Park Juhyung, Yoon Ki-Yong, Kwak Myung-Jun, Kang Jihun, Kim Suhee, Chaule Sourav, Ha Seong-Ji, Jang Ji-Hyun
School of Energy and Chemical Engineering, Department of Energy Engineering, Graduate School of Carbon Neutrality, UNIST, Ulsan 44919, Republic of Korea.
ACS Appl Mater Interfaces. 2023 Feb 22;15(7):9341-9349. doi: 10.1021/acsami.2c20524. Epub 2023 Feb 7.
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) 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), NiFe(OH)/NFMX/FeO achieved a maximum photocurrent density of 3.09 mA cm at 1.23 V, which is 2.78-fold higher than that of α-FeO (1.11 mA cm). Furthermore, the poor stability of MXene in an aqueous solution for water splitting was resolved by uniformly coating it with NiFe(OH), after which it showed outstanding stability for 60 h at 1.23 V. This study demonstrates the successful use of NFMX as a hole transport material combined with an OEC for highly efficient water splitting.
由于具有减少表面电荷复合的潜力,析氧共催化剂(OECs)与赤铁矿光阳极的联用备受关注。然而,用OECs修饰并不能提高赤铁矿低的表面电荷转移和体电荷分离速率,赤铁矿的固有缺陷仍然限制了高效光电化学(PEC)水分解。在此,我们通过在赤铁矿和OEC之间插入零维(0D)纳米碎片化MXene(NFMX)作为空穴传输材料,成功克服了赤铁矿用于水分解时缓慢的析氧反应性能。0D NFMX由二维(2D)MXene片材制成,并通过离心辅助方法沉积在三维(3D)赤铁矿光阳极表面,而不改变2D MXene片材的固有性能。在众多OECs中,NiFe(OH)因其高效的电荷传输行为和高稳定性,被选作本体系中提高赤铁矿PEC性能的OEC。由于NFMX和NiFe(OH)之间的强大协同作用,NiFe(OH)/NFMX/FeO在1.23 V时实现了3.09 mA cm的最大光电流密度,这比α-FeO(1.11 mA cm)高2.78倍。此外,通过用NiFe(OH)均匀包覆解决了MXene在用于水分解的水溶液中的稳定性差的问题,之后它在1.23 V下表现出60小时的出色稳定性。本研究证明了NFMX作为空穴传输材料与OEC联用成功用于高效水分解。