Short communicationA novel nitrogen-containing electrocatalyst for oxygen reduction reaction from blood protein pyrolysis
Introduction
The oxygen reduction reaction (ORR) at the cathode plays a key role in metal–air batteries [1] and fuel cells [2]. Carbon-supported platinum particles are the most effective catalyst for the ORR [3], but sluggish oxygen reduction, high cost, and low abundance limit the commercialization of these technologies. Many research efforts have been done on the reduction of Pt loading and exploration of novel non-precious catalysts to reduce fuel cell cost. It is interesting that heat-treated carbon materials have received enormous attention as non-precious electrode materials for ORR, especially for N-doped carbon nanotubes and N-doped graphene [4], [5], [6], [7]. Additional N-containing materials were fabricated by several bioproteins, such as collagen [8] and hemoglobin [9], [10]. Quite recently, several groups have reported the preparation and oxygen reduction electrocatalytic behavior of N-containing electrocatalysts using hemin biomaterial as an effective precursor or N-enriched amino acids as nitrogen sources [11], [12], [13], [14], [15]. These works mainly focus on the use of natural porphyrinatoiron complexes contained inside hemin or the selection of nitrogen sources to form the catalytic sites.
Many heat-treated materials have reasonably good electrocatalytic activity towards ORR, but their stability is still far below the requirements for the practical application of new energy. The exhibited catalytic properties may be substantially attributed to the presence of C–N active sites in the carbon structure [4], [16], [17], [18], [19]. However, the detailed C–N bonding configuration responsible for the ORR catalytic activity of N-containing carbons remains elusive. Additionally, to create N-containing electrocatalysts, in addition to the requirement of complex procedures and expensive equipment, the precursors also need to be handled carefully because of their toxic and corrosive nature [5]. Therefore, the development of a simple and effective method for fabricating electrocatalysts to replace the commercial Pt-based catalysts has remained a challenge.
Blood protein (BP) from animals can be obtained from the meat industry, and it includes an abundance of hemoprotein and various amino acids. These substances can successfully produce active electrocatalysts for ORR in acidic and alkaline environments. BP material could be a potential precursor for preparing highly active electrocatalysts for ORR, as supported by our previous reports [20]. To overcome the current obstacles, in this work, we develop a new approach to synthesize a novel N-containing electrocatalyst (BP350C1000) BP material with high ORR catalytic activity and stability through the use of high-temperature pyrolysis. Our results indicate that BP350C1000 with higher percentage of pyrrolic-N improves ORR activity substantially, suggesting that pyrrolic-N plays an active role in ORR electrocatalysis.
Section snippets
Materials
Porcine BP was supplied by the Food Testing Center of Chongqing Bureau of Quality and Technology Supervision, China. Carbon black (Vulcan XC-72R) was purchased from Cabot® and pretreated in a solution containing 10% HNO3 and 30% H2O2 at 80 °C for 12 h.
Catalyst preparation
First, 0.5 g of BP was decomposed in flowing N2 at 350 °C for 5 h. The yielded pyropolymer as a precursor was mixed with the pretreated carbon black support (mass ratio of 1:1) by ball milling. The obtained substance was further treated in flowing
Catalyst characterization
In Fig. 1(a), the XRD patterns of three N-containing electrocatalysts show similar phase compositions. The only other peaks observed are two amorphous-carbon peaks, centered at 2θ values of ≈24° and ≈44°, which are ascribed to the graphitic planes (002) and (101), respectively [20]. The broad peak at 24° reveals the domination of the disordered carbon phase in electrocatalysts, while the weak broad peak at 44° suggests the existence of graphitic layers with smaller sizes and lower
Conclusions
Herein, we report a facile method to design an ORR electrocatalyst from the pyrolysis of the BP350 pyropolymer combined with a carbon support. The nitrogen exists mainly in the pyridinic- and pyrrolic-N configurations in all carbonized materials. It is interesting that the high-temperature pyrolysis process changes a significant amount of the pyridinic-N to the pyrrolic-N configuration. BP350C1000 contains a higher percentage of the pyrrolic-N configuration, which is promising for four-electron
Acknowledgments
This work was supported by the Natural Science Fund of China (Project No. 21273292) and the Fundamental Research Funds for the Central Universities (Project No. CDJXS12220002). We also thank Wenjing Yang and Lin Chen for helpful discussions.
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