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Regulating the distribution of reactive oxygen species generated from H2O2 activation is the prerequisite to ensuring the efficient and safe use of H2O2 in the chemistry and life science fields. Herein, we demonstrate that constructing a dual Cu−Fe site through the self‐assembly of single‐atomic‐layered Cu5 nanoclusters onto a FeS2 surface achieves selective H2O2 activation with high efficiency. Unlike its unitary Cu or Fe counterpart, the dual Cu−Fe sites residing at the perimeter zone of the Cu5/FeS2 interface facilitate H2O2 adsorption and barrierless decomposition into ⋅OH via forming a bridging Cu‐O‐O‐Fe complex. The robust in situ formation of ⋅OH governed by this atomic‐layered catalyst enables the effective oxidation of several refractory toxic pollutants across a broad pH range, including alachlor, sulfadimidine, p‐nitrobenzoic acid, p‐chlorophenol, p‐chloronitrobenzene. This work highlights the concept of building a dual catalytic site in manipulating selective H2O2 activation on the surface molecular level towards efficient environmental control and beyond. [ABSTRACT FROM AUTHOR]

The efficiencies of semiconductor photocatalysis are always severely restricted by the rapid recombination of charge carriers in the bulk phase, while local polarization is an efficient scenario to conquer the above issue to boost the photocatalytic performance. Here, as a proof‐of‐concept demonstration, local charge polarization induced by the intrinsic zwitterionic resonance structure of photocatalysts is reported. A novel squaraine‐based covalent organic framework (SQ‐COF‐1) photocatalyst with an interesting zwitterionic resonance structure is creatively developed. Meanwhile, the comparison samples (SQ‐COF‐2 and PDA‐COF) based on similar COF structure with tunable local polarity are accordingly designed and prepared. The local charge polarization generated from the zwitterionic resonance structure profoundly redistributes and separates the charge carriers, as evidenced by experimental and theoretical results collectively. Benefiting by the largest local polarization, SQ‐COF‐1 exhibits superior visible‐light‐driven photocatalytic activities than SQ‐COF‐2, PDA‐COF, and commonly used polymeric carbon nitride photocatalyst. This work presents a local charge polarization protocol for engineering charge behavior to promote photocatalysis, which shows great promise for the future design of high‐performance photocatalytic materials. [ABSTRACT FROM AUTHOR]

Efficient molecular oxygen activation is crucial for catalytic oxidation reaction, but highly depends on the construction of active sites. In this study, we demonstrate that dual adjacent Fe atoms anchored on MnO2 can assemble into a diatomic site, also called as MnO2-hosted Fe dimer, which activates molecular oxygen to form an active intermediate species Fe(O = O)Fe for highly efficient CO oxidation. These adjacent single-atom Fe sites exhibit a stronger O2 activation performance than the conventional surface oxygen vacancy activation sites. This work sheds light on molecular oxygen activation mechanisms of transition metal oxides and provides an efficient pathway to activate molecular oxygen by constructing new active sites through single atom technology. Efficient oxygen activation is crucial for catalytic oxidation reaction, but highly depends on the construction of active sites. Here, dual adjacent Fe atoms anchored on MnO2 can assemble into a diatomic site, which activates molecular oxygen to form an active intermediate species Fe(O = O)Fe for CO oxidation. [ABSTRACT FROM AUTHOR]

The use of solar energy to drive organic reactions under mild conditions provides a sustainable pathway for green synthesis and has been one of the primary goals pursued by scientists. In this research, the cadmium indium sulfide (CdIn2S4) photocatalyst was prepared using a simple solvothermal method and was thoroughly characterized using X-ray powder diffraction, UV-visible absorption spectra, nitrogen adsorption–desorption isotherms, scanning electron microscopy, transmission electron microscopy and X-ray spectroscopy measurements. The photocatalytic performance of the CdIn2S4 photocatalyst was evaluated using photocatalytic synthesis of Schiff base compounds in a coupled system of aromatic alcohols and nitrobenzene under visible light irradiation. The yield of N-benzylideneaniline reached up to 32% in the coupled system of benzyl alcohol and nitrobenzene under visible light illumination for 8 h. Furthermore, the changes for the amounts of aromatic aldehydes and AL as intermediate products during the photocatalytic process were also investigated. Using isotopic tracing, a possible reaction mechanism for the photocatalytic synthesis of N-benzylideneaniline and the redox reactions in the coupled system of benzyl alcohol and nitrobenzene was proposed. It is hoped that this strategy can provide an effective pathway for the traditional organic synthesis and transformation using photocatalytic technology under mild conditions. [ABSTRACT FROM AUTHOR]

Competing Interests: Conflict of interest The authors declare that they have no conflict of interest.

Ammonia nitrogen (NH 4 + -N) is a ubiquitous environmental pollutant, especially in offshore aquaculture systems. Electrochemical oxidation is very promising to remove NH 4 + -N, but suffers from the use of precious metals anodes. In this work, a robust and cheap electrocatalyst, iron single-atoms distributed in nitrogen-doped carbon (Fe-SAs/N-C), was developed for electrochemical removal of NH 4 + -N from in wastewater containing chloride. The Fe-SAs/N-C catalyst exhibited superior activity than that of iron nanoparticles loaded carbon (Fe-NPs/N-C), unmodified carbon and conventional Ti/IrO 2 -TiO 2 -RuO 2 electrodes. And high removal efficiency (> 99%) could be achieved as well as high N 2 selectivity (99.5%) at low current density. Further experiments and density functional theory (DFT) calculations demonstrated the indispensable role of single-atom iron in the promoted generation of chloride derived species for efficient removal of NH 4 + -N. This study provides promising inexpensive catalysts for NH 4 + -N removal in aquaculture wastewater., (Copyright © 2022. Published by Elsevier B.V.)

Removal of non-biodegradable heavy metals has been the top priority in wastewater treatment and the development of green technologies remains a significant challenge. We demonstrate that phosphorylated nanoscale zero-valent iron (nZVI) is promising for removal of heavy metals (Ni II , Cu II , Cr VI , Hg II ) via a boosted Kirkendall effect. Phosphorylation confines tensile hoop stress on the nZVI particles and "breaks" the structurally dense spherical nZVI to produce numerous radial nanocracks. Exemplified by Ni II removal, the radial nanocracks favor the facile inward diffusion of Ni II and the rapid outward transport of electrons and ferrous ions through the oxide shell for surface (Ni II /electron) and boundary (Ni II /Fe 0 ) galvanic exchange. Accompanied by a pronounced hollowing phenomenon, phosphorylated nZVI can instantly reduce and immobilize Ni II throughout the oxide shell with a high capacity (258 mg Ni g -1  Fe). For real electroplating factory wastewater treatment, this novel nZVI performs simultaneous Ni II and Cu II removal, producing effluent of stable quality that meets local discharge regulations., (© 2021 Wiley-VCH GmbH.)

The use of solar energy to drive organic reactions under mild conditions provides a sustainable pathway for green synthesis and has been one of the primary goals pursued by scientists. In this research, the cadmium indium sulfide (CdIn2S4) photocatalyst was prepared using a simple solvothermal method and was thoroughly characterized using X-ray powder diffraction, UV-visible absorption spectra, nitrogen adsorption-desorption isotherms, scanning electron microscopy, transmission electron microscopy and X-ray spectroscopy measurements. The photocatalytic performance of the CdIn2S4 photocatalyst was evaluated using photocatalytic synthesis of Schiff base compounds in a coupled system of aromatic alcohols and nitrobenzene under visible light irradiation. The yield of N-benzylideneaniline reached up to 32% in the coupled system of benzyl alcohol and nitrobenzene under visible light illumination for 8 h. Furthermore, the changes for the amounts of aromatic aldehydes and AL as intermediate products during the photocatalytic process were also investigated. Using isotopic tracing, a possible reaction mechanism for the photocatalytic synthesis of N-benzylideneaniline and the redox reactions in the coupled system of benzyl alcohol and nitrobenzene was proposed. It is hoped that this strategy can provide an effective pathway for the traditional organic synthesis and transformation using photocatalytic technology under mild conditions.

Ternary chalcogenide semiconductor, cadmium indium sulfide (CdIn 2 S 4 ), was prepared by a simple solvothermal method using ethylene glycol as a solvent, as well as indium chloride tetrahydrate (InCl 3 . 4H 2 O), cadmium nitrate tetrahydrate [Cd(NO 3 ) 2 . 4H 2 O], and thiacetamide (TAA) as precursors. The resulted sample was subject to a series of characterizations. It is the first time to use CdIn 2 S 4 sample as a visible light-driven photocatalyst for simultaneous selective redox transformation of organic aromatic compounds. The results indicate that the as-synthesized CdIn 2 S 4 photocatalyst not only has excellent photocatalytic performance compared with pure In 2 S 3 and CdS for the selective oxidation of aromatic alcohols in an oxygen environment, but also shows high photocatalytic redox activities under nitrogen atmosphere. A possible mechanism for the photocatalytic redox reaction in the coupled system was proposed. It is hoped that our current work could extend the applications of CdIn 2 S 4 photocatalyst and provide new insights for selective transformations of organic compounds.