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Photocatalytic H2O2 generation is compelling for sustainable solar-to-chemical conversion, but it is an emerging challenge to realize efficient conversion without the consumption of any alcohols. Also, the in-depth mechanism for the structure-induced activity enhancement is still unclear but remains pivotal for practical application. Herein, cyano groups and S atoms were collectively introduced into carbon nitride (MTCN), and the vital roles and detailed mechanism were investigated. Specifically, MTCN exhibited a laudable H2O2 generation of 68.12 mM gcat−1 h−1, together with an apparent quantum yield of 49.01% at 420 nm. Intriguingly, it was observed that the existence of some contaminants can promote H2O2 generation and, in turn, accelerate degradation. Additionally, it is revealed that the S atoms and cyano group could facilitate oxygen adsorption and H+ adsorption, respectively. This study shows a promising strategy to construct modified g-C3N4 and exhibits a clear mechanism for H2O2 generation paired with simultaneous contaminant treatment. [ABSTRACT FROM AUTHOR]

The improper disposal of plastic waste raises significant concerns due to its severe threat to ecosystems and public health. Artificial photosynthesis, compared with the conventional strategies (e.g., pyrolysis) operated under harsh conditions, has emerged as a green and sustainable approach to convert plastic waste into commodity chemicals under ambient conditions. In this study, we have developed a partially oxidized CuIn5S8 nanosheet photocatalyst (O-CuIn5S8) to promote the conversion of polyethylene terephthalate (PET) waste into value-added chemicals while producing hydrogen fuel. After oxygen incorporation, the as-obtained O-CuIn5S8 catalyst demonstrates significantly improved activity, with a hydrogen evolution rate of 2.57 ± 0.02 mmol g−1 h−1, which is 7 times higher than that of the pristine CuIn5S8. Furthermore, O-CuIn5S8 allows an effective transformation of pretreated PET into a range of valuable commodity chemicals, including formate, acetate, and glycolate, via a hole-induced oxidation mechanism. This work paves the way for the rational development of photocatalysts to manage plastic pollution and meanwhile reclaim the carbon source within PET plastic waste. [ABSTRACT FROM AUTHOR]

Ruthenium (Ru), benefitting from efficient water dissociation ability, is considered a good candidate for alkaline hydrogen evolution reaction (HER); however, the strong binding of H intermediates over Ru sites leads to a limited desorption behavior and thus an unsatisfactory HER activity. Here, we propose a strategy to fabricate a well-defined hetero-interface via anchoring Ru nanoparticles on Co4N nanorods grown on nickel foam (Ru/Co4N/NF). The as-prepared Ru/Co4N/NF catalyst is demonstrated to effectively catalyze water splitting into hydrogen in an alkaline electrolyte, with an overpotential of 145 mV to reach 100 mA cm−2 and a Tafel slope of 25 mV dec−1, far surpassing bare Ru/NF and Co4N/NF. Experimental observations combined with computational simulations reveal that the charge migration from Ru to Co4N contributes to the formation of electron-deficient Ru sites and shifts the d-band center away from the Fermi level, which is conducive to hydrogen desorption. Meanwhile, the electron coupling effect between Ru and Co4N reduces the H2O adsorption energy and allows more electrons to participate in H2O molecule activation. [ABSTRACT FROM AUTHOR]

The accumulation of plastic wastes in landfills and the environment threatens our environment and public health, while leading to the loss of potential carbon resources. The urgent necessary lies in developing an energy‐saving and environmentally benign approach to upgrade plastic into value‐added chemicals. Artificial photosynthesis holds the ability to realize plastic upcycling by using endless solar energy under mild conditions, but remains in the initial stage for plastic upgrading. In this review, we aim to look critically at the photocatalytic conversion of plastic wastes from the perspective of resource reutilization. To begin with, we present the emerging conversion routes for plastic wastes and highlight the advantages of artificial photosynthesis for processing plastic wastes. By parsing photocatalytic plastic conversion process, we demonstrate the currently available routes for processing plastic, including plastic photodegradation, tandem decomposition of plastic and CO2 reduction, selective plastic oxidation, as well as photoreforming of plastic. This review concludes with a personal perspective for potential advances and emerging challenges in photocatalytic plastic conversion. [ABSTRACT FROM AUTHOR]

Fabricating heterostructures with dense interfacial catalytic sites is essential for implementation of high-performance hydrogen evolution reaction (HER). However, the strong correlation between adsorbed hydrogen atoms and electronegative nonmetal atoms gives rise to the unfavorable hydrogen desorption behavior on the heterointerface, especially on the metal sulfide heterointerface. Herein, we present a simple way to incorporate nitrogen into the NiS2/CoS2 heterostructure (N–NiS2/CoS2) to form an electron-reconfiguration heterointerface. The electronic structure of active sites on the N–NiS2/CoS2 interface can be effectively tuned by N doping, thus realizing a promoted water adsorption and dissociation capability, and near-optimal hydrogen desorption behavior on the N–NiS2/CoS2 interface. Consequently, the as-prepared N–NiS2/CoS2 heterointerface demonstrates an impressive HER performance with a low overpotential of 73 mV at a current density of 10 mA cm−2 and a small Tafel slope of 65 mV dec−1. This work sheds light on the positive effects of interfacial element dopants on the HER performance, and also provides valuable insights for rational design of a high-performance heterointerface electrocatalyst. [ABSTRACT FROM AUTHOR]