Liu Yuhan, Yao Yuting, Zhang Xinyue, Blackman Christopher, Perry Robin S, Palgrave Robert G
Department of Chemistry, University College London, Christopher Ingold Building, 20 Gordon Street, London WC1H 0AJ, U.K.
London Centre for Nanotechnology and Department of Physics and Astronomy, University College London, 17-19 Gordon Street, London WC1H 0AH, U.K.
ACS Appl Mater Interfaces. 2023 Aug 2;15(30):37069-37076. doi: 10.1021/acsami.3c07425. Epub 2023 Jul 24.
Halide perovskites are promising photoelectrocatalytic materials. Their further development requires understanding of surface processes during electrochemistry. Thin films of tellurium-based vacancy-ordered perovskites with formula ATeI, A = Cs, methylammonium (MA), were deposited onto transparent conducting substrates using aerosol-assisted chemical vapor deposition. Thin film stability as electrodes and photoelectrodes was tested in dichloromethane containing tetrabutylammonium PF (TBAPF). Using photoemission spectroscopy, we show that the formation of a solid electrolyte interphase on the surface of the CsTeI, consisting of CsPF, enhances the stability of the electrode and allows extended chopped-light chronoamperometry measurements at up to 1.1 V with a photocurrent density of 16 μA/cm. In contrast, (CHNH)TeI does not form a passivating layer and rapidly degrades upon identical electrochemical treatment. This demonstrates the importance of surface chemistry in halide perovskite electrochemistry and photoelectrocatalysis.
卤化物钙钛矿是很有前景的光电催化材料。它们的进一步发展需要了解电化学过程中的表面过程。使用气溶胶辅助化学气相沉积法将化学式为ATeI(A = Cs、甲铵(MA))的碲基空位有序钙钛矿薄膜沉积到透明导电基板上。在含有四丁基铵PF(TBAPF)的二氯甲烷中测试了薄膜作为电极和光电极的稳定性。通过光发射光谱,我们表明在CsTeI表面形成由CsPF组成的固体电解质界面,提高了电极的稳定性,并允许在高达1.1 V的电压下进行长达16 μA/cm光电流密度的扩展斩光计时电流法测量。相比之下,(CHNH)TeI不会形成钝化层,并且在相同的电化学处理下会迅速降解。这证明了表面化学在卤化物钙钛矿电化学和光电催化中的重要性。