Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Zeqian Zhang,Hongshan Wu,Qiming Chen,Xiaowei Li,Yimin Cai,Lihua Yuan,Wen Feng
Efficient and selective palladium (Pd) recovery from high-level liquid waste (HLLW) constitutes a crucial task for both precious resource recovery and environmental remediation, but remains challenging to achieve high efficiency, sufficient selectivity, and fast kinetics. Herein, we report a new pyrazinamide ligand (denoted as PA) as the first example of employing pyrazine-based ligand for Pd 2 + separation with impressive efficiency. Using an ionic liquid C 8 mimNTf 2 as diluent, the developed pyrazinamide-ionic liquid (PA-IL) extraction system exhibited attractive merits for Pd 2+ separation such as a wide range of workable acidities from 0.2 M to 5 M HNO 3 , ultra-fast extraction kinetics with equilibrium time of 3 min, and good Pd 2+ selectivity over 16 ions coexisting in simulated HLLW and other non-metallic anions. Slope analysis indicated that the extraction mechanism involves the cation exchange of C 8 mim + and the coextraction of NO 3 - anions in the course of Pd 2+ extraction. Results from a set of spectroscopic investigations and single crystal X-ray diffraction analysis suggest the formation of complexes with stoichiometry of both 1:1 and 2:1 (PA/Pd 2+ ) in solution and in solid state, of which the formation of 2:1 complex is the most thermodynamically favored according to DFT theoretical calculations. This work provides a highly promising pyrazinamide-based extraction system for efficient and selective Pd 2+ separation from HLLW, and brings more understanding about the complexation and coordination behaviors between N-based ligands and Pd 2+ ions.
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MOLECULES
·
2025
·Vol. 30
·期 7
·1533
·
IF 4.6
Yuyang Gan,Yimin Cai,Song Huang,Xiaowei Li,Wen Feng,Lihua Yuan
Nitrogen donor-based ligands are highly promising extractants for palladium separation from high-level liquid waste (HLLW). However, the electronic effect of these ligands, a critical factor influencing their complexation ability with Pd(II), remains largely unexplored. Herein, three picolinamide-based ligands were designed and synthesized, each featuring substituents with distinct electronic effects at thepara-position of the pyridine (electro-donating methoxyl group for L-I, hydrogen for L-II, and electro-withdrawing ester group for L-III). The concurrent processes of Pd(II) coordination and ligand protonation enable the manipulation of pyridine nitrogen electronegativity, resulting in a tunable Pd(II) extraction performance. Notably, L-I exhibits the highest extraction efficiency at low acidities (≤1 M HNO3) but the lowest extraction at high acidities (≥3 M HNO3), whereas L-III shows the poorest efficiency at low acidities but the best performance at high acidities. The Job plot analysis and ESI-HRMS results reveal a 1:1 and 2:1 (L/Pd) stoichiometry in the Pd(II) complexation process. The single crystal X-ray analysis of Pd(NO3)2(L-II)2complex confirms a four-coordinated Pd(II) center, with two pyridine nitrogen atoms and two monodentate nitrate oxygens forming a quadrangular geometry. Density functional theory (DFT) calculations further indicate that the formation of 2:1 (L/Pd) complexes is energetically favored, and the stronger basicity of the nitrogen atoms correlates with a higher Pd(II) binding affinity and increased susceptibility to protonation.
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Environmental Science-Nano
·
2024
·
IF 5.8
Ya-Fei Cheng,Meng Li,Hai-Tian Xu,Shu-Yang Fang,Yu Zhang,Zheng-Zhe Zhang,Ren-Cun Jin
Among numerous engineered nanoparticles (NPs), CuNPs have been identified as a kind of high-risk inhibitor to anammox bacteria; however, the potential effects of salinity on the toxicity of CuNPs to anammox consortia remain unclear. Their short-term and long-term effects on anammox consortia were investigated by batch assays and continuously-fed bioreactors. The addition of 5.0–7.4 g L−1 NaCl immediately shielded the acute inhibition of 2.0–4.6 mg L−1 CuNPs on anammox activity. However, the coexistence of 5.0 g L−1 NaCl significantly aggravated the inhibitory effect of 3.0 mg L−1 CuNPs on anammox activity after exposure of about one month through reducing the content of extracellular polysaccharides. Even, the membrane permeability was significantly increased with the further increase of NaCl to 8.0 g L−1. Although the relative abundance of anammox bacteria at the DNA level was relatively higher, most of the anammox cells may not be able to perform metabolic functions normally due to membrane damage. Thus, appropriate salinity would attenuate the adverse impacts caused by the short-term shock of CuNPs, while pre-treatment is required to avoid the synergistic stress of high CuNPs when treating high salt wastewater.
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Colloid and Interface Science Communications
·
2025
·
IF 4.7
Jun Sun,Sulei Zhang,Yichen Wang,Denghai Sheng,Shengjie Liu,Yu Rao,Aiqing Li,Yuchun Pan,John L. Brash,Xiaoli Liu,Hong Chen
Thrombus formation often leads to the failure of intravascular implants. Natural endothelium provides multifaceted antithrombotic functions through nitric oxide/ prostacyclin secretion to inhibit platelet activation, glycosaminoglycan mediated anticoagulation, and tissue-type plasminogen activator driven fibrinolysis. Therefore, surfaces mimicking these multiple endothelial functions are expected to have enhanced antithrombotic properties. In this study, polyvinyl chloride surface was rendered porous through solvent/nonsolvent-induced phase separation and loaded with a metal-organic framework, CuBTTri to catalyze nitric oxide release from a precursor. Furthermore, using layer-by-layer self-assembly, multiple bilayers of a poly(lysine- co -oligo(ethylene glycol) methyl ether methacrylate) copolymer (fibrinolysis-promoting), and sodium heparin (endothelial cell growth-promoting), were deposited on the un-etched side of the polyvinyl chloride. This modified surface was shown to be capable of releasing nitric oxide, destroying nascent thrombus, inhibiting smooth muscle cell growth, and promoting endothelial cell adhesion. This study represents a novel approach to developing multifunctional blood-contacting surfaces that mimic multiple properties of the endothelium.
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DALTON TRANSACTIONS
·
2025
·
IF 3.3
Yaqoot khan,Yunyun Du,Li Yan,Niu Zhang,Menglei Zhang,Hongwei Ma,Hui Li
Understanding the coordination geometry of nucleotide mono-, di-, and triphosphates is pivotal for unraveling the intricate relationships between molecular structure and biological function, particularly in metal–ligand interactions and their role in biomolecular recognition. This study investigates the structure of nucleotide-metal polymers and their selective interactions with amino acids, specifically Tryptophan (Trp) and Tyrosine (Tyr). We synthesized and comprehensively analyzed five coordination polymers of cytidine-nucleotides: cytidine monophosphate (CMP), deoxycytidine monophosphate (dCMP), cytidine diphosphate (CDP), and cytidine triphosphate (CTP): {[Cu(CMP)(bpa)(H₂O)₃](CMP)·3H₂O}n (1), {[Cu₂(dCMP)(4,4′-bipy)₂(H₂O)₂]·4H₂O}n (2), {[Cu₂(CDP)₂(azpy)(H₂O)]·3H₂O}n (3), {[Cd₂(CDP)₂(bpa)₂(H₂O)₂]·8H₂O}n (4), and {[Cu(CTP)(2,2′-bipy)]·2H₂O}n (5), where (3), (4) and (5) mark the first report of CDP and CTP coordination complexes. Single crystal X-ray diffraction unveiled the structure of the polymers to be one-dimensional (1, 5) or two-dimensional (2, 3, 4). Circular dichroism (CD) spectroscopy in both the solid and solution states elucidates the chirality-driven assembly in these nucleotide-metal polymers. The selective interactions of coordination polymers with Tryptophan (Trp) and Tyrosine (Tyr) were studied using spectroscopic titrations. Experimental and computational analyses reveal distinct interactions between all five coordination polymers and the amino acids, highlighting their biosensing potential. Binding affinity variations across the polymers offer insights into nucleotide-metal coordination chemistry and suggest applications in molecular recognition and functional materials.
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Materials
·
2025
·Vol. 18
·期 15
·3679
·
IF 3.2
Guangxin Wu,Gaosheng Li,Lijun Wei,Hao Chen,Yujie Wang,Yunze Qiao,Yu Hua,Chenyang Shi,Yingde Huang,Wenjie Yang
This study synthesized FeNiCuAlX high-entropy alloys (HEAs) (where X = Cr, Co, Mn) using arc melting and investigated their high-temperature oxidation behavior in air at 900 °C. The oxidation kinetics of all alloys followed a parabolic rate, with the oxidation rate constants (kp) of FeNiCuAlCr, FeNiCuAlCo, and FeNiCuAlMn being approximately two to three orders of magnitude lower than that of the FeNiCu alloy. Specifically, FeNiCuAlCr exhibited the lowest kp value of 1.72 × 10−6mg2·cm4/s, which is significantly lower than those of FeNiCuAlCo (3.29 × 10−6mg2·cm4/s) and FeNiCuAlMn (1.71 × 10−5mg2·cm4/s). This suggests that the addition of chromium promotes the formation of a dense Al2O3/Cr2O3oxide layer, significantly enhancing the oxidation resistance. Furthermore, corrosion resistance was assessed through potentiodynamic polarization and electrochemical impedance spectroscopy in a 3.5% NaCl solution. FeNiCuAlCr demonstrated exceptional resistance to localized corrosion, as indicated by its low corrosion current density (45.7 μA/cm2) and high pitting potential (−0.21 V), highlighting its superior corrosion performance.
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International Journal of Smart and Nano Materials
·
2025
·
IF 6.6
Jiefeng Gong,Zhiyuan Huang,Huihuang Yu,Hongmingzhe He,Yige Xiong,Longqiu Li,Guanhua Zhang,Guangyu Zhang
High-precision three-dimensional (3D) printing has enabled the fabrication of architected microlattices with complex geometries and tunable functionalities, offering new opportunities for electrochemical energy storage devices. In particular, 3D polymer octet-truss lattice frameworks exhibit exceptional mechanical robustness, structural regularity, and customizable porosity, making them promising candidates for electrode applications. However, current fabrication techniques often face challenges in achieving the required precision and structural integrity for advanced applications. In this study, projection micro stereolithography (PμSL) was utilized to fabricate high-resolution 3D electrode substrates based on octet-truss microlattices. The printed structures were systematically optimized for both mechanical stability and printing accuracy. Electrochemical plating and magnetron sputtering were employed as surface modification techniques to improve the physicochemical characteristics of the lattices and introduce lithium-affinitive functionality. The resulting 3D microlattice electrodes demonstrate high structural precision and enhanced electrochemical performance, highlighting their strong potential for integration into advanced lithium metal batteries and related energy storage systems.
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Inorganic Chemistry Frontiers
·
2025
·
IF 6.4
Mengqi Man,Yong Guo,Tianran Hu,Ying Sun,Aikai Yang,Xiqing Chen,Xingchao Wang
The preparation of SiOx materials that exhibit enduring stable cycling performance and high initial coulombic efficiency (ICE) through cost-effective methods remains a substantial hurdle. Herein, a hybrid carbon-coated SiO-20/G@TMA composite was synthesized using an integrated strategy that combines high-energy ball milling and high-temperature carbonization, employing graphene (G) and trimeric acid (TMA) as carbon sources. The three-dimensional crosslinked conductive network, formed by the mechanically flexible graphene and the carbon-rigid TMA, induces the generation of a LiF-rich SEI film. This film reduces interfacial side reactions and improves the ICE to 74.2%. Furthermore, the SiO-20/G@TMA electrode, characterized by a rigid–flexible hybrid structure, demonstrates excellent capacity retention and impressive rate performance over extended cycling periods. The discharge capacity of the SiO-20/G@TMA anode reaches 848.3 mA h g−1 at a current density of 0.5 A g−1, with a reversible capacity of 77% (about 649.1 mA h g−1) maintained after 600 cycles. When paired with a LiNi0.8Co0.1Mn0.1O2 (NCM811) cathode, the SiO-20/G@TMA anode achieves a reversible capacity of 140.0 mA h g−1 at the current density of 0.2 A g−1. After 100 cycles, the capacity retention rate is 85% and the energy density is 474.7 Wh kg−1.
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Matter
·
2025
·
IF 17.5
Shining Wu,Yuting Zhang,Guanwu Li,Yifeng Hou,Mengyang Cao,Chengyu Wei,Pengkun Yang,Lu Huang,Yingpeng Wu
High-entropy alloys (HEAs) have a wide range of applications due to their excellent physical and chemical properties. However, traditional synthesis routes always require high temperatures over 923 K or have high equipment requirements. Here, we developed a liquid metal gallium (Ga)-mediated strategy using only a commercial vortex mixer and metal powders to synthesize HEAs near room temperature (303 K) with low power (7 W). A variety of HEAs were successfully prepared, and the yield can be expanded to over 10 g each time. The mechanistic investigation proved that Ga continued to flow under the mechanical force and exposed fresh surfaces to contact the metal, thereby promoting the process of metal dissolution in Ga and forming HEAs. These as-prepared HEAs can be used for catalysis in electrochemical oxygen evolution reactions with low overpotential and high durability. This strategy provides an innovative method for low-energy synthesis of HEAs at room temperature.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2025
·
IF 11.3
Zhenmin Xu,Ting Zhang,Junyu Lang,Mengli Xu,Ya Xie,Chunyan Wu,Huangrong Wang,Han Yu,Zhenfeng Bian
Carboxylates are commonly formed as intermediates during the oxidation of volatile organic compounds (VOCs) and are often regarded as significant barriers to the complete mineralization of organic pollutants. In this study, we present a novel cobalt-doped copper-based catalyst that employs an in situ benzoic acid-mediated oxygen activation strategy for the photocatalytic degradation of toluene under visible-light irradiation. Unlike traditional systems in which carbonyl intermediates contribute to catalyst deactivation, we demonstrate that benzoic acid, generated during toluene oxidation, acts as a potent ligand to modulate the electronic structure of cobalt sites. This interaction significantly enhances oxygen activation and promotes the generation of reactive oxygen species (ROS), facilitating the complete oxidation of toluene to CO2 with nearly 100% efficiency. In situ characterization and density functional theory (DFT) calculations reveal that the migration of benzoic acid from copper to cobalt sites under visible light is critical for the oxidation process. This migration induces a pronounced electron-donating effect, enabling activation of the Co center, which drives efficient ROS production and autocatalytic mineralization of benzoic acid. The resulting Co-Vo-Cu catalyst demonstrates exceptional catalytic activity and stability, outperforming previous systems in VOCs degradation. This work offers new insights into the role of organic intermediates in oxygen activation and presents a promising strategy for the development of next-generation photocatalysts for VOCs elimination.
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Petroleum Science
·
2025
·
IF 6.1
Zhi-Cai Zhang,Jia-Kun Wu,Chao Wang,Zhi-Qiang Hou,Yao Tang,Hao Li,Jiao Yang,Jun Gao,Yi-Kan Yang,Yang-Bin Liu,Xiao-Ping Ouyang,Hai-Kuo Wang
With the global oil and gas industry increasingly targeting ultra-deep well development, the demand for wear resistance in polycrystalline diamond compact (PDC) bits is increasing. However, further improvement of the mechanical properties of PDC incurs prohibitively elevated costs and stringent technological challenges. Here, we present a two-stage high-pressure infiltration (HPI) methodology involving cobalt removal pretreatment followed by lubricant infiltration. The successful infiltration of lubricants into diamond micropores has been systematically verified, and the effects of lubricant phase composition, infiltration pressure, and temperature on infiltration depth have been thoroughly investigated. Fractal dimension analysis characterizes the pore structure of cobalt-removed diamonds, revealing a strong correlation between the fractal dimension and friction coefficient reduction. Tribological testing confirms the formation of lubricating films at friction interfaces, achieving a 71.5% reduction in the coefficient of friction for lubricant-containing diamond materials. This straightforward strategy opens a gate to developing the next generation of self-lubricating diamond materials.
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Journal of Materials Chemistry A
·
2025
·
IF 9.5
Hanqian Li,Bangzhi Ge,Wenqi Xie,Ruoyan Li,Chao Li,Wanqi Jie,Dongxu Zhang,Yi Qin,Yuan Yu,Chongjian Zhou
Liquid-like thermoelectric materials continuously draw significant attention because of their extraordinary performance. However, liquid-like Cu atoms usually aggregate into clusters, resulting in charge carrier concentration far above the optimized value. Herein, we demonstrate that the dynamic Cu atoms can be homogenized throughout the matrix by a phase-dependent diffusion process. We directly visulized that the typical equilibrium process periodically aggregates Cu atoms into clusters along the grain boundaries, leaving abundant vacancies within the dynamic cation sublattice and thereby causing carrier concentrations that are much higher than the optimal value. We developed a solid-state non-equilibrium quenching process to freeze the homogeneous Cu sublattice in the symmetry cubic phase to ambient environment and removed the unfavorable Cu segregation. This substantially decreases the hole concentration from 1.2 × 1022 cm−3 for the equilibrium sample to 0.8 × 1022 cm-3 for the quenched sample, approaching the calculated optimal value. Notably, the highly uniform Cu sublattice reduces the lattice thermal conductivity to predicted minima of 0.3 W·m−1·K−1 from 300 to 1000 K. The reduced hole concentration and lattice thermal conductivity collectively give rise to a high ZT value of 1.5 at 1000 K, lying in the ballpark of all previously reported stoichiometric copper chalcogenides.
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