Photogeneration of Reactive Species from Biochar-Derived Dissolved Black Carbon for the Degradation of Amine and Phenolic Pollutants

Wan, Dong; Wang, Jie; Dionysiou, Dionysios D.; Kong, Yaqian; Yao, Wenlong; Selvinsimpson, Steplinpaulselvin; Chen, Yong

doi:10.1021/acs.est.1c01942

Cited by 83 publications

(51 citation statements)

References 67 publications

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“…Hence, the oxidants of lower selectivity but higher steady-state concentrations may play a dominant role in the degradation of target pollutants. The competitive contribution of radicals is ubiquitous in AOPs-related studies. ,,,− Moreover, special attention should be paid to DOM which exhibits rather complicated role in practical application. DOM could accelerate the degradation of pollutants via photosensitization to generate reactive species, serving as electron shuttle mediators, − or hamper the oxidation via reduction of the intermediates or competitive adsorption and degradation …”

Section: Selective Oxidation Via Tuning the Reactivity Of Reactantsmentioning

confidence: 99%

Toward Selective Oxidation of Contaminants in Aqueous Systems

Yang

Qian

Shan

et al. 2021

Environ. Sci. Technol.

214

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The presence of diverse pollutants in water has been threating human health and aquatic ecosystems on a global scale. For more than a century, chemical oxidation using strongly oxidizing species was one of the most effective technologies to destruct pollutants and to ensure a safe and clean water supply. However, the removal of increasing amount of pollutants with higher structural complexity, especially the emerging micropollutants with trace concentrations in the complicated water matrix, requires excessive dosage of oxidant and/ or energy input, resulting in a low cost-effectiveness and possible secondary pollution. Consequently, it is of practical significance but scientifically challenging to achieve selective oxidation of pollutants of interest for water decontamination. Currently, there are a variety of examples concerning selective oxidation of pollutants in aqueous systems. However, a systematic understanding of the relationship between the origin of selectivity and its applicable water treatment scenarios, as well as the rational design of catalyst for selective catalytic oxidation, is still lacking. In this critical review, we summarize the state-of-the-art selective oxidation strategies in water decontamination and probe the origins of selectivity, that is, the selectivity resulting from the reactivity of either oxidants or target pollutants, the selectivity arising from the accessibility of pollutants to oxidants via adsorption and size exclusion, as well as the selectivity due to the interfacial electron transfer process and enzymatic oxidation. Finally, the challenges and perspectives are briefly outlined to stimulate future discussion and interest on selective oxidation for water decontamination, particularly toward application in real scenarios.

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Section: Selective Oxidation Via Tuning the Reactivity Of Reactantsmentioning

confidence: 99%

Toward Selective Oxidation of Contaminants in Aqueous Systems

Yang

Qian

Shan

et al. 2021

Environ. Sci. Technol.

214

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“…To explore the effects of the amendments on the photochemistry of paddy water, we first used LFP and EPR spectroscopy to identify the photogenerated RIs. As shown in Figure S2a, photoexcited paddy water showed unidentified transients with a broad unstructured absorption band centered at 440 nm, similar to the transient absorption spectra of typical DOM samples. , Owing to the complexity of the transient signals, the absorption band may consist of a superposition of signals from 3 DOM* or DOM radicals produced upon laser excitation . These results suggest that 3 DOM* or DOM radicals would be formed from paddy water under irradiation.…”

Section: Resultsmentioning

confidence: 54%

“…25,26 Owing to the complexity of the transient signals, the absorption band may consist of a superposition of signals from 3 DOM* or DOM radicals produced upon laser excitation. 27 These results suggest that 3 DOM* or DOM radicals would be formed from paddy water under irradiation. EPR analysis was used to further identify the formed RIs.…”

Section: ■ Introductionmentioning

confidence: 81%

Mechanistic Study of the Effects of Agricultural Amendments on Photochemical Processes in Paddy Water during Rice Growth

Zeng

Fang

et al. 2022

Environ. Sci. Technol.

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The photochemical properties of paddy water might be affected by the commonly used amendments in rice fields owing to the associated changes in water chemistry; however, this important aspect has rarely been explored. We examined the effects of agricultural amendments on the photochemistry of paddy water during rice growth. The amendments significantly influenced the photogenerated reactive intermediates (RIs) in paddy water, such as triplet dissolved organic matter (3DOM*), singlet oxygen, and hydroxyl radicals. Compared with control experiments without amendments, the application of straw and lime increased the RI concentrations by up to 16.8 and 11.1 times, respectively, while biochar addition had limited effects on RI generation from paddy water in in situ experiments under sunlight. Fluorescence emission–excitation matrix spectroscopy, Fourier transform ion cyclotron resonance mass spectrometry, and structural equation modeling revealed that upon the addition of straw and lime amendments, humified DOM substances contained lignins, proteins, and fulvic acids, which could produce more RIs under irradiation. Moreover, the amendments significantly accelerated the degradation rate of 2,4-dichlorophenol but led to the 3DOM*-mediated formation of more toxic and stable dimeric products. This study provides new insights into the effects of amendments on the photochemistry of paddy water and the pathways of abiotic degradation of organic contaminants in paddy fields.

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“…Thus, the UV-LEDs with variable wavelengths can enhance contaminant photodegradation by facilitating the match of excitation wavelength with the absorbance and/or quantum yield maxima of contaminants and/or root exudates. It can be predicted that some 3 DOM* or 1 O 2 -labile contaminants (e.g., atenolol, diphenhydramine, cimetidine, and cyanopeptides) could be efficiently photodegraded in the waters with Pistia stratiotes. , For the contaminants that belong to the · OH-dominated degradation compound (e.g., caffeine, N,N-diethyl-m-toluamide, and telmisartan), , they are likely to have higher photodegradation rates in the waters with Eichhornia crassipes. Overall, this study provides new insights into the wavelength-dependent photoreactivity of the root exudates of aquatic plants under UV-LED irradiation.…”

Section: Discussionmentioning

confidence: 99%

Wavelength-Dependent Photoreactivity of Root Exudates from Aquatic Plants under UV-LED Irradiation

et al. 2022

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Aquatic plants and their root exudates play important roles in the removal of trace organic contaminants in aquatic environments. However, the wavelength-dependent photogeneration of reactive species (RS) and photodegradation of organic contaminants by root exudates are poorly understood. This paper presents the first evidence that the photogeneration of 3DOM*, 1O2, and ·OH by root exudates varied under UV light-emitting diode (UV-LED) irradiation in the wavelength range of 265–400 nm. The quantum yields of 3DOM* and 1O2 of the four plants’ root exudates, including Scindapsus aureus, Pistia stratiotes, Eichhornia crassipes, and Nymphaea tetragona, reached the highest value at an irradiation wavelength of 275 nm and further decreased with increasing wavelength, while the ·OH quantum yield decreased gradually from 3.2–5.5 × 10–4 at 265 nm to 1.4–2.6 × 10–6 at 400 nm. The root exudate of Pistia stratiotes showed higher quantum yields of 3DOM* and 1O2 than that of the other three plants, while the highest ·OH quantum yield was observed in that of Eichhornia crassipes. The excitation wavelength affected the indirect degradation of organic contaminants by altering the photogeneration of RS in root exudate solutions. These findings highlight the wavelength-dependent photoreactivity of root exudates and improve the understanding of their photochemical processes in aquatic environments.

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Photogeneration of Reactive Species from Biochar-Derived Dissolved Black Carbon for the Degradation of Amine and Phenolic Pollutants

Cited by 83 publications

References 67 publications

Toward Selective Oxidation of Contaminants in Aqueous Systems

Toward Selective Oxidation of Contaminants in Aqueous Systems

Mechanistic Study of the Effects of Agricultural Amendments on Photochemical Processes in Paddy Water during Rice Growth

Wavelength-Dependent Photoreactivity of Root Exudates from Aquatic Plants under UV-LED Irradiation

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