Title : High-entropy transition-metal sulfide nanoparticles deposited on ultra-thin g-C3N4 nanosheets for efficient CO2 photoreduction
Abstract:
Progression towards a sustainable and efficient CO2 photoreduction reaction (CO2-PR) is hindered by overcoming challenges such as the development of affordable and cost-effective catalysts. Among the various materials applied for CO2-PR during the last decade, almost no heed has been paid to the high- entropy materials.High-entropy transition-metal sulfides (HETMSs) feature homogeneous multi-metallic compounds as single-phase solid solutions with no less than five types of cations in a sulfide structure. Unfortunately, their synthesis process is unfavorable because thermodynamic immiscibility of metallic elements prevents the achievement of high specific surface area and efficient electronic configuration. Herein, through the sulfidation of a self-templated glycerate-assisted metal-organic structure, hierarchical nanoparticles of high-entropy transition-metal sulfide (np-HETMS) were synthesized and grown on ultra- thin g-C3N4 nanosheets(UCN). The peculiar morphology and the synergic electronic interaction of multi- metallic constituents confirmed the synthesis of an appropriate hybrid nanostructure (np-HETMS/UCN) for highly efficient CO2-PR. The crystalline investigation of synthesized np-HETMS exhibited the formation of a crystalline-amorphous system in the term of unique single-phase pyrite (CoFeNiMnCu)S2. The attained amorphous structure was much more conducive to advancement in charge transfer to and from active sites, effective orientation toward CO2 adsorption and facility of atomic disorder for unique electronic structure. In addition, the np-HETMS in the hybrid nanostructure presented superior light-harvesting encompassing the entire solar spectrum, efficacious photon utilization using charge dissociation and steering, therefore serving as active centers for substantial involvement in CO2-PR. As anticipated, the capability of np-HETMS/UCN nanocomposite in realizing competitive syngas production compared with other state-of-the-art nanomaterials demonstrated the high performance of our strategy. According to the long-lasting experiment and time-equivalent consecutive cycling runs, the architecture of the np- HETMS/UCN nanocomposite demonstrated considerable resistance to catalyst inactivation/destruction. The innovative architecture of np-HETMS was based on the requisite of efficient CO2-PR, shedding light on the applicability of high-entropy materials in photocatalysis.
Audience Take Away:
- This research broadens the audience’s perspective about general limitations in designing and developing sustainable CO2-photoreducing reactions.
- This research introduces a possible solution to improve the catalyst: high-entropy configuration.
- This research presents an unprecedently procedure for synthesizing high-entropy metal sulfide in favor of CO2-PR.
- Individuate the gaps in a research area and find solutions to overcome efficiency/sustainability challenges.
- Acquire familiarity with state-of-the-art materials synthesis strategies.
- This research maintains:
- The fundamental theory and applications of sustainable photocatalysis.
- The new generation of synthesis route for the inclusion of high-entropy materials in catalyst
- The engineering strategy can be applied to the other domains
- This research specifically focuses on the validation of an important category of materials (high-entropy materials), design of innovative hybrid structure to be appropriate and highly efficient in CO2-PR.
- The strategy behind the design of our final hybrid nanocomposites can be expanded in similar fields and assist other researchers to improve the performance of their catalysts accordingly.
