Tremendous progress has been achieved in renewable-energy-powered electrolysis systems for clean hydrogen production. The anodic oxygen evolution reaction (OER) still remains a major bottleneck. However, biomass oxidation reactions have shown increased interest in supplanting OER due to thermodynamically favorable biomass upgrading reactions, enabling a more cost-effective hydrogen generation route and concurrently offering opportunities for stable chemical production. Given the immense advances in material design, two-dimensional (2D)-based heterostructure materials stand out, usually with strong interfacial chemical interactions and significant electronic coupling between composites, synergistically creating unexpected properties and remarkable optimization of pre-existing functionalities. Accordingly, herein, a series of 2D heterostructures were elaborately constructed by solution-based self-assembly of transition metal dichalcogenides (TMDs) and layered double hydroxides (LDHs); subsequently, they functioned as highly efficient bifunctional catalysts for HER and 5-hydroxymethylfurfural (HMF) conversion to 2,5-furandicarboxylic acid (FDCA). Particularly, intense hydrogen production and nearly 100% HMF-upgraded Faradic efficiency were realized by the well-designed NiFe LDH@MoS2 catalyst. This presentation will focus on the exploration of the origin of the synergetic effect observed in typical bifunctional NiFe LDH@MoS2 catalysts for HER and HMF upgradation. The judicious combined employment of microscopic and X-ray techniques is highlighted to gain a comprehensive and in-depth understanding of structural and electronic structural changes at heterostructure interfaces. Specifically, ex situ X-ray techniques and transmission electron microscopy are implemented to investigate the atomic-scale structures and electronic structural characteristics of resulting catalytic materials; meanwhile, in situ (operando) X-ray techniques are adopted to track the dynamic structural evolution of catalysts and monitor the atom-to-atom or atom-to-reactant electronic interactions in real time under diverse operating conditions. This presented work is anticipated to offer new insights into the further development and application of versatile heterostructures as high-performance catalytic materials in hybrid water electrolysis systems for efficient renewable energy generation and large-scale production of fuels and industrially important chemicals.

Bifunctional heterostructures self-assembled from transition metal dichalcogenides and layered double hydroxide for highly efficient hydrogen production and 5-(hydroxymethyl)furfural upgradation

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