查找使用阿拉丁产品的科研文献

Cu Doping-Induced Transformation from [Ag62S12(SBut)32]2+ to [Ag62−xCuxS12(SBut)32]4+ Nanocluster

Jun Zhou,Sha Yang,Yesen Tan,Huaisheng Cheng,Jinsong Chai,Manzhou Zhu

The change in the valence state of nanocluster can induce remarkable changes in the properties and structure. However, achieving the valence state changes in nanoclusters is still a challenge. In this work, we use Cu 2+ as dopant to “oxidize” [Ag 62 S 12 (SBu t ) 32 ] 2+ (4 free electrons) to obtain the new nanocluster: [Ag 62−x Cu x S 12 (SBu t ) 32 ] 4+ with 2 free electrons. As revealed by its structure, the [Ag 62−x Cu x S 12 (SBu t ) 32 ] 4+ (x=10∼21) has a similar structure to that of [Ag 62 S 12 (SBu t ) 32 ] 2+ precursor and all the Cu atoms occupy the surface site of nanocluster. It′s worth noting that with the Cu atoms doping, the [Ag 62−x Cu x S 12 (SBu t ) 32 ] 4+ nanocluster is more stable than [Ag 62 S 12 (SBu t ) 32 ] 2+ at higher temperature and in electrochemical cycle. This result has laid a foundation for the subsequent application and exploration. Overall, this work reveals crystals structure of a new Ag−Cu nanocluster and offers a new insight into the electron reduction/oxidation of nanocluster.

Multi-site occupancies of Dy3+ in Ca3Gd(AlO)3(BO3)4 and their optical thermometric applications

Ye Zhiqi,Cheng Zhiyuan,Liu Tong,Shi Tian,Gao Fuhao,Khan Wasim Ullah,Zhang Yueli

Lanthanide-doped Ca 3 Ln(AlO) 3 (BO 3 ) 4 phosphors are adopted for numerous new types of applications with outstanding optical properties. Herein, the novel Ca 3 Gd(AlO) 3 (BO 3 ) 4 :Dy 3+ phosphors were synthesized by the high-temperature solid-state method. X-ray diffraction, scanning electron microscopy, transmission electron microscopy, diffuse reflection spectroscopy, and as well as photoluminescence (PL) spectra and lifetime curves are used to exemplify the resulting samples. This research explores the samples microstructure and the influence of Dy 3+ doping at the Ca and Gd sites. The PL spectrum results indicated that Ca 3 Gd(AlO) 3 (BO 3 ) 4 :Dy 3+ can be effectively excited by 349 nm UV light and emits bright white light results of Dy 3+ ions with the 4f–4f transition. The optimum doping content of the Dy 3+ in the Ca 3 Gd(AlO) 3 (BO 3 ) 4 host samples were 7 mol%, and the concentration quenching (CQ) mechanism was mainly owing to dipole–dipole interaction. Interestingly, the Ca 3 Gd 0.93 (AlO) 3 (BO 3 ) 4 :0.07Dy 3+ showed exceptional thermal-quenching resistance of > 87.3% intensity at 350 K. The temperature-sensing properties of Ca 3 Gd 0.93 (AlO) 3 (BO 3 ) 4 :0.07Dy 3+ ranging from 300 to 500 K were analyzed and had shown a decent maximum S A value about 1.35% K −1 at 500 K between 455 and 669 nm fluorescence intensity ratio. Hence, the novel Ca 3 Gd 0.93 (AlO) 3 (BO 3 ) 4 :0.07Dy 3+ materials could be a competent candidate for low-cost and non-contact optical thermometry in a high-temperature environment.

Effects of hydrogen sulfide (H2S) on respiration control of state 3/4 in mitochondria from bovine heart

Y Su,Y Cheng,D Wang,F Zhang,Y Su,Z Li

Dual engine drive: The synergy of Mn and Ti 4 O 7 achieves highperformance acidic water oxidation

Xin Li,Zhongya Jia,Yi Wang,Kuo Liu,Xi Li,Tao Qi

The development of electrocatalysts that simultaneously exhibit high activity and robust stability for the oxygen evolution reaction (OER) is critical to advancing proton exchange membrane water electrolysis (PEMWE). In this work, Mn-doped RuO2 is composited with acid-resistant and highly conductive Ti4O7 via a simple molten salt method, yielding a Mn-RuO2/Ti4O7 hybrid electrocatalyst. Electrochemical measurements reveal that Mn-RuO2/Ti4O7 achieves a low overpotential of 194 mV at 10 mA cm⁻² and maintains stable operation for over 220 h at this current density. In situ spectroscopic analysis and computational studies further indicate that Mn doping modulates the electronic interplay between RuO2 and Ti4O7, which not only suppresses over-oxidation of Ru at high potentials but also promotes the deprotonation kinetics of reaction intermediates, thereby significantly enhancing the overall catalytic performance. This work offers an effective strategy for balancing activity and stability in acidic OER electrocatalys.

Copper doped palladium metallene with enhanced catalytic activity for the electrochemical detection and degradation of 4-nitrophenol

Hongyi Li,Changjin Zhou,Jiadong Chen,Junlun Zhu,Yunxia Jin,Yingxi Wang,Zhengfang Tian,Shengfu Wang,Wei Wen

Metallene, as a new type of metal material, has unique structure and properties, which brings new research directions and application prospects for environmental wastewater treatment, catalysis, energy storage and conversion. Here, we developed copper doped palladium metallene (Cu-doped Pd metallene) by reasonable and effective interface design for electrochemical detection of 4-nitrophenol (4-NP) and degrading 4-NP in presence of sodium borohydride. The synergistic interaction both the catalytic activity sites of copper and the high conductive properties of Pd metallene exhibited, transforming into an ideal candidate for the electrochemical detection and catalytic reduction of 4-NP. Inspired by these advantages, electrochemical detection of 4-NP was exhibited better analytical performance, which displayed the detection range from 10 to 1000 μM. In addition, the Cu-doped Pd metallene showed the best activity with k app  = 0.54 s −1 . Notably, the Cu-doped Pd metallene exhibited outstanding catalytic efficiency for the degradation of 4-NP that was three times greater than that of pure Pd metallene. Under the condition of high temperature and high concentration of salt, Cu-doped Pd metallene still maintained high catalytic activity. Those results indicated that Cu-doped Pd metallene exhibited superior catalytic activity, considerable stability, elevated turnover frequency, and improved green sustainability for the detection and degradation of 4-NP. This will be of immense importance to the realization of metallene toward potential high-value applications and the advancement of nanocatalyst research.

Ionic interactions drive SC[4]A to regulate polyamide networks for achieving high-efficiency Li+/Mg2+ separation

Wei Shao,Xiuling Liu,Zhaojing Jing,Ziyang Guo,Xiaowen Huo,Weihao Zhang,Haitao Wang,Na Chang

The selective separation of lithium and magnesium by conventional nanofiltration (NF) membranes remains a major challenge for lithium extraction from salt-lake brine. This difficulty results from the extremely fast and disordered nature of the interfacial polymerization process, which hampers precise control over the pore size of the separation layer. In this study, to utilize the hollow internal cavity of the macrocycle, calix[4]arene was directly sulfonated to prepare hydrophilic sulfonated calix[4]arene (SC[4]A), which was incorporated as an aqueous-phase additive into the piperazine (PIP) solution. NF membranes were then fabricated via interfacial polymerization (IP) on a self-made polysulfone (PSf) substrate. The results demonstrated that SC[4]A effectively accelerated the kinetics of the IP reaction. More importantly, SC[4]A, which was ionically bonded into the polyamide (PA), served as the additional mass transfer channel and formed a separation layer with a smaller free volume, narrower pore size distribution, and enhanced negative surface charge. The prepared TFC-0.5 membrane exhibited a Li + /Mg 2+ separation factor as high as 28.90, a 2.19-fold increase over the pristine membrane. Additionally, the incorporation of SC[4]A improved the hydrophilicity of the membrane surface, imparting superior antifouling properties to the modified membrane. By precisely regulating the IP process and tailoring the free volume of the separation layer, this study provides a new strategy for developing high-performance lithium‑magnesium separation NF membranes.

Toll-Like Receptor 4/p65 Signalling Pathway Mediates Recurrent Spontaneous Abortion by Regulating Forkhead Box Protein P3

Caiqun Huang,Ying Lyu,E Fen Cheng

Background:Although multiple factors contribute to recurrent spontaneous abortion (RSA), recent studies have highlighted a role for regulatory T cells (Tregs) in maintaining immune tolerance during pregnancy. Understanding the intricate relationship between RSA and Tregs offers promising avenues for diagnosis and therapeutic strategies in reproductive medicine.Methods:We successfully established a mouse model of RSA, and all animals were euthanized on gestational day 13. Uterine horns were examined upon dissection to determine the number of viable fetuses and resorption sites, after which the post-implantation loss rate (abortion rate) was calculated. Placental morphology was evaluated via hematoxylin and eosin staining, whereas gene expression was analysed by immunohistochemistry. Treg abundance was determined by flow cytometry. Gene expression and cytokine levels in EL4 cells and patient samples were evaluated by quantitative real-time polymerase chain reaction (qPCR) and Western blotting.Results:The abortion rate of RSA mice was 31.64%. In addition, Treg numbers were reduced in both RSA mice and patients, while the expression of Toll-like receptor 4 (TLR4) and p65 was upregulated, further suppressing forkhead box protein P3 (FOXP3) expression. Blocking p65 expression with small interfering RNA (siRNA) targeting p65 prevented the lipopolysaccharide (LPS)-induced downregulation of FOXP3 in EL4 cells. The TLR4 inhibitor IAXO102 was ineffective at increasing FOXP3 expression in EL4 cells following p65 overexpression p65.Conclusions:The results of this study suggest that activation of the TLR4/p65 signalling in RSA inhibits FOXP3 expression and contributes to abortion. Importantly, the findings indicate that Treg suppression in RSA is p65-dependent.

KBi(IO3)3(OH) and NaBi(IO3)4: from the centrosymmetric chain to a noncentrosymmetric double layer

Ying-Jie Jia,Yi-Gang Chen,Ting Wang,Yao Guo,Xiao-Fang Guan,Xian-Ming Zhang

Two new alkali–metal bismuth iodates KBi(IO3)3(OH) (1) and NaBi(IO3)4 (2) have been synthesized by a hydrothermal method via tuning of alkali–metal ions. Compound 1 crystallizes in the space group P and features a [Bi(IO3)3(OH)]n chain with eight-membered Bi–O–I–O–Bi–O–I–O rings. The [Bi(IO3)3(OH)]n chain consists of paddlewheel-like dimeric Bi2(OH)2(IO3)4 units linked by IO3 pairs. Compound 2 in the polar space group Cc features a [Bi(IO3)4]− double layer with Bi4I4 eight-membered rings (8-MRs). NaBi(IO3)4 exhibits a strong second harmonic generation (SHG) response of ∼5.0 × KDP (KH2PO4) and a wide transmittance window (0.4–12 μm), and structure analyses and theoretical calculations reveal that polarization results mainly from the proper alignment of the IO3 groups. The calculated electronic structure based on the DFT method indicates that the BiOn and IO3 groups dominate their optical properties.

Fabrication of highly dispersed Pd nanoparticles supported on reduced graphene oxide for catalytic reduction of 4-nitrophenol

Wenhuan Dong,Saisai Cheng,Cheng Feng,Ningzhao Shang,Shutao Gao,Chun Wang

Well-dispersed and ultrafine metal nanoparticles can significantly improve the catalytic performance of heterogeneous catalyst. In this paper, highly dispersed Pd nanoparticles were successful anchored on reduced graphene oxide using a co-deposition and sacrificial method, in which cobalt was used as the sacrificial agent. This method can effectively prevent the Pd nanoparticles from aggregation, and the resulted catalyst exhibited exceedingly high catalytic activity for the reduction of 4-nitrophenol at room temperature with NaBH 4 as hydrogen resource. The turnover frequency reaches 9900   h −   1 at 298   K, which is among the highest values ever reported thus far for heterogeneously catalyzed reduction of 4-nitrophenol under ambient conditions.

1-Methyl-4-R-1,2,4-triazolium (R = −CH2CH2OCH3, −CH2COOCH2CH3)-Based Ionic Liquids as Plasticizers for Solid Propellants

Long Liu,Jinhu Bai,Ze Su,Yuan Yao,Zhixiang Zhou,Yangfeng Xia,Yanqiang Zhang

In this paper, a series of energetic ionic liquid plasticizers of 1-methyl-4-methoxyethyl-1,2,4-triazolium chloride (1), 1-methyl-4-methoxyethyl-1,2,4-triazolium bis(trifluoromethylsulfonyl)imide (1a), 1-methyl-4-methoxyethyl-1,2,4-triazolium nitrate (1b), 1-methyl-4-ethyl acetate-1,2,4-triazolium chloride (2), 1-methyl-4-ethyl acetate-1,2,4-triazolium bis(trifluoromethylsulfonyl)imide (2a), and 1-methyl-4-ethyl acetate-1,2,4-triazolium nitrate (2b) were synthesized and characterized. The results show that compounds 1a, 1b, 2a, and 2b have lower melting points (Tm, −72.60 to −32.67 °C) and good thermal stability (Td, 161–348 °C) and are suitable as plasticizers for hydroxyl-terminated polybutadiene (HTPB) curing systems. Among these four ionic liquids, ester-functionalized cations can help to improve the tensile strength (2a, 0.943 MPa; 2b, 1.113 MPa) of the cured system, while ether-functionalized cations are more beneficial to improve elongation at break (1a, 522.90%; 1b, 484.45%). Ester-functionalized ionic liquids are more beneficial to reduce the glass transition temperature of HTPB elastomers. The storage modulus of HTPB elastomers containing NO3– is higher, while that of HTPB elastomers containing NTf2– is lower. The crosslink densities of HTPB/TDI/2a and HTPB/TDI/2b plasticized by ester-functionalized ionic liquids are larger, which are 9369 and 9616 mol/m3, respectively. There are hydrogen bond interactions between the ionic liquid and the HTPB elastomer, and these interactions changed the distribution of the hard and soft segments in the polymer molecules.

Synergistically enhanced electrochemical sensor based on a covalent organic framework/carbon nanotube composite for 4-nitrophenol detection

Xue Jun-Chang,Jiang Yue,Xia Huan,Hou Lu,Li Heng-Ye,Wang Zhong-Xia,Kong Fen-Ying,Wang Wei

An electrochemical sensor was developed for the sensitive voltammetric determination of 4-nitrophenol (4-NP) by integrating an in situ grown nanocomposite of amino-functionalized carbon nanotubes (NH 2 -CNTs) and a zinc porphyrin-tetrathiafulvalene covalent organic framework (TTCOF-Zn). This hybrid design strategically couples the electron donor–acceptor (D-A) architecture of TTCOF-Zn, featuring pre-engineered electron transport channels, with the exceptional electrical conductivity of NH 2 -CNTs via covalent bonding, synergistically enhancing charge transfer efficiency. Leveraging the high conductivity, abundant active sites, and hierarchical porosity of the TTCOF-Zn/NH 2 -CNTs nanocomposite, the modified electrode achieves an exceptional detection limit of 17 nM (linear range, 50 nM–1 mM) using differential pulse voltammetry, surpassing most reported sensors. The sensor also demonstrates excellent reproducibility, long-term stability, and strong anti-interference capability against common co-existing species. Its practical applicability was demonstrated through quantitative analysis of 4-NP in real lake water samples, with results validated by the HPLC method, underscoring the potential of D-A COF/CNT covalent hybrids for high-performance environmental monitoring. Graphic

Simultaneously Photocatalytic H2 Production and C–C Coupling of 4-Pyridinemethanol on Pt Doped CdS/TiO2 Heterojunction

Li Qing,Yang Yuke,Li Huajing,Yang Yiwen,Ma Siyu,Su Qiuxing,Shi Yonghong,Li Yuangang

The synergistic coupling of photocatalytic hydrogen production with high-value-added organic conversion provides a new research direction for the efficient use of solar energy and green chemical synthesis. However, key challenges remain in the same catalytic system, such as severe carrier recombination and difficulty in precisely controlling the interfacial reaction pathways. To address these issues, we construct CdS/TiO 2 heterojunction photocatalysts with Pt species introduced by ion exchange and photodeposition. As a result, the Cd(Pt)S/TiO 2 –Pt composite photocatalyst is successfully prepared. Under visible light irradiation, the catalyst achieves highly selective conversion of 4-pyridinemethanol to the C–C coupling product 1, 2-di(4-pyridyl)-1,2-ethanediol, with a selectivity of 89.22%. Under optimized reaction conditions, the maximum H 2 production rate of the catalyst reaches 4.66 mmol·g –1 ·h –1 . Mechanistic studies show that the photogenerated holes enriched on the surface of Cd(Pt)S drive the sp 3 C–H dehydrogenation of 4-pyridinemethanol to form •CH(OH)C 5 H 4 N radicals, which then undergo radical coupling to form new C–C bonds. Meanwhile, the photogenerated electrons transfer through TiO 2 to the Pt active sites to participate in hydrogen evolution. This study provides new insights into regulating the selective conversion of radicals via interfacial electronic engineering and designing photocatalytic coupled reaction systems.