Hydrogen peroxide electrogeneration from O2 electroreduction: A review focusing on carbon electrocatalysts and environmental applications.

Hydrogen peroxide (H2O2) stands as one of the foremost utilized oxidizing agents in modern times. The established method for its production involves the intricate and costly anthraquinone process. However, a promising alternative pathway is the electrochemical hydrogen peroxide production, accomplished through the oxygen reduction reaction via a 2-electron pathway. This method not only simplifies the production process but also upholds environmental sustainability, especially when compared to the conventional anthraquinone method. In this review paper, recent works from the literature focusing on the 2-electron oxygen reduction reaction promoted by carbon electrocatalysts are summarized. The practical applications of these materials in the treatment of effluents contaminated with different pollutants (drugs, dyes, pesticides, and herbicides) are presented. Water treatment aiming to address these issues can be achieved through advanced oxidation electrochemical processes such as electro-Fenton, solar-electro-Fenton, and photo-electro-Fenton. These processes are discussed in detail in this work and the possible radicals that degrade the pollutants in each case are highlighted. The review broadens its scope to encompass contemporary computational simulations focused on the 2-electron oxygen reduction reaction, employing different models to describe carbon-based electrocatalysts. Finally, perspectives and future challenges in the area of carbon-based electrocatalysts for H2O2 electrogeneration are discussed. This review paper presents a forward-oriented viewpoint of present innovations and pragmatic implementations, delineating forthcoming challenges and prospects of this ever-evolving field.

Decontamination of wastewater containing contaminants of emerging concern by electrooxidation and Fenton-based processes - A review on the relevance of materials and methods.

In recent years, there has been an increasingly growing interest regarding the use of electrochemical advanced oxidation processes (EAOPs) which are considered highly promising alternative treatment techniques for addressing environmental issues related to pollutants of emerging concern. In EAOPs, electrogenerated oxidizing agents, such as hydroxyl radical (HO•), can react non-selectively with a wide range of organic compounds, degrading and mineralizing their structures to unharmful molecules like CO2, H2O, and inorganic ions. To this date, a broad spectrum of advanced electrocatalysts have been developed and applied for the treatment of compounds of interest in different matrices, specifically aiming at enhancing the degradation performance. New combined methods have also been employed as alternative treatment techniques targeted at circumventing the major obstacles encountered in Fenton-based processes, such as high costs and energy consumption, which still contribute significantly toward inhibiting the large-scale application of these processes. First, some fundamental aspects of EAOPs will be presented. Further, we will provide an overview of electrode materials which have been recently developed and reported in the literature, highlighting different anode and cathode structures employed in EAOPs, their main advantages and disadvantages, as well as their contribution to the performance of the treatment processes. The influence of operating parameters, such as initial concentrations, pH effect, temperature, supporting electrolyte, and radiation source, on the treatment processes were also studied. Finally, hybrid techniques which have been reported in the literature and critically assess the most recent techniques used for evaluating the degradation efficiency of the treatment processes.

Assessing the oxygen reduction reaction by a 2-electron mechanism on ceria surfaces.

The 2-electron pathway of the oxygen reduction reaction is an unwanted process in the development of fuel cells. In contrast, it has gained the scientific community's attention due to its importance as a promising way of removing emergent pollutants and endocrine disruptors from water bodies and a more sustainable alternative for large-scale commercial hydrogen peroxide production. Cerium oxide has shown remarkable potential and selectivity experimentally for this mechanism, and its possible applications, exceeding the previous reference materials. In this work, we studied the 2-electron pathway for oxygen reduction on different ceria-cleaving directions (100), (110), (221), and (331) by first principles methods based on density functional theory. Our results show that the (100) surface is the most favorable for reduction, with the (331) crystallographic plane also showing potential for good catalytic activity. This fact could be essential for designing new nanostructures, with higher portions of those planes exposed, for higher catalytic activity.