Supports promote single-atom catalysts toward advanced electrocatalysis

Electrocatalytic Oxygen Reduction to Hydrogen Peroxide: From Homogeneous to Heterogeneous Electrocatalysis

Electrocatalytic hydrogen peroxide (H2O2) synthesis via the two‐electron oxygen reduction reaction (2e ORR) pathway is becoming increasingly important due to the green production process. Here, cationic vacancies on nickel phosphide, as a proof‐of‐concept to regulate the catalyst's physicochemical properties, are introduced for efficient H2O2 electrosynthesis. The as‐fabricated Ni cationic vacancies (VNi)‐enriched Ni2−xP‐VNi electrocatalyst exhibits remarkable 2e ORR performance with H2O2 molar fraction of >95% and Faradaic efficiencies of >90% in all pH conditions under a wide range of applied potentials. Impressively, the as‐created VNi possesses superb long‐term durability for over 50 h, suppassing all the recently reported catalysts for H2O2 electrosynthesis. Operando X‐ray absorption near‐edge spectroscopy (XANES) and synchrotron Fourier transform infrared (SR‐FTIR) combining theoretical calculations reveal that the excellent catalytic performance originates from the VNi‐induced geometric and electronic structural optimization, thus promoting oxygen adsorption to the 2e ORR favored “end‐on” configuration. It is believed that the demonstrated cation vacancy engineering is an effective strategy toward creating active heterogeneous catalysts with atomic precision.

Cation‐Vacancy‐Enriched Nickel Phosphide for Efficient Electrosynthesis of Hydrogen Peroxides

We reported the selective electrochemical reduction of oxygen (O2 ) to hydroxyl radicals (. OH) via 3-electron pathway with FeCo alloy encapsulated by carbon aerogel (FeCoC). The graphite shell with exposed -COOH is conducive to the 2-electron reduction pathway for H2 O2 generation stepped by 1-electron reduction towards to . OH. The electrocatalytic activity can be regulated by tuning the local electronic environment of carbon shell with the electrons coming from the inner FeCo alloy. The new strategy of . OH generation from electrocatalytic reduction O2 overcomes the rate-limiting step over electron transfer initiated by reduction-/oxidation-state cycle in Fenton process. Fast and complete removal of ciprofloxacin was achieved within 5 min in this proposed system, the apparent rate constant (kobs ) was up to 1.44±0.04 min-1 , which is comparable with the state-of-the-art advanced oxidation processes. The degradation rate almost remains the same after 50 successive runs, suggesting the satisfactory stability for practical applications.

Selective Electrocatalytic Reduction of Oxygen to Hydroxyl Radicals via 3-Electron Pathway with FeCo Alloy Encapsulated Carbon Aerogel for Fast and Complete Removing Pollutants.

Photocatalytic two-electron oxygen reduction reaction (2e - ORR) has been regarded as a promising strategy to solve the disadvantage of Fenton technology (constant addition of H 2 O 2 ). Herein, a photocatalysis-self-Fenton system was constructed on garland g-C 3 N 4 with carbon defects (GCN-PSFs) for pollutants degradation. Carbon defects in the obtained GCN not only accelerate charge separation but also improve 2e - ORR. As expected, the apparent rate constant for 2,4-DCP degradation by GCN-PSFs enhances to 0.070 min −1 , which is 5.4, 3.3 and 2.6 times as that of BCN, BCN-PSFs and GCN. The capture experiments and electron spin resonance indicate that the high activity is attributed to abundant ∙OH radicals, which are formed from the in-situ produced H 2 O 2 . Density functional theory (DFT) calculation confirms that the carbon defects in GCN is favorable for photocatalytic 2e - ORR to H 2 O 2 . This work provides a new insight for high-efficient degradation of organic pollutants by PSFs. • A photocatalysis-self-Fenton system was constructed based on garland g-C 3 N 4 . • Carbon defects accelerate charge separation and improve the O 2 adsorption ability. • Carbon defects in the Garland g-C 3 N 4 is favorable for photocatalytic 2e - ORR. • The photocatalysis-self-Fenton system is efficient for 2,4-Dichlorophenol degradation. • Abundant ∙OH radials were produced by efficient utilization of in-situ generated H 2 O 2 . 

Boosting 2e− Oxygen Reduction Reaction in Garland Carbon Nitride With Carbon Defects for High-efficient Photocatalysis-self-Fenton Degradation of 2,4-Dichlorophenol

Hydrogen peroxide (H2O2) production by electrocatalytic two-electron oxygen reduction shows promise as a replacement for energy-intensive anthraquinone oxidation or H2/O2 direct synthesis. Here, we report on graphene-supported Ni single-atom (SA) electrocatalysts, which are synthesized by a simple surfactant-free reduction process with enhanced electrocatalytic activity and stability. Unlike conventional Ni nanoparticles or alloy catalysts, the well-dispersed Ni-SA sites lack adjacent Ni atoms. This structure promotes H2O2 production by a two-electron oxygen reduction pathway under an alkaline condition (pH = 13). This catalyst exhibited enhanced H2O2 selectivity (>94%) with a considerable mass activity (2.11 A mgNi-1 at 0.60 V vs reversible hydrogen electrode), owing to the presence of oxygen functional groups and isolated Ni sites. Density functional theory calculations provide insights into the role of this catalyst in optimizing the two-electron oxygen reduction reaction pathway with high H2O2 selectivity. This work suggests a new method for controlling reaction pathways in atomically dispersed non-noble catalysts.

Graphene-Supported Single Nickel Atom Catalyst for Highly Selective and Efficient Hydrogen Peroxide Production.

Polyethyleneimine-reinforced Sn/Cu foam dendritic self-supporting catalytic cathode for CO2 reduction to HCOOH.

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Graphene-Supported Single Nickel Atom Catalyst for Highly Selective and Efficient Hydrogen Peroxide Production.

Polyethyleneimine-reinforced Sn/Cu foam dendritic self-supporting catalytic cathode for CO2 reduction to HCOOH.