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Science Bulletin · 2024 · IF 18.8

Hybrid ion/electron interfacial regulation stabilizes the cobalt/oxygen redox of ultrahigh-voltage lithium cobalt oxide for fast-charging cyclability

Zhihong Bi,Anping Zhang,Gongrui Wang,Cong Dong,Pratteek Das,Xiaoyu Shi,Zhong-Shuai Wu

High-voltage and fast-charging LiCoO 2 (LCO) is key to high-energy/power-density Li-ion batteries. However, unstable surface structure and unfavorable electronic/ionic conductivity severely hinder its high-voltage fast-charging cyclability. Here, we construct a Li/Na-B-Mg-Si-O-F-rich mixed ion/electron interface network on the 4.65 V LCO electrode to enhance its rate capability and long-term cycling stability. Specifically, the resulting artificial hybrid conductive network enhances the reversible conversion of Co 3+/4+ /O 2−/ n − redox by the interfacial ion–electron cooperation and suppresses interface side reactions, inducing an ultrathin yet compact cathode electrolyte interphase. Simultaneously, the derived near-surface Na + /Mg 2+ /Si 4+ -pillared local intercalation structure greatly promotes the Li + diffusion around the 4.55 V phase transition and stabilizes the cathode interface. Finally, excellent 3 C (1 C = 274 mA g −1 ) fast charging performance is demonstrated with 73.8% capacity retention over 1000 cycles. Our findings shed new insights to the fundamental mechanism of interfacial ion/electron synergy in stabilizing and enhancing fast-charging cathode materials.

研究领域: 材料科学 · 电化学 · 能源存储
✓ 已验证 DOI 高影响因子
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JOURNAL OF ALLOYS AND COMPOUNDS · 2025 · IF 6.3

Supercritical Hydrothermal Synthesis, Magnetism, and Rotating Magnetocaloric Effect of Fluorocarbonates K4RE2(CO3)3F4 (RE = Ce, Pr, Nd, Sm, Eu, Tb, and Dy) with Rare-earth Dimers RE2O12F4

Jingfang Tong,Weijie Lin,Ruixin Guo,Zhongzheng Deng,Haitao Zhou,Shu Guo,Xiaojun Kuang

Strong magnetic anisotropy in low-dimensional magnets leads to a significant rotating magnetocaloric effect, presenting new opportunities for the exploration of more efficient and streamlined refrigeration systems. In this study, we have successfully synthesized a series of centimeter-scale rare-earth-containing fluorocarbonates, K 4 RE 2 (CO 3 ) 3 F 4 ( RE = Ce, Pr, Nd, Sm, Eu, Tb, and Dy) through a supercritical hydrothermal method, featuring unique RE 2 O 12 F 4 magnetic dimers. The above materials' fundamental magnetism has been systematically investigated, and no long-range magnetic transitions were captured above 1.8   K. Based on the low-temperature specific heat results, the long-range magnetic ordering was found around 0.84   K and 0.97   K for K 4 Tb 2 (CO 3 ) 3 F 4 and K 4 Dy 2 (CO 3 ) 3 F 4 , respectively. Furthermore, the anisotropic magnetism of K 4 Tb 2 (CO 3 ) 3 F 4 and K 4 Dy 2 (CO 3 ) 3 F 4 reveals significant magneto-crystalline anisotropy, with the magnetic field ( B ) aligned along the RE 2 O 12 F 4 magnetic dimer, which acts as the easy magnetic axis. The maximum rotating field entropy change, − Δ S R max for K 4 Tb 2 (CO 3 ) 3 F 4 reaches approximately 9   J   kg -1 K -1 around 17   K, while for K 4 Dy 2 (CO 3 ) 3 F 4 , it is approximately 5.5   J   kg -1 K -1 near 11   K, both under a 7   T field applied along the c -axis. These findings highlight the potential of these compounds for magnetic refrigeration applications through a rotating crystallographic direction.

研究领域: 材料科学 · 物理学
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JOURNAL OF HAZARDOUS MATERIALS · 2023 · IF 13.6

Efficient removal of petroleum hydrocarbons from soil by percarbonate with catechin-promoted Fe(III)/Fe(II) redox cycling: Activation of ferrous and roles of ·OH and ·CO3-

Tong Zhang,Yuan Chen,Tao Wang,Chang Liu,Dan He,Bin Liu,Yuanyuan Liu

Advanced oxidation processes are widely used to remove petroleum hydrocarbons from soil, but usually consume large quantities of ferrous and acidify the soil. This study tested an advanced oxidation approach based on percarbonate in laboratory experiments. It removed 88% petroleum hydrocarbons in soil with a pH increase from 8.2 to 10.2. ·OH and ·CO 3 - were the main reactive species, and degraded 41% and 37% PHCs from soil respectively. The o-dihydroxybenzene structure in catechin was found to reduce ferric to ferrous, and prolong the generation of ·OH from 120 s to over 1800 s. The petroleum hydrocarbons were degraded to intermediates including alkanes and olefins through hydrogen-abstraction by ·OH and ·CO 3 - , and by dimerization and β-scission of alkyl radicals. These intermediates were then oxidized to CO 2 and H 2 O by ·OH and ·CO 3 - . The main residual intermediates in the soil were low-molecular-weight n-alkanes and branched alkanes, and they were found to inhibit the growth of oats ( Avena sativa L. ) much less than the original petroleum hydrocarbons. These findings provide a fundamental basis for designing effective technologies which use percarbonate to remove organic pollutants .

研究领域: 环境科学 · 土壤修复
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SEPARATION AND PURIFICATION TECHNOLOGY · 2025 · IF 9

A novel CoOOH/PTFE catalytic membrane for persulfate activation to sustainably degrade 17α-ethinylestradiol: Oxygen vacancies promote synergistic pathways of radical and nonradical mechanisms

Chuan-hua Yang,Yujie Cui,Zhengxi Chen,Yiluo Hu,Xuejun Pan,Siping Ji,Feng-zhi Jiang

Peroxymonosulfate (PMS)-based advanced oxidation processes (PMS-AOPs) currently face issues regarding transition-metal ion valence conversion and practical application in water treatment. To address them, we synthesized a CoOOH catalyst with a unique three-dimensional porous flower-like morphology for PMS activation to degrade 17α-ethinylestradiol (EE2) in wastewater. By adding PMS to CoOOH in small amounts, 95.68 % of EE2 (3 mg/L) was degraded within 9 min. The catalytic efficiency of CoOOH was considerably higher than those of a material synthesized via the conventional precipitation method and commercial Co 3 O 4 . CoOOH also exhibited a wide pH adaptability range, good cyclic stability, and a low cobalt ion leaching concentration. It demonstrated excellent PMS activation performance, chemical stability, and safety. Mechanistic studies revealed that numerous surface hydroxyl groups and abundant oxygen vacancies in CoOOH facilitated efficient electron transfer, rapidly achieved the Co 3+ /Co 2+ redox cycle, and generated a large amount of highly oxidative nonradical ( 1 O 2 ) and radical (•O 2 − ) species, thereby efficiently degrading organic pollutants. Finally, by combining PMS-AOPs with membrane separation, a CoOOH/PTFE membrane–PMS system was fabricated for continuous EE2 degradation in lake water; it could operate continuously for 24 h in treating 1.25 L of Dianchi Lake water (Kunming, Yunnan) containing 3-mg/L EE2 while maintaining an EE2 removal rate of 92.35 %. The synthesized CoOOH/PTFE catalytic membrane facilitated transition-metal ion redox cycling and efficient organic-pollutant degradation as well as enabled convenient catalyst recovery, thereby reducing secondary pollution in the degradation process. Overall, this research provides a feasible strategy for the practical application of PMS-AOPs.

CAS / MDL: 1415-93-6 70693-62-8
研究领域: 环境科学 · 化学工程 · 催化 · 水处理技术 · 材料科学
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NEW JOURNAL OF CHEMISTRY · 2019 ·Vol. 44 ·期 4 ·1245-1252 · IF 3.069

A novel cobalt doped MOF-based photocatalyst with great applicability as an efficient mediator of peroxydisulfate activation for enhanced degradation of organic pollutants

Shi-Wen Lv,Jing-Min Liu,Ning Zhao,Chun-Yang Li,Zhi-Hao Wang,Shuo Wang

The issue of environmental pollution is currently more and more serious, and developing an effective method with universal applicability for removing various contaminants is pretty necessary. Herein, a novel photocatalyst denoted as Co-doped MIL-53-NH2(Fe : Co 4 : 1) was constructed via a feasible solvothermal method, which served as an efficient mediator to activate peroxydisulfate for degrading various organic pollutants. Results from the current work indicated that doping Co with an appropriate proportion could enhance the optical absorption intensity of MIL-53-NH2 and reduce the band gap. Furthermore, a Co ion acting as a mediator could facilitate the charge transfer through a Co3+/Co2+ redox pathway, and thereby suppress the recombination of photogenerated electron–hole pairs. More interestingly, the Co-doped MIL-53-NH2 exhibited excellent and extensive degradation abilities for various organic pollutants including bisphenol A (BPA), antibiotics and organic dyes in the presence of peroxydisulfate (PS) under visible light irradiation. It was also found that ˙OH and SO4−˙ were the major contributors to the catalytic process. Total organic carbon (TOC) analysis indicated that the majority of the contaminants were degraded into CO2 and H2O. Even in the real samples, the developed Co-doped MIL-53-NH2/PS/solar system still possessed excellent performance for the degradation of BPA. Possible photocatalytic mechanisms and the kinetics were also investigated. Besides, the Co-doped MIL-53-NH2 had good catalytic reusability and stability. To sum up, this study provides a promising approach for removing organic pollutants from wastewater.

研究领域: 环境科学 · 材料科学 · 化学工程 · 光化学
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ANALYTICA CHIMICA ACTA · 2023 · IF 6.2

Determination of uric acid in serum by SERS system based on VO-MnCo2O4/Ag nanozyme

Yaoyu Tan,Mengyao Qi,Huan Jiang,Baihui Wang,Xia Zhang

The level of uric acid is crucial to human health. Octahedral oxygen vacancy MnCo 2 O 4 /Ag (V O -MnCo 2 O 4 /Ag) nanozyme was successfully prepared by simple hydrothermal, calcination and self-reduction methods. V O -MnCo 2 O 4 /Ag nanozyme is rich in Mn 2+ /Mn 3+ and C O 2+ /C O 3+ redox electron pairs, large specific surface area and oxygen vacancies. V O -MnCo 2 O 4 /Ag nanozyme showed high uricase-like activity and peroxidase-like activity. At the same time, the SERS signal of the detected molecule could be significantly enhanced after the catalytic reaction of the V O -MnCo 2 O 4 /Ag nanozyme. The K m values of V O -MnCo 2 O 4 /Ag nanozyme for H 2 O 2 and TMB were 0.04 mM and 0.027 mM respectively. Based on the uric acid oxidase-like and peroxidase-like activities of V O -MnCo 2 O 4 /Ag, we developed a label-free, sensitive, and reliable SERS uric acid detection system. The detection linear range of uric acid is 0.01 μM–1000 μM and the detection of limit is 7.8 × 10 −9  M. The results show that the sensing system has good accuracy, sensitivity, selectivity , and stability. It can be applied to the determination of samples under different conditions. This study provides profound insights into the design of enzyme-like activity regulation and SERS properties regulation of nanozymes, provides guidance for the study of reaction kinetics and catalytic mechanism of nanozymes, and has broad application prospects in the field of nanozymes and SERS sensing analysis.

研究领域: 纳米技术 · 分析化学 · 生物化学 · 材料科学 · 医学诊断
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