction reaction

doi:10.1016/S1872-2067(21)63880-9

Abstract

Abstract:

Metal-N₄ (M-N₄) macrocyclic complexes are interesting electrocatalysts due to their well-defined structures and rich molecular tuning. Among them, metal phthalocyanines have been widely studied for the carbon dioxide reduction reaction (CO₂RR) in heterogeneous systems and demonstrated good electrocatalytic performance. However, other complexes like metal corroles and metal porphyrins are much less explored, and often show inferior performances. In this study, three cobalt macrocyclic complexes, cobalt phthalocyanine, cobalt meso-tetraphenylporphyrin, and cobalt meso-triphenylcorrole (CoPc, CoTPP and CoTPC) are investigated in heterogeneous electrocatalysis of CO₂RR. Although CoPc/carbon nanotube (CNT) hybrid exhibits high electrocatalytic activity, CNT hybridization does not work for CoTPC and CoTPP that hold weak interactions with CNTs. By the drop-dry method with a high molecular loading of 5.4 × 10^-7 mol cm^-2, CoTPC and CoTPP could deliver appreciable electrode activities. Poly(4-vinylpyridine) (PVP) introduction is further demonstrated as a facile method to afford enhanced activities for CoTPP at low molecular loadings through enhancing molecule-substrate interactions. The partial current density of carbon monoxide for CoTPP+CNT/PVP is around 8 times higher than the sample without PVP at -0.67 V versus reversible hydrogen electrode. This work provides solutions to enhance the electrode activities of molecular electrocatalysts with weak substrate interactions in heterogeneous systems.

Key words: CO₂ reduction, Cobalt phthalocyanine, Cobalt corrole, Cobalt porphyrin, Heterogeneous electrocatalysis

Zhichao Lin, Zhan Jiang, Yubo Yuan, Huan Li, Hongxuan Wang, Yirong Tang, Chunchen Liu, Yongye Liang. Cobalt-N₄ macrocyclic complexes for heterogeneous electrocatalysis of the CO₂ reduction reaction[J]. Chinese Journal of Catalysis, 2022, 43(1): 104-109.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(21)63880-9

https://www.cjcatal.com/EN/Y2022/V43/I1/104

Figures/Tables 4

Fig. 1. (a) Chemical structures of CoPc, CoTPC and CoTPP; (b) LSVs of CoPc/CNT, CoTPC/CNT and CoTPP/CNT in a CO2-saturated 0.5 M KHCO3 solution at v = 5 mV s-1; (c) Cyclic voltammograms of 10 mM DMF solutions of CoTPC and CoTPP containing 0.1 M Bu4NPF6, recorded on a GC electrode at v = 0.10 V s-1 under Ar (dash) or CO2 (solid).

Fig. 2. The fabrication process of drop-dry samples on CFP. Each sphere stands for one molecule: CoPc (green), CoTPC (red) and CoTPP (blue).

Fig. 3. (a) LSVs of CoPc+CNT, CoTPC+CNT and CoTPP+CNT mixtures with different molecular contents in a CO2 saturated 0.5 M KHCO3 solution at v = 5 mV s-1; Chronoamperometric curves (b) and FEs (c) of CoPc+CNT-e, chronoamperometric curves (d) and FEs (e) of CoTPC+CNT-e, and chronoamperometric curves (f) and FEs (g) of CoTPP+CNT-e at different voltages in a CO2 saturated 0.5 M KHCO3 solution; (h) Partial current densites of CO. Currents were taken average from 40 min eletrocatalysis at appoximately -0.67 V (vs. RHE); (i) AC impedance tests of CoPc+CNT-c, CoTPC+CNT-c and CoTPP+CNT-c mixtures on glassy carbon electrodes in CO2 saturated 0.5 M KHCO3 solution with a scanning frequency range from 200 kHz to 100 Hz with an a.c. amplitude of 5 mV. The solid lines are guides to the eye.

Fig. 4. (a) Schematic diagram for Cobalt-N4 macrocyclic complexes immobilized on CNT with the assistance of PVP; (b) LSVs of CoPc+CNT/PVP, CoTPC+CNT/PVP, CoTPP+CNT/PVP, CoTPP+CNT-a and CoPc/CNT MDEs in CO2 saturated 0.5 M KHCO3 solution at v = 5 mV s-1; Chronoamperometric curves (c) and FEs (d) at different voltages of CoTPP+CNT/PVP.

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Cobalt-N₄ macrocyclic complexes for heterogeneous electrocatalysis of the CO₂ reduction reaction

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