Electrochemical water-splitting reactions (hydrogen evolution reaction (HER) and oxygen evolution reaction (OER)) and oxygen redox reactions (oxygen reduction reaction (ORR) and OER) are core processes for electrochemical water-splitting devices, rechargeable metal–air batteries, and regenerative fuel cells. Developing highly efficient non-noble multifunctional catalysts in the same electrolyte is an open challenge. Herein, efficient Co–N–C electrocatalysts with a mixed structure comprising Co–N moieties and Co nanoparticles encapsulated in a N-doped carbon layer were prepared via pyrolysis of a new structure of Co-coordinated bis­(imino)­pyridine polymer constructed by 2,6-diacetylpyridine and 3,3′-diaminobenzidine. Results demonstrate that Co ion sources have a remarkable impact on the final Co–N–C performance. The Co–N–C catalyst prepared using cobalt acetate as a precursor displays remarkable overall multifunctional performance. It needs only a cell voltage of 1.66 V (obtained from the half-cell test) for the water-splitting reaction (HER/OER) to reach 10 mA·cm–2 in 1.0 M KOH, and the overall oxygen redox activity (OER/ORR) is 0.72 V in 0.1 M KOH, outperforming the reported nonprecious metal catalysts. The excellent activity is attributable to the synergistic effects between active sites with encapsulated metallic Co for HER and OER and Co–N moieties for ORR.

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Thermo-Electrochemical cells (Thermocells/TECs) transform thermal energy into electricity by means of electrochemical potential disequilibrium between electrodes induced by a temperature gradient (ΔT). Heat conduction across the terminals of the cell is one of the primary reasons for device inefficiency. Herein, we embed Poly(Vinylidene Fluoride) (PVDF) membrane in thermocells to mitigate the heat transfer effects - we refer to these membrane-thermocells as MTECs. At a ΔT of 12 K, an improvement in the open circuit voltage (Voc) of the TEC from 1.3 mV to 2.8 mV is obtained by employment of the membrane. The PVDF membrane is employed at three different locations between the electrodes i.e. x = 2 mm, 5 mm, and 8 mm where ‘x’ defines the distance between the cathode and PVDF membrane. We found that the membrane position at x = 5 mm achieves the closest internal ∆T (i.e. 8.8 K) to the externally applied ΔT of 10 K and corresponding power density is 254 nWcm−2; 78% higher than the conventional TEC. Finally, a thermal resistivity model based on infrared thermography explains mass and heat transfer within the thermocells.

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