Spin-controlled CO2-to-CO conversion using aqueous-stable chiral CsPbBr3 quantum dot/nitrogen-doped reduced graphene oxide heterostructures

초록

Solar-driven CO2 reduction using halide perovskite quantum dots (QDs) is hindered by inefficient charge extraction and poor stability in aqueous environments. Here, we present dual-ligand-engineered CsPbBr3 QDs, where 4-bromobutyric acid (BBA) enhances aqueous stability and chiral (S)-(-)-2-bromopropionic acid (S-BPA) induces chirality for chirality-induced spin selectivity (CISS). Integrating these chiral, water-stable QDs with Ndoped reduced graphene oxide forms a spin-controlled heterostructure exhibiting an apparent spin polarization of 81.80% derived from the magnetization-dependent current asymmetry, a CO production rate of 120.74 mu mol g- 1 h- 1, and improved CO selectivity under solar-driven CO2 reduction. Operando ATR-FTIR analysis indicates accelerated *COOH-to-*CO conversion and rapid *CO desorption, while electrochemical impedance spectroscopy reveals significantly reduced interfacial charge-transfer resistance, attributed to spin-selective charge transport. Strong ligand coordination also suppresses aqueous degradation of CsPbBr3 QDs, extending operational stability to 144 h. Collectively, these findings establish dual-ligand engineering as an effective strategy for enabling spincontrolled CO2-to-CO conversion using chiral perovskite QDs in aqueous media.

키워드