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Nickel oxide (NiOX) has a crucial role in enhancing the efficiency and stability of p‐i‐n inverted perovskite solar cells (PSCs), which hold great potential for commercialization. However, improving contact passivation between perovskites and NiOX is a challenge due to a hindered buried interface. In order to address this issue, self‐assembled monolayers (SAMs) are introduced as a buffer layer to prevent direct contact and non‐radiative recombination. While, the large dipole moment of SAMs increases the work function of NiOX, which is crucial for enhancing hole transport performance, given the low interfacial potential barrier for hole transfer. By a combination of the first‐principles calculations, drive‐level capacitance profiling, and transient absorption spectrum characterization, the understanding of the ion‐dipole interactions and interface passivation mechanism of potassium fluoride (KF) ultra‐thin buffer layer between SAMs and perovskites is provided. The efficiency of inverted PSCs as high as 23.25% is obtained, and the unencapsulated devices kept 90% of initial efficiency following 1400 h aging under nitrogen, which demonstrate remarkable long‐term stability as well. This novel strategy highlights the significance of SAMs dipole moment at the NiOX/perovskites interface and provides a new approach to address buried interfaces for high‐efficiency and long‐term stability in inverted PSCs. [ABSTRACT FROM AUTHOR]

Constructing heterojunction is an attractive strategy for promoting photoelectrochemical (PEC) performance in water splitting and organic pollutant degradation. Herein, a novel porous BiVO4/Boron-doped Diamond (BiVO4/BDD) heterojunction photoanode containing masses of ultra-micro electrodes was successfully fabricated with an n-type BiVO4 film coated on a p-type BDD substrate by magnetron sputtering (MS). The surface structures of BiVO4 could be adjusted by changing the duration of deposition (Td). The morphologies, phase structures, electronic structures, and chemical compositions of the photoanodes were systematically characterized and analyzed. The best PEC activity with the highest current density of 1.8 mA/cm2 at 1.23 VRHE was achieved when Td was 30 min, and the sample showed the highest degradation efficiency towards tetracycline hydrochloride degradation (TCH) as well. The enhanced PEC performance was ascribed to the excellent charge transport efficiency as well as a lower carrier recombination rate, which benefited from the formation of BiVO4/BDD ultra-micro p-n heterojunction photoelectrodes and the porous structures of BiVO4. These novel photoanodes were expected to be employed in the practical PEC applications of energy regeneration and environmental management in the future. [ABSTRACT FROM AUTHOR]