Plastic valorization presents a significantly untapped opportunity to address environmental issues while creating the necessary economic push for a circular carbon economy. Compared with the conventional routes for processing plastics (e.g., pyrolysis and gasification), a photoreforming strategy, namely, photocatalytic plastic oxidation paired with water splitting, aims to achieve plastic valorization into commodity chemicals under mild conditions while offering hydrogen fuels. Here, we implement MoS2-tipped CdS nanorod photocatalysts in an aqueous medium to reform pretreated plastics that range from polyesters (e.g., polylactic acid (PLA) and polyethylene terephthalate (PET)) to polyolefins (e.g., polyethylene (PE)). The architecture of MoS2/CdS takes advantage of the anisotropic morphology and rapid charge transfer features of nanorods, by collecting the electrons at the MoS2 tip for hydrogen evolution and utilizing the entire sidewall of CdS nanorods with rich holes toward plastic oxidation. It is shown that continuous H2 can be evolved from photoreforming of PLA, PET (commercial PET granules and real-world PET bottles), and PE, while these plastic substrates are accordingly converted into a series of valuable chemicals. This work provides an effective way to harness solar energy to realize the transformation of trash (plastics) to treasure (gaseous/liquid chemicals).

Electrochemical valorization of polyethylene terephthalate (PET) waste streams into commodity chemicals offers a potentially sustainable route for creating a circular plastic economy. However, PET wastes upcycling into valuable C2 product remains a huge challenge by the lack of an electrocatalyst that can steer the oxidation economically and selectively. Here, it is reported a catalyst comprising Pt nanoparticles hybridized with γ‐NiOOH nanosheets supported on Ni foam (Pt/γ‐NiOOH/NF) that favors electrochemical transformation of real‐word PET hydrolysate into glycolate with high Faradaic efficiency (> 90%) and selectivity (> 90%) across wide reactant (ethylene glycol, EG) concentration ranges under a marginal applied voltage of 0.55 V, which can be paired with cathodic hydrogen production. Computational studies combined with experimental characterizations elucidate that the Pt/γ‐NiOOH interface with substantial charge accumulation gives rise to an optimized adsorption energy of EG and a decreased energy barrier of potential determining step. A techno‐economic analysis demonstrates that, with the nearly same amount of resource investment, the electroreforming strategy towards glycolate production can raise revenue by up to 2.2 times relative to conventional chemical process. This work may thus serve as a framework for PET wastes valorization process with net‐zero carbon footprint and high economic viability.

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.

Photoreforming (PR) is a process that splits water into hydrogen coupled with oxidation of solid waste into value-added products, which provides a way to mitigate resource depletion of solid waste and accumulation of CO 2 in the atmosphere. The realization of solid waste PR by harnessing the redox capabilities of photocatalyst is crucial to address the environmental pollution issue and reduce our reliance on fossil fuels. In this review, we overview the continuous progress from the latest studies in constructing the PR system for upgrading of solid waste. We classify the different kinds of solid wastes and illustrate the PR mechanism. Furthermore, we discuss the advantages for cooperatively coupling of hydrogen production with solid waste valorization. We also highlight some state-of-the-art photocatalysts for valorization of biomass, plastics, and food wastes. Finally, we focus on the development of high-performance catalysts needed in the PR domain to tackle the future challenges.

Spinel Co3O4 has emerged as a promising electrocatalyst towards alkaline water oxidation, but its activity is restricted by the undesirable electronic configuration of octahedral Co3+ site. Herein, we simultaneously manipulate...