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In terms of facilitated photogenerated charge carrier dynamics and induced proton reduction potential, photocatalytic H2 evolution could be improved by dimensionality tuning from 3D nanocubes to 1D nanorods.

The isolation of graphene from graphite triggered enormous interest in the study of 2D materials due to their remarkable physical properties. These 2D materials feature many unique properties, such as atomically thin flakes, a layered structure, a long-range order and a dangling bond-free surface, which are promising for broad applications in various fields including (opto)electronics, spintronics, catalysis and so on. Specially, organic 2D layered materials have the prominent advantage of their designable and tailorable chemical structure at the atomic level. The preparation of organic 2D layered material thin films has become a very hot research topic in the materials fields because of their great potential to be integrated into advanced nanodevices. Considering the lack of large single crystal samples, it is not possible to obtain large-scale films from the traditional top-down exfoliation methods. Various groups and our previous studies prove the efficiency of interfacial synthesis methods for high-quality organic 2D layered material thin film preparation by restricting the reaction at the two-phase boundary area within a plane. As the performance of resultant films is highly related to their "quality" in aspects of continuity, crystallinity, uniformity, and thickness, the selection of interfaces and conditions is vitally important. Until now, many interfacial synthesis methods have been developed and modified for the controlled growth of high-quality organic 2D layered material thin films. This feature article reviews the recent advances in organic 2D layered material thin film preparation by interfacial methods. First, how the features of the interface affect the growth behavior of organic 2D layered materials is analyzed. Then, varieties of organic 2D layered material thin films with different chemical structures grown at various interfaces are discussed. Finally, the challenges and prospects in the interfacial synthesis of high-quality organic 2D layered materials are also explored.

Owing to the high synthetic value of deuteration in the pharmaceutical industry, we describe herein the conversion of a range of aromatic ketones to deuterium-labeled products in good to excellent yields. Efficient and site-selective deuteration of benzyl alcohols by D2O with visible light irradiation of quantum dots (QDs), together with gram-scale synthesis and photocatalyst recycling experiments indicated the potential of the developed method in practical organic synthesis.

The Complexity to Diversity (CtD) strategy, a strategy for the synthesis of stereochemically complex and structurally diverse small molecules from natural products using ring-distortion reactions, was applied in the synthesis of a 47-member compound collection from the natural product griseofulvin. A Tsuji-Trost allylation and oxa-Michael cyclization tandem reaction was used for the first time in the CtD strategy to generate complex ring fused compounds.

With a Ag/g-C3N4 nanometric semiconductor as the photocatalyst, 2-arylquinolines were synthesized through a photoxidation-Povarov cascade reaction of N-benzylanilines and alcohols under visible light irradiation. Under the blue light of a 3 W LED, good yields were achieved for various substrates in oxygen at room temperature. This methodology provides a green and mild alternative for the formation of 2-arylquinoline derivatives. Remarkably, the Ag/g-C3N4 nanocomposite can be conveniently recovered and reused several times with satisfying yields.

Bioinspired transformation of small-molecules to energy-related feedstocks is an attractive research area to overcome both the environmental issues and the depletion of fossil fuels. The highly effective metalloenzymes in nature provide blueprints for the utilization of bioinspired metal complexes for artificial photosynthesis. Through simpler structural and functional mimics, the representative herein is the pivotal development of several critical small molecule conversions catalyzed by metal complexes, e.g., water oxidation, proton and CO2 reduction and organic chemical transformation of small molecules. Of great achievement is the establishment of bioinspired metal complexes as catalysts with high stability, specific selectivity and satisfactory efficiency to drive the multiple-electron and multiple-proton processes related to small molecule transformation. Also, potential opportunities and challenges for future development in these appealing areas are highlighted.

Catalytic conversion of carbon dioxide (CO2) to value-added chemicals under mild conditions is highly desired, albeit with significant challenges. Here, in terms of exposure of abundant active sites and excellent photo-to-thermal conversion properties, flower-like Co2C has been firstly used for effectively catalysing the cycloaddition of CO2 with epoxides to produce cyclic carbonates with yields of up to 95% under solar light. Density functional theory (DFT) calculations reveal that Lewis acid sites of the surface Co atoms can activate both CO2 and epoxide, thus opening up the possibility of a CO2-epoxide cycloaddition reaction.

Photoelectrochemistry enables the formation of a variety of active intermediates for organic synthesis in an environmentally friendly manner. Herein, a photoelectrochemical cell is fabricated to realize activation of P-H/C-H bonds for cross-coupling hydrogen evolution. As compared with an electrochemical cell, nearly 90% external bias input is saved to drive the C-P bond construction with good to excellent yields.

A simple, mild and efficient approach to access fluorinated dibenz[b,e]azepines via visible-light photoredox catalysis is presented. Inexpensive and commercially available fluoroalkyl anhydrides in concert with pyridine N-oxide are employed as the source of the fluoroalkyl radicals. A one-pot process involving the trifluoroacetylation of unprotected secondary benzyl amines followed by radical cyclization could also afford the desired fluorinated dibenz[b,e]azepines.

We report a new molecular design for optically triggered nm-scale translation of a submolecular component relative to another. We used a rotaxane-like molecule terminated at one end with stiff stilbene that served both as a chromophore to trigger the translation of the pillar[5]arene "wheel" and as a stopper to prevent its dethreading.

To identify the short-lived, highly-active iron intermediate generated in situ for water oxidation, we describe here a new complex 1 by subtle modulation of the TPA ligand and succeed in capturing the high-valent FeIV(O) species, which is responsible for the O-O bond formation and oxygen evolution with higher efficiency.

With visible light irradiation of a catalytic amount of Ir(ppy)3 at room temperature, a number of N-aryl enamines were transformed into their corresponding indoline products in good to excellent yields without requiring any extra additives. This is the first example of the synthesis of indolines via the intramolecular cyclization of enamines under visible light irradiation.

A novel pillared-layered entangled luminescent metal–organic framework [Zn2(bpdc)2(BPyTPE)] (1) (BPyTPE = (E)-1,2-diphenyl-1,2-bis(4-(pyridin-4-yl)phenyl)ethene) has been designed and constructed. The solvent-free 1 exhibits strong blue-green emission with an excellent fluorescence quantum yield of 99% and provides a facile and reversible method to sensitively and quantitatively detect trace pesticide of 2,6-dichloro-4-nitroaniline.

Three novel bis(Triol)-functionalized Anderson cluster derivatives (POM-L-POM, POM-L, L-POM-L) were efficiently synthesized, which manifest interesting self-assembly and synergistic effects. They provided strong support in synthons, applications in syntheses and properties for designing organic-inorganic hybrid chains.

Due to their enhanced light harvesting, favored interfacial charge transfer and excellent proton reduction activity, hybrid photocatalysts of metallic 1T-MoS2 nanosheets and inorganic-ligand stabilized CdSe/ZnS QDs obtained via a self-assembly approach can produce H2 gas with a rate of ∼155 ± 3.5 μmol h−1 mg−1 under visible-light irradiation (λ = 410 nm), the most exceptional performance of solar H2 evolution using MoS2 as a cocatalyst known to date.

Ultrathin SnNb2O6 nanosheets with a thickness of ∼3 nm were synthesized via a facile hydrothermal route using ultrathin K4Nb6O17 nanosheets as the precursor. This ultrathin nanosheets with a large specific surface area of 71.1 m(2) g(-1) showed improved visible-light photocatalytic H2-production activity in lactic acid aqueous solution, which is about 4 and 14 times higher than that of 50 nm-thick SnNb2O6 nanosheets and bulk SnNb2O6 powders, respectively. The higher activity of ultrathin nanosheets was mainly attributed to their larger specific surface area and much better charge transfer efficiency.

An amphiphilic polymeric micelle is utilized as a microreactor to load a hydrophobic [FeFe]-hydrogenase mimic in water. The local concentration enhancement and strong interaction between the mimic and the photosensitizer as well as the water-mediated fast proton migration caused by the microreactor improve photocatalytic hydrogen production remarkably in water.

By combining visible light catalysis and transfer hydrogenation, we are able to convert a series of alkynes to their corresponding alkenes in high chemical yields. Then the visible light catalytic transfer hydrogenation reaction can couple photoisomerization to produce E-alkenes or Z-alkenes exclusively depending on the aryl or alkyl substituted alkynes.

A copper(i) cysteine complex generated by mixing Cu(ii) ions with cysteine in aqueous solution greatly enhanced the activity of CdSe photocatalysts for H2 production in aqueous solution under visible light excitation. The complex can enhance the H2 evolution rate by as much as 150 times, by acting as an oxidation co-catalyst and increasing charge carrier lifetimes. The copper(i) cysteine complex can also be applied to enhance the H2 production performance of other semiconductor photocatalyst systems, thereby affording a new research direction in the development of co-catalysts for solar hydrogen production.

A redox strategy was designed to generate strong basicity on mesoporous silica by using the redox interaction of a precursor with methanol vapor. The formation of strongly basic sites was realized at 400 °C, which breaks the tradition of thermally induced decomposition that usually requires much higher temperatures (>600 °C).

We report the first application of layered double hydroxide as a photocatalyst in the transformation of primary aromatic amines to their corresponding imines with high efficiency and selectivity by using oxygen in an air atmosphere as a terminal oxidant under light irradiation.