Direct Electron Transfer Coordinated by Oxygen Vacancies Boosts Selective Nitrate Reduction to N2 on a Co–CuOx Electroactive Filter

Li, Yang; Ma, Jinxing; Wu, Zhichao; Wang, Zhiwei

doi:10.1021/acs.est.1c05841

Cited by 67 publications

(24 citation statements)

References 49 publications

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“…Recent studies revealed that electrocatalytic NO 3 – reduction can occur via both direct electron transfer and/or atomic H*-mediated indirect reduction pathways. , During the electrochemical reduction of NO 3 – in aqueous media, protons were reduced to generate atomic H*, which could break the N–O bond and could be used as a reducing agent for NO 3 – . EPR was used to identify the formation of H* with 5,5-dimethyl-1-pyrroline- N -oxide (DMPO) as a radical trapping reagent .…”

Section: Resultsmentioning

confidence: 99%

Fluidic MXene Electrode Functionalized with Iron Single Atoms for Selective Electrocatalytic Nitrate Transformation to Ammonia

Ren,

Tian,

Jin

et al. 2023

Environ. Sci. Technol.

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The growth of renewable energy industries and the ongoing need for fertilizer in agriculture have created a need for sustainable production of ammonia (NH 3 ) using low-cost, environment-friendly techniques. The electrocatalytic nitrate (NO 3 − ) reduction reaction (NO 3 RR) has the potential to improve both the management of environmental nitrogen and the recycling of synthetic nutrients. However, NO 3 RR is frequently hindered by the incomplete NO 3 − conversion, sluggish reaction kinetics, and suppression of the hydrogen evolution reaction (HER). Inspired by specific local electronic structures that are adjustable for singleatom catalysts, this work presents a nanohybrid electrocatalytic filter with iron single atoms (FeSA) immobilized on MXene. The fabricated FeSA/MXene filter exhibited maximum NH 3 Faradaic efficiency and selectivity (82.9 and 99.2%, respectively) that were higher than those for filters made of Fe nanoparticles anchored on MXene (FeNP/MXene) (69.2 and 81.3%, respectively) and MXene alone (32.8 and 52.4%, respectively), measured at an initial pH of 7 and an applied potential of −1.4 V vs Ag/AgCl. Density functional theory calculations revealed that, compared to the FeNP/ MXene filter, the FeSA/MXene filter prevented the competition from the HER and reduced the activation energy of the potentiallimiting step (*NO to *NHO) that made the NH 3 synthesis thermodynamically favorable . This work highlights an alternative strategy for achieving a synergistic NO 3 − removal and nutrient recovery with durable catalytic activity and stability.

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Section: Resultsmentioning

confidence: 99%

Fluidic MXene Electrode Functionalized with Iron Single Atoms for Selective Electrocatalytic Nitrate Transformation to Ammonia

Ren,

Tian,

Jin

et al. 2023

Environ. Sci. Technol.

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“…As oxidative radicals, such as superoxide and hydroxyl radicals can only be produced at the cathode under aerobic condition or at the anode, , the C-F bond breakage could be attributed to either direct or indirect electrochemical reduction in this study. The electrochemical reduction mechanisms involved direct electron transfer and indirect reduction via atomic H*. ,− The atomic H* involved in the electroreduction process was detected by the electron paramagnetic resonance (EPR) spin trapping. As shown in Figure S6, nine characteristic peaks of DMPO-H signal of atomic H* trapped by DMPO were detected at both OTAB-modified carbon paper cathode and pure carbon paper cathode.…”

Section: Resultsmentioning

confidence: 99%

Electroreductive Defluorination of Unsaturated PFAS by a Quaternary Ammonium Surfactant-Modified Cathode via Direct Cathodic Reduction

Wang

Xiao

Lin

et al. 2023

Environ. Sci. Technol.

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Remediation of per- and polyfluoroalkyl substances (PFAS) in groundwater remains a technological challenge due to the trace concentrations of PFAS and the strength of their C–F bonds. This study investigated an electroreductive system with a quaternary ammonium surfactant-modified cathode for degrading (E)-perfluoro(4-methylpent-2-enoic acid) (PFMeUPA) at a low cathodic potential. A removal efficiency of 99.81% and defluorination efficiency of 78.67% were achieved under −1.6 V (vs Ag/AgCl) at the cathode modified by octadecyltrimethylammonium bromide (OTAB). The overall degradation procedure started with the adsorption of PFMeUPA onto the modified cathode. This adsorption process was promoted by hydrophobic and electrostatic interactions between the surfactants and PFMeUPA, of which the binding percentage, binding mode, and binding energy were determined via molecular dynamics (MD) simulations and density functional theory (DFT) calculations. The step-wise degradation pathway of PFMeUPA, including reductive defluorination and hydrogenation, was derived. Meanwhile, C–F bond breaking with direct electron transfer only was achieved for the first time in this study, which also showed that the CC bond structure of PFAS facilitates the C–F cleavage. Overall, this study highlights the crucial role of quaternary ammonium surfactants in electron transfer and electrocatalytic activities in the electroreductive system and provides insights into novel remediation approaches on PFAS-contaminated groundwater.

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“…More accessible reactive sites in the catalyst indicate higher catalytic activity in the GOR. The following research on electrochemical analysis is normalized by the ECSA. − …”

Section: Resultsmentioning

confidence: 99%

ZIF-8-Derived Three-Dimensional Nitrogen-Doped Porous Carbon as a Pt Catalyst Support for Electrocatalytic Oxidation of Glucose in a Glucose Fuel Cell

Dong

et al. 2023

ACS Appl. Energy Mater.

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Durable catalysts with high catalytic activity and high oxygen tolerance are required in the glucose oxidation reaction, which is the rate-determining step in abiotic glucose fuel cells (GFCs). Herein, a ZIF-8-derived three-dimensional nitrogen-doped porous carbon (NCZIF‑8) material with a large surface area of 944 m2 g–1 is successfully synthesized as a catalyst support. Low loading rates (10 wt %) of Pt nanoparticles (NPs) are in situ reduced onto the NCZIF‑8 support (10% Pt/NCZIF‑8). The addition of the NCZIF‑8 support promotes the uniform dispersion of Pt NPs, which enhances the durability of the catalyst by preventing the aggregation of Pt NPs. Moreover, the full exposure of Pt active sites improves the catalytic efficiency, enhancing the catalytic activity during the electrocatalytic oxidation of glucose. The porous structure in NCZIF‑8 facilitates the kinetic transport of glucose. Pt NPs anchored in pores reduce the influence of oxygen during the glucose oxidation reaction. After a 300-cycle CV test, the peak current density of the 10% Pt/NCZIF‑8-decorated anode decreases only by 7.83%, which demonstrates the good durability. A dual-chamber GFC with the 10% Pt/NCZIF‑8 anode and the Pt cathode delivered a maximum power density (P max) of 0.54 μW cm–2 with an open-circuit voltage (V oc) of 323.8 mV and a short-circuit current density (J sc) of 6.5 μA cm–2. The prepared 10% Pt/NCZIF‑8 catalyst can be used as a promising catalyst in the electrocatalytic oxidation of glucose.

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Direct Electron Transfer Coordinated by Oxygen Vacancies Boosts Selective Nitrate Reduction to N₂ on a Co–CuO_x Electroactive Filter

Cited by 67 publications

References 49 publications

Fluidic MXene Electrode Functionalized with Iron Single Atoms for Selective Electrocatalytic Nitrate Transformation to Ammonia

Fluidic MXene Electrode Functionalized with Iron Single Atoms for Selective Electrocatalytic Nitrate Transformation to Ammonia

Electroreductive Defluorination of Unsaturated PFAS by a Quaternary Ammonium Surfactant-Modified Cathode via Direct Cathodic Reduction

ZIF-8-Derived Three-Dimensional Nitrogen-Doped Porous Carbon as a Pt Catalyst Support for Electrocatalytic Oxidation of Glucose in a Glucose Fuel Cell

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