Imines and secondary amines have attracted widespread attention in the fields of medicine owing to their unique unit structures and biological activities. However, the design of catalysts for targeted synthesis...
A major challenge that limits the applications of nanostructured electrocatalysts is precise surface structure regulation. The critical performance-impeding factors for the important electrochemical ozone production (EOP) lie in the leaching-induced poor stability as well as the competing oxygen evolution and ozone production reactions over the most promising platinum-based electrocatalysts. Although composition diversification by alloying appears to be a prevailing strategy to optimize platinum-based electrocatalysts, a practical restriction turns out to be the inevitable surface segregation and termination of platinum-enriched structures due to their lower surface energies. In this work, we introduce the nanoconfinement of intermetallic platinum–nickel nanostructures encapsulated by boron carbide, which effectively frustrates the surface segregation of alloy nanostructures and well maintains the pristine termination of the alloy. Precise atomic-level structural elucidation and model construction of the encapsulated alloy nanostructures are achieved by quantitative electron microscopy. The composite nanoalloy with a unique surface termination evokes synergetic catalytic effects that promote the charge transfer between the surface and adsorbed oxygen intermediates, which entails outstanding EOP performance with a high Faraday efficiency of 14.8% in neutral media and long-term stability of up to 120 h as a qualified electrocatalyst for the EOP electrolyzer devices. More importantly, the current work paves a new route to overwhelm the thermodynamically limited surface structures of bare nanoalloy catalysts through diverse nanoconfinement strategies.
Ozone is one of the most powerful oxidants for disinfection and sterilization. Water electrolysis represents an attractive method for electrochemical ozone production (EOP). Looking for highly active and cost‐effective alternative electrocatalysts to replace toxic PbO2 on the anode of the EOP electrolyzer is important. Here, a series of scalable, low‐toxicity ABO3 perovskite electrocatalysts was successfully synthesized, and their EOP performances were evaluated on the basis of their d‐band center values. Experimental results show that the gaseous ozone output of PrCoO3 is almost 1.3 times higher compared with that of commercial β‐PbO2. Theoretical calculations indicate that the volcanic‐type EOP performance of ABO3 can be attributed to the d‐band center of Co modified by lanthanide elements. Moreover, PrCoO3 demonstrates a remarkable performance in the electrodegradation of various organic pesticides and antibiotics, revealing potential application in advanced oxidation processes.
Diamond electrodes have been receiving increased attention because of their favorable properties for wastewater treatment. However, the surface properties of the diamond anode have not been fully determined. Herein, an extensive study was conducted to explore hybrid two-dimension nanodiamonds (2D NDs) with variable sp 3 /sp 2 ratios as metal-free electrochemical ozone production (EOP) electrocatalysts. The 2D ND-1100 electrocatalyst with interface heterojunction of sp 3 /sp 2 exhibited outstanding EOP performance compared with the normal ND@G with sp 3 @sp 2 core−shell structure. Theoretical calculations further revealed that a high sp 3 /sp 2 ratio could effectively prohibit the O 2 */O 3 * intermediate dissociation. O 3 * with five-ring configurations exhibited lower adsorption energies than O 2 * under the high sp 3 /sp 2 ratio condition, indicating the high O 3 selectivity. The optimal sp 3 /sp 2 ratio was predicted to be 4:5 to 8:1 for O 3 selective formation. In addition, the 2D ND-1100 electrocatalyst demonstrated remarkable performance in electrodegrading organic pollutants, indicating its broad potential for efficient and advanced oxidation applications. This work provides an effective strategy for the removal of organic pollutants in wastewater based on high-performance hybrid two-dimension nanodiamonds with appropriate sp 3 /sp 2 rations.
Developing a bifunctional electrocatalyst that can effectively produce O3 and H2O2 is significant for the electrochemical synthesis of O3 and H2O2 for the synergistic oxidative degradation of organic pollutants. In this study, SnO with various exposed facets was synthesized by tailoring the crystal facet microenvironment for oxygen intermediates adsorption for electrochemical ozone production (EOP) and two‐electron oxygen reduction reaction (2e− ORR). The Faraday efficiency of SnO‐1 with a high (110) facet ratio for O3 was 22.0%, while SnO‐4 with a high (002) facet ratio achieved a selectivity of 93.6% for H2O2. The theoretical calculation indicates that their excellent performances originated from the strong adsorption of the (110) facet on O* and O2* and the suitable adsorption and desorption strength of the (002) facet on OOH*, respectively. This study provides an attractive strategy for the development of a bifunctional electrocatalyst for advanced electrochemical oxidation by tailoring the crystal facet microenvironment.
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