Owing to the limited availability of natural sources, the widespread demand of the flavouring, perfume and pharmaceutical industries for unsaturated alcohols is met by producing them from α,β-unsaturated aldehydes, through the selective hydrogenation of the carbon-oxygen group (in preference to the carbon-carbon group). However, developing effective catalysts for this transformation is challenging, because hydrogenation of the carbon-carbon group is thermodynamically favoured. This difficulty is particularly relevant for one major category of heterogeneous catalyst: metal nanoparticles supported on metal oxides. These systems are generally incapable of significantly enhancing the selectivity towards thermodynamically unfavoured reactions, because only the edges of nanoparticles that are in direct contact with the metal-oxide support possess selective catalytic properties; most of the exposed nanoparticle surfaces do not. This has inspired the use of metal-organic frameworks (MOFs) to encapsulate metal nanoparticles within their layers or inside their channels, to influence the activity of the entire nanoparticle surface while maintaining efficient reactant and product transport owing to the porous nature of the material. Here we show that MOFs can also serve as effective selectivity regulators for the hydrogenation of α,β-unsaturated aldehydes. Sandwiching platinum nanoparticles between an inner core and an outer shell composed of an MOF with metal nodes of Fe, Cr or both (known as MIL-101; refs 19, 20, 21) results in stable catalysts that convert a range of α,β-unsaturated aldehydes with high efficiency and with significantly enhanced selectivity towards unsaturated alcohols. Calculations reveal that preferential interaction of MOF metal sites with the carbon-oxygen rather than the carbon-carbon group renders hydrogenation of the former by the embedded platinum nanoparticles a thermodynamically favoured reaction. We anticipate that our basic design strategy will allow the development of other selective heterogeneous catalysts for important yet challenging transformations.
Remarkable progress has been made in developing high performance organic field-effect transistors (OFETs) and the mobility of OFETs has been approaching the values of polycrystalline silicon, meeting the requirements of various electronic applications from electronic papers to integrated circuits. In this review, the key points for development of high mobility OFETs are highlighted from aspects of molecular engineering, process engineering and interface engineering. The importance of other factors, such as impurities and testing conditions is also addressed. Finally, the current challenges in this field for practical applications of OFETs are further discussed.
Organic semiconductors have attracted a lot of attention since the discovery of highly doped conductive polymers, due to the potential application in field-effect transistors (OFETs), light-emitting diodes (OLEDs) and photovoltaic cells (OPVs). Single crystals of organic semiconductors are particularly intriguing because they are free of grain boundaries and have long-range periodic order as well as minimal traps and defects. Hence, organic semiconductor crystals provide a powerful tool for revealing the intrinsic properties, examining the structure-property relationships, demonstrating the important factors for high performance devices and uncovering fundamental physics in organic semiconductors. This review provides a comprehensive overview of the molecular packing, morphology and charge transport features of organic semiconductor crystals, the control of crystallization for achieving high quality crystals and the device physics in the three main applications. We hope that this comprehensive summary can give a clear picture of the state-of-art status and guide future work in this area.
Organic photoresponse materials and devices are critically important to organic optoelectronics and energy crises. The activities of photoresponse in organic materials can be summarized in three effects, photoconductive, photovoltaic and optical memory effects. Correspondingly, devices based on the three effects can be divided into (i) photoconductive devices such as photodetectors, photoreceptors, photoswitches and phototransistors, (ii) photovoltaic devices such as organic solar cells, and (iii) optical data storage devices. It is expected that this systematic analysis of photoresponse materials and devices could be a guide for the better understanding of structure-property relationships of organic materials and provide key clues for the fabrication of high performance organic optoelectronic devices, the integration of them in circuits and the application of them in renewable green energy strategies (critical review, 452 references).
The integration of high charge carrier mobility and high luminescence in an organic semiconductor is challenging. However, there is need of such materials for organic light-emitting transistors and organic electrically pumped lasers. Here we show a novel organic semiconductor, 2,6-diphenylanthracene (DPA), which exhibits not only high emission with single crystal absolute florescence quantum yield of 41.2% but also high charge carrier mobility with single crystal mobility of 34 cm2 V−1 s−1. Organic light-emitting diodes (OLEDs) based on DPA give pure blue emission with brightness up to 6,627 cd m−2 and turn-on voltage of 2.8 V. 2,6-Diphenylanthracene OLED arrays are successfully driven by DPA field-effect transistor arrays, demonstrating that DPA is a high mobility emissive organic semiconductor with potential in organic optoelectronics.
A kind of sulfonated graphene (around 3 nm thick) with high dispersion properties has been synthesized. It is demonstrated to adsorb persistent organic aromatic pollutants effectively from aqueous solutions. The adsorption capability of the prepared sulfonated graphene nanomaterials approaches ∼2.3–2.4 mmol g−1 for naphthalene and 1‐naphthol, which is one of the highest capabilities of today's nanomaterials. This highly effective adsorbent may be a promising candidate to remove aromatic chemicals from large volumes of aqueous solutions. It opens a new door for cost effective environmental pollution management with graphene in the near future.
Human eyes undertake the majority of information assimilation for learning and memory. Transduction of the color and intensity of the incident light into neural signals is the main process for visual perception. Besides light‐sensitive elements that function as rods and cones, artificial retinal systems require neuromorphic devices to transform light stimuli into post‐synaptic signals. In terms of plasticity timescale, synapses with short‐term plasticity (STP) and long‐term potentiation (LTP) represent the neural foundation for experience acquisition and memory formation. Currently, electrochemical transistors are being researched as STP–LTP devices. However, their LTP timescale is confined to a second‐to‐minute level to give unreliable non‐volatile memory. This issue limits multiple‐plasticity synapses with tunable temporal characteristics and efficient sensory‐memory systems. Herein, a ferroelectric/electrochemical modulated organic synapse is proposed, attaining three prototypes of plasticity: STP/LTP by electrochemical doping/de‐doping and ferroelectric‐LTP from dipole switching. The device supplements conventional electrochemical transistors with 10000‐second‐persistent non‐volatile plasticity and unique threshold switching properties. As a proof‐of‐concept for an artificial visual‐perception system, an ultraflexible, light‐triggered organic neuromorphic device (LOND) is constructed by this synapse. The LOND transduces incident light signals with different frequency, intensity, and wavelength into synaptic signals, both volatile and non‐volatile.
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