Cross-linked ultrathin polyphosphazene-based nanosheet with promoted charge separation kinetics for efficient visible light photocatalytic CO2 reforming to CH4

Organic polymer materials as a promising type of photocatalyst are still limited by the poor transport efficiency of photoinduced carrier. Herein, a series of cross-linked ultrathin polyphosphazene-based nanosheets is developed by regulating the N-containing skeleton. The aromatic ring, pyrimidine ring and s-triazine ring are bonded with cyclotriphosphazene to form large-sized 2D nanosheets, respectively. Experimental results and theoretical calculations have determined the pyrimidine ring that has a stronger ability to adsorb CO2 and can provide a suitable band gap and a stronger built-in electric field, so as to realize the rapid separation of photoproduced carrier. 2PC sample with the pyrimidine ring delivered near 100% selectivity for CO2-to-CH4 conversion with an impressive rate of 626 mu mol g(-1 )without cocatalyst and photosensitizer under visible light illumination, surpassing many reported photocatalysts. Briefly, this work offers a fresh means for the construction of high-performance polymers by regulating the internal framework.

Automated summary

In this study, a new type of ultrathin polyphosphazene-based nanosheets photocatalyst was successfully developed by regulating the internal framework. The experimental results showed that the nanosheets exhibited excellent CO2 adsorption ability and rapid separation of photoproduced carrier, leading to efficient CO2-to-CH4 conversion. The photocatalyst demonstrated high performance in visible light illumination, surpassing many reported photocatalysts.