Pyrolysis-Free Mechanochemical Conversion of Small Organic Molecules into Metal-Free Heteroatom-Doped Mesoporous Carbons for Efficient Electrosynthesis of Hydrogen Peroxide

New and Revised Aspects of the Electrochemical Synthesis of Hydrogen Peroxide: From Model Electrocatalytic Systems to Scalable Materials

“…(a) LSVs at 1600 rpm in alkaline media (except for the dotted line made in acid media), and (b) the percentage of H 2 O 2 . All data reproduced with permission from refs (Copyright 2021, American Chemical Society), (Copyright 2017, American Chemical Society), (Copyright 2023, American Chemical Society), (Copyright 2018, Springer Nature), (Copyright 2018, Springer Nature), (Copyright 2021, American Chemical Society), (Copyright 2021, American Chemical Society), (Copyright 2021, American Chemical Society), (Copyright 2018, Elsevier), (Copyright 2020, American Chemical Society), and (Copyright 2021, Elsevier). (c–f) Possible defects in carbon materials and (g, h) optimized configurations and adsorption energies for O 2 and *OOH on the models of pyridinic-N/pyrrolic-N and pyridinic-N/pyrrolic-N/F for fluorine, nitrogen-doped carbon.…”

“…The synthesis of N-doped materials is almost always obtained by pyrolysis of small molecules or polymers, and it is difficult to find other methods since the incorporation of heteroatoms is favored at relatively high temperatures. As an alternative, we report a work in which a pyrolysis-free mechanochemical method is used . The authors propose a ball-milling-based method in which the precursors are milled under nitrogen in the presence of Mg, which acts as a templating agent.…”

“…The combinate action of N (O 2 adsorption promotion) and F atoms (*OOH desorption promotion) (Figure 6g,h), brings a high selectivity for H 2 O 2 electroproduction. 123 With the mechanochemical doping approach previously presented, 121 nitrogen/fluorine-doped carbons have been prepared showing good activity. Fluorine was introduced also as a standalone dopant, by the same authors (F-Cs, Figure 6a,b) and by Zhao et al 133 Besides doping, one very important parameter to control is the porosity of the carbonaceous material.…”

Recent Advances with Biomass‐Derived Carbon‐Based Catalysts for the High‐Efficiency Electrochemical Reduction of Oxygen to Hydrogen Peroxide

“…[99] As a result, a positive electron density is created in the carbon matrix, which can act as an active site to attract O 2 molecules, which are then chemisorbed and reduced. [95,100,101] Compared to the doping of O and N elements, the study of carbon materials monodoped with P, B, and S heteroatoms derived from biomass resources for H 2 O 2 production is less. For example, litchi shell was investigated as the precursor of an electrocatalyst based on Pdoped carbon toward ORR to generate H 2 O 2 .…”

Thermoplasmonic In Situ Fabrication of Nanohybrid Electrocatalysts over Gas Diffusion Electrodes for Enhanced H2O2 Electrosynthesis

“…The resulting polarization favors optimum O 2 adsorption, triggering the selective reduction pathway. While nitrogen is the most investigated heteroatom, various non-metal elements have been screened and their effect evaluated in the realm of 2e – ORR, including fluorine. , Notably, F-doped carbons show a high positive charge over the carbon framework due to the highest electronegativity of fluorine atoms, which show great potential for ORR, especially facilitating the desorption of the *OOH intermediate . Besides doped carbon, TMNs are well-suited as electrocatalysts due to their exceptional electrical conductivity, chemical stability, wear resistance, and mechanical robustness. − The limited performance of TMNs compared to commercial Pt/C can be improved through doping , or by partial oxidation, leading to oxynitride phases. ,− Furthermore, a fully or partially oxidized surface layer can increase the selectivity toward the 2e – ORR over the 4e – ORR, as shown in the case of titanium nitride/oxynitride (TiN/TiO x N y ) electrocatalysts. ,,, …”