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Fluorine atoms doping was reported in experiment to reduce the band gap, improve the oxidation potential of hole, and polarize the electron distribution of polymeric carbon nitride (PCN). However, the relationships between different types of F doping and the roles of F doping in electronic and optical properties remain elusive. In this work, we investigate several F doping types in PCN and analyze their different roles in electronic and optical properties with the first-principles calculations. The results show that two stable and cooperative F doping types are found, one is to form the C (sp

A four-stage oscillating feedback millireactor with splitters (S-OFM) was designed to improve the mixing performance based on chaotic advection. Three-dimensional CFD simulations were used to investigate its flow characteristics and mixing performance, and the generation mechanisms of secondary flows were examined. The results show that the mixing index (MI

A simple, mild, green, and efficient method for the synthesis of 2-aminobenzamides is highly desirable. Herein, we report the development of an efficient, one-pot strategy starting from 2-aminobenzaldehydes and amines with acetic acid in ethyl acetate/acetone using irradiation with UV light for the synthesis of 2-aminobenzamides in high yields; 32 examples proceeded successfully by this photo-induced protocol in up to 92% yield. The reaction was also readily achieved on a gram scale. The utility of the 2-aminobenzamide building block in organic synthesis was shown by their use in the preparation of quinazolinone derivatives. The method was applied to amino acid derivatives as the amine component, which smoothly gave N-(2-aminobenzoyl)acetate derivatives at room temperature. Finally, a plausible mechanism is proposed.

The first trivalent and pentavalent tricarbabismatranes bearing the N(CH2C6H4−)3 ligand were synthesized.

We have developed a transition-metal free protocol for efficient cross-dehydrogenative coupling of 3-aryl benzofuran-2(3H)-ones and toluenes/phenols using DTBP as an oxidant.

Selective condensation/bicycloaromatization of two different arylalkynes is firstly developed under ligand-free copper(i)-catalysis, which allows the direct synthesis of C–N axial biaryl compounds in high yields with excellent selectivity and functional group tolerance. Due to the critical effects of Cu(i) catalyst and HFIP, many easily occurring undesired reactions are suppressed, and the coupled five–six aromatic rings are constructed via the selective formation of two C(sp2)–N(sp2) bonds and four C(sp2)–C(sp2) bonds. The achievement of moderate enantioselectivity verifies its potential for the simplest asymmetric synthesis of atropoisomeric biaryls. Western blotting demonstrated that the newly developed compounds are promising targets in biology and pharmaceuticals. This unique reaction can construct structurally diverse C–N axial biaryl compounds that have never been reported by other methods, and might be extended to various applications in materials, chemistry, biology, and pharmaceuticals., Selective condensation/bicycloaromatization of two different arylalkynes is firstly developed under ligand-free copper(i)-catalysis, which allows the direct synthesis of C–N axial biaryl compounds in high yields with excellent selectivity and functional group tolerance.

Phosphanylnaphtho[2,1-d]oxazoles, a P,N-chelating ligand, were synthesized through one-pot phosphonation/Cu-catalyzed oxidative condensation, followed by methylation and reduction.

Edge and bridge units embedded in carbon nitride frameworks have been well-designed via a facile polymerization method to boost exciton dissociation and charge separation.

The photocatalytic oxidation of toluene (TL) to benzaldehyde (BAD) has the advantages of mild reaction conditions, green chemistry, and high selectivity of the target products.

A simple and efficient methodology for the synthesis of large sterically hindered triarylamines in a single step was developed. A direct N,N-diarylation of 8-aminoquinoline with sterically hindered...

Herein, with air-stable chalcogenated stibines (

We have developed a protocol for efficient synthesis of indolin-2-ones from benzofuranones and aryl amines using iodine as a mediator. A diverse range of benzofuranones and aryl amines undergo cros...

Simultaneous photocatalytic reactions of H2 evolution and real wastewater degradation have drawn much attention to practical energy and environmental applications. While these applications of photocatalyst often suffer from the high charge-carrier recombination and poor efficiency in reactants activation, resulting in unsatisfactory photocatalytic activity or need expensive platinum co-catalyst. Here, the unsaturated iron ion based coordination polymer (FeTMT) with weak Fe-N sites has been fabricated by a facile wet-chemical method. It exhibits outstanding photocatalytic performance for the simultaneous production of H2 (1272 μmol g-1 h-1) and degradation of real wastewater from brewing liquor (degradation efficiency is 60%) without using any cocatalyst, which is larger than that reported system. The density functional theory (DFT) calculations revealed that the unsaturated Fe-N bridge could transfer the electrons from C3N3S3 rings to Fe3+, boosting the separation and transportation efficiency of charge carriers. On the other hand, the N functional group close to the metal centers in FeTMT could regarded as a proton relay to enhance the surface of hydrophily. Further in-situ test demonstrated that unsaturated Fe sites could adsorb H+ to form H-Fe-H bond, while Fe-N sites serve as the catalytic active centers in FeTMT. This finding opens an avenue to construct a novel coordination polymer and deep understanding for the practical industrial photocatalysis application

A new tripodal C-anionic ligand, 2-{bis(benzothiazolyl)(methoxy)methyl}phenyl (L), was stably generated by the reaction of the ligand precursor (L'), the corresponding bromide (2-BrC6H4)(MeO)C(C7H4NS)2 (C7H4NS = 2-benzothiazolyl), with nBuLi at -104 °C in the presence of TMEDA (N,N,N',N'-tetramethylethylenediamine). The ligand lithium salt reacted with BiCl3 to give a 2 : 1 complex L2BiCl. A 1 : 1 complex LBiCl2 was obtained in good yield by the redistribution reaction between L2BiCl and BiCl3. X-ray diffraction analysis revealed that the ligand L coordinated in an expected κ3-C,N,N' coordination mode in LBiCl2, while it coordinated in κ3-C,N,O and κ2-C,O coordination modes in L2BiCl. The ligand precursor reacted with BiX3 (X = Cl, Br) to give 1 : 1 complexes L'BiX3 and was found to act as a neutral tripodal C(π),N,N-ligand.

Rational tailoring of the atomic structure of photocatalysts with multiple functions to enhance the carrier transfer efficiency and surface activation of carbon nitride (C3N4) is promising and a challenge. Here, we make the first report of a facile strategy to construct amphiphilic carbon and C–O–C chain linked terminal melem units in functional carbon nitride (COCN) via copolymerizing formaldehyde with melem. By integrating the amphiphilic carrier bridge of carbon and C–O–C chains into the framework, the photogenerated carrier mobility and activated species (superoxide radicals, singlet oxygen) as well as surface interaction are significantly improved. Consequently, the optimal tailoring of C3N4 attains superior photocatalytic activity for hydrogen production (34.9 μmol h−1) and selective oxidation of sulfide to sulfoxide using air (nearly 100% conversion and selectivity after 3 h of illumination), which is about 7 times higher than that of pristine C3N4. This study provides deep insight into and strategies for the atomic tailoring of carrier transfer and surface reaction over organic-based photocatalysts.

The introduction of oxygen vacancies (Ov) has been regarded as an effective method to enhance the catalytic performance of photoanodes in oxygen evolution reaction (OER). However, their stability under highly oxidizing environment is questionable but was rarely studied. Herein, NiFe-metal-organic framework (NiFe-MOFs) was conformally coated on oxygen-vacancy-rich BiVO4 (Ov-BiVO4 ) as the protective layer and cocatalyst, forming a core-shell structure with caffeic acid as bridging agent. The as-synthesized Ov-BiVO4 @NiFe-MOFs exhibits enhanced stability and a remarkable photocurrent density of 5.3±0.15 mA cm-2 at 1.23 V (vs. RHE). The reduced coordination number of Ni(Fe)-O and elevated valence state of Ni(Fe) in NiFe-MOFs layer greatly bolster OER, and the shifting of oxygen evolution sites from Ov-BiVO4 to NiFe-MOFs promotes Ov stabilization. Ovs can be effectively preserved by the coating of a thin NiFe-MOFs layer, leading to a photoanode of enhanced photocurrent and stability.

We disclose a novel method for the synthesis of fluorescent N,N'-chelate organoboron compounds in high efficiency by treatment of aminoquinolates with NaBAr4/R'COOH in the presence of an iodine cat...

In this work, a functionalized metal-organic layer (MTTB MOL) was first synthesized and characterized, where MTTB means that it was synthesized from TTB (4,4’,4”-s-triazine-2,4,6-triyl-tribenzoate)...

Dimethyl sulfoxide (DMSO), as extremely important aprotic polar solvent and reaction medium, has attracted widespread attention from chemists in recent years due to its wide range of uses and the multiple functions it displays in various chemical processes. Especially in the past decade, dimethyl sulfoxide has become increasingly favored as a synthon in organic chemistry, resulting in great progress in this research field. In this context, this review provides a comprehensive summary of the literature on the recent progress in organic synthesis using dimethyl sulfoxide as a synthon, covering all the reports from 1 January 2016 to 11 May 2022. This type of reaction is mainly performed by transferring one or more units of dimethyl sulfoxide, such as oxygen (-O-, =O), methyl (-CH

Bismuth oxyhalide (BiOX)-based heterostructures have attracted much attention due to their promotion effect on photocatalytic performance. Nonetheless, there is a lack of theoretical understanding on the relationship between the BiOX-induced interface and the enhancement of photocatalytic activity. In the present work, density functional theory (DFT) calculations were conducted to investigate the energy band structure, charge transfer and optic properties of layered MoS 2 /BiOX (X = Cl, Br, I) van der Waals (vdW) heterojunctions. All the MoS 2 /BiOX heterojunctions have lower band gaps, smaller effective mass and better light absorption ability than BiOX monolayers. Moreover, electrons transfer from MoS 2 to BiOX, and MoS 2 /BiOX heterojunctions show typical type-II band arrangement. Importantly, MoS 2 /BiOI presents significant performance in the carrier mobility and light absorption ability among the three heterostructures, which can facilitate effective separation of photo-generated electron-hole pairs and enhance photocatalytic activity. It is disclosed that the band edges MoS 2 /BiOX are suitable for the photocatalytic decomposition of water into oxygen. It is especially so for MoS 2 /BiOI which can affect full photocatalytic water splitting. The results clarify why the combination of MoS 2 and BiOX for the generation of MoS 2 /BiOX vdW heterojunctions could result in excellent photocatalytic activity, and disclose why MoS 2 /BiOI is the best among the three for photocatalytic water splitting.

The activation of C–H bonds is an efficient approach for the production of value-added organics. The partial oxidation of hydrocarbons to oxygen-containing products at mild conditions is a profound...

Multi-component nanomaterials with intricate multishell architectures hold great potential for the development of advanced photocatalytic materials. However, most of the multishell hollow materials reported so far are single-component, and it is rare to come across multi-component ones with hybrid compositions. Herein, we demonstrate a facile in situ supramolecular self-assembly strategy to synthesize hollow, porous and double-shell octahedron of CdS@C3N4 composition. By virtue of compositional and structural advantages, the CdS@C3N4 composites exhibit outstanding activity and stability in photocatalytic H2 generation and selective oxidation of saturated C H bonds.

Metal-organic framework (MOF) is one of the most promising porous materials in photocatalysis. In this study, copper was deposited on as well as encapsulated in a semiconductor-like MOF (UiO-66) to fabricate the Cu/Cu@UiO-66 catalyst via an advanced double-solvent approach followed by one-step reduction. Even with ultralow amount of copper, Cu/Cu@UiO-66 shows significantly enhanced photocatalytic activity as well as stability for partial oxidation of aromatic alcohols under visible light irradiation. The result is attributed to the integration of plasmonic effect (Cu nanoparticles on UiO-66) and Schottky junction (Cu quantum dots encapsulated in UiO-66) which can be considered as a promising noble-metal-free way for the enhancement of visible-light-driven photocatalytic activity of MOFs.

We report the synthesis of mesoporous alumina (MA)-supported sodium tripolyphosphate (STPP)/chitosan (Ch) composite (denoted as MA@STPP/Ch) by a layer-by-layer self-assembly method. The multilayered MA@STPP/Ch is nontoxic and shows excellent CO2 adsorption capacity (maximum: 278.96 mg g−1 at 50 °C) and reusability, better than that of MA (97.24 mg g−1 at 50 °C). The enhanced CO2 adsorption could be ascribed to the synergism between porous structure and functional groups of Ch.