ELECTROCHIMICA ACTA
·
2024
·
IF 5.5
Lei Zhang,Bing Sun,Qinghua Liu,Lin Song,Teibang Zhang,Xiaobo Duan
Extensive research has focused on the lithium (Li) metal anode, but progress in developing this technology has been hindered by the formation of lithium dendrites and their irreversible effects. In this study, an inorganic LiF-Li 3 N-rich solid electrolyte interface (SEI) is established in ether electrolyte through the direct use of 2,3-difluoro-5-(trifluoromethyl)pyridine (DP) to enable uniform Li deposition and enhance interfacial properties for a stable Li metal anode. Theoretical calculations show that DP has a higher tendency to decompose on lithium metal. An alternative approach involving the inclusion of additional anions into the solvation sheath of Li + ions using weakly solvating solvents is proposed. During Li plating, DP is reduced to form a LiF and Li 3 N-rich SEI, resulting in a heterogeneous SEI layer on the Li metal anode surface. This approach allows stable cycling of Li|Li cells for over 1800 h at current densities of 5 mA cm −2 and 15 mAh cm −2 . The method presented here has potential significance in the identification of suitable electrolytes for future research on lithium metal anodes.
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GREEN CHEMISTRY
·
2024
·
IF 9.3
Genyan Hao,Tao Zhao,Qiang Fang,Yunzhen Jia,Dandan Li,Dazhong Zhong,Jinping Li,Qiang Zhao
Exploring Earth-abundant and efficient electrocatalysts to replace Ir and Ru for the acidic oxygen evolution reaction (OER) is essential to reduce the cost of clean hydrogen production. Here, we show that trace amounts of electronegative non-metallic element fluorine (F)-doped Co3O4 nanoneedles improve the activity and stability of Co3O4. The F-doped Co3O4 nanoneedles supported on carbon paper (F-Co3O4/CP) exhibit an overpotential of 350 mV at 10 mA cm−2 for the acidic OER. In addition, their performance remains consistent after continuous operation for 80 h. Detailed investigations reveal that introducing an anion promotes the enrichment of OH on the surface of Co3O4 and prevents acid corrosion, thereby enhancing the intrinsic OER activity and stability. Theoretical calculations further indicate that F doping can effectively improve electron transfer and optimize the energy barrier for the formation of *OOH intermediates, which significantly improves OER performance. This study provides guidance for designing efficient and stable non-noble metal acidic water oxidation catalysts.
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NEW JOURNAL OF CHEMISTRY
·
2025
·
IF 2.5
Qiuyao Jiao,Yan Liu,Ran Yu,Lei Li
For supported heterogeneous catalyst, metal-support interaction (MSI) is very important factors for catalytic performance. Commercial γ-alumina was reduced with hydrogen in advance, providing strong anchoring sites for metal (metal oxide) species. This research demonstrates the use of pre-reduced alumina as catalyst carrier to anchor metal Co species in FTS compared with unreduced one. The defective alumina supported catalyst displayed a supeior performance. The Co/RAl2O3-550 catalyst showed surprisingly high CO conversion of 56.0%, C5+ hydrocarbons selectivity of 93.2%, and a low methane selectivity of 2.7% at a remarkable high activity (CTY = 1.1 × 10-5 molCO gCo-1 s−1). It revealed the strong reduction of alumina generated more defective sites, which was strongly anchored with metal cobalt species under MSI. Besides, the reduction of alumina also boosted the number of surface L-acidity, promoting the CO absorption rate through CO dissociation. These results reveal the unique property of defective Al2O3 supported cobalt catalysts, and provide a practical strategy to explore stable and efficient FTS catalysts.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2025
·
IF 8
Yuxin Lin,Luyao Wang,Sining Meng,Jianjia Liu,Xinyu Li,Wenjuan Wang,Miaoyang Hu,Xi Wang,Weixia Duan,Shangcheng Xu,Jun Wang,Rong Gao
Bisphenol F (BPF), one of the major substitutes for bisphenol A (BPA), is increasingly used in pharmaceuticals, food packaging, and chemical manufacturing. Emerging evidence suggests its potential neuropsychiatric risks. However, the underlying mechanisms remain poorly characterized. Thus, the present study was performed to investigate the roles of the kynurenine (KYN) pathway in BPF induced anxiety- and depression-like behaviors, especially the keys roles of the toxic metabolite 3-hydroxykynurenine (3−HK). The mice were administrated with BPF (10, 40, 160 μg/kg/day) for 30 consecutive days, and the behaviors as well as the changes of the KYN pathway were examined. Noteworthily, even low-dose of BPF exposure (40 μg/kg/day) elicited pronounced anxiety- and depression-like behaviors, molecularly shown as the synaptic marker proteins (PSD95, SYN) and dendritic spine proteins (Drebrin) loss in the prefrontal cortex and hippocampus, along with impaired synaptic connection. The UHPLC-MS/MS metabolomic profiling revealed the aberrant metabolism of the KYN pathway, as shown by the elevated neurotoxic metabolite 3-HK and decreased neuroprotective metabolite kynurenic acid (KynA). Mechanistic analyses demonstrated that the 3-HK rate-limiting enzyme KMO was upregulated while the KynA rate-limiting enzyme KAT2 was downregulated in mouse brain. Notably, pharmalogical inhibition of KMO (GSK180) or blockage kynurenine generation with the TDO2 inhibitor (680C91) substantially ameliorated the BPF induced anxiety- and depression-like behaviors and synaptic impairments. Collectively, the present study unravels a previously unrecognized the BPF induced anxiety- and depression-like behaviors in mice via KMO and 3-HK increase. Therefore, targeting the KMO may provide novel interventive strategy for BPF induced neurobehavioral disorders.
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INORGANIC CHEMISTRY
·
2025
·
IF 4.7
Yu Kang,Bin Li,Haoyu Li,Yuxiao Guo,Qiange He,Li Wang,Guo Wang,Xiaoyan Tang,Chao Xu
The design of multidentate hydrophilic ligands with high binding affinity and selectivity is fundamentally important for efficient metal separation and the development of highly stable radiopharmaceuticals. A widely adopted strategy involves introducing water-solubilizing groups into originally effective lipophilic ligands, aiming to preserve the metal-binding affinity while imparting aqueous solubility. In this work, we demonstrate that such an intuitive solubilization approach can fail if an appropriate hydrogen-bonding network is not established. Using a phenanthroline diimine ligand system as a model, we reveal, at a molecular level, how inter- and intramolecular hydrogen bonding critically influences both water solubility and metal affinity. This is supported by a comprehensive suite of spectroscopic titrations, single-crystal X-ray diffraction, and DFT calculations. To the best of our knowledge, this is the first in-depth study to correlate molecular structure and hydrogen-bonding interactions with overall ligand solubility and metal affinity/selectivity. The insights gained here offer valuable guidance for the rational design of hydrophilic ligands in applications ranging from nuclear waste remediation to f-block-metal-based radiopharmaceuticals and contrast agents.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
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IF 21.1
Ye Chen,Xiaokang Sha,Junpo Guo,Xupo Liu,Meinan Chang,Jiayao Qiu,Jingru Zhang,Bowen Cai,Jiashu Tang,Yi Liu,Huaiyu Shao,Deli Wang
Rational design of heteroatom-doped catalysts with prominent reaction kinetics holds immense potential for enhancing biomass electrooxidation processes. Here, we introduce a F-doped NiO nanosheet architecture enriched with F-Ni δ+ -O coordination motifs as an advanced electrocatalyst for the oxidation of 5-hydroxymethylfurfural (HMF). XPS depth profiling and differential charge density calculations reveal that the distinctive F-Ni δ+ -O configuration induces asymmetric charge redistribution at Ni sites, effectively reducing the activation energy for Ni 3+ OOH species and their subsequent interaction with HMF. Meanwhile, pH-dependent and in-situ Raman measurements demonstrate that F sites function as proton relays, facilitating proton transfer and enabling efficient proton-coupled electron transfer kinetics. The synergistic electronic and proton effects endow excellent catalytic performance, with an oxidation current density of 66.45 mA cm −2 and a reaction rate of 5.23 × 10 −4 s −1 , far higher than that of the original NiO. Notably, the catalyst retains over 95 % Faradaic efficiency and yield of 2,5-furandicarboxylic acid (FDCA) after twenty consecutive cycles. This work establishes a dual regulation strategy via heteroatom doping to simultaneously modulate electronic configuration and proton transfer dynamics, offering novel insights into the design of high-performance electrocatalysts for biomass valorization.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
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IF 21.1
Ziwen An,Qihao Xie,Shaohan Xu,Baoling Niu,Lingzhi Sun,Jingui Zheng,Guohua Zhao
Perfluorooctanoic acid (PFOA), a synthetic persistent and bio-accumulative chemical, has raised global concerns. PFOA oxidation by advanced oxidation technology (AOPs) begins with decarboxylation, followed by CF 2 groups unzipping cycle and C–F cleavage. Since reactive radicals (even •OH) cannot initiate decarboxylation and abundant low-toxicity organics hinders decarboxylation, presents significant challenges for defluorination. We designed a functionalized high-index (201) TiO 2 photoanode (S-TiO 2,201 ) capable of molecular recognition and activation, which switches PFOA adsorption from carboxyl groups to preferential adsorption via the perfluoroalkyl backbone. This adsorption configuration selectively recognizes PFOA and accelerates decarboxylation via direct hole oxidation. In situ electron paramagnetic resonance (EPR) confirmed faster decarboxylation and •OH quantification showed hole utilization efficiency rising from 9.6 % to 39.3 % after functionalization. PFOA was selectively removed from 200 μg/L to 1.2 μg/L with 1000-fold humic acid interference. This work presents a strategy for efficient and selective PFOA removal by precisely modulating its adsorption configuration.
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NEW JOURNAL OF CHEMISTRY
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2025
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IF 2.5
Xiang Gao,Jiajia Zhao,Hao Song,Xintong Zhou,Yuehua Deng,Jiali Liu,Yanrui Li
Graphitic carbon nitride (CN), a promising photocatalyst for CO2 reduction, suffers from inefficient light harvesting and sluggish charge separation dynamics, which severely restricts its application. Ionic liquids (ILs) have been used for the assisted preparation of photocatalysts, thus effectively altering their geometric and electronic properties. Herein, the 1-butyl-3-methylimidazolium hexafluorophosphate ([Bmim]PF6) IL was introduced as a modifier to successfully construct a P- and F-co-doped porous CN catalyst via simple calcination of the IL and urea without any organic solvents and templates. The optimized catalyst exhibited an enhanced photocatalytic activity for CO2 reduction via gas–solid mode under visible light irradiation, achieving CO and CH4 evolution rates of 39.9 and 2.63 μmol g−1 h−1 (CO selectivity of 94%), which were 7.8 and 4.8 times higher than those of pristine CN, respectively. PFCN also demonstrated excellent reusability and stability. Comprehensive characterization revealed that the strategy of doping of P and F atoms significantly enlarged the surface area, improved CO2 adsorption, broadened visible-light harvesting, and accelerated charge transfer and separation efficiency. This work highlights the potential of ILs as multifunctional agents for designing high-performance doped CN photocatalysts.
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Journal of Environmental Chemical Engineering
·
2025
·Vol. 13
·期 6
·120116
·
IF 7.2
Wujian Zhang,Yongchao Zhao,Jidong Wang,Kangjun Wang,Hangjia Shen,Zongjian Liu,Wenfeng Han,Ying Li,Aimin Chen,Haodong Tang
The dehydrofluorination of 1,1-difluoroethane (R152a) is a Lewis acid–catalyzed reaction in which both catalytic activity and stability are governed by the coordination and acidity of aluminum sites. In this work, a mechanochemical fluorination strategy was developed to construct a partially fluorinated Al-based catalyst with tunable acid properties. By controlling the fluorine-aluminum ratio during ball milling, the in situ formation of AlF 2 (OH) was achieved, serving as a structural stabilizer and electronic modulator. The coexistence of F-Al-O units and unsaturated Al centers provides medium-strength Lewis acid sites, which favor selective C-F bond activation while suppressing side reactions. Comprehensive characterizations (XRD, XPS, 27 Al NMR, and NH 3 -TPD) confirmed that the defect-related F-Al-O structure maintains structural integrity and balanced acidity during reaction. Consequently, the optimized catalyst exhibits excellent activity, selectivity, and long-term stability in R152a dehydrofluorination.
研究领域:
催化化学
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材料化学
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无机化学
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化学工程
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ACS Applied Materials & Interfaces
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2025
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IF 8.2
Li-Qian Cheng,Xinyuan Xie,Kai Chen,Xuxia Hao,Min Jiang,Yanping Tang,Haijiao Xie,Zhaoyin Wen
The pursuit of high-power and prolonged service life lithium ion batteries has driven extensive research into novel anode materials. Titanium niobium oxide (TNO) has arisen as a prospective contender due to its high reaction potential and low strain performance, which effectively avoid side reactions and suppress the formation of lithium dendrite. However, challenges such as poor conductivity and structural instability during high-rate cycling have hindered their practical application. In this study, high-performance V5+ and F– codoping of the TiNb2O7 (V/F-TNO) anode is obtained by a facile solvothermal method and exhibits outstanding electrochemical properties in both liquid- and solid-state batteries. Under the synergistic effect of V5+ and F– doping, impurity bands and additional oxygen vacancies are introduced to enhance the conductivity, while the particle size is reduced, which significantly improves its rate performance. In addition, a more stable crystal structure improves its cycle life. Thereby, the V/F-TNO anode displays a high reversible capacity of 322.8 mAh g–1 at 0.1 C and a superior rate capability of 222.6 mAh g–1 at 20 C. During long-term cycles, the V/F-TNO anode presents an outstanding discharge capacity of 178.5 mAh g–1 after 1500 cycles at 10 C, equivalent to a capacity retention rate of 78.2%. LiFePO4 (LFP)|Li1.3Al0.3Ti1.7(PO4)3 composite polymer electrolyte (LATPCPEs)|V/F-TNO solid-state batteries (SSBs) are assembled and display ideal capacities of 129.3 mAh g–1 at 0.2 C and 83.5 mAh g–1 at 5 C. Moreover, they retain an extraordinary capacity of 101.7 mAh g–1 after 200 cycles at 0.5 C, corresponding to a high-capacity retention ratio of 86%. This study demonstrates that the V/F-TNO anode is a promising candidate for high-power liquid and solid-state batteries.
研究领域:
材料科学
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电化学
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储能
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电池技术
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DYES AND PIGMENTS
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2017
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IF 3.473
H.C. Ma,Z.M. Yang,H.Y. Cao,L. Lei,Z.Q. Lei
The development of CO 2 -active fluorescent sensors is paramount to the climate assessment. And also, because of the biological and environmental importance, trace detection F − is a great challenge task but very necessary for human daily life. This paper presented a water-soluble fluorescent sensor fabricated by triphenylamine derivative of NBTA 3− and quaternary ammonium salt (CTAC), which was further explored as a green and multi-functional sensing platform, and demonstrated excellent CO 2 response ability and trace amount of F − recognition with obvious visualized exhibitions. Especially, our research result has potential application in the CO 2 sensing by contact and vapor modes. Both of techniques exhibited reliable and sensitive and quick CO 2 sensing capability. We hope our research result is of real-time monitoring CO 2 in our surroundings.
研究领域:
分析化学
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环境科学
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材料科学
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Surfaces and Interfaces
·
2025
·
IF 6.3
Kai Yang,Junhao Wang,Dian Yu,Pengqiuyue Pu,Hang Li,Zihao Chen,Yangyang Tang,Zhao Fang
As mineral resources are developed and exploited, the proportion of low-grade zinc ore increases. The concentrations of F - exceeding the optimal range may pose a risk to zinc hydrometallurgy . In the present research, Al 2 O 3 -ZnO microspheres (AZO) characterized by a substantial specific surface area were synthesized through a hydrothermal-roasting technique and applied in industrial zinc sulphate fluoride removal. The optimal adsorption conditions for AZO and the underlying adsorption mechanism were investigated. The results indicated that the adsorption at 12 g·L -1 dosage, original pH=5.32 of the solution and 323 K for 75 min, when the fluoride concentration was reduced to below 50 mg·L -1 , the fluoride removal percentage reached 73.32 %, and the adsorption capacity was 8.55 mg·g -1 . Kinetic studies revealed that AZO exhibited surface inhomogeneity, functioning as a heterogeneous adsorbent, with the fluoride adsorption process being predominantly chemical in nature. The isotherm model suggested that the removal process was characterized by homogeneous adsorption of a monomolecular layer, with a theoretical maximum adsorption capacity of AZO estimated at 9.479 mg·g -1 . FT-IR and XPS analyses demonstrated that the defluorination process occurs through ion exchange between F - and -OH, as well as the formation of Zn/Al-F complexes. Consequently, AZO present a novel approach for developing an effective adsorbent for defluorination in industrial ZnSO 4 solutions.
研究领域:
环境化学
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湿法冶金
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材料科学
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吸附技术
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废水处理
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