Abstract

The use of oxygen evolution co-catalysts (OECs) with hematite photoanodes has received much attention because of the potential to reduce surface charge recombination. However, the low surface charge transfer and bulk charge separation rate of hematite are not improved by decorating with OECs, and the intrinsic drawbacks of hematite still limit efficient photoelectrochemical (PEC) water splitting. Here, we successfully overcame the sluggish oxygen evolution reaction performance of hematite for water splitting by inserting zero-dimensional (0D) nanofragmented MXene (NFMX) as a hole transport material between the hematite and the OEC. The 0D NFMX was fabricated from two-dimensional (2D) MXene sheets and deposited onto the surface of a three-dimensional (3D) hematite photoanode via a centrifuge-assisted method without altering the inherent performance of the 2D MXene sheets. Among many OECs, NiFe(OH)x was selected as the OEC to improve hematite PEC performance in our system because of its efficient charge transport behavior and high stability. Because of the great synergy between NFMX and NiFe(OH)x, NiFe(OH)x/NFMX/Fe2O3 achieved a maximum photocurrent density of 3.09 mA cm-2 at 1.23 VRHE, which is 2.78-fold higher than that of α-Fe2O3 (1.11 mA cm-2). Furthermore, the poor stability of MXene in an aqueous solution for water splitting was resolved by uniformly coating it with NiFe(OH)x, after which it showed outstanding stability for 60 h at 1.23 VRHE. This study demonstrates the successful use of NFMX as a hole transport material combined with an OEC for highly efficient water splitting.

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