An N,S-Anchored Single-Atom Catalyst Derived from Domestic Waste for Environmental Remediation

Cui, Peixin; Yang, Qiang; Liu, Cun; Wang, Yu; Fang, Guodong; Dionysiou, Dionysios D.; Wu, Tongliang; Zhou, Yiyi; Ren, Junxiang; Hou, Haijun; Wang, Yujun

doi:10.1021/acsestengg.1c00255

Cited by 42 publications

(23 citation statements)

References 45 publications

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“…There is a linear relationship between positions of the absorption edge and Mn valences, and the valence of Mn in PABC-750 is determined as +2.48 (Figure S5 and Table S2), suggesting that Mn(II) is the main form of Mn in PABC-750. The ab initio XANES calculation was employed for the quantitative analysis of the 3D local structure around Mn . The fitting result indicates the Mn–N 4 structure with four Mn–N bond lengths of 1.93, 1.95, 2.01, and 2.02 Å (Figure b) is the active site in PABC-750.…”

Section: Resultsmentioning

confidence: 99%

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Atomically Dispersed Manganese on Biochar Derived from a Hyperaccumulator for Photocatalysis in Organic Pollution Remediation

Cui

Liu

et al. 2022

Environ. Sci. Technol.

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Phytoremediation is a potentially cost-effective and environmentally friendly remediation method for environmental pollution. However, the safe treatment and resource utilization of harvested biomass has become a limitation in practical applications. To address this, a novel manganese-carbon-based single-atom catalyst (SAC) method has been developed based on the pyrolysis of a manganese hyperaccumulator, Phytolacca americana. In this method, manganese atoms are dispersed atomically in the carbon matrix and coordinate with N atoms to form a Mn–N4 structure. The SAC developed exhibited a high photooxidation efficiency and excellent stability during the degradation of a common organic pollutant, rhodamine B. The Mn–N4 site was the active center in the transformation of photoelectrons via the transfer of photoelectrons between adsorbed O2 and Mn to produce reactive oxygen species, identified by in situ X-ray absorption fine structure spectroscopy and density functional theory calculations. This work demonstrates an approach that increases potential utilization of biomass during phytoremediation and provides a promising design strategy to synthesize cost-effective SACs for environmental applications.

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Section: Resultsmentioning

confidence: 99%

“…The ab initio XANES calculation was employed for the quantitative analysis of the 3D local structure around Mn. 35 The fitting result indicates the Mn−N 4 structure with four Mn−N bond lengths of 1.93, 1.95, 2.01, and 2.02 Å (Figure 2b) is the active site in PABC-750.…”

Section: ■ Introductionmentioning

confidence: 98%

Atomically Dispersed Manganese on Biochar Derived from a Hyperaccumulator for Photocatalysis in Organic Pollution Remediation

Cui

Liu

et al. 2022

Environ. Sci. Technol.

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“…Notably, the lowest E ads and strongest interaction in Model D suggests that the PMS molecules preferred to adsorb onto this configuration, thus exposing the electron channel. [ 21 ] Furthermore, the crystal orbital Hamilton population (COHP) analysis of the O–O band in the four models was also investigated. [ 22 ] The less negative COHP of Model D presented more activation of the O–O band in PMS, which was further in coordination with the above results (Figure 5b).…”

Section: Resultsmentioning

confidence: 99%

Defect Engineering Modulated Iron Single Atoms with Assist of Layered Clay for Enhanced Advanced Oxidation Processes

Zhang

Wang

et al. 2022

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Single‐atom catalysts (SACs) feature maximum atomic utilization efficiency; however, the loading amount, dispersibility, synthesis cost, and regulation of the electronic structure are factors that need to be considered in water treatment. In this study, kaolinite, a natural layered clay mineral, is applied as the support for g‐C3N4 and single Fe atoms (FeSA‐NGK). The FeSA‐NGK composite exhibits an impressive degradation performance toward the target pollutant (>98% degradation rate in 10 min), and catalytic stability across consecutive runs (90% reactivity maintained after three runs in a fluidized‐bed catalytic unit) under peroxymonosulfate (PMS)/visible light (Vis) synergetic system. The introduction of kaolinite promotes the loading amount of single Fe atoms (2.57 wt.%), which is a 14.2% increase compared to using a bare catalyst without kaolinite, and improved the concentration of N vacancies, thereby optimizing the regulation of the electronic structure of the single Fe atoms. It is discovered that the single Fe atoms successfully occupied five coordinated N atoms and combined with a neighboring N vacancy. Consequently, this regulated the local electronic structure of single Fe atoms, which drives the electrons of N atoms to accumulate on the Fe centers. This study opens an avenue for the design of clay‐based SACs for water purification.

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“…Second, we note that most SACs studied for persulfate activation were built upon the M−N−C structure, while SACs can be coordinated to other heteroatoms such as O, S, P, or B (e.g., S/N codoping for Co SAC, 270 N/B or N/P codoping for Cu SAC 271 ). The electronegativities of these elements follow the order: O (χ O = 3.44) > N (χ N = 3.04) > S (χ O = 2.58) > C (χ C = 2.55) > P (χ P = 2.19) > B (χ B = 2.04).…”

Section: ■ Challenges and Research Directionsmentioning

confidence: 99%

Outlook on Single Atom Catalysts for Persulfate-Based Advanced Oxidation

Kim

2022

ACS EST Eng.

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Single atom catalysts (SACs) have emerged as a promising catalyst material architecture for energy, chemical, and environmental applications. In the past several years, SACs have been increasingly explored for persulfate-based advanced oxidation processes (AOPs) due to their superior persulfate activation and pollutant degradation performance compared to benchmark dissolved ion and nanoparticle catalysts. However, there still exist uncertainties on the mechanism of persulfate activation by SACs, which involves a complex interplay of sulfate and hydroxyl radicals, singlet oxygen, high-valent metal species, and/or mediated electron transfer. Questions also remain as to how persulfate ions molecularly align on the single atom site, how persulfate ions are converted into reactive species, and what design parameters lead to higher efficiency for persulfate activation and pollutant degradation. In this critical review, we examine past SAC materials employed for persulfate-based AOPs and discuss how they function differently compared to their ion and nanoparticle counterparts. We further our discussion on current limitations, opportunities, and future research needs in (i) filling the knowledge gaps in the mechanisms of persulfate-SAC interactions; (ii) augmenting fundamental research with theoretical simulation and in situ characterization techniques; (iii) improving material design tailored for environmental applications; and (iv) proactively considering the challenges associated with engineering practices and complex water matrixes.

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An N,S-Anchored Single-Atom Catalyst Derived from Domestic Waste for Environmental Remediation

Cited by 42 publications

References 45 publications

Atomically Dispersed Manganese on Biochar Derived from a Hyperaccumulator for Photocatalysis in Organic Pollution Remediation

Atomically Dispersed Manganese on Biochar Derived from a Hyperaccumulator for Photocatalysis in Organic Pollution Remediation

Defect Engineering Modulated Iron Single Atoms with Assist of Layered Clay for Enhanced Advanced Oxidation Processes

Outlook on Single Atom Catalysts for Persulfate-Based Advanced Oxidation

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