State Key Laboratory of Crystal Materials, Shandong University, Jinan, 250100, P.R. China.
School of Physics, Shandong University, Jinan, 250100, P.R. China.
Chemistry. 2023 Jul 11;29(39):e202300999. doi: 10.1002/chem.202300999. Epub 2023 May 17.
Severe poisonousness and prolonged instability existing in organic-inorganic lead-based perovskite are two matters seriously hindering its potential future application in photocatalysis. Therefore, it is particularly important to explore ecology-friendly, air-stable and highly active metal-halide perovskites. Herein, a new and stable lead-free perovskite Cs SnBr decorated with reduced graphene oxide (rGO), is synthesized and employed in the photocatalytic organic conversion. The as-prepared Cs SnBr is ultrastable, exhibiting no clear changes after being placed in the air for six months. The Cs SnBr /rGO composite shows excellent photocatalytic activity in photo-driven-oxidation of 5-hydroxymethylfurfural (HMF) to high value enclosed 2,5-diformylfuran (DFF), achieving>99.5 % conversion of HMF and 88 % DFF selectivity in the presence of green oxidant O . Comprehensive characterizations disclose a multistep reaction mechanism, demonstrating that the molecular oxygen, photogenerated carriers, ⋅O and O altogether synergistically participate in the effective photo-driven conversion of HMF to DFF. This work expands the material gallery towards selective organic conversion and environmentally friendly perovskite options for photocatalytic application.
有机-无机铅基钙钛矿中存在严重的毒性和长期不稳定性,这两点严重阻碍了其在光催化领域的潜在应用。因此,探索生态友好、稳定和高效的金属卤化物钙钛矿尤为重要。本文合成了一种新型、稳定的无铅钙钛矿 CsSnBr ,并负载还原氧化石墨烯(rGO),用于光催化有机转化。所制备的 CsSnBr 超稳定,在空气中放置六个月后没有明显变化。CsSnBr/rGO 复合材料在光驱动氧化 5-羟甲基糠醛(HMF)生成高附加值的 2,5-二醛基呋喃(DFF)中表现出优异的光催化活性,在绿色氧化剂 O 的存在下,HMF 的转化率超过 99.5%,DFF 的选择性为 88%。综合表征揭示了一个多步反应机制,表明分子氧、光生载流子、 ⋅O 和 O 共同协同参与了 HMF 到 DFF 的有效光驱动转化。这项工作扩展了光催化应用中选择性有机转化和环境友好型钙钛矿材料的选择范围。