Bottom‐Up Construction of Triazine‐Based Frameworks as Metal‐Free Electrocatalysts for Oxygen Reduction Reaction

Abstract

A bottom-up method is used to construct novel metal-free catalysts for deeper study of oxygen reduction reaction (ORR) catalysis. Through controlling the structural evolution of a 2D covalent triazine-based framework, the conductivity, nitrogen configurations, and multidoping structures of the as-prepared catalysts can be easily tuned, which makes a great platform for both studying the mechanisms of the ORR and optimizing the performances of the metal-free catalysts.

Conversion of amorphous polymer networks to covalent organic frameworks under ionothermal conditions: a facile synthesis route for covalent triazine frameworks

“…[9][10][11][12][13][14][15][16][17][18][19][20] CTFs have also been applied as solid base catalysts for the conversion of CO 2 21 and as metal free catalysts for ORR. 22,23 The high surface area and nitrogen amount make CTFs attractive for the storage of gases 6,[24][25][26][27][28] or generally as sorbent materials. [29][30][31] Furthermore, due to the conjugated planar structure, CTFs are organic semiconductors.…”

Non-Precious Electrocatalysts for Oxygen Reduction Reaction in Alkaline Media: Latest Achievements on Novel Carbon Materials

“…A nitrogen-containing molecule, terephthalonitrile, as the basic building block and through first trimerization into a 2D covalent triazine-based framework and 0.1 M KOH, oxygen saturated; 10 mV·s −1 , 1600 rpm J d = 4.0 mA·cm −2 E 1/2 = 0.767 V vs. RHE [41] Among all carbon materials, graphene is the most promising for accommodating various nanoparticles to achieve high electron transport rate, electrolyte contact area and structural stability, all of which lead to markedly improved ORR performance. Replacing carbon with graphene in 3D structures combined with M-N-doped-carbon further enhances their electrocatalytic activity and stability (M-N-doped-3D graphene).…”

“…More precisely, the development of porous organic networks, which stems from the polymerization of rigid organic molecules, offers the opportunity of 3D controllable structured electrocatalysts preparation [42]. Recently, Hao et al [41] exploited the 2D structure of triazine-based framework (metal organic) and convert it to a 3D porous electrocatalyst. Its stability at 0.6 V vs. RHE was excellent as kept stable by 100% for 11 h of operation, as well as its tolerance in presence of 3.0 M methanol.…”

“…However, they differ in their kinetic current values: the 3D nanosheets Co 3 O 4 -doped-graphene [38] exhibited a kinetic current density of 34 mA·cm −2 at 0.75 V vs. RHE, while the 3D-structured Co-N-doped highly ordered macro-mesoporous carbon of 23.2 mA·cm −2 . [38], [29], [27], [41], [28], [40], [35], [39], [34]). …”

“…Additionally, most of those that were examined for methanol tolerance were found totally unaffected by methanol's presence. [38], [29], [27], [41], [28], [40], [35], [39], [34]). …”