Latest ArticlesThis work demonstrates a two-step method to produce oxide-derived Cu nanowires on Cu mesh surface to offer a monolithic catalyst that outstandingly improves the hydrogen production from reforming formaldehyde and water under ambient conditions. Our results not only reveal that the special oxide-derived nanostructure can significantly improve the formaldehyde reforming performance of Cu, but also display that the hydrogen production has a linear relationship with oxygen pressure. Specially, a maximum of 36 times increment in hydrogen generation rate is observed than that without oxygen during the reaction. Density functional theory calculations show that the formaldehyde molecule is adsorbed on Cu surface only when the adsorbed oxygen is in adjacency, and hydrogen release process is the rate-determining step. This work highlights that the activity of deliberately synthesized catalyst can further be promoted by dynamic chemical modulation of surface states during working.
Using a ditopic organic linker 4-(1H-pyrazol-4-yl)benzoic acid (H2pba), FICN-6, a metal-organic framework containing both Cu2(O2CR)4 and Cu3(OH)(pyz)3(O2CR) secondary building units (SBUs), was synthesized. FICN-6 adopts in an unusual intercatenated structure with SBUs from two distinct networks connecting to each other. Presence of Cu3 clusters makes FICN-6 a good heterogeneous catalyst for oxygen activation and aerobic oxidative C-C coupling of organic boronic acids.
Efficient cathode-catalysts with multi-functional properties are essential for Li-CO2 battery, while the construction of them with simultaneously enhanced CO2 reduction and evolution kinetics is still challenging. Here, a kind of hybrid nanosheets based on Ru nanoparticles, Fe-TAPP and grapheme oxide (GO) has been designed through a one-pot self-assembly strategy. The Ru, Fe-porphyrin and GO based hybrid nanosheets (denoted as Ru/Fe-TAPP@GO) with integrated multi-components offer characteristics of ultrathin thickness (~4 nm), high electro-redox property, uniformly dispersed morphology, and high electrical conductivity, etc. These features endow Ru/Fe-TAPP@GO with ultra-low overpotential (0.82 V) and fully reversible discharge/charge property with a high specific-capacity of 39,000 mAh/g within 2.0–4.5 V at 100 mA/g, which are much superior to Ru@GO and Fe-TAPP@GO. The achieved performance was presented as one of the best cathode-catalysts reported to date. The synergistically enhanced activity originated from the integrated hybrid nanosheets may provide a new pathway for designing efficient cathode-catalysts for Li-CO2 batteries.
Three discrete tetrahedral metallo-supramolecular cages were designed and constructed using truxene-pended base ligands. Owing to the synergistic rigidifying effect of unsymmetric cyano-substituted oligo(p-phenylene-vinylene) (u-COPV) suspended by the truxene skeleton, the resulting supramolecular cages were confirmed to exhibit significant aggregation-induced emission (AIE) accompanied by an interesting solvatochromic fluorescent behavior as well as a porous honeycomb-like state during aggregation. In particular, the anti-counterfeiting performance and emission behaviors of the cages in the solid state under external hydrostatic pressure were investigated.
Trifluoromethylation/sulfonylation of alkynes from trifluoromethyl thianthrenium triflate and sulfur dioxide under extremely mild reaction conditions provides a facile access to trifluoromethyl-substituted vinyl sulfonohydrazides in moderate to good yields. This multicomponent reaction of trifluoromethyl thianthrenium triflate, alkynes, sulfur dioxide and hydrazines proceeds efficiently under visible light irradiation in the presence of photocatalyst at room temperature with broad substrate scope and excellent functional group compatibility. This reaction is highly stereoselective, and only (E)-isomers are obtained. Additionally, these trifluoromethyl-substituted vinyl sulfonohydrazides are further evaluated for anti-bacteria activity. In vitro activities of these compounds against Staphylococcus aureus (G+) and Escherichia coli (G−) are examined.
As a monoatomic bridge, fluoride ion can transmit efficient magnetic interaction between lanthanide ions but its effect on tuning the magnetization dynamics has not been well understood. Herein, two monofluoride-bridged dinuclear dysprosium complexes [Dy2F(bbpen)2(EtOH)2]Br·EtOH (1) and [Dy2F(bbppy)2]Br·2EtOH (2) with Dy-F-Dy angles of ~178° and their diamagnetic-ion diluted analogues 1´ and 2´ were synthesized. Magnetic studies reveal that 1 and 1´ barely show any magnetization dynamics, but 2 and 2´ exhibit strong magnetization dynamics. Systematical experimental analysis combined with ab initio calculations reveals that the different magnetization dynamics between 1 and 2 mainly originate from the effect of magnetic anisotropy by terminal ligand and bridging group of the chelating ligand, and the fluoride bridge can effectively suppress the quantum tunneling of the magnetization and turn on Orbach process in 2.
The water promotion effects, where water can provide a solution-mediated reaction pathway in various heterogeneous chemical catalysis, have been presented and attracted wide attention recently, yet, the rational design of catalysts with a certain ability of enhancing water-induced reaction process is full of challenges and difficulties. Here, we show that by incorporating alkali (Na, K) cations as an electronic and/or structural promoter into Pd/rGO-ZnCr2O4 (rGO, reduced graphene oxide), the obtained Pd(Na)/rGO-ZnCr2O4 as a representative example demonstrates an outstanding benzyl alcohol oxidation activity in the Pickering emulsion system in comparison to the alkali-free counterpart. The response experiments of water injection confirm the enhanced activity, and the Na-modified catalyst can further enhance the promotion effects of water on the reaction. The effects of alkali cations for Pd nanoparticles are identified and deciphered by a series of experimental characterizations (XPS, in situ CO-DRIFTS, and CO-TPR coupled with MS), showing that there is abundant −OH on the surface of the catalyst, which is stabilized by the formation of Pd−OHx. The alkali-stabilized Pd−OHx is helpful to enhance the water-induced reaction process. According to the results of in situ Raman as well as UV-vis absorption spectra, the Na-modulated Pd(Na)/rGO-ZnCr2O4 enables the beneficial characteristics for distorting the benzyl alcohol structure and enhancing the adsorption of benzyl alcohol. Further, the mechanism for enhanced water promotion effects is rationally proposed. The strategy of alkali cations-modified catalysts can provide a new direction to effectively enhance the chemical reaction involving small molecule water.
The abnormal activation of BRD4 accelerates the progression of acute myeloid leukemia (AML), developing more precise therapeutics to intervene BRD4 promise to be an excellent opportunity to avoid current limitations of chemotherapy in clinic. Herein, a range of small-molecule PROTACs with the privileged 8-methyl-pyrrolo[1,2-a]pyrazin-1(2H)-one scaffold were rationally designed, which harbored different carbon or ethylenedioxy chains to degrade BRD4 mediated by the E3 ubiquitin ligase CRBN. Among them, the most potential B24 exhibited remarkable BRD4 degradation and excellent anti-proliferative activities in MV4-11 cells, with values of DC50 and IC50 for 0.75 nmol/L and 0.4 nmol/L, respectively, which were better than the BRD4 inhibitor (+)-JQ-1. Notably, this compound could time-dependently degrade the target protein in the BRD4-, CRBN-, and proteasome-dependent manner. Besides, B24 dramatically decreased the level of proto-oncogene c-Myc, and induced cell apoptosis by arresting the cell cycle in G0/G1 phase, down-regulating Bcl-2 and up-regulating Bax to amplify apoptotic effectors. This proof-of-concept study also highlighted the feasibility of BRD4-based PROTACs as a more powerful strategy against AML.
As the main target cells of immune regulation, macrophages play an important role in the bone regeneration process. Macrophages can be polarized into the M1 and M2 types under the stimulation of different factors. They have proinflammatory and anti-inflammatory effects, respectively, and play key roles in different stages of bone regeneration. The ratio of M1 to M2 macrophages can be regulated by immunomodulatory biomaterials to promote bone repair and regeneration. In this paper, we review the recent literature on the chemical, physical and biological properties of biomaterials and the regulation of macrophage polarization under the influence of other factors. We also cover new methods for preparing immunomodulatory biomaterials for bone regeneration. This paper will provide new design ideas for the development of biomaterials with immunological properties and will support the clinical translation of bone-related medical biomaterials.
Difluorocarbene has emerged as a valuable intermediate to synthesize fluorides. However, difluorocarbene-derived synthesis of 19F/18F-trifluoromethyl triazoles has not been explored. Herein, we reported the Cu(I)-promoted difluorocarbene-derived 19F/18F-trifluoromethylation of iodotriazoles using KF/K18F as the fluorine source. This approach rapidly generated a wide range of 5-trifluoromethyl-1, 2, 3-triazoles in good yields showing high functional group compatibility. The reaction was effective for late-stage functionalization of bioactive molecules and 18F-trifluoromethylation of iodotriazoles. This work provides a practical synthetic methodology for the development of triazole drugs and 18F-radiotracers for positron emission tomography.
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