New Journal of Chemistry最新文献

The exploration of clean, environmentally friendly, efficient and economical metal electrocatalysts is becoming more and more in-depth, but catalyst activity and stability are still the main goals. Herein, a thin regular pentagonal rough nanosheet array (La-CoNiOOH@FeSe@NiSe/NF) grown on a three-dimensional porous conductive surface was designed and synthesized. The prepared electrode material exhibited good catalytic activity in 1 M KOH solution, required only 270 mV of overpotential to provide 10 mA cm⁻² current density for the oxygen evolution reaction (OER), and showed excellent stability for at least 90 hours during the OER process. The characterization test results proved that the incorporation of La changed the surface electronic structure, optimized the interface, modulated the active site on the surface of the material, and exposed a large number of active sites, thus improving the activity and stability of the catalyst material. At the same time, such a rough surface also gives the material excellent wettability and anti-bubble adhesion, which is also a key factor in maintaining the catalytic activity and OER stability of the material. This method provides a new idea for developing an efficient and economical electrolytic hydroelectricity catalyst.

The development of lead-free primary explosives is urgent from industrial and military aspects. Herein, a typical energetic molecule with the dinitromethyl group and tetrazole ring was selected as the ligand for different alkali metals (Na, K, Rb, and Cs) to achieve a series of energetic coordination polymers (ECPs), namely, ECP 1 to ECP 4. The DNMT molecule showed outstanding coordination ability with metal ions to form diverse metal complexes and coordination frameworks. It was found that the conformation of the energetic ligand as well as the framework structure can be tuned by the deprotonation of DNMT and the corresponding metal centers. Interestingly, a rare metal–π(tetrazole) coordinate bond was also observed in ECP 3, which is valuable for designing new ECPs and energetic metal complexes (EMCs). A new method has been developed for predicting the energetic properties of EMCs and ECPs. The calculation results indicate that the DNMT-based ECPs have good detonation performance and can be used as lead-free primary explosives. Moreover, the perforated lead plate test reveals the extensive application of the DNMT-based ECPs in emerging laser-initiated explosives. Compared to pure DNMT, the DNMT-based ECPs show significantly enhanced thermal stability. The mechanisms behind different detonation performances and thermal stabilities among the DNMT-based ECPs were also discussed. All the results will be valuable for the future development of ECPs in the applications of lead-free primary explosives.

Metal–organic frameworks (MOFs) have been perceived as promising electrode materials in lithium ion batteries (LIBs) due to their tunable three-dimensional porous frameworks and large surface areas. However, the coordinate bonds between metallic ions and organic ligands in MOFs are easily broken during the redox process, resulting in structural breakage and poor electrochemical performance. In this study, graphene oxide (GO) has been applied as a matrix to anchor Ni²⁺ through carboxyl groups, thereby forming Ni-MOFs in situ on the surface and effectively enhancing the structural stability of Ni-MOFs. When used as an anode in an LIB, Ni-MOFs/GO can present a specific capacity of 740.8 mA h g⁻¹ at 50 mA g⁻¹ with almost no capacity degradation after 100 cycles. This performance can be attributed to the large d–π electron conjugation, which not only contributes to rapid electron transfer but also benefits the delocalization of charge. Additionally, the GO matrix can effectively prevent the agglomeration of Ni-MOF particles, which also aids the structural stabilization of Ni-MOFs in the charge/discharge process, thus enhancing the electrochemical performance of Ni-MOFs/GO.

Janus kinase (JAK) inhibitors have been extensively used to treat hematologic cancers, but issues such as drug resistance and limited efficacy persist. Designing multi-target inhibitors with synergistic effects is an appropriate solution. Histone deacetylase (HDAC) inhibitors are also extensively employed as anticancer agents, so multi-target inhibitors based on JAK2 and HDAC6 may offer enhanced efficacy and safety. In this study, we established classification and regression models to facilitate the identification of dual JAK2 and HDAC6 inhibitors. Features were selected using mutual information (MI) algorithm, and 40 classification models were constructed using 5 feature methods and 8 Machine Learning (ML) algorithms to identify dual JAK2 and HDAC6 inhibitors. Among them, the KNN (K-nearest neighbors) model exhibited the best performance (ACC = 0.988, MCC = 0.970, AUC = 0.978). Additionally, four regression models were built using recursive feature elimination (RFE) to predict the inhibitory activity of JAK2 and HDAC6 inhibitors. Extreme gradient boosting (GBDT) and light gradient boosting machine (LGBM) models exhibited the best performance, with R²_test-JAK2 = 0.752 and R²_test-HDAC6 = 0.743, respectively. Furthermore, we utilized the SHapley Additive exPlanations (SHAP) method to elucidate the features that impact the classification and regression models. Based on this method, key fingerprint structures influencing the classification model and descriptors related to inhibitory activity were identified. Subsequently, molecular docking was employed to investigate how dual JAK2 and HDAC6 inhibitors interact with JAK2 and HDAC6 proteins. In conclusion, the classification and regression models established in this study can effectively facilitate the discovery of dual JAK2 and HDAC6 inhibitors, emphasizing the significant promise of machine learning in the discovery of dual inhibitors.

In recent years, hydrogels have been employed to fabricate flexible capacitors (FCs) and wearable sensors. However, achieving a balance between the electrochemical and mechanical properties of hydrogels remains a challenge. Herein, polyacrylamide/sodium alginate (PAM/SA) dual-network hydrogels with good mechanical properties and high electrochemical properties were obtained by nitric acid (HNO₃) mediation. The –COO– groups on the SA network inside the hydrogel are partially acidified to –COOH under the action of HNO₃, which increases the hydrogen bond density of the hydrogel. The PAM/SA hydrogel exhibited a maximum mechanical strength of 83.4 KPa and a maximum elongation at break of 471.3%. Furthermore, the conductivity (σ) of PAM/SA dual-network hydrogels increased from 36.48 mS cm⁻¹ to 96.4 mS cm⁻¹, and the specific capacitance of the flexible capacitor (FC) composed of the hydrogels increased by about 142.1%. Finally, the hydrogel was prepared as a wearable motion sensor, which is capable of accurately detecting the different motion states of a person. Consequently, the hydrogel has a multitude of applications in the field of FCs and wearable sensors.

Cu-based catalysts have been promising materials for electrocatalytic reduction of carbon dioxide into C₂₊ products. However, the low selectivity of Cu-based catalysts for a single C₂₊ product limits their application. Herein, this work presents a strategy to modify the coordination environment of Cu-based MOF catalysts through the introduction of different doping atoms, aiming to improve the selectivity towards ethanol products. The CuIn-BTC-DBD catalyst exhibits an ethanol FE of 87% with a partial current density of −17 mA cm⁻² at −1.4 V vs. RHE. Through experimental investigations, we reveal the modulation of the coordination environment of Cu-based MOFs through the doping of In atoms. This strategy improves the selectivity for ethanol products. This study provides a new approach to designing bimetallic Cu-based MOF electrocatalysts with high efficiency, mild conditions, and stable CO₂RR to ethanol products.

The generation of hydrogen from water using sunlight offers a promising approach for scalable and sustainable carbon-free energy production. The success of solar-to-fuel technology hinges on the design of efficient, durable, and cost-effective photoelectrochemical (PEC) cells that can absorb sunlight and drive water-splitting reactions. In this context, we present a promising heterojunction by integrating Cu₂O with a ZnO overlayer mimicking a 3D–2D heterojunction, addressing the challenges associated with copper-based metal oxides in PEC water-splitting reactions. The heterojunction thin films were deposited on ITO glass substrates using a low-cost, scalable spray pyrolysis technique. We varied the thickness of the ZnO layer by adjusting the total spray time from 30 to 120 seconds on the pre-deposited Cu₂O thin films. Our study identified 90 seconds as the optimal spray time, yielding a peak photocurrent of 1.25 mA cm⁻² and an ABPE of 0.98% at an overpotential of 270 mV. Density functional theory (DFT) studies were also conducted to elucidate the mechanism behind the improved photocurrent of the heterojunction.

Solid or quasi-solid electrolytes are acclaimed for their ability to overcome limitations associated with liquid electrolytes, while still retaining crucial characteristics of the latter. Particularly within the realm of energy storage, these electrolytes have garnered substantial interest over the past decade. This study presents an investigation into two hybrid eutectogels obtained from the encapsulation of an ionic-liquid-(IL-) based binary deep eutectic solvent (DES) within a solid matrix of titania (TiO₂) or silica (SiO₂) through a non-aqueous sol–gel route. The DES is prepared by mixing the IL 1-butyl-3-methylimidazolium methanesulfonate ([BMIM][MeSO₃]) and N-methylacetamide (NMAc) in a carefully optimized molar ratio of 1 : 2. The properties of the eutectogels are thoroughly examined employing analytical techniques including field emission scanning electron microscopy (FESEM), energy dispersive X-ray (EDX) spectroscopy, field emission transmission electron microscopy (FETEM), Fourier transform infrared (FTIR) spectroscopy, Raman spectroscopy, X-ray diffraction (XRD), thermogravimetric analysis (TGA), cyclic voltammetry (CV), and electrochemical impedance spectroscopy (EIS). Remarkably, the structural integrity of the DES remains unaltered following its incorporation into the matrices. The eutectogels exhibit a double-layer capacitive behavior within a wide operating potential window (OPW) of 3 V. Specific capacitance and ionic conductivity as high as 16.32 F g⁻¹ and 1.27 mS cm⁻¹ are obtained at room temperature with specific energy and specific power of 20.39 W h kg⁻¹ and 3.31 kW kg⁻¹ respectively, thus underscoring their potential utility in applications concerning electrochemical supercapacitors.

Using (bis)diethoxyphosphoryl ferrocene [Fc(OP(OEt)₂)₂] and transition metal carboxylates – [M₂(μ-OOCR)₄(CH₃CN)₂], M = Cu^II, R = ^tBu, (C₅H₄)Mn(CO)₃ (Cym) or [M₃(μ-OOCR)₆(CH₃CN)₂], M = Ni^II, Co^II, R = Cym, a series of heterometallic polymers with metal cores {Cu₂Fe}_n (1), {Cu₂Mn₄Fe}_n (2) {Ni₂Mn₄Fe}_n (3), and {Co₂Mn₄Fe}_n (4) were obtained under mild conditions. Compounds 1 and 2 showed antibacterial activity against a Mycobacterium smegmatis strain in vitro.