Latest ArticlesThe first example of TBAI/H2O cooperative electrocatalytic coupling-annulation of quinoxalin-2(1H)-ones with N-arylglycines was developed. A broad range of tetrahydroimidazo[1,5-a]quinoxalin-4(5H)-ones were obtained in good to excellent yields with exclusive chemoselectivities and excellent regioselectivities. The H-hydrogen bond served as a key factor for the electrocatalytic production of aminomethyl radical at lower oxidative potential.
MIL-88A(Fe)@sponge (MS) was synthesized by a dip-coating method, which displayed efficient photocatalytic Cr(Ⅵ) reduction efficiency under both low power LED UV light and real solar light irradiation. It was observed that MS (0.2 g/L) could remove 100% Cr(Ⅵ) (10 mg/L) by adding 0.4 mmol/L tartaric acid (TA) without adjusting pH (pH 5.05) within 6.0 min and 3.0 min under UV light and real solar light irradiation, respectively. Besides, the photo-induced e− and radicals (O2•− and CO2•−) were found to play the momentous roles in the MS/TA/UVL/Cr(Ⅵ) system by the scavenger experiments and electron spin resonance (ESR) tests. MS was also filled into a fixed-bed reactor to test the possibility of long-term Cr(Ⅵ) reduction operation in TA/UVL system. As expected, the results revealed that MS could still maintain 100% activity up to 60 h. These results demonstrated that MIL-88A(Fe) might be the potentially efficient catalyst for large-scale wastewater treatment in the near future.
A novel chromatography stationary phase with a quasi-graphitized carbon modified shell has been developed. Coal pitch was directly carbonized on the surface of porous silica with in-situ carbonization. The carbonized coal pitch coating exhibits some degree of graphitization with a 78 nm-thick layer on the surface of silica and a 0.5 nm-thick layer on the inner surface of the mesopores. Based on the special structure of the graphitized carbon coating, the novel stationary phase can provide multiple interactions such as hydrophobic interaction, π-π interaction and dipole-dipole interaction. The novel composite material exhibited unique separation selectivity and excellent separation efficiency for polar compounds, including imidazoles, nucleosides and pesticides. Besides, the packed column also exhibited great repeatability with the RSDs of the retention time of nucleosides between 0.07%-0.50% (n = 5). Finally, satisfied result was achieved in the separation of fullerenes on the new column, suggesting the great potential in the industrial-scale purification of fullerenes.
Hydrogen production from water electrolysis using renewable electricity is a highly promising route to solve the energy crisis of human society. The tetragonal 3d-transition metal selenide with metallic feature has been discovered to efficiently catalyze the hydrogen evolution electrocatalysis; however, its performance is still unsatisfactory and further improvement is necessary. Herein, the hydrogen evolution reaction of the functional tetragonal 3d-transition metal selenide with the heteroatom-dopant as well as cationic vacancy is fully investigated by means of density functional theory calculations. Our results identify 53 promising candidates endowed with good activity due to the absolute free energy of hydrogen adsorption |∆GH| ≤ 0.30 eV wherein 15 candidates with |∆GH| ≤ 0.09 eV possess compelling performance in comparison with the benchmark Pt material. Interestingly, the functional CuSe systems account for 29 out of 53 candidates, being high attractive for experimental synthesis. According to the analysis of electronic structure, the enhanced performance stems from the upshift of the sp orbitals, which benefits for the improved affinity toward hydrogen capture. This work provides new direction and guidance for the design of novel electrocatalysts.
Decarbonylation of aldehydes is a basic organic transformation, which has been developed for more than six-decade. However, as comparing to well-studied aromatic aldehydes, fewer examples for catalytic decarbonylation of aliphatic aldehydes were reported, mainly on simple or special substrates. For α-bulky or highly functionalized ones, stoichiometric Rh(Ⅰ) were usually required for decent yields. Herein, we present a rare example of Ir(Ⅰ)-catalyzed direct decarbonylation of α-quaternary aldehydes with broad substrate scope and good functional group compatibility via judicious selection of ligand. The α-chirality is memorized in this decarbonylation process. In addition, we report a broad-spectrum decarbonylation of α-secondary and α-tertiary aldehydes containing multifunctional groups with an improved Rh(Ⅰ)/DPPP recipe. Finally, we realized selective decarbonylation of α-tertiary aldehydes in the presence of α-quaternary one via the reactivity differences.
The binding interactions between 4-aminopyridine (4-AP) and a series of cucurbit[n]urils (Q[5], Q[6], TMeQ[6], Q[7], Q[8]) have been studied using 1H NMR spectroscopy, UV–vis absorption spectroscopy, isothermal titration calorimetry (ITC) and X-ray crystallography. The data indicates that the Q[5]@4-AP complex exhibits exo binding, which is not observed in the other four host-guest complexes. Furthermore, X-ray crystallography clearly reveals how the Q[n]s bind with 4-AP to form complexes, for example Q[5] forms an outer-surface complex, whilst Q[6], TMeQ[6] and Q[7] formed 1:1 host and guest type complexes, and Q[8] formed a stable 1:2 ternary complex due to its large cavity, which can accommodate two 4-AP molecules.
Copper is one of the most efficient catalysts widely investigated in electrochemical CO2 reduction, however, the further development of copper-based catalysts is constrained by severe stability problems. In this work, we developed a method for the synthesis of highly ordered CuAu intermetallic nanoalloys (o-CuAu) under mild conditions (< 250 ℃), which can convert carbon dioxide to carbon monoxide with high selectivity and can operate stably for 160 h without current decay. The improved stability is believed to be due to the increased mixing enthalpy and stronger atomic interactions between Cu and Au atoms in the intermetallic nanoalloy. In addition, XPS results, Tafel slope and in situ IR spectroscopy demonstrate that high valence gold atoms on o-CuAu surface promote the reduction of CO2. In contrast, the disordered CuAu nanoalloy (d-CuAu) underwent atomic rearrangement to form a Cu-rich structure on the surface, leading to reduced stability. These findings may provide insight into the rational design of stable CO2RR electrocatalysts through proper structural engineering.
In the present work, two Tröger's base-based macrocycles (TBBMs) with different bridging ethylene glycol chains (T1, n = 1; T3, n = 3) were successfully synthesized and studied via the crystal analysis. These two TBBMs possess rare rectangular-like cavities and show chiral selection during the crystallization. T1 with short glycol chain (n = 1) crystallized as racemates, while T3 with long glycol chain (n = 3) was found as meso isomer. In contrast to T1 and T3, for T2 (n = 2) both rac-T2 and meso isomer R2NS2N-T2 has been observed in our previous report. Thus, the synthesis of new TBBMs T1 and T3 with different bridging ethylene glycol chains not only makes the study of TBBMs more systematically, but also helps to understand the relationship between the size of the rectangular cavity and the chiral selection of Tröger's base-based macrocycles during their crystallization.
Researches have investigated the formation, transportation and spreading of bubble on solid surface with specific wettability. However, bubble transfer on wettability-heterogeneous surfaces has been rarely reported, which also plays significant role in water electrolysis, heat transfer, micro-bubble collection, etc. In this work, we carefully investigate the behavior of bubble transfer from the aerophobic or aerophilic region to the superaerophilic region through fabricating the wettability-heterogenous surfaces. Surface energy was elucidated to be transformed to the kinetic energy during bubble transfer process. Theoretical analysis on the average velocity of bubble transfer was consistent with the experimental results. The influence of wettability of solid substrate, bubble volume and superaerophilic stripe width on bubble transfer are carefully investigated. Moreover, wettability-heterogeneous surfaces were explored to be applied in micro-CO2 bubble collection and H2 bubble removement in water splitting.
Zinc indium sulfide (ZnIn2S4), a novel photocatalyst, has attracted considerable attention and been extensively studied over the past few years owing to its various advantages such as nontoxicity, structural stability, easy availability, suitable band gap and fascinating photocatalytic activity. This review mainly focuses on the recent state-of-art progress of ZnIn2S4-based photocatalysts. First, we briefly introduced preparation methods of ZnIn2S4 with diverse morphological structures. Then, considering the photocatalytic activity of pristine ZnIn2S4 would be confined by rapid recombination of photo-generated electron-hole pairs and limited light absorption range, different modulation strategies such as layer and size control, doping, vacancy engineering and hetero-nanostructures were expounded in detail. Afterwards, the applications of ZnIn2S4 in various fields such as H2 production, CO2 reduction, value-added products synthesis, pollutant purification and N2 fixation are clearly summarized. In the end, we sorted out the conclusions and outlook, aiming to provide some new insights for this fascinating material.
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