Design of highly selective and stable CsPbI3 perovskite catalyst for photocatalytic reduction of CO2 to C1 products

Finding efficient photocatalytic carbon dioxide reduction catalysts is one of the core issues in addressing global climate change. Herein, the pristine CsPbI₃ perovskite and doped CsPbI₃ perovskite were evaluated in carbon dioxide reduction reaction (CO₂RR) to C₁ products by using density functional theory. Free energy testing and electronic structure analysis methods have shown that doped CsPbI₃ exhibits more effective catalytic performance, higher selectivity, and stability than undoped CsPbI₃. Additionally, it is discovered that CsPbI₃ (100) and (110) crystal surfaces have varied product selectivity. The photo-catalytic effectiveness is increased by the narrower band gap of Bi and Sn doped CsPbI₃, which broadens the absorption spectrum of visible light and makes electron transport easier. The calculation results indicate that Bi doped CsPbI₃ (100) and CsPbI₃ (110) crystal faces exhibit good selectivity towards CH₄, with free energy barriers as low as 0.55 eV and 0.58 eV, respectively. Sn doped CsPbI₃ (100) and CsPbI₃ (110) crystal planes exhibit good selectivity for HCOOH and CH₃OH, respectively. The results indicate that the Bi and Sn doped CsPbI₃ perovskite catalyst can further improve the CO₂ photocatalytic activity and high selectivity for C₁ products, making it a suitable substrate material for high-performance CO₂RR.