Latest ArticlesPhotoreduction of CO2 into value-added products offers a promising approach to overcome both climate change and energy crisis. However, low conversion efficiency, poor product selectivity, and unclear mechanism limit the further advancement of CO2 photoreduction. The development of two-dimensional (2D) materials and construction of single atom sites are two frontier research fields in catalysis. Combining the advantages of 2D materials and single atom sites is expected to make a breakthrough in CO2 photoreduction. In this review, we summarized the design and application, proposed challenges and opportunities, and laid a foundation for further research and application of 2D materials confining single atoms (SACs@2D) for CO2 photoreduction.
Ammonia is one of the most essential chemicals in the modern society but its production still heavily relies on energy-consuming Haber-Bosch processes. The photocatalytic reduction of nitrogen with water for ammonia production has attracted much attention recently due to its synthesis under mild conditions at room temperature and atmospheric pressure using sunlight. Herein, we report a high-performance Au/MIL-100(Cr) photocatalyst, comprising MIL-100(Cr) and Au nanoparticles in photocatalytic nitrogen reduction to ammonia at ambient conditions under visible light irradiation. The optimized photocatalyst (i.e., 0.10Au/MIL-100(Cr)) achieved the excellent ammonia production rate with 39.9 µg gcat−1 h−1 compared with pure MIL-100(Cr) (2.73 µg gcat−1 h−1), which was nearly 15 times that on pure MIL-100(Cr). The remarkable activity could be attributed to the adsorption-plasmonic synergistic effects in which the MIL-100(Cr) and Au are responsible to the strong trapping and adsorption of N2 molecules and photo-induced plasmonic hot electrons activating and decomposing the N2 molecules, respectively. This study might provide a new strategy for designing an efficient plasmonic photocatalyst to improve the photocatalytic performance of N2 fixation under visible light irradiation.
In the design of conjugated molecules, modular production enables materials to easily realize structure modification and precisely tune their photoelectrical property. Construction of a novel and universal building block is crucial to design and manufacture high performance and stable conjugated molecules for optoelectronic application. Herein, we originally demonstrated a universal 4-qualifiable fluorene-based building block, which is a fundamental molecular segment to functionalize and obtain novel conjugated materials. Compared to the traditional modification at 9-site, additional 4-position functionalization provided an exciting blueprint to not only tune electronic structure and excited state via p-n molecular design engineering and space charge-transfer strategy, but also allow for optimizing intermolecular arrangement and obtaining solution-processing ability. The introduction of the 4-site substituent in fluorene based semiconductors may endow materials with unique properties. Finally, we successfully prepared two stable deep-blue light-emitting conjugated polymer, PODOPF and PODOF, by utilizing the 4-substituent fluorene based building block. It is believable that the performance, stability and processibility of reported outstanding fluorene-based conjugated molecules can be further optimized based on this universal building block.
By using a perylene diimine (PDI) syn-atropisomer as highly preorganized precursor, we successfully constructed a visible-light-active organic macrocycle PDI-M. The formation of macrocyclic structure effectively avoids self-aggregation of PDI cores and enhances the absorption in visible region. As a photocatalyst, PDI-M exhibits excellent activity on aerobic selective oxidation of sulfide into sulfoxide under visible light irradiation at room temperature. Mechanism studies show that both superoxide and singlet oxygen act as reactive oxygen species. This work provides a typical case toward the maximum utilization of photosensitive groups under mild conditions.
Herein, we report a borane-promoted reductive deoxygenation coupling reaction to synthesize sulfides. This reaction features excellent functional group compatibility, high efficiency, broad substrate scope, and application in late-stage functionalization of biomolecules. Preliminary mechanistic studies suggest diaryl sulfides are the intermediates of this reaction. Moreover, the real active aryl sulfide anions may be generated in situ with the aid of B2pin2 and react with alkyl tosylates through a concerted SN2 pathway.
Nanoscale low-dimensional chiral architectures are increasingly receiving scientific interest, because of their potential applications in many fields such as chiral recognition, separation and transformation. Using 6, 12-dibromochrysene (DBCh), we successfully constructed and characterized the large-area two-dimensional chiral networks on Au(111) and one-dimensional metal-liganded chiral chains on Cu(111) respectively. The reasons and processes of chiral transformation of chiral networks on Au(111) were analyzed. We used scanning tunneling spectroscopy (STS) to analyze the electronic state information of this chiral structure. This work combines scanning tunneling microscopy (STM) with non-contact atomic force microscopy (nc-AFM) techniques to achieve ultra-high-resolution characterization of chiral structures on low-dimensional surfaces, which may be applied to the bond analysis of functional nanofilms. Density functional theory (DFT) was used to simulate the adsorption behavior of the molecular and energy analysis in order to verify the experimental results.
A green and highly efficient strategy for the preparation of bridged spirocyclic compounds via visible-light-induced cyclization of 2-(2-(arylethynyl)benzylidene)malononitrile derivatives with 2,6-di(tert-butyl)-4-methylphenol (BHT) at room temperature was developed. The photoinduced radical reactions generated the corresponding products in good yields under simple and mild reaction conditions.
The concise syntheses of eight 13-methylprotoberberine (13-MePB) and eight enantioenriched 13-methyltetrahydroprotoberberine (13-MeTHPB) alkaloids have been achieved in a tactically modular fashion. This synthetic work features a one-pot metal-free Pictet-Spengler/Friedel-Crafts hydroxyalkylation/dehydration/oxidation sequence and a following highly enantioselective Ir-catalyzed hydrogenation. Given such brevity and modularity, our developed synthetic route would be greatly beneficial to the efficient syntheses of existing natural products and new fully synthetic variants of 13-MePB and 13-MeTHPB family.
Although surface-enhanced Raman spectroscopy (SERS) has been applied for gathering fingerprint information, even in single molecule analysis, the decayed Raman signals in aqueous solutions largely obstruct the on-site insight reaction process. In this study, large-scaled semiconductor films with multi-walled (TiO2/WO3/TiO2) nanopore distribution are fabricated by combining electrochemical anodization and sputtering technique, and then employed as the SERS substrates for detection of molecules at the solid/liquid interfaces. Given the remarkably improved electrochromic property of the multi-walled film, such SERS substrates were endowed with tunable oxygen vacancy (VO) density and distribution via simply applying electrochemical bias voltage, which enabled one to achieve an enhanced charge transfer efficiency and thus a remarkably increased Raman signal even in solution. The VO-rich SERS substrate is highly repeatable, thus providing a reliable platform for in-situ monitoring of the target molecules or intermediates at the solid/liquid interfaces.
The need for temporal resolution and long-term stability in super-resolution fluorescence imaging has motivated research to improve the photostability of fluorescent probes. Due to the inevitable photobleaching of fluorophores, it is difficult to obtain long-term super-resolution imaging regardless of the self-healing strategy of introducing peroxide scavengers or the strategy of fluorophore structure modification to suppress TICT formation. The buffered fluorogenic probe uses the intact probes in the buffer pool to continuously replace the photobleached ones in the target, which greatly improves the photostability and enables stable dynamic super-resolution imaging for a long time. But the buffering capacity comes at the expense of reducing the number of fluorescent probes in targets, resulting in low staining fluorescence intensity. In this paper, we selected BODIPY 493, a lipid droplet probe with high fluorescence brightness, to explore the dynamic process of lipid droplet staining of this probe in cells. We found that BODIPY 493 only needs very low laser power for lipid droplet imaging due to the high molecular accumulation in lipid droplets and the high brightness, and the spatiotemporal resolution is greatly improved. More importantly, we found that BODIPY 493 also has a certain buffering capacity, which enables BODIPY 493 to be used for super-resolution imaging of lipid droplet dynamics. This work reminds researchers to coordinate the buffering capacity and brightness of fluorogenic probes.
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