Synergistic effects for boosted persulfate activation in a designed Fe–Cu dual-atom site catalyst

Wu, Huihui; Yan, Jingjing; Xu, Xin; Yuan, Qinqin; Wang, Jinhang; Cui, Jun; Lin, Aoxiang

doi:10.1016/j.cej.2021.132611

Cited by 85 publications

(53 citation statements)

References 53 publications

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“…Recently, the copper (Cu)-based high-density SACs have also been proved to have considerable catalytic activity for the activation of PMS. [229,230,233] For example, Pan et al synthesized highdensity (%6 atoms nm À2 ) Cu atom anchored on the N-dopped biochar (SACu@NBC), which showed excellent catalytic activity for PMS activation and the complete removal of bisphenol A (BPA) within 30 min (see Figure 23H,I). [229] The mechanism of electron transfer in SACu@NBC/PMS system was accurately identified by anodic oxidation analogy, and the Cu single atom is the active center of catalyst, which can obviously improve the electron transfer and reaction activity of carbon carrier.…”

Section: Brief Summary Of Afcs On Electrocatalysismentioning

confidence: 99%

“…The nanozyme and TMB were added to 1 mL NaAc buffer (pH ¼ 4.5) Catalytic rate constant (K cat ¼ 1.474 Â 10 À1 s À1 ); Antibacterial activity against Escherichia coli perdisulfate (PDS) activation. [233] DFT calculations showed that the Cu atoms can effectively optimize the distribution of Fe 3 d bonding orbitals and keep low state of Fe atoms, thus promoting the adsorption and pyrolysis of PDS and the oxidative decomposition of pollutants. At present, a variety of metal SACs (M-N x ) can produce singlet oxygen ( 1 O 2 ) with long service life and high efficiency and can be used as active oxygen species for efficient degradation of organic pollutants.…”

Section: °Cmentioning

confidence: 99%

“…[228,231] The single-site adsorption mode is beneficial for the utilization of each single metal site in moderate atomic density (1-5 atoms nm À2 ), where the PMS molecules can be divided into OH* and SO 4 * moieties spontaneously to assist the production of O immediate and 1 O 2 (see Figure 23M). Importantly, for ultrahigh-density (10-20 atoms nm À2 ) SACs (see Table 1) [9,11,37,49,56,57,84,176,207] or bimetallic/DACs (see the inset in Figure 23L), [233] their average atomic distance (or atomic pair distance) is often less than 0.3 nm, which provides an opportunity to adsorb two O atoms of PDS molecules by two adjacent metal sites (or the atom pair). In particular, adjacent metal atoms (or bimetallic atoms) often lead to changes in the electronic structure that favor molecular adsorption and chemical bond activation.…”

Section: °Cmentioning

confidence: 99%

“…It is worth mentioning that the size or space matching between isolated metal sites and substrate molecules is critical to catalytic performances in multiple catalytic reaction types. [56,84,174,233] For Li-S batteries, the polysulfide of Li 2 S n (n ¼ 4-8) molecules generated during charge and discharge are much larger than the size of metal sites of SACs. Therefore, the catalytic effect of SACs with completely isolated sites on sulfur cathode may not be the best.…”

Section: Polysulfide Catalytic Conversionmentioning

confidence: 99%

“…Furthermore, the high‐density (≈4 atoms nm −2 ) Fe/Cu bimetallic single sites on N‐dopped porous carbon were designed and synthesized by Wu et al, where Cu–N plays a key role in improving the catalytic capacity of Fe/Cu–N–C catalyst for perdisulfate (PDS) activation. [ 233 ] DFT calculations showed that the Cu atoms can effectively optimize the distribution of Fe 3 d bonding orbitals and keep low state of Fe atoms, thus promoting the adsorption and pyrolysis of PDS and the oxidative decomposition of pollutants.…”

Section: Heterogeneous Catalysis Applications Of Afcsmentioning

confidence: 99%

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Emerging Ultrahigh‐Density Single‐Atom Catalysts for Versatile Heterogeneous Catalysis Applications: Redefinition, Recent Progress, and Challenges

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In recent years, single‐atom catalysts (SACs) with high metal loading have emerged in different heterogeneous catalysis fields and shown extraordinary catalytic properties. When there are enough coordination atoms (or functional groups) on the supports, it is possible to achieve a limit monolayer atom loading on the surface of supports with ultrahigh atom density (5–15 atoms nm−2) and extremely close site distance (0.2–0.5 nm), by using appropriate synthesis methods and procedures. These high‐density metal atoms usually have no or less metal bonds, which are mostly isolated by support atoms to form 3D foam‐like atomic constructions. Herein, a new notion of metal atomic foam catalysts (AFCs) is propsed to redefine these ultrahigh‐density SACs accommodated by specific supports. This new paradigm of 3D atomic construction for SACs has potential significance for both theoretical research and industrial applications. The latest major advancements in the controllable synthesis of AFCs on various supports (e.g., polymer, carbon, and metallic compound) via different methods (bottom‐up or top‐down approaches) are summarized. The latent catalytic principles and typical application cases of AFCs are emphasized in a wide range of heterogeneous catalysis fields (e.g., thermocatalysis, photocatalysis, electrocatalysis, etc.). The challenges and prospects of this newly 3D ultrahigh‐density AFCs materials in practical industrial application are pointed out as well.

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Section: Brief Summary Of Afcs On Electrocatalysismentioning

confidence: 99%

Section: °Cmentioning

confidence: 99%

Section: °Cmentioning

confidence: 99%

Section: Polysulfide Catalytic Conversionmentioning

confidence: 99%

Section: Heterogeneous Catalysis Applications Of Afcsmentioning

confidence: 99%

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Emerging Ultrahigh‐Density Single‐Atom Catalysts for Versatile Heterogeneous Catalysis Applications: Redefinition, Recent Progress, and Challenges

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Recent Advance of Atomically Dispersed Dual‐Metal Sites Carbocatalysts: Properties, Synthetic Materials, Catalytic Mechanisms, and Applications in Persulfate‐Based Advanced Oxidation Process

Wei

Cui

et al. 2023

Adv Funct Materials

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Recently, atomically dispersed dual‐metal sites carbocatalysts (DMSCs) make a wave in the field of persulfate‐based advanced oxidation processes (PS‐AOPs) in light of their ≈100% atomic utilization efficiency, high density of active sites, and superior catalytic activity. This review aims to provide a state‐of‐the‐art overview on the development of DMSCs for activating PS. Initially, the types and properties of DMSCs are summarized, as well as the role of doping different heteroatoms is discussed. Subsequently, the properties of different carbon carriers and the methods for the synthesis of DMSCs are outlined. After that, the mechanism and application of DMSCs for the activation of PS toward organic contaminants degradation are revealed. Particularly, the mechanism of nonradical pathway is described, and the necessity of coupling DMSCs‐based PS‐AOPs to other processes for practical water treatment is emphasized. Finally, the formidable challenges and future research directions of DMSCs are proposed. This review is expected to provide insight into the preparation of DMSCs in the field of nanomaterials and to broaden the path for their environmental applications.

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Single‐Atom Catalysts Originated from Metal–Organic Frameworks for Sulfate Radical‐Based Advanced Oxidation Processes: Critical Insights into Mechanisms

Chen,

Kang,

Cheng

et al. 2023

Adv Funct Materials

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The widely discussed single‐atom catalysts (SACs) are regarded as a kind of attractive material for sulfate radical‐based advanced oxidation processes (SR‐AOPs) owing to their maximum atomic utilization efficiency and outstanding stability. Currently, metal–organic frameworks (MOFs) have appeared as prospective precursors for building SACs due to extensive chelating sites, functional adjustability, and structural tunability. However, there are few critical and systematic reviews about the application of MOF‐derived SACs in SR‐AOPs, especially in‐depth analysis of the mechanisms. Therefore, this review seeks to offer a thorough summary of the development of MOF‐derived SACs in SR‐AOPs. First, the unique advantages of MOFs as derivative precursors for SACs are discussed thoroughly. Afterward, the current synthesis strategies are elaborated categorically to unveil the formation process of single atoms and their coordination environments. Notably, the roles of different reaction sites including the generation of reactive species and mediating electron transfer are further analyzed to explain mechanisms comprehensively. Thereafter, the characterization techniques and theoretical calculations for mechanisms studies are also highlighted. Eventually, critical insights into present challenges and future developments are proposed, which are expected to enhance the catalytic efficiency of MOF‐derived SACs in SR‐AOPs.

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Synergistic effects for boosted persulfate activation in a designed Fe–Cu dual-atom site catalyst

Cited by 85 publications

References 53 publications

Emerging Ultrahigh‐Density Single‐Atom Catalysts for Versatile Heterogeneous Catalysis Applications: Redefinition, Recent Progress, and Challenges

Emerging Ultrahigh‐Density Single‐Atom Catalysts for Versatile Heterogeneous Catalysis Applications: Redefinition, Recent Progress, and Challenges

Recent Advance of Atomically Dispersed Dual‐Metal Sites Carbocatalysts: Properties, Synthetic Materials, Catalytic Mechanisms, and Applications in Persulfate‐Based Advanced Oxidation Process

Single‐Atom Catalysts Originated from Metal–Organic Frameworks for Sulfate Radical‐Based Advanced Oxidation Processes: Critical Insights into Mechanisms

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