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Emerging single‐atom catalysts (SACs) are promising in water remediation through Fenton‐like reactions. Despite the notable enhancement of catalytic activity through increasing the density of single‐atom active sites, the performance improvement is not solely attributed to the increase in the number of active sites. The variation of catalytic behaviors stemming from the increased atomic density is particularly elusive and deserves an in‐depth study. Herein, single‐atom Fe catalysts (FeSA‐CN) with different distances (dsite) between the adjacent single‐atom Fe sites are constructed by controlling Fe loading. With the decrease in dsite value, remarkably enhanced catalytic activity of FeSA‐CN is realized via the electron transfer regime with peroxymonosulfate (PMS) activation. The decrease in dsite value promotes electronic communication and further alters the electronic structure in favor of PMS activation. Moreover, the two adjacent single‐atom Fe sites collectively adsorb PMS and achieve single‐site desorption of the PMS decomposition products, maintaining continuous PMS activation and contaminant removal. Moreover, the FeSA‐CN/PMS system exhibits excellent anti‐interference performance for various aquatic systems and good durability in continuous‐flow experiments, indicating its great potential for water treatment applications. This study provides an in‐depth understanding of the distance effect of single‐atom active sites on water remediation by designing densely populated SACs. [ABSTRACT FROM AUTHOR]

Abstract: Ag–AgBr was deposited onto mesoporous alumina (MA) and titanium-doped MA by a deposition–precipitation method. The photocatalytic activity and the dissolution of Ag+ from different catalysts were investigated during the photodegradation of 2-chlorophenol (2-CP) and phenol in ultrapure water and tap water with visible-light irradiation. With the increase in doped titanium, the Ag+ dissolution decreased with a decrease in the photocatalytic activity. Ag–AgBr/MA-Ti1 was considered the better catalyst for practical applications because its Ag+ dissolution was minimal (0.4mgL−1 in ultrapure water and 5μgL−1 in tap water), although its photoactivity was slightly less than that of Ag–AgBr/MA. The dissolution of Ag+ was related to a charge–transfer process based on the study of cyclic voltammetry analyses under a variety of experimental conditions. The results suggested that several types of anions in the water, including CO3 2−, SO4 2−, and Cl−, could act as electron donors that trap the photogenerated holes on Ag nanoparticles to facilitate electron circulation; this would decrease the release of Ag+. Our studies indicated that the catalyst had a higher activity and stability in water purification. [Copyright &y& Elsevier]

[Display omitted] • Surface microelectric fields (SMEF) on catalyst were formed by electrostatic force. • The formation of SMEF maximize the removal of refractory pollutants in wastewater. • The SMEF can link electron transfer between refractory pollutants and microorganisms. • The interspecific electron transport was induced by SMEF to can speed up degradation. The stable structure and toxic effect of refractory organic pollutants in wastewater lead to the problem of high energy consumption in water treatment technology. Herein, we propose a synergistic purification of refractory wastewater driven by microorganisms and surface microelectric fields (SMEF) over a dual-reaction-center (DRC) catalyst HCLL-S8-M prepared by an in situ growth method of carbon nitride on the Cu-Al 2 O 3 surface. Characterization techniques demonstrate the successful construction of SMEF with strong electrostatic force over HCLL-S8-M based on cation-π interactions between metal copper ions and carbon nitride rings. With the catalyst as the core filler, an innovative fixed bed bioreactor is constructed to purify the actual kitchen-oil wastewater. The removal efficiency of the wastewater even with a very low biodegradability (BOD 5 /COD = 0.33) can reach 60% after passing through this bioreactor. An innovative reaction mechanism is revealed for the first time that under the condition of a small amount of biodegradable organic matter, the SMEF induces the enrichment of electric active microorganisms (Desulfobulbus and Geobacter) in the wastewater, accelerates the interspecies electron transfer of intertrophic metabolism with the biodegradable bacteria through the extracellular electron transfer mechanism such as cytochrome C and self-secreted electron shuttle. The electrons of the refractory organic pollutants adsorbed on the surface of the catalyst are delocalized by the SMEF, which can be directly utilized by microorganisms through EPS conduction. The SMEF generated by electron polarization can maximize the utilization of pollutants and microorganisms in wastewater and further enhance degradation without adding any external energy, which is of great significance to the development of water self-purification technology. [ABSTRACT FROM AUTHOR]

In common advanced oxidation processes, excess reagents and energy are often added to the reaction system to maintain the continuity of the reaction. These additions result in a large waste of resources and energy, which has become a bottleneck in the development of water treatment technology. In this study, we propose a new strategy to solve this problem based on a novel dual-reaction-center (DRC) Fe-ZnS quantum dots (Fe–ZnS QDs) catalyst that forms a non-equilibrium surface with an electron-polarized distribution. Through experimental and theoretical studies, it was verified that the activation of trace amounts of H 2 O 2 could break the energy barrier for pollutants to transfer electrons. The dissolved oxygen (DO) in the reaction system could be activated by gaining energy on the surface of the Fe–ZnS QDs catalyst, and was converted to 1O 2 to attack organic pollution. In addition, the pollutants themselves supplied electrons to H 2 O 2 through the surface of the Fe–ZnS QDs catalyst to generate more •OH radicals for pollutant degradation, thus providing two fast paths for pollutant degradation. The system could drive the reaction through a trace amount of H 2 O 2 , thereby activating DO to generate 1O 2 while effectively using the energy of pollutants. Therefore, the proposed system offers a new direction for the development of environmentally-friendly catalysts and greatly reduces the consumption of resources and energy. [Display omitted] • Fe–ZnS QDs is successfully developed as a Fenton catalyst for the first time. • The surface of ZnS QDs is regulated by trace Fe to form a non-equilibrium surface with an electron-polarized distribution. • The Fe–ZnS QDs/H 2 O 2 system exhibits excellent activity for pollutants degradation. • Inert oxygen species in reaction system are easily activated to 1O 2 to attack pollutants. [ABSTRACT FROM AUTHOR]

Layered structural BiOBr with {110} facet exposure is a promising functional material for highly selective adsorption and separation of heavy metal ions in water purification. In this study, the distinct adsorption behaviors of As(III), As(V), and Cr(VI) on {110} facet were theoretically and experimentally investigated. The results suggested that uncharged As(III) was dominantly adsorbed on the [Bi 2 O 2 ]2+ surface replacing the hydroxyl group, whereas Cr(VI) and As(V) oxyanions preferentially intercalated on {110} facet by exchange with Br- ions between the layers. Moreover, due to interfacial coupling configuration ([BiO-CrO 4 -OBi]-O-As(OH) 2) between the surface and interlayer on {110} facet, the synergic removal of Cr(VI) and As(III) could be accelerated under photoexcitation to induce a direct electron transfer from surface AsIII to interlayer CrVI, forming AsV and CrIII. Subsequently, approximately 69.3% of Cr(III) and 98.6% of As(V) were readily desorbed in acidic conditions and a high concentration of Br- solution, respectively, to achieve simultaneous detoxification and selective separation. [Display omitted] • Oxyanions (CrO 4 2- and HAsO 4 2-) preferentially intercalated between BiOBr layers by exchange with Br- ion. • Interfacial coupling configuration was constructed by the intercalated Cr(VI) and surface adsorbed As(III) on {110} facet. • Synergic removal was accelerated by electrons transfer from surface As(III) to interlayer Cr(VI) for both detoxification. • Selective separation of chromium and arsenic was based on interlayer anion-exchange property. [ABSTRACT FROM AUTHOR]

• Co2+-N-C π is constructed via atomically dispersed Co bonding with C-based graphene-like structure. • Co2+-N-C π (Co−π) structure plays key role for PMS activation and pollutant degradation. • Electron donation effect of pollutants is realized through π-π interaction in SACo-NGs system. • High efficiency and low consumption are realized in SACo-NGs/PMS water treatment system. Orbital interaction involving metal cation−π is an important form for electron transfer regulation. To accelerate the interfacial electron transfer of peroxymonosulfate (PMS) activation for water treatment, we report a new strategy through bonding atomically dispersed cobalt with nanospheric C-based graphene-like structures (SACo-NGs) to form metal cation−π structure, driving rapid and directional transfer of the electrons of pollutants to PMS on the catalyst surface. The catalyst SACo-NGs is synthesized by an enhanced hydrothermal-sintering method and the formation of metal cation−π structure is demonstrated by X-ray absorption fine structure (EXAFS), X-ray photoelectron spectroscopy (XPS), electron paramagnetic resonance spectroscopy (EPR) and Raman spectroscopy. It is found that Co−π structures (Co2+-N-C π) play a key role for the efficient activation of PMS, which results in pollutants being greatly removed in a few minutes. During the reaction, pollutants can donate electrons for the system through π−π interaction accompanying by the direct oxidative degradation of pollutants. The obtained electrons are quickly transferred to the atomically dispersed cobalt sites through the formed cation−π structure, which promotes the activation of PMS. This is a successful practice in the field of PMS activation using cation−π structure to accelerate electron transfer and achieve rapid degradation of pollutants. [ABSTRACT FROM AUTHOR]

• Multiple vacancy associates were introduced by constructing porous β-Bi 2 O 3 -{220}. • Porous β-Bi 2 O 3 -{220} was highly effective for pollutants removal under visible light. • Multiple vacancy associates enhanced surface polarization for efficient charge separation. • The electron transfer from pollutants to the catalyst was promoted by their strong interaction. • HO 2 and holes were confirmed to be the main active species. Porous β-Bi 2 O 3 with highly exposed {220} facets was fabricated for the first time and the formation of surface multiple Bi-O vacancy associates was confirmed by the photoluminescence, positron annihilation spectra, and theoretical calculations. Compared with traditional nonporous β-Bi 2 O 3 -{201}, the photocatalytic rate of porous β-Bi 2 O 3 -{220} was more than twice faster and the photoconversion efficiency increased by 20 times. And various refractory organic pollutants can be effectively degraded and mineralized under visible light. Multiple Bi-O vacancy associates were demonstrated to change electronic structure and enhance the polarization of the related atoms and orbitals. The photogenerated charge separation and transfer was thus improved to produce more surface active species. Simultaneously, the electron transfer from pollutants to the catalyst was found to be accelerated, finally leading to the outstanding photocatalytic performances of porous β-Bi 2 O 3 -{220}. These findings provide useful insights into the development of visible-light-driven photocatalysts for water purification. [ABSTRACT FROM AUTHOR]