Ever-growing demands for rechargeable zinc-air batteries call for efficient bifunctional electrocatalysts. Among various electrocatalysts, single atom catalysts (SACs) have received increasing attention due to the merits of high atom utilization, structural tunability and remarkable activity. Rational design of bifunctional SACs relies heavily on an in-depth understanding of reaction mechanisms, especially dynamic evolution under electrochemical conditions. This requires a systematic study in dynamic mechanisms to replace current trial and error modes. Herein, fundamental understanding of dynamic oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) mechanisms for SACs are first presented combining in situ and/or operando characterizations and theoretical calculations. By highlighting structure-performance relationships, rational regulation strategies are particularly proposed to facilitate the design of efficient bifunctional SACs. Furthermore, future perspectives and challenges are discussed. This review provides a thorough understanding of dynamic mechanisms and regulation strategies for bifunctional SACs, which are expected to pave the avenue for exploring optimum single atom bifunctional oxygen catalysts and effective ZABs. This article is protected by copyright. All rights reserved.

Bifunctional Single Atom Catalysts for Rechargeable Zinc-Air Batteries: From Dynamic Mechanism to Rational Design.

An original strategy was reported to manipulate ORR selectivity of N-doped hollow mesoporous carbon spheres (N-HMCS) via heteroatom (P and S) doping. Heteroatom doping can not only modulate electronic structure of N-HMCS and proportion/configuration of doped N, but also regulate ORR pathway. Specifically, rich-graphitic N sites and electron-rich C–P bond domains in N,P-HMCS act as electron donors, making *OOH more unstable and easier to desorb into H2O2. This severely distorts the sp2 lattice of graphene, catalyzing a two-electron ORR synergistically. Conversely, a strong interaction between electron-deficient C–S bond domain and *OOH intermediate due to the introduction of highly electronegative S hinders the desorption of *OOH, leading to the breakage of the O–O bond and promoting four-electron ORR along with the rich-pyridinic N receptor site. The reaction activity and kinetics mechanism present a positive correlation with proportion of graphitic N, revealing graphitic N is the primary active site with a much faster electron transfer capacity. 

Steering the Oxygen Reduction Reaction Pathways of N-Carbon Hollow Spheres by Heteroatom Doping

Oxygen reduction reaction via the two‐electron route (2e− ORR) provides a green method for the direct production of hydrogen peroxide (H2O2) along with in situ utilization. The effective catalysts with high ORR activity, 2e− selectivity, and stability are essential for the application of this technology. Single‐atom catalysts (SACs) have attracted intensively attention for H2O2 electrosynthesis owing to the unique geometric and electronic configurations. In this review, the mechanism and theoretical predictions for 2e− ORR over SACs are first introduced. Then, the recent advances of various SACs for the electrosynthesis of H2O2 are documented. And the correlation between the central atom, coordination atoms, and coordination environment of SACs and the corresponding electrocatalytic ORR performance including activity, selectivity, and stability are emphatically analyzed and summarized. Finally, the major challenges and opportunities regarding the future design of SACs for the H2O2 production are pointed out.

Single‐Atom Catalysts for H2O2 Electrosynthesis via Two‐Electron Oxygen Reduction Reaction

The organic pollutants removal by conventional methods (adsorption, coagulation, filtration, microorganism and enzymes) showed important limitation due to the reluctance of these molecules. An alternative to this issue is represented by the photocatalytic technology considered as an advanced oxidation process (AOP). The photoreactors design and concepts vary based on the working regime (static or dynamic), photocatalyst morphology (powders or bulk) and volume. This mini-review aims to provide specific guidelines on the correlations between the photoreactor concept characteristics (working regime, volume and flow rate), irradiation scenarios (light spectra, irradiation period and intensity) and the photocatalytic process parameters (photocatalyst materials and dosage, pollutant type and concentration, pollutant removal efficiency and constant rate). The paper considers two main photoreactor geometries (cylindrical and rectangular) and analyses the influence of parameters optimization on the overall photocatalytic efficiency. Based on the systematic evaluation of the input data reported in the scientific papers, several perspectives regarding the photocatalytic reactors’ optimization were included.

https://www.mdpi.com/2073-4344/11/5/556/pdf

The Influence of Photocatalytic Reactors Design and Operating Parameters on the Wastewater Organic Pollutants Removal—A Mini-Review

Recent trends and applications of electrolyzed oxidizing water in fresh foodstuff preservation and safety control.

In this work, a type of doped carbon material with rich edged P atoms co-functionalized by O and N atoms was synthesized via simple solvothermal treatment of P2O5 in formamide,...

Oxygenated P/N co-doped carbon for efficient 2e‒ oxygen reduction to H2O2

Effects of electrolyzed water treatment on pesticide removal and texture quality in fresh-cut cabbage, broccoli, and color pepper

Molecular imprinting polymer (MIP) has been increasingly employed for sulfonylurea herbicides (SUHs) detection in different matrices. A novel MIP that was effective as a highly class-selective sorbent in molecularly imprinted solid-phase extraction (MISPE) was successfully prepared for isolation and purification of SUHs, namely, metsulfuron-methyl, chlorsulfuron, chlorimuron-ethyl, prosulfuron, and pyrazosulfuron-ethyl, in rice, corn and soybean samples. The MIP was synthesized by precipitation polymerization using metsulfuron-methyl as the template, 4-vinylpyridine as the functional monomer, ethylene glycol dimethacrylate as the crosslinker, and MeCN as the porogen. The polymerization system of the MIP was optimized, and its adsorption performances were evaluated by comparing its adsorption isotherms and adsorption kinetics with those of a non-imprinted polymer (NIP). Following MISPE for extracting and enriching SUHs from rice, corn and soybean samples, high-performance liquid chromatography-tandem mass spectrometry (HPLC-MS/MS) was performed. Acceptable recoveries were observed at SUHs contaminant concentrations of 10, 20 and 40 μg/L: from 77.56 to 99.81%, with relative standard deviations of <13.8% (n = 5) for all samples. The limits of detection for the five SUHs were 0.21-0.26 μg/L. The results demonstrated that the proposed MISPE-HPLC-MS/MS method is an effective approach for the simultaneous and sensitive determination of the five SUHs in rice, corn and soybean samples.

/pdf/preparation-of-molecularly-imprinted-polymer-for-selective-2tgqtdkf.pdf

Preparation of Molecularly Imprinted Polymer for Selective Solid-Phase Extraction and Simultaneous Determination of Five Sulfonylurea Herbicides in Cereals

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Oxygenated P/N co-doped carbon for efficient 2e‒ oxygen reduction to H2O2

Effects of electrolyzed water treatment on pesticide removal and texture quality in fresh-cut cabbage, broccoli, and color pepper

Preparation of Molecularly Imprinted Polymer for Selective Solid-Phase Extraction and Simultaneous Determination of Five Sulfonylurea Herbicides in Cereals