Chemically Robust, Cu-based Porous Coordination Polymer Nanosheets for Efficient Hydrogen Evolution: Experimental and...

Area of Science:

• Materials Science
• Nanotechnology
• Electrochemistry

Background:

• Porous coordination polymer (PCP) nanosheets offer numerous active sites and short diffusion paths, enabling applications in energy conversion and mass transfer.
• Challenges exist in developing chemically stable PCP nanosheets with high active site density and large lateral dimensions.

Purpose of the Study:

• To design and prepare chemically stable PCP nanosheets with dense, accessible active sites.
• To evaluate the performance of these nanosheets in electrocatalytic hydrogen evolution.
• To elucidate the mechanism and role of active sites using theoretical calculations.

Main Methods:

• A combined bottom-up and top-down integral strategy was employed for PCP nanosheet synthesis.
• Characterization of nanosheet properties including active site density, thickness, and pore size.
• Electrocatalytic hydrogen evolution measurements.
• Density functional theory (DFT) calculations for mechanistic studies.

Main Results:

• Successfully synthesized chemically stable PCP nanosheets with ultrathin nature (5 nm) and significant pores (18 Å).
• Achieved a high density of exposed Cu²⁺ active sites (2.1 × 10⁶ per μm²).
• Demonstrated remarkable performance in electrocatalytic hydrogen evolution reactions.

Conclusions:

• The developed PCP nanosheets are promising candidates for efficient electrocatalytic hydrogen evolution.
• The study provides insights into the mechanism of hydrogen evolution and the crucial role of Cu²⁺ active sites.
• The integrated synthesis strategy offers a viable route for producing advanced functional nanomaterials.