Tin-lead(Sn-Pb)mixed perovskites are extensively investigated in near-infrared(NIR)photodetectors(PDs)owing to their excellent photoelectric performance.However,achieving high-performance Sn-Pb mixed PDs remains chall...Tin-lead(Sn-Pb)mixed perovskites are extensively investigated in near-infrared(NIR)photodetectors(PDs)owing to their excellent photoelectric performance.However,achieving high-performance Sn-Pb mixed PDs remains challenging,primarily because of the rapid crystallization and the susceptibility of Sn^(2+) to oxidation.To ad⁃dress these issues,this study introduces the multifunctional molecules 2,3-difluorobenzenamine(DBM)to modulate the crystallization of Sn-Pb mixed perovskites and retard the oxidation of Sn^(2+),thereby significantly enhancing film quality.Compared with the pristine film,Sn-Pb mixed perovskite films modulated by DBM molecules exhibit a high⁃ly homogeneous morphology,reduced roughness and defect density.The self-powered NIR PDs fabricated with the improved films have a spectral response range from 300 nm to 1100 nm,a peak responsivity of 0.51 A·W^(-1),a spe⁃cific detectivity as high as 2.46×10^(11)Jones within the NIR region(780 nm to 1100 nm),a linear dynamic range ex⁃ceeding 152 dB,and ultrafast rise/fall time of 123/464 ns.Thanks to the outstanding performance of PDs,the fabri⁃cated 5×5 PDs array demonstrates superior imaging ability in the NIR region up to 980 nm.This work advances the development of Sn-Pb mixed perovskites for NIR detection and paves the way for their commercialization.展开更多
Carbonylation reactions,crucial for carbonyl group incorporation,struggle with the inherent complexity of achieving selective mono-or double-carbonylation on single substrates,often due to competing reaction pathways....Carbonylation reactions,crucial for carbonyl group incorporation,struggle with the inherent complexity of achieving selective mono-or double-carbonylation on single substrates,often due to competing reaction pathways.Herein,our study introduces a strategy employing palladium amides,harnessing their unique reactivity control,to direct the selective carbonylation of amines for the targeted synthesis of urea and oxamide derivatives.The palladium amide structure was elucidated using single-crystal X-ray diffraction.Controlled experiments and cyclic voltammetry studies further elucidate that the oxidation of palladium amide or its insertion into a carbonyl group diverges into distinct pathways.By employing sodium percarbonate as an eco-friendly oxidant and base,we have successfully constructed a switchable carbonylation system co-catalyzed by palladium and iodide under room temperature.The utilizing strategy in this study not only facilitates effective control over reaction selectivity but also mitigates the risk of explosions,a critical safety concern in traditional carbonylation methods.展开更多
基金Supported by National Key Research and Development Program of China(2022YFA1404201)National Natural Science Foundation of China(62205187,U23A20380,U22A2091,62222509,62127817,62075120)+3 种基金Changjiang Scholars and Innovative Research Team in University of Ministry of Education of China(IRT_17R70)Fundamental Research Program of Shanxi Province(202103021223032,202303021222031)Project Funded by China Postdoctoral Science Foundation(2022M722006)Fund for Shanxi“1331 Project”Key Subjects Construction。
文摘Tin-lead(Sn-Pb)mixed perovskites are extensively investigated in near-infrared(NIR)photodetectors(PDs)owing to their excellent photoelectric performance.However,achieving high-performance Sn-Pb mixed PDs remains challenging,primarily because of the rapid crystallization and the susceptibility of Sn^(2+) to oxidation.To ad⁃dress these issues,this study introduces the multifunctional molecules 2,3-difluorobenzenamine(DBM)to modulate the crystallization of Sn-Pb mixed perovskites and retard the oxidation of Sn^(2+),thereby significantly enhancing film quality.Compared with the pristine film,Sn-Pb mixed perovskite films modulated by DBM molecules exhibit a high⁃ly homogeneous morphology,reduced roughness and defect density.The self-powered NIR PDs fabricated with the improved films have a spectral response range from 300 nm to 1100 nm,a peak responsivity of 0.51 A·W^(-1),a spe⁃cific detectivity as high as 2.46×10^(11)Jones within the NIR region(780 nm to 1100 nm),a linear dynamic range ex⁃ceeding 152 dB,and ultrafast rise/fall time of 123/464 ns.Thanks to the outstanding performance of PDs,the fabri⁃cated 5×5 PDs array demonstrates superior imaging ability in the NIR region up to 980 nm.This work advances the development of Sn-Pb mixed perovskites for NIR detection and paves the way for their commercialization.
基金The National Key Research and Development Program of Ministry of Science and Technology(No.2022YFA1504602)Natural Science Foundation of Jiangsu Province(No.BK20211094)National Natural Science Foundation of China(No.22302214,21972152,U22B20137).
文摘Carbonylation reactions,crucial for carbonyl group incorporation,struggle with the inherent complexity of achieving selective mono-or double-carbonylation on single substrates,often due to competing reaction pathways.Herein,our study introduces a strategy employing palladium amides,harnessing their unique reactivity control,to direct the selective carbonylation of amines for the targeted synthesis of urea and oxamide derivatives.The palladium amide structure was elucidated using single-crystal X-ray diffraction.Controlled experiments and cyclic voltammetry studies further elucidate that the oxidation of palladium amide or its insertion into a carbonyl group diverges into distinct pathways.By employing sodium percarbonate as an eco-friendly oxidant and base,we have successfully constructed a switchable carbonylation system co-catalyzed by palladium and iodide under room temperature.The utilizing strategy in this study not only facilitates effective control over reaction selectivity but also mitigates the risk of explosions,a critical safety concern in traditional carbonylation methods.
