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The accumulation of plastic waste poses a pressing environmental challenge. Catalytic conversion stands out as an ideal approach for plastics upcycling, particularly through solar‐driven plastics photoreforming. However, due to the common effects of multiple reactive oxygen species (ROS), selectively generating high‐value chemicals becomes challenging. In this study, we developed a universal strategy to achieve >85 % selective production of diesel olefins (C15–C28) from polyolefin waste plastics via single ROS. Using tetrakis (4‐carboxyphenyl) porphyrin supramolecular (TCPP) with different central metals as an example to regulate single ROS generation, results show Ni‐TCPP facilitates triplet exciton production, yielding 1O2, while Zn‐TCPP generates ⋅O2− due to its strong built‐in electric field (IEF). 1O2 directly dechlorinates polyvinyl chloride (PVC) due to the electro‐negativity of chlorine atoms and the low dissociation energy of C−Cl bonds, while ⋅O2− promotes direct dehydrogenation of polyethylene (PE) due to the electro‐positivity of hydrogen atoms and the high dissociation energy of C−H bonds. This method is universally applicable to various single ROS systems. Installation experiments further affirm the application potential, achieving the highest diesel olefin production of 76.1 μmol h−1. Such a universally adaptive approach holds promise for addressing the global plastic pollution problem. [ABSTRACT FROM AUTHOR]

Improving peroxymonosulfate (PMS) activation efficiency to enhance simultaneous generation of radicals and non‐radicals is essential for removing new pollutants (NPs) in complex waters. However, achieving this with standard lattice‐structured heterogeneous catalysts remains challenging due to inefficient electron transfer. Here, CuCo2O4 properties are successfully tuned by controlling lattice distortion, enabling simultaneous PMS oxidation and reduction. Unlike the slow rate of electron transfer in heterogeneous metal catalysts with standard lattice structures, the highly active binary lattice distortion in CuCo2O4 alters the structure and electron distribution, exposes more Cu and Co sites, lowers the PMS adsorption barriers, and realizes the synergistic production of SO4•−/•OH), and 1O2. The k‐value for ciprofloxacin is as high as 17.83 min−1 M−1, 29.42 times higher than that with non‐binary lattice distortion. Additionally, the developed intermittent reactor consistently maintains a removal rate above 95% over five cycles in actual wastewater treatment scenarios. This work provides a new avenue for achieving the removal of new pollutants in complex water bodies. [ABSTRACT FROM AUTHOR]

Two‐electron oxygen reduction reaction (2e− ORR) is a promising method for the synthesis of hydrogen peroxide (H2O2). However, high energy barriers for the generation of key *OOH intermediates hinder the process of 2e− ORR. Herein, we prepared a copper‐supported indium selenide catalyst (Cu/In2Se3) to enhance the selectivity and yield of 2e− ORR by employing an electronic metal–support interactions (EMSIs) strategy. EMSIs‐induced charge rearrangement between metallic Cu and In2Se3 is conducive to *OOH intermediate generation, promoting H2O2 production. Theoretical investigations reveal that the inclusion of Cu significantly lowers the energy barrier of the 2e− ORR intermediate and impedes the 4e− ORR pathway, thus favoring the formation of H2O2. The concentration of H2O2 produced by Cu/In2Se3 is ~2 times than In2Se3, and Cu/In2Se3 shows promising applications in antibiotic degradation. This research presents a valuable approach for the future utilization of EMSIs in 2e− ORR. [ABSTRACT FROM AUTHOR]

By rationally adjusting the coordination environment and constructing the more electron‐enriched active site in single‐atom catalysts, the effect of heterogenous peroxymonosulfate (PMS)‐based Fenton‐like reactions can be effectively improved, yet remains a severe challenge. In this study, the electron‐rich Ru dual‐atom site is successfully immobilized onto N‐doped carbon (Ru2N6‐C) for PMS activation in water purification. The presence of electron‐rich Ru dual‐atom sites not only provides more electrons for PMS but also facilitates the formation of a Yeager adsorption configuration on the catalyst surface, which enhances O─O bond cleavage and leads to an increase in •SO4− and •OH generation. Moreover, the Ru2N6‐C catalyst exhibits exceptional durability and reliability, achieving an ultra‐high efficiency with a turnover frequency of 153.95 min−1 M−1 for the naproxen degradation. A membrane reactor is further developed for the purification of wastewater, which is expected to provide a viable approach to controlling water pollution through the design of metal dual‐atom sites carbon‐based catalysts. [ABSTRACT FROM AUTHOR]

Peroxymonosulfate (PMS) mediated radical and nonradical active substances can synergistically achieve the efficient elimination of antibiotic resistance genes (ARGs). However, enhancing interface electron cycling and optimizing the coupling of the oxygen‐containing intermediates to improve PMS activation kinetics remains a major challenge. Here, Co doped CeVO4 catalyst (Co−CVO) with asymmetric sites was constructed based on Ce 4f−O 2p−Co 3d gradient orbital coupling. The catalyst achieved approximately 2.51×105 copies/mL of extracellular ARGs (eARGs) removal within 15 minutes, exhibited ultrahigh degradation rate (k=1.24 min−1). The effective gradient 4f‐2p‐3d orbital coupling precisely regulates the electron distribution of Ce−O−Co active center microenvironment, while optimizing the electronic structure of Co 3d states (especially the occupancy of eg), promoting the adsorption of oxygen‐containing intermediates. The generated radical and nonradical generated by interfacial electron cycling enhanced by the reduction reaction of PMS at the Ce site and the oxidation reaction at the Co site achieved a significant mineralization rate of ARGs (83.4 %). The efficient removal of ARGs by a continuous flow reactor for 10 hours significantly reduces the ecological risk of ARGs in actual wastewater treatment. [ABSTRACT FROM AUTHOR]

The huge amount of plastic wastes has become a pressing global environmental problem, leading to severe environmental pollution and resource depletion through conventional downcycling technologies like incineration and landfilling. In contrast, selective upcycling of various plastics offers a promising solution for converting waste plastics into valuable products. This review provides a comprehensive overview of the recent advancements in innovative catalytic technologies, including thermocatalysis, electrocatalysis, and photocatalysis. Special emphasis is placed on elucidating the reaction mechanisms, activating designated chemical bonds for high selectivity, and elaborating the above techniques in terms of reaction conditions and products. Finally, the application prospects and future development trends in plastic catalysis are discussed, providing valuable insights for realizing a sustainable circular plastic economy. [ABSTRACT FROM AUTHOR]

Molecular oxygen (O2) activation technology is of great significance in environmental purification due to its eco‐friendly operation and cost‐effective nature. However, the activation of O2 is limited by spin‐forbidden transitions, and efficient molecular oxygen activation depends on electronic behavior and surface adsorption. Herein, we prepared cationic defect‐rich Bi4Ti3O12 (BTO‐MV2) catalysts containing Ti vacancies (VTi) for O2 activation in water purification. The VTi on BTO nanosheets can induce electron spin polarization, increasing the number of spin‐down photogenerated electrons and reducing the recombination of electron‐hole pairs. An active surface VTi is also formed, serving as a center for adsorbing O2 and extracting electrons, effectively generating ⋅OH, O2⋅− and 1O2. The degradation rate constant of tetracycline achieved by BTO‐MV2 is 3.3 times faster than BTO, indicating a satisfactory prospect for practical application. This work provides an efficient pathway to activate molecular oxygen by constructing new active sites through cationic vacancy modification technology. [ABSTRACT FROM AUTHOR]

Enhancing the peroxymonosulfate (PMS) activation efficiency to generate more radicals is vital to promote the Fenton‐like reaction activity, however, how to promote the PMS adsorption and accelerate the interfacial electron transfer to boost its activation kinetics remains a great challenge. Herein, we prepared Cu‐doped defect‐rich In2O3 (Cu‐In2O3/Ov) catalysts containing asymmetric Cu−Ov−In sites for PMS activation in water purification. The intrinsic catalytic activity is that the side‐on adsorption configuration of the O−O bond (Cu−O−O−In) at the Cu‐Ov‐In sites significantly stretches the O−O bond length. Meanwhile, the Cu‐Ov‐In sites increase the electron density near the Fermi energy level, promoting more and faster electron transfer to the O−O bond for generating more SO4⋅− and ⋅OH. The degradation rate constant of tetracycline achieved by Cu‐In2O3/Ov is 31.8 times faster than In2O3/Ov, and it shows the possibility of membrane reactor for practical wastewater treatment. [ABSTRACT FROM AUTHOR]

The implementation of carbon neutrality to achieve the goal of controlling global warming in the Paris Climate Agreement is currently the most important international climate issue. Efficient utilization of solar energy through photocatalysts is of great significance to the adjustment of energy structure. Single‐atom photocatalysts have excellent catalytic activity and selectivity in a variety of applications, including sustainable energy conversion, chemical synthesis, CO2 reduction, environmental remediation, and other areas, owing to their unique electronic structure and high atom usage. Here, we elaborated on the content and implementation direction of the carbon neutrality policy and demonstrated the design principles of single‐atom photocatalysts. Recent single‐atom synthesis strategies are summarized, and representative characterization methods have been shown to further reveal the structure–performance relationship. Then, we focus on the application of single‐atom photocatalysts in CO2 reduction, sustainable energy conversion, and environmental remediation. Finally, the opportunities and challenges in the application of single‐atom photocatalysts were discussed based on its current development. [ABSTRACT FROM AUTHOR]

Single‐atom photocatalysts have shown their fascinating strengths in enhancing charge transfer dynamics; however, rationally designing coordination sites by metal doping to stabilize isolated atoms is still challenging. Here, a one‐unit‐cell ZnIn2S4 (ZIS) nanosheet with abundant Cu dopants serving as the suitable support to achieve a single atom Pt catalyst (Pt1/Cu–ZIS) is reported, and hence the metal single atom–metal dopant interaction at an atomic level is disclosed. Experimental results and density functional theory calculations highlight the unique stabilizing effect (Pt–Cu interaction) of single Pt atoms in Cu‐doped ZIS, while apparent Pt clusters are observed in pristine ZIS. Specifically, Pt–Cu interaction provides an extra coordination site except three S sites on the surface, which induces a higher diffusion barrier and makes the single atom more stable on the surface. Apart from stabilizing Pt single atoms, Pt–Cu interaction also serves as the efficient channel to transfer electrons from Cu trap states to Pt active sites, thereby enhancing the charge separation and transfer efficiency. Remarkably, the Pt1/Cu–ZIS exhibits a superb activity, giving a photocatalytic hydrogen evolution rate of 5.02 mmol g−1 h−1, nearly 49 times higher than that of pristine ZIS. [ABSTRACT FROM AUTHOR]

The activity of heterogeneous photocatalytic H2O2 activation in Fenton‐like processes is closely related to the local electron density of reaction centre atoms. However, the recombination of electron‐hole pairs arising from random charge transfer greatly restricts the oriented electron delivery to active center. Here we show a defect engineered iron single atom photocatalyst (Fe1‐Nv/CN, single Fe atoms dispersed on carbon nitride with abundant nitrogen vacancies) for the activation of H2O2 under visible light irradiation. Based on DFT calculations and transient absorption spectroscopy results, the engineered nitrogen vacancies serve as the electron trap sites, which can directionally drive the electrons to concentrate on Fe atoms. The formation of highly concentrated electrons density at Fe sites significantly improves the H2O2 conversion efficiency. Therefore, the optimized single atom catalyst exhibiting a higher ciprofloxacin degradation activity, which was up to 18 times that of pristine CN. [ABSTRACT FROM AUTHOR]

Single‐atom CoN4 active sites have demonstrated excellent efficiency in peroxymonosulfate activation. However, the identification of CoN4 active sites and the detailed singlet oxygen generation mechanism in peroxymonosulfate activation remains ambiguous. We demonstrate a strategy to regulate the generation of reactive oxygen species by atomically dispersed cobalt anchored on nitrogen‐doped carbon. As indicated by experiment and DFT calculations, CoN2+2 was the active site and singlet oxygen was the predominant reactive oxygen species with a proportion of 98.89 %. Spontaneous dissociation of adsorbed peroxymonosulfate on the CoN2+2 active sites was energetically unfavorable because of the weakly positive Co atoms and CoN2+2 coordination, which directed PMS oxidation by a non‐radical pathway and with simultaneous singlet oxygen generation. The generated singlet oxygen degraded several organic pollutants with high efficiency across a broad pH range. [ABSTRACT FROM AUTHOR]

Defects in nanomaterials often lead to properties that are absent in their pristine counterparts. To date, most studies have focused on the effect of single defects, while ignoring the synergy of multiple defects. In this study, a model of photocatalytic O2 activation was selected to unravel the role of dual defects by decorating bismuth oxide with surface O vacancies and bulk O substitution simultaneously. The introduction of dual defects led to a spatial and electronic synergistic process: i) O substitution induced a local electric field in the bulk of BiO2−x, which promoted bulk separation of electrons and holes immediately after their generation; ii) O vacancies efficiently lowered the conduction band, served as the capture center for electrons, and thus facilitated the adsorption and activation of O2. This effect was greatly promoted by the coexistence of bulk O substitution, and DFT calculations showed that only O substitution near an O vacancy could have this effect. [ABSTRACT FROM AUTHOR]

Electrochemically functional porous membranes of low cost are appealing in various electrochemical devices used in modern environmental and energy technologies. Herein we describe a scalable strategy to construct electrochemically active, hierarchically porous carbon membranes containing atomically dispersed semi‐metallic Se, denoted SeNCM. The isolated Se atoms were stabilized by carbon atoms in the form of a hexatomic ring structure, in which the Se atoms were located at the edges of graphitic domains in SeNCM. This configuration is different from that of previously reported transition/noble metal single atom catalysts. The positively charged Se, enlarged graphitic layers, robust electrochemical nature of SeNCM endow them with excellent catalytic activity that is superior to state‐of‐the‐art commercial Pt/C catalyst. It also has long‐term operational stability for hydrazine oxidation reaction in practical hydrazine fuel cell. [ABSTRACT FROM AUTHOR]

A highly efficient Z‐scheme photocatalytic system constructed with 1D CdS and 2D CoS2 exhibited high photocatalytic hydrogen‐evolution activity of 5.54 mmol h−1 g−1 with an apparent quantum efficiency of 10.2 % at 420 nm. More importantly, its interfacial charge migration pathway was unraveled: The electrons are efficiently transferred from CdS to CoS2 through a transition atomic layer connected by Co–S5.8 coordination, thus resulting in more photogenerated carriers participating in surface reactions. Furthermore, the charge‐trapping and charge‐transfer processes were investigated by transient absorption spectroscopy, which gave an estimated charge‐separation yield of approximately 91.5 % and a charge‐separated‐state lifetime of approximately (5.2±0.5) ns in CdS/CoS2. This study elucidates the key role of interfacial atomic layers in heterojunctions and will facilitate the development of more efficient Z‐scheme photocatalytic systems. [ABSTRACT FROM AUTHOR]

The unexpected phenomenon and mechanism of the alkali metal involved NH3 selective catalysis are reported. Incorporation of K+ (4.22 wt %) in the tunnels of α‐MnO2 greatly improved its activity at low temperature (50–200 °C, 100 % conversion of NOx vs. 50.6 % conversion over pristine α‐MnO2 at 150 °C). Experiment and theory demonstrated the atomic role of incorporated K+ in α‐MnO2. Results showed that K+ in the tunnels could form a stable coordination with eight nearby Osp3 atoms. The columbic interaction between the trapped K+ and O atoms can rearrange the charge population of nearby Mn and O atoms, thus making the topmost five‐coordinated unsaturated Mn cations (Mn5c, the Lewis acid sites) more positive. Therefore, the more positively charged Mn5c can better chemically adsorb and activate the NH3 molecules compared with its pristine counterpart, which is crucial for subsequent reactions. [ABSTRACT FROM AUTHOR]

Innentitelbild: Atomically Dispersed Semimetallic Selenium on Porous Carbon Membrane as an Electrode for Hydrazine Fuel Cells (Angew. In ihrem Forschungsartikel auf S. 13600 zeigen W. Zhou, H. Wang et al., dass die Membranen als Elektroden für die Hydrazinoxidation in praxistauglichen Hydrazin-Brennstoffzellen genutzt werden können. Atomare Dispergierung, Elektrokatalyse, Hydrazinoxidation, Poröse Kohlenstoffmembranen, Selen. [Extracted from the article]

Herein, an example of Cu‐doped few‐layer ZnIn2S4 nanosheets is used to reveal the origin of optimum and excess doping for photocatalysts at atomic level. Results show that the metal‐S4 coordination maintains well with 0.5 wt% Cu substituted Zn atoms in the lattice. The introduced Cu atoms bring electronic acceptor states close to the valence band (VB) maximum and thus ensures higher charge density and efficient carrier transport, resulting in an optimum hydrogen evolution rate of 26.2 mmol h−1 g−1 and an apparent quantum efficiency of 4.76% at 420 nm. However, a distorted atomic structure and largely upshift of VB maximum with Cu‐S3.6 coordination are found with excess doping concentration (3.6 wt%). These bring the heavy charge recombination and consequentially dramatic reduced activity. This work provides a new insight into elemental doping study and takes an important step toward the development of ultrathin 2D photocatalysts. Few‐layer ZnIn2S4 nanosheets with tunable copper doping are used to disclose the origin of optimum and excess doping for photocatalysis at atomic level. Experimental and theoretical evidence reveal that optimal and excess doping is derived from the different local coordination configuration of dopants, extent of distortion, and the change of electronic structure. [ABSTRACT FROM AUTHOR]

Herein, an example of Cu‐doped few‐layer ZnIn2S4 nanosheets is used to reveal the origin of optimum and excess doping for photocatalysts at atomic level. Results show that the metal‐S4 coordination maintains well with 0.5 wt% Cu substituted Zn atoms in the lattice. The introduced Cu atoms bring electronic acceptor states close to the valence band (VB) maximum and thus ensures higher charge density and efficient carrier transport, resulting in an optimum hydrogen evolution rate of 26.2 mmol h−1 g−1 and an apparent quantum efficiency of 4.76% at 420 nm. However, a distorted atomic structure and largely upshift of VB maximum with Cu‐S3.6 coordination are found with excess doping concentration (3.6 wt%). These bring the heavy charge recombination and consequentially dramatic reduced activity. This work provides a new insight into elemental doping study and takes an important step toward the development of ultrathin 2D photocatalysts. Few‐layer ZnIn2S4 nanosheets with tunable copper doping are used to disclose the origin of optimum and excess doping for photocatalysis at atomic level. Experimental and theoretical evidence reveal that optimal and excess doping is derived from the different local coordination configuration of dopants, extent of distortion, and the change of electronic structure. [ABSTRACT FROM AUTHOR]