Hierarchically Nanoporous Titanium-Based Coordination Polymers for Photocatalytic Synthesis of Benzimidazole

Authors：Li, Zhijing; Ye, Zecheng; Chen, Limin^*; Cui, Jie^*; Chen, Jinzhu^*

Source：ACS Applied Nano Materials, 2020, 3(11): 10720-10731.

DOI：10.1021/acsanm.0c01953

• carbon dioxide
• coordination polymer
• hierarchically nanoporous materials
• ionic liquids
• photocatalysis

Construction of macroporosity-added hierarchical porous coordination polymers (CPs) as nanocatalysts is of great significance for their improved catalytic performance by promoting mass transfer and molecular accessibility. We present an efficient and one-step fabrication process of hierarchically macro/mesoporous titanium-based CP materials by using CO2-derived "distillable" ionic liquids (ILs) as a "reactive" solvent through a template-free strategy. The as-synthesized sponge-like CPs, composed of titanium terephthalate units, show a macropore-size range from 120 to 470 nm with a mean mesopore size of 7.6 nm. The defect-formation mechanism is proposed for macro/mesoporous CP formation via IL-induced uniquely synergistic effects of CO2 bubble perturbation, base-etching, pore-expanding, and reconstruction in one step. The hierarchical CP-derived macro/mesoporous semiconductor integrates a high thermostability and special porosity, which make it an efficient photocatalyst for green synthesis of benzimidazole from 1,2-phenylenediamine and ethanol (or triethylamine) under visible light irradiation.

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