Nature is capable of storing solar energy in chemical bonds via photosynthesis through a series of C–C, C–O and C–N bond-forming reactions starting from CO 2 and light. Direct capture of solar energy for organic synthesis is a promising approach. Lead (Pb)-halide perovskite solar cells reach 24.2% power conversion efficiency, rendering perovskite a unique type material for solar energy capture. We argue that photophysical properties of perovskites already proved for photovoltaics, also should be of interest in photoredox organic synthesis. Because the key aspects of these two applications are both relying on charge separation and transfer. Here we demonstrated that perovskites nanocrystals are exceptional candidates as photocatalysts for fundamental organic reactions, for example C–C, C–N and C–O bond-formations. Stability of CsPbBr 3 in organic solvents and ease-of-tuning their bandedges garner perovskite a wider scope of organic substrate activations. Our low-cost, easy-to-process, highly-efficient, air-tolerant and bandedge-tunable perovskites may bring new breakthrough in organic chemistry.
Cost-effective and efficient photocatalysis are highly desirable in chemical synthesis. Here we demonstrate that readily prepared suspensions of APbBr 3 (A = Cs or methylammonium (MA)) type perovskite colloids (ca. 2−100 nm) can selectively photocatalyze carbon−carbon bond formation reactions, i.e., α-alkylations. Specifically, we demonstrate α-alkylation of aldehydes with a turnover number (TON) of over 52,000 under visible light illumination. Hybrid organic/ inorganic perovskites are revolutionizing photovoltaic research and are now impacting other research fields, but their exploration in organic synthesis is rare. Our lowcost, easy-to-process, highly efficient and bandedgetunable perovskite photocatalyst is expected to bring new insights in chemical synthesis.
With the rapid development of data‐driven human interaction, advanced data‐storage technologies with lower power consumption, larger storage capacity, faster switching speed, and higher integration density have become the goals of future memory electronics. Nevertheless, the physical limitations of conventional Si‐based binary storage systems lag far behind the ultrahigh‐density requirements of post‐Moore information storage. In this regard, the pursuit of alternatives and/or supplements to the existing storage technology has come to the forefront. Recently, organic‐based resistive memory materials have emerged as promising candidates for next‐generation information storage applications, which provide new possibilities of realizing high‐performance organic electronics. Herein, the memory device structure, switching types, mechanisms, and recent advances in organic resistive memory materials are reviewed. In particular, their potential of fulfilling multilevel storage is summarized. Besides, the present challenges and future prospects confronted by organic resistive memory materials and devices are discussed.
Solar driven carbon–carbon (C–C) bond formation is a new direction in solar energy utilization. Earth abundant nanocrystal based photocatalysts are highly sought after as they can potentially eliminate expensive noble metal catalysts. A detailed understanding of the underlying reaction mechanisms could provide guidance in designing new systems that can activate a larger class of small molecules. Here, we employ transient absorption spectroscopy to study a model C–C bond formation reaction, i.e., α-alkylation of aldehydes catalyzed by colloidal CsPbBr3 nanocrystals (NCs). We find that both electrons and holes undergo ultrafast charge transfer (∼50 ps) from photoexcited perovskite NCs to reactant molecules. A charge separated state lives for more than 0.8 μs, enabling a radical mechanism to form the C–C bonds. We discuss the differences between the NCs photoredox catalysts and the molecular catalyst.
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