The
design and development of carbon materials with high-efficiency
oxygen reduction activity is still a problem. Folic acid (FA) has
unique structural characteristics, and it can provide multiple coordination
sites for metal ions. Here, folic acid (FA) was used as a metal complex
ligand, and Cu–Co-based N-doped porous carbon nanosheets (Cu–CoNCNs)
were synthesized by the solvothermal method, the molten salt template-assisted
calcination method, and the chemical etching method. The Cu–CoNCNs
synthesized by this method have highly efficient oxygen reduction
reaction (ORR) activity. In 0.1 mol/L KOH electrolytes, the catalyst
exhibits excellent ORR activity and has a fairly high half-wave potential
(0.905 V vs reversible hydrogen electrode (RHE)). X-ray photoelectron
spectroscopy (XPS), Raman spectroscopy, infrared spectroscopy, and
X-ray diffraction (XRD) were used to investigate the reasons why the
catalyst has excellent catalytic activity and long-life stability.
It was proved that the impressive ORR activity of Cu–CoNCNs
comes from Cu doping, which can regulate the surface electronic structure
of the catalyst, thereby optimizing the binding ability between the
intermediate and adsorbed species and improving the catalytic activity.
The introduction of sulfur is beneficial to regulate the electronic structure of M-Nx active site, thus improving oxygen reduction reactions (ORR) catalytic activity. Herein, we adopted a hydrogel method to synthesize ORR catalyst of Co metal atom dispersed on N and S co-doped tremelliform carbon (Co/NSTFC). The as-synthesized catalyst was characterized by TEM, XRD and BET, and results demonstrated that cobalt atoms are highly dispersed on porous N and S co-doped tremelliform carbon, and the specific surface area is as high as 1613 m2 g−1. And XPS analysis confirms the formation Co-Nx coordination bond, while the sulfur atom is successfully doped on the carbon support. The XPS analysis of N 1s and Co 2p prove that the introduction of sulfur atoms can improve the efficiency of electron transferring to graphite nitrogen, and to the vicinity of Co-Nx, thus increasing d-band center of Co metal atoms, consequently improving the oxygen reduction activity. The Co/NSTFC catalyst exhibits high-efficient ORR activity with half-wave potential (E1/2) of 0.882 V in 0.1 M KOH. Furthermore, the measured number of electron transfer is close to 4, and a low yield of hydrogen peroxide and superior stability were confirmed with the Co/NSTFC catalyst. This study provides new insights into the design and synthesis of high the performant ORR catalysts and promoting the development of energy conversion.
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