CERAMICS INTERNATIONAL
·
2021
·
IF 4.527
Yubin Wen,Yufu Liu
Typical high-entropy fluorite oxides with five metal cations have exhibited improved thermomechanical properties . In this work, we have successfully prepared single-phase high-entropy (Zr 0.2 Ce 0.2 Hf 0.2 Y 0.2 Al 0.2 )O 2-δ fluorite oxides through the combination of sol-gel method and calcination , using metal nitrate/chloride, citric acid and absolute ethanol as the primary raw materials. A series of characterizations were employed for chemical, morphological and structural analysis of the calcined products. The five cationic elements were shown to be uniformly distributed in the nearly pure fluorite oxide without apparent segregation at the micro/nano-meter scales after 1500 °C calcination. Annealing and water quenching within the test temperature range did not witness any appreciable phase transition. It is revealed that the concentration of Ce 3+ in Ce ions reaches 33.84% and δ is equal to 0.234, yielding a nominal composition of (Zr 0.2 Ce 0.2 Hf 0.2 Y 0.2 Al 0.2 )O 1.766 . Cation and anion configurational entropy were found to be 1.609 R and 0.722 R, respectively, where R is the ideal gas constant, for a sum of the total configurational entropy of 2.331 R in the high-entropy system. Line defects inside the crystals and 3 types of crystalline boundary structures have been observed and identified among the mostly atomically sharp grain boundaries.
研究领域:
材料科学
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化学
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DOI
高影响因子
ANALYTICAL AND BIOANALYTICAL CHEMISTRY
·
2022
·Vol. 414
·期 29
·8309-8315
·
IF 4.478
Zhang Huixin,Du Lin,Wei Zhihao,Wang Xuemei,Sojic Neso,Zhou Xin,Wang Zonghua
Electrochemiluminescence (ECL) of luminol is a well-established methodology in analytical chemistry and bioimaging. Developing novel strategies to enhance the ECL signal of this model emitter is a challenging but rewarding task. In this work, we introduced the high-intensity focused ultrasound (HIFU), as a pretreatment means and a non-invasive way to trigger and boost the ECL signal with a 40-fold significant enhancement in the luminol-O 2 system without the addition of exogenous co-reactants. The superoxide anion (O 2 −• ) generated in situ by HIFU was the key initiator for boosting the ECL emission as demonstrated in this study for the first time. This promising co-reactant-free strategy could find potential applications for ultrasensitive ECL detection in the analysis of complex biological entities. Graphical abstract
研究领域:
分析化学
·
生物成像
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超声技术
·
生物分析
✓ 已验证
DOI
PubMed
高影响因子
Journal of the American Chemical Society
·
2024
·
IF 14.4
Yao Song,Xiao Yang,Huan Liu,Suxia Liang,Yafeng Cai,Wenqiang Yang,Kaixin Zhu,Liang Yu,Xiaoju Cui,Dehui Deng
Electrochemical conversion of CH4 to easily transportable and value-added liquid fuels is highly attractive for energy-efficient CH4 utilization, but it is challenging due to the low reactivity and solubility of CH4 in the electrolyte. Herein, we report a high-pressure electro-Fenton (HPEF) strategy to establish a hetero-homogeneous process for the electrocatalytic conversion of CH4 by O2 at room temperature. In combination with elevation of reactant pressure to accelerate reaction kinetics, it delivers an unprecedented HCOOH productivity of 11.5 mmol h–1 gFe–1 with 220 times enhancement compared to that under ambient pressure. Remarkably, an HCOOH Faradic efficiency of 81.4% can be achieved with an ultralow cathodic overpotential of 0.38 V. The elevated pressure not only promotes the electrocatalytic reduction of O2 to H2O2 but also increases the reaction collision probability between CH4 and •OH, which is in situ generated from the Fe2+-facilitated decomposition of H2O2.
研究领域:
环境科学
·
电化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nature Chemistry
·
2026
·
IF 24.5
Wang Nan,Cui Chunyu,Xu Runjing,Wang Xiaofang,Wu Chaoxin,Pu Qihao,Wang Wentao,Cao Yongjie,Liao Mochou,Wang Fengmei,Wang Yonggang,Chen Yuhui,Ji Xiao,Xia Yongyao,Wang Fei
Magnesium–oxygen (Mg–O 2 ) batteries are considered promising candidates for next-generation energy storage systems due to their high specific energy, low cost and intrinsic safety. However, poor rechargeability remains a critical barrier, largely due to the lack of suitable electrolytes and undesired irreversible cathode reactions. Here we report a rechargeable non-aqueous Mg–O 2 battery enabled by a tailored electrolyte featuring a cage-like Mg 2+ solvation environment. We find that varying ether solvent chain lengths, alongside a tridentate chelating agent, can act coordinately to form a dynamic solvation microreactor. This solvation environment is consistent with the reversible formation of nanocrystalline magnesium peroxide at the cathode and remains compatible with reversible magnesium plating/stripping. The resulting Mg–O 2 batteries achieve a high initial discharge voltage approaching 2.0 V, an ultralow overpotential of 0.35 V, a remarkable round-trip energy efficiency of 80% and over 450 stable cycles. These results highlight a solvation-structure-guided strategy for enabling rechargeable Mg–O 2 batteries and potentially other multivalent metal–air systems.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
MATERIALS CHEMISTRY AND PHYSICS
·
2025
·
IF 4.7
Qingfang Jiang,Wujian Zhang,Weijian Ge,Yiping Jin,Wenfeng Han,Ying Li,Haodong Tang
Sintering deactivation of loaded precious metal catalysts is a pressing issue in the field, significantly reducing catalyst activity. Among them, the redispersion of carbon-loaded precious metal catalysts under a high-temperature atmosphere suffers from the problem of carbon carriers being prone to carbonization. In this study, the sintered PdZn/AC catalysts could be redispersed at low temperatures by adding the additive Zn. Combined with TEM, XRD, XPS, and other characterization means, it was found that the main reason for the redispersion of the sintered catalysts was that the Zn additive could form an alloy with Pd, which promoted the formation of high-valent Pd species, which exfoliated into small particles by oxidation in the O 2 –CO atmosphere. In addition, the factors that influenced the process (Zn content, redispersion temperature, treatment time, and number of treatments) were investigated using the controlled variable method. The present work presents a new idea for recycling sintered precious metal catalysts.
研究领域:
催化化学
·
材料科学
·
化学工程
·
表面化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMOSPHERE
·
2024
·
IF 8.1
Chunyun Gu,Jiabin Li,Wei Zhou,Jiayi An,Liting Tian,Feng Xiong,Wenbo Fei,Yangfan Feng,Jie Ma
1,2,3-Trichloropropane (TCP) is an emerging groundwater pollutant, but there is a lack of reported studies on the abiotic natural attenuation of TCP by iron minerals. Furthermore, perturbation by O 2 is common in the shallow subsurface by both natural and artificial processes. In this study, natural magnetite was selected as the reactive iron mineral to investigate its role in the degradation of TCP under O 2 perturbation. The results indicated that the mineral structural Fe(II) on magnetite reacted with dissolved oxygen to generate O 2 − · and HO·. Both O 2 − · and HO· contributed to TCP degradation, with O 2 − · playing a more important role. After 56 days of reaction, 66.7% of TCP was completely dechlorinated. This study revealed that higher magnetite concentrations, smaller magnetite particle sizes, and lower initial TCP concentrations favored TCP degradation. The presence of <10 mg/L natural organic matter (NOM) did not affect TCP degradation. These findings significantly advance our understanding of the abiotic natural attenuation mechanisms facilitated by iron minerals under O 2 perturbation, providing crucial insights for the study of natural attenuation.
研究领域:
环境科学
·
化学
✓ 已验证
DOI
高影响因子
Journal of Physical Chemistry C
·
2024
·
IF 3.3
Wan Zhong,Yizhuo Fu,Xueqian Chen,Chao Lu
Electrochemiluminescence (ECL) of the luminol-dissolved O2 system has been applied in many fields, but the role of reactive oxygen species (ROS) in potential-resolved ECL of luminol-dissolved O2 remains ambiguous due to the complexity of the ROS production and the difficulty in detecting ROS. In this work, the function of ROS in potential-dependent luminol-O2 ECL was investigated in detail. Interestingly, the four ECL peaks were observed in the potential-resolved ECL profiles, including a cathodic ECL peak at −0.5 V (ECL-1), two anodic ECL peaks at 0.45 V (ECL-2) and 1.3 V (ECL-3), and a broad and flat peak starting from 1.11 V and ending at 0.35 V (ECL-4, a secondary peak) on the reverse scan backward from upper potentials. The impact of ROS on the different ECL channels was investigated. It was found that superoxide radical (O2•–) could promote all of the above four ECL peaks, while hydroxyl radical (HO•) could only facilitate ECL-1, ECL-3, and ECL-4. Additionally, pathways of all ECL peaks were proposed. The investigation on the role of ROS in potential-resolved ECL of luminol-dissolved O2 will guide the rational regulation and potential applications of luminol ECL in various fields.
研究领域:
分析化学
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电化学
·
生物分析
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Wenjing Yang,Yibing Ji,Chenhang Ding,Xujie Zhang,Wurikaixi Aiyiti,Chongxian He,Cijun Shuai
Reactive oxygen species (ROS) mediated tumor therapeutic strategies have been extensively studied. However, its effectiveness in eliminating tumor cells is inevitably restricted by the hypoxia or the insufficient hydrogen peroxide (H 2 O 2 ) content. To fundamentally address these challenges, an O 2 -independent and stimuli-responsive nanosystem (named CuS@PMS) is ingeniously constructed by loading peroxymonosulfate (PMS: HSO 5 − ) into hollow mesoporous copper sulfide (CuS) to mediate the generation of sulfate radicals (SO 4 − ). The CuS@PMS was then introduced into polycaprolactone (PCL) to prepare into breast meshes by selective laser sintering. Specifically, the released Cu 2+ ions combining with the photothermal property of CuS synergistically activate PMS, ensuring the cascade amplification of SO 4 − . Unlike conventional ROS, the production of SO 4 − independent on the content of O 2 and H 2 O 2 in the tumor microenvironment, characterizing a longer half-life and faster reaction rate, thereby possessing more advantages in antitumor. The results showed that the SO 4 − yield of PCL/CuS@PMS group significantly higher than that of PCL/PMS group, especially under near-infrared (NIR) light. Moreover, the antitumor efficiency of PCL/CuS@PMS + NIR group was 43 % higher than that of PCL/PMS group in an O 2 -independent manner. The study provided a more efficient, highly adaptable and versatile approach for tumor treatment.
研究领域:
生物医学工程
·
纳米技术
·
肿瘤治疗
✓ 已验证
产品关联
DOI
高影响因子
Nature Synthesis
·
2025
·
IF 20
Wang Ruizhao,Dai Jie,Zhao Long,Hu Zhiwei,Chen Chien-Te,Kuo Chang-Yang,Zhan Guangming,Shi Yanbiao,Wang Jiaxian,Zou Yunjie,Xu Mingkai,Zou Xingyue,Zheng Qian,Zhou Bing,Wang Kaiyuan,Zhao Rui,Zhang Yan,Shen Yunhao,Yao Yancai,Zhang Lizhi
Electrochemical O 2 activation offers a green approach for efficient synthesis of singlet oxygen ( 1 O 2 ). However, it is commonly determined by adsorption-dependent O 2 activation and transformation and can suffer from the sluggish desorption of surface-bound *OOH. Here we report an adsorption-independent O 2 activation pathway for 1 O 2 electrosynthesis via an O 2 mono-hydrogenation process on compressive-strained rutile TiO 2 (CSR-TiO 2 ). This CSR-TiO 2 achieved an 1 O 2 generation rate of 148.26 μmol l −1 min −1 with near 100% Faradaic efficiency, outperforming the strain-free counterpart (35.97 μmol l −1 min −1 ) and other previously reported materials. Such superior performance of CSR-TiO 2 stemmed from compressive strain, which can suppress the formation of reductive unsaturated sites for the O 2 adsorption and enhance the reductive ability of atomic hydrogen (H*), favouring the O 2 mono-hydrogenation pathway and bypassing the traditional surface-bound *OOH desorption pathway. The generated 1 O 2 could be utilized for the selective oxidation of thioanisole and its derivatives, offering a promising strategy for green organic synthesis.
研究领域:
材料科学
·
电化学
·
绿色合成
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Energy Materials
·
2022
·
IF 6.959
Zhi Gu,Xing Xin,Jing Yang,Dingcheng Guo,Shujiao Yang,Jinghua Wu,Yong Sun,Xiayin Yao
The practical application of lithium–oxygen (Li–O2) batteries is limited by the formation of lithium dendrites and the use of flammable and unstable organic liquid electrolytes, which would cause safety issues and poor cycling stability. Herein, we present a bilayer organic/inorganic hybrid solid-state electrolyte to improve the safety and enhance the electrochemical performance of Li–O2 batteries. Si-doped NASICON-type electrolyte Li1.511Al0.5Ge1.5Si0.01P2.99O12 (LAGP-Si) serves as an inorganic rigid backbone to guarantee high ionic conductivity and provide a barrier between active oxygen and lithium anode. Poly(ethylene glycol) methyl ether methacrylate (PEGMEM) is chosen as a polymer buffer layer due to its compatibility with lithium. Benefiting from the synergistic effect between LAGP-Si and PEGMEM, the obtained hybrid electrolyte exhibits high ionic conductivity and good stability against lithium anode. Consequently, the polarization of the Li symmetric cell is dramatically reduced by replacing pure LAGP-Si with a bilayer hybrid electrolyte. The solid-state Li–O2 batteries employing a PEGMEM@LAGP-Si electrolyte deliver a greater initial discharge–charge capacity of 7.3 mAh cm–2 and enhanced cyclic performance for 39 cycles with a restricted capacity of 0.4 mAh cm–2. The present work delivers a promising category of hybrid solid electrolytes for high-performance solid-state Li–O2 batteries.
研究领域:
材料科学
·
电化学
·
储能
·
固态电池
✓ 已验证
DOI
高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
·
2019
·Vol. 25
·期 12
·3112-3118
·
IF 5.16
Zhipeng Lin,Hao Zhang,Guofeng Liang,Yanqi Jin,Hongbin Zeng,Jiawang Li,Jian Chen,Weihong Zhang,Fangyan Xie,Yanshuo Jin,Hui Meng
Graphical Composite nanostructured cathode : FeOOH nanocubes with a core–shell structure and anchored on carbon ribbons have been prepared. The carbon ribbons improve the conductivity of the system and make more of the FeOOH surface available for electrochemical reaction. An Li/O 2 battery with FeOOH as the cathode material shows a specific capacity of 14816 mAh g −1 cathode and a long-term stability of 67 cycles over 400 h (see figure). A composite of FeOOH nanocubes anchored on carbon ribbons has been synthesized and used as a cathode material for Li/O 2 batteries. Fe 2+ ion-exchanged resin serves as a precursor for both FeOOH nanocubes and carbon ribbons, which are formed simultaneously. The as-prepared FeOOH cubes are proposed to have a core–shell structure, with FeOOH as the shell and Prussian blue as the core, based on information from XPS, TEM, and EDS mapping. As a cathode material for Li/O 2 batteries, FeOOH delivers a specific capacity of 14816 mA h g −1 cathode with a cycling stability of 67 cycles over 400 h. The high performance is related to the low overpotential of the oxygen reduction/evolution reaction on FeOOH. The cube structure, the supporting carbon ribbons, and the -OOH moieties all contribute to the low overpotential. The discharge product Li 2 O 2 can be efficiently decomposed in the FeOOH cathode after a charging process, leading to higher cycling stability. Its high activity and stability make FeOOH a good candidate for use in non-aqueous Li/O 2 batteries.
研究领域:
材料科学
·
能源存储与转换
✓ 已验证
DOI
PubMed
高影响因子
JOURNAL OF POWER SOURCES
·
2020
·
IF 8.247
Chang Wu,Yuyang Hou,Jicheng Jiang,Haipeng Guo,Hua-Kun Liu,Jun Chen,Jiazhao Wang
Li–O 2 batteries has been widely investigated for its ultra-high capacity as next generation batteries. Nevertheless, some problems like sluggish kinetic reaction and instability hugely impede the practical use of Li–O 2 batteries. In this work, Mo 2 C/MoO 2 @RGO heterostructures was fabricated by in-situ growth of Mo 2 C between MoO 2 and RGO during calcination and being employed as cathode to explore the synergistic effect in Li–O 2 batteries. As a result, Mo 2 C/MoO 2 @RGO exhibits good specific capacity with 2365 mAh g −1 , high round-trip efficiency (89% at first cycle) and improved cycling performance. Density functional theory calculations indicated that the Mo 2 C/MoO 2 @RGO heterostructures have better capability of oxygen adsorption than sole constituent (Mo 2 C@RGO or MoO 2 @RGO), which triggers the formation of film-like amorphous discharge products, leading to lower overpotential and stable performance. Our study reveals the important role of heterostructures in Li–O 2 batteries system and demonstrates a promising design strategy for heterostructured catalyst.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）