Mo Vacancy-Mediated Activation of Peroxymonosulfate for Ultrafast Micropollutant Removal Using an Electrified MXene Filter Functionalized with Fe Single Atoms

Jin, Limin; You, Shijie; Ren, Nanqi; Ding, Bin; Liu, Yanbiao

doi:10.1021/acs.est.2c03904

Cited by 100 publications

(42 citation statements)

References 43 publications

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“…Electrochemical PMS activation for flow-through water treatment requires robust catalysts for widespread implementation. 16 We first compared the FESEM images of CuNW filters before and after the reactions to evaluate their robustness (Figure S25). The results suggested negligible changes of the surface chemistry, revealing the filter's stable structural and chemical nature.…”

Section: ■ Materials and Methodsmentioning

confidence: 99%

“…Second, the design of the reactor configuration plays a significant role. A conventional batch reactor is usually diffusion-limited, while the flow-through configurations are dominantly by convection. , The use of the flow-through configuration has been shown to increase the degradation kinetics of sulfamethoxazole (SMX) by 17-fold compared to a conventional batch system . Third, the introduction of an applied potential (AP) has been proven to be effective in facilitating the cycling of transition metal catalysts from high to low valence states .…”

Section: Introductionmentioning

confidence: 99%

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Copper Nanowire Networks: An Effective Electrochemical Peroxymonosulfate Activator toward Nitrogenous Pollutant Abatement

Zheng

You

Chen

et al. 2023

Environ. Sci. Technol.

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Herein, we developed an electrochemical filtration system for effective and selective abatement of nitrogenous organic pollutants via peroxymonosulfate (PMS) activation. Highly conductive and porous copper nanowire (CuNW) networks were constructed to serve simultaneously as catalyst, electrode, and filtration media. In one demonstration of the CuNW network’s capability, a single pass through a CuNW filter (τ < 2 s) degraded 94.8% of sulfamethoxazole (SMX) at an applied potential of −0.4 V vs SHE. The exposed {111} crystal plane of CuNW triggered atomic hydrogen (H*) generation on sites, which contributed to effective PMS reduction. Meanwhile, with the involvement of SMX, a Cu–N bond was formed by the interactions between the −NH2 group of SMX and the Cu sites of CuNW, accompanied by the redox cycling of Cu2+/Cu+, which was facilitated by the applied potential. The different charges of the active Cu sites made it easier to withdraw electrons and promote PMS oxidation. Theoretical calculations and experimental results were combined to suggest a mechanism for pollution abatement with CuNW networks. The results showed that system efficacy for the degradation of a wide array of nitrogenous pollutants was robust across a broad range of solution pH and complex aqueous matrices. The flow-through operation of the CuNW filter outperformed conventional batch electrochemistry due to convection-enhanced mass transport. This study provides a new strategy for environmental remediation by integrating state-of-the-art material science, advanced oxidation processes, and microfiltration technology.

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Section: ■ Materials and Methodsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Copper Nanowire Networks: An Effective Electrochemical Peroxymonosulfate Activator toward Nitrogenous Pollutant Abatement

Zheng

You

Chen

et al. 2023

Environ. Sci. Technol.

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“…[ 62 ] Jin et al characterized Fe single atoms on the surface of bimetallic MXene, and found that the absorption edge position was located between the absorption edge of bivalent and trivalent FeO x . [ 63 ] The peak at 1.42 Å is corresponded to the FeO bond, and the fitting results indicated that FeO 6 was the main structure (Figure 7c,d). Single Fe atoms synthesized by Kuznetsov et al exhibited different oxidation states and coordination environments.…”

Section: Characterizations Of Isolated Metal Atoms In Mxenesmentioning

confidence: 99%

Section: Characterizations Of Isolated Metal Atoms In Mxenesmentioning

confidence: 99%

Applications of MXene‐Based Single‐Atom Catalysts

Bai

Guan

2023

Small Structures

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Catalytic science, including heterogeneous catalysis, homogeneous catalysis, and enzyme catalysis, is involved in various fields of production and life, including energy, pharmaceuticals, environmental protection and so on. Thereinto, heterogeneous catalysis, which is usually driven by metal-based catalysts, effectively reduces production costs due to its easy recovery nature and thus plays a dominant role in industrial production. However, the distribution of active sites in heterogeneous catalysts is uncontrollable, and it is difficult to utilize the structure-activity relationship to adjust the catalyst performance. Through reducing the size of the nonmetallic catalyst and increasing the exposure of the active site, the catalytic performance can be significantly improved. Thus, design and synthesis of catalysts on atomic scale is an efficient strategy to improve catalytic activity.In 2011, Zhang et al. prepared atomically dispersed Pt species and proposed the concept of single-atom (SA) catalyst for the first time, defining single-atom catalysts (SACs) as a supported catalyst in which metal species are dispersed in the form of isolated atoms. [1] Compared with traditional catalysts, SACs have an atomic utilization efficiency of 100%, and can achieve high catalytic performance under low metal load, which greatly reduces the production cost. [2] Shi et al. loaded only 4.1 wt% Pt SAs on the surface of MoSe 2 , showing excellent alkaline electrocatalytic hydrogen evolution performance. [3] In addition, SACs have the properties of reusability and controllable structure, which combine the advantages of homogeneous and heterogeneous catalysis. [4,5] Usually, single-metal sites have uniform and adjustable coordination structures, showing the superiority of catalyzing specified reactions and improving product selectivity. By changing the activation temperature, Ren et al. synthesized Pt SAs with different electronic environment and oxidation state on Fe 2 O 3 in a controllable manner. [6] Moreover, Pd SAs with different coordination are synthesized by replacing different organic ligands, and the Pd@POL-1 coordinated with organic phosphine showed high catalytic selectivity for the hydrosilylation reaction of internal alkyne. [7] Due to the high cohesive energy, individual metal atoms tend to aggregate to form nanoclusters. [8] To obtain stable and highly dispersed metal atoms, it is usually necessary to anchor the isolated metal atoms onto a substrate, where strong charge transfer would occur through the bonding of the metal atoms to the reactive sites on the substrate. Metal oxide, metal-organic framework, molybdenum disulfide, graphene, and so on are common carriers that can be used to fix metal atoms. [9][10][11][12][13] Among them, 2D materials show good application prospects due to large specific surface area. [14,15] As a new type of 2D materials, metallic carbides, nitrides, or carbonic nitrides (MXenes), with the general structure of M n þ 1 X n T x , where M is transition metal (TM), X is carbon/nitrogen elemen...

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“…Micropollutants (MPs, such as pharmaceuticals, personal care products, and pesticides), exposure to these chemicals present in amounts (ng/L to μg/L) above the natural background levels in water bodies, pose a high risk to both ecological security and clean water supply ( 1 , 2 ). Advanced oxidation process (AOP) based on peroxymonosulfate (PMS) is a promising water treatment technology for MP decontamination ( 3 , 4 ).…”

mentioning

confidence: 99%

Generating dual-active species by triple-atom sites through peroxymonosulfate activation for treating micropollutants in complex water

Zhou

Song

Wang

et al. 2023

Proc. Natl. Acad. Sci. U.S.A.

205

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The peroxymonosulfate (PMS)-triggered radical and nonradical active species can synergistically guarantee selectively removing micropollutants in complex wastewater; however, realizing this on heterogeneous metal-based catalysts with single active sites remains challenging due to insufficient electron cycle. Herein, we design asymmetric Co–O–Bi triple-atom sites in Co-doped Bi 2 O 2 CO 3 to facilitate PMS oxidation and reduction simultaneously by enhancing the electron transfer between the active sites. We propose that the asymmetric Co–O–Bi sites result in an electron density increase in the Bi sites and decrease in the Co sites, thereby PMS undergoes a reduction reaction to generate SO 4 •- and •OH at the Bi site and an oxidation reaction to generate 1 O 2 at the Co site. We suggest that the synergistic effect of SO 4 •- , •OH, and 1 O 2 enables efficient removal and mineralization of micropollutants without interference from organic and inorganic compounds under the environmental background. As a result, the Co-doped Bi 2 O 2 CO 3 achieves almost 99.3% sulfamethoxazole degradation in 3 min with a k-value as high as 82.95 min −1 M −1 , which is superior to the existing catalysts reported so far. This work provides a structural regulation of the active sites approach to control the catalytic function, which will guide the rational design of Fenton-like catalysts.

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Mo Vacancy-Mediated Activation of Peroxymonosulfate for Ultrafast Micropollutant Removal Using an Electrified MXene Filter Functionalized with Fe Single Atoms

Cited by 100 publications

References 43 publications

Copper Nanowire Networks: An Effective Electrochemical Peroxymonosulfate Activator toward Nitrogenous Pollutant Abatement

Copper Nanowire Networks: An Effective Electrochemical Peroxymonosulfate Activator toward Nitrogenous Pollutant Abatement

Applications of MXene‐Based Single‐Atom Catalysts

Generating dual-active species by triple-atom sites through peroxymonosulfate activation for treating micropollutants in complex water

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