Functionality Driven Dimensionality Modulation for Charge Transportation in Silver Cluster Assemblies

Cluster-assembled materials (CAMS) are an emerging category of modular solids that interconnect atomic precision with functional tunability. This work highlights ligand-induced dimensionality control in Ag12 cluster-based assemblies, achieved through functionalization of the organic linker. Two distinct cluster assemblies were fabricated from the geometrically distinct Ag12 core utilizing pyrazine and 2 amino-pyrazine linkers. A three-dimensional (SSICG20) framework was achieved through the accumulation of Ag12 cluster core pyrazine as a bridging ligand, while the latter one constructs a two-dimensional (SSICG21) sheet-like structure. Both frameworks exhibit distinct architectures with modulating charge transfer capability, particularly evidenced through their applicability in the charge transport measurements via linear device preparation and electro catalytic urea oxidation reaction. In investigations of the I-V measurements, both SSICG20 and SSICG21 demonstrated stable ON/OFF ratios throughout 1000 cycles, followed by SSICG20 showing superior memory response. Aligned with its superior switching response, SSICG20 showed promising catalytic efficiency in the electro catalytic urea oxidation reaction in harsh alkaline seawater conditions, with a significantly reduced onset potential of 110 mV at a current density of 10 mA, surpassing its 2D counterpart. A sustainable solar-driven overall water electrolysis experiment was also employed, which showed quite an optimistic efficiency. Collectively, this work provides a fundamental insight into the interplay of charge transportation on silver cluster assembly via dimensionality Modulation.