Nitrogen-Doped Hollow Carbon Nanoparticles with Excellent Oxygen Reduction Performances and Their Electrocatalytic Kinetics

Abstract

To propel the commercialization of fuel cells, the development of efficient nonprecious metal catalysts, specifically cathodic oxygen reduction catalysts, is turning into reality because the great advancements have been made on nitrogen-doped carbon materials recently. In this study, we demonstrated that nitrogen-doped hollow carbon nanoparticles (N-HCNPs) exhibit excellent electrocatalytic performance for oxygen reduction reaction (ORR) in alkaline fuel cells. Cyclic voltammetry and rotating ring-disk electrode voltammetry showed that the ORR activity of N-HCNPs approaches that of commercial Pt–C catalyst and is much better compared with nitrogen-free counterparts due to the incorporation of nitrogen atoms into graphitic structures. Kinetic studies indicated that the involvement of nitrogen induces a totally different oxygen adsorption mechanism and a four-electron dominated reaction pathway for N-HCNPs in comparison with nitrogen-free HCNPs, very similar to the observations in Pt–C. Moreover, N-HCNPs exhibited good operation stability and excellent tolerance to methanol crossover and CO poisoning for ORR superior to that of Pt–C. Our findings suggest that N-HCNPs catalyst is a promising alternative for the Pt-based catalysts in fuel cells.

High oxygen reduction activity of few-walled carbon nanotubes with low nitrogen content

“…Research on metal-free catalysts for ORR has thus become a very active topic in catalysis, especially with the emergence of nitrogen-doped carbon nanomaterials as one of the promising electrocatalysts. Recent research has investigated nitrogen doping of different carbon nanomaterials (CNM) such as carbon nanotubes (CNTs) [5][6][7][8][9][10][11][12][13][14], carbon nanofibers (CNFs) [15,16], graphene [17,18], mesoporous carbon [19], carbon nanocages [20], and hollow carbon nanoparticles [21]. The studies are particularly numerous for Nitrogen-doped CNTs (N-CNTs) among these materials.…”

Highly efficient cathode catalyst layer based on nitrogen-doped carbon nanotubes for the alkaline direct methanol fuel cell

“…graphene [10,[23][24][25][26][27][28][29][30][31][32][33], carbon nanotubes [11,20,21,[34][35][36][37][38][39][40][41][42][43], carbon nanofibers [12,[44][45][46][47], mesoporous carbon [15,22], graphitic carbon [48,49], carbon spheres [19,[50][51][52][53], carbon nanocages 4 [54], flower-like carbon [55], carbon aerogel [56,57], vesicular carbon [58], nanodiamonds [59]) relatively few have been tested in actual fuel cell conditions [58,[60][61][62]…”

Nitrogen-doped graphene with enhanced oxygen reduction activity produced by pyrolysis of graphene functionalized with imidazole derivatives

“…Moreover, addition of nitrogen varies the charge distribution of the carbon network so that the C atoms adjacent to N become more positively charged, resulting in an enhanced interaction with the adsorbing molecule and thus lower activation barrier for its decomposition [96]. 41 Recently, a variety of metal-free nitrogen doped CNMs have been synthesized in the form of CNTs [97][98][99][100][101][102], CNFs [103,104], graphene [105,106], mesoporous carbon [107], carbon nanocages [108], carbon spheres, hollow carbon nanoparticles [109], etc. In this thesis the synthesis and electrocatalytic activity of N-FWCNTs and N-GNPs for the ORR have been investigated.…”