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CHINESE CHEMICAL LETTERS · 2023 · IF 9.1

Dual-additives enable stable electrode-electrolyte interfaces for long life Li-SPAN batteries

Zhenqiang Guo,Huicong Yang,Qian Wei,Shengjun Xu,Guangjian Hu,Shuo Bai,Feng Li

ABSTRACT Sulfurized polyacrylonitrile (SPAN) is proposed as a promising cathode material for lithium sulfur batteries. However, the continuous side reactions at the electrolyte-electrode interfaces as well as the slow redox kinetics of SPAN cathode deteriorate the electrochemical performance. In this study, an electrolyte with dual-additives comprising 2-fluoropyridine (2-FP) and lithium difluorobis (oxalato) phosphate (LiDFBOP) was used to improve the performance of Li||SPAN cells. 2-FP has a lower lowest occupied molecular orbital energy than that of the solvents in the electrolyte, leading to its prior reduction. A LiF-rich film can be formed on the electrode, effectively improving the stability of the electrolyte-electrode interfaces and prolonging the life. Simultaneously, LiDFBOP could form an electrolyte-electrode interface film containing a large amount of Li x PO y F z species, compensating for the kinetic deterioration caused by the lower ionic conductive of LiF formed at the electrolyte-electrode interface. Hence, an electrode-interface film with good chemical stability and high Li + transport was established by LiF and Li x PO y F z -rich species. The Li||SPAN cell with the electrolyte containing dual-additives demonstrates an excellent capacity retention of 97.5% after 200 cycles at 1.0 C, 25 °C, comparing to 56.2% capacity retention without additives. Moreover, the rate capacities of cells with dual-additives can reach 1128.1 mAh/g at 5 C, comparing to only 813.5 mAh/g using electrolyte without additives. Our results shown that the dual-additives in electrolyte provide a promising strategy for practical application of lithium sulfur batteries with SPAN cathodes.

研究领域: 材料科学 · 电化学 · 能源存储
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ENVIRONMENTAL SCIENCE & TECHNOLOGY · 2024 · IF 10.8

Controllable Pyridine N-Oxidation–Nucleophilic Dechlorination Process for Enhanced Dechlorination of Chloropyridines: The Cooperation of HCO4– and HO2–

Ying Chen,Lei Tian,Wen Liu,Yi Mei,Qiu-Ju Xing,Yi Mu,Ling-Ling Zheng,Qian Fu,Jian-Ping Zou,Daishe Wu

Dechlorination of chloropyridines can eliminate their detrimental environmental effects. However, traditional dechlorination technology cannot efficiently break the C–Cl bond of chloropyridines, which is restricted by the uncontrollable nonselective species. Hence, we propose the carbonate species-activated hydrogen peroxide (carbonate species/H2O2) process wherein the selective oxidant (peroxymonocarbonate ion, HCO4–) and selective reductant (hydroperoxide anion, HO2–) controllably coexist by manipulation of reaction pH. Taking 2-chloropyridine (Cl–Py) as an example, HCO4– first induces Cl–Py into pyridine N-oxidation intermediates, which then suffer from the nucleophilic dechlorination by HO2–. The obtained dechlorination efficiencies in the carbonate species/H2O2 process (32.5–84.5%) based on the cooperation of HCO4– and HO2– are significantly higher than those in the HO2–-mediated sodium hydroxide/hydrogen peroxide process (0–43.8%). Theoretical calculations confirm that pyridine N-oxidation of Cl–Py can effectively lower the energy barrier of the dechlorination process. Moreover, the carbonate species/H2O2 process exhibits superior anti-interference performance and low electric energy consumption. Furthermore, Cl–Py is completely detoxified via the carbonate species/H2O2 process. More importantly, the carbonate species/H2O2 process is applicable for efficient dehalogenation of halogenated pyridines and pyrazines. This work offers a simple and useful strategy to enhance the dehalogenation efficiency of halogenated organics and sheds new insights into the application of the carbonate species/H2O2 process in practical environmental remediation.

研究领域: 环境科学 · 化学工程
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Advanced Energy and Sustainability Research · 2025 · IF 5.7

Electric and Temperature Field-Modulated Periodic Repair of the Electrode/Electrolyte Interface toward Long Cycle Stability of Low-Temperature Li-Ion Batteries

Zhenqiang Guo,Chengling Yang,Yu Fan,Yancai Zhang,Haolun Zou,Yukun Yan,Hongbin Zhang,Zhenhui Liu,Zinuo Chen,Sitong Peng,Ziyi Dang,Hengyi Li

This study tackles the poor low-temperature performance of lithium-ion batteries through a synergistic strategy that modulates electrode–electrolyte interfacial chemistry via coordinated temperature and electric field control. The research uncovers distinct interfacial evolution mechanisms: at −20 °C, strengthened solvent–Li + affinity causes solvation structure reorganization and interfacial deterioration, whereas at 25 °C, enhanced anion participation promotes formation of stable inorganic-rich interphases. Reduced electric field intensity further facilitates the construction of stable interfaces. Based on these findings, a variable-temperature constant-current cycling protocol with periodic room-temperature activation is developed. This approach effectively restores stable interfaces and substantially minimizes polarization, enabling commercial lithium iron phosphate (LFP) batteries to maintain nearly 100% initial capacity after 150 cycles at −20 °C—significantly surpassing conventional strategies (80.4% retention). Notably, this optimization method regulates interfacial chemistry through external field parameters without electrolyte formulation changes, demonstrating both theoretical innovation and engineering practicality. This work provides a novel paradigm for low-temperature battery design by decoupling interfacial regulation from material modification.

CAS / MDL: 372-48-5
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APPLIED ORGANOMETALLIC CHEMISTRY · 2022 ·Vol. 36 ·期 7 ·e6759 · IF 4.072

Synthesis, characterization, and antitumor biological evaluation of novel fluorine-containing platinum (IV) complexes

Lihua Chen,Pan Zhao,Jing Yang,Xiali Liao,Bo Yang,Chuanzhu Gao

A series of antitumor platinum (IV) complexes based on ammonia and fluoropyridine carrier groups with biotin and chloride ions as axial groups have been designed and synthesized in this paper. The structures of platinum (IV) complexes were fully characterized by 1 H NMR, ESI-MS, and IR. Such Pt (IV) complexes have certain tumor targeting properties, and the Pt (II) complexes released in the reducing microenvironment could combine with DNA. Compared with cisplatin, complexes S3 and S4 exhibited similar cytotoxicity against SW480, HCT116, and HepG2 cancer cell lines according to in vitro antitumor activity evaluation. Particularly, Complex S2 showed 1.5–3.0 times higher cytotoxicity than cisplatin and picoplatin against selected cell lines. According to the structure–activity relationship, the introduction of fluorine atoms and axial chloride has an important influence on the strong cytotoxic activity of Pt (IV) complex. In addition, the axial biotin molecule increased the targeting of the complex to tumor cells. Overall, the novel fluorine-containing Pt (IV) complex S2 is an attractive antitumor lead compound with further research value.

研究领域: 药物化学 · 肿瘤学 · 生物无机化学
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