Bioinspired Construction of Synergistic Polyoxometalate–LDH Interface Derived Microreactor Heterojunctions as Efficient Water Splitting Electrocatalysts
Excessive fossil fuels consumption for energy needs is accelerating global warming and detrimental effects on the environment. Achieving carbon neutrality requires access to sustainable and renewable resources. H2 is regarded as future clean energy due to its high energy density and low environmental impact. Water electrolysis for H2 production has been attracting the pursuit of renewable energy technologies, but scaling up requires efficient energy conversion and storage systems for widespread adoption. Electrocatalytic water splitting is an energy-efficient method for producing green H2, offering precise control over reaction conditions and deeper insights into HER and OER mechanism.1-2 However, developing structurally stable, corrosion resistance, high conductivity, high surface area, porous and cost-effective catalysts remains challenge. To date, Platinum-based catalysts showed exceptional HER performance, but their high cost, scarcity hinder large scale use. Consequently, development of non-noble metal-based electrocatalysts with high activity under mild conditions is vital for improving HER efficiency and reducing overall cost of large-scale H2 production.3-4
Polyoxometalates (POMs), metal oxide clusters with structural diversity and strong redox properties promise in developing non-noble metal-based electrocatalysts. To address, their challenges in low surface area and solubility, numerous efforts have been used to assemble/heterogenize POMs onto various supports and their crystalline derivatives have shown improved electrocatalytic activity, but challenges remain persist in time-consuming methods, harsh conditions, low efficiency and lower intrinsic HER than Pt-based catalysts.4-5 Therefore, developing precise strategies to construct POMs and their derivatives with atomically uniform active sites via intimate interfacial interactions of conductive substrates is vital for fast e- transfer and catalytic efficiency. However, organizing matter across length scales, using host-guest compatibility and employing a suitable bottom-up protocol under mild conditions remains a challenge and is rare in this field. Creating hetero-interface between POM and LDH within confined microreactors, while maintaining their structural integrity at high current densities may offer notable advantage in improving their both inherent stability and HER performance. As a co-catalyst, LDH provide metal redox sites for improving charge transfer efficiency at the interface. Such interfaces can reduce charge carrier distance and promote efficient electrocatalytic activity. This study, proposes a bioinspired assembly strategy to construct synergistic 3D-POM@LDH heterointerfaces using thin (⁓1nm) exfoliated LDH nanosheets within a confined microreactor environment. Additionally, their corresponding crystalline derivatives (MO3 and spinel AB2O4) under calcinations will be explored to evaluate their bi-functional performance in electrocatalytic overall water splitting.