Materials Today Communications
·
2024
·
IF 3.7
Zhiqin Wen,Zhenyu Wu,Bo Ma,Jiedong Qin,Li Tang,Taoyi Lu,Yuhong Zhao
A novel 6-cationic single-phase high-entropy fluorite oxides (HEFOs) (Ce 0.16 Zr 0.16 La 0.16 Sm 0.16 Nd 0.16 Y 0.16 )O 2- δ (CZLSNYO) have been prepared by using solid-state reactions, and the structure and mechanical properties of the HEFOs were studied in depth. CZLSNYO exhibits a single-phase cubic fluorite structure with a smooth and crack-free surface and distinct grain boundaries after sintering at 1400 °C, 1500 °C and 1600 °C for 12 hours. The concentration of Ce 3+ in Ce ions is calculated to be 22.23 % ± 1.11 %, and the value of δ is 0.3519 ± 0.0176, yielding a nominal composition of (Ce 0.16 Zr 0.16 La 0.16 Sm 0.16 Nd 0.16 Y 0.16 )O 1.6481 ± 0.0176 . With the increase of sintering temperature, the average grain size of CZLSNYO initially enlarges and then reduces, and its Vickers hardness exhibits a comparable trend. By comparing with the 5-cations (Ce 0.2 Zr 0.2 La 0.2 Sm 0.2 Nd 0.2 )O 2- δ HEFOs, 6-cationic single-phase CZLSNYO sintered at 1500 °C possess large hardness (16.32 GPa) and fracture toughness (8.07 MPa m 1/2 ), since the addition of Y element increases the configuration entropy of the system, and Y has a greater hardness, resulting in a cocktail effect.
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TRANSACTIONS OF TIANJIN UNIVERSITY
·
2025
·Vol. 31
·期 3
·278-291
·
IF 8.5
Chi Shuxiu,Wang Chenhui,Liao Jie,Sun Peng,Fei Yaohan,Han You,Zhang Jinli,Wu Jiangjiexing,Li Wei
Aiming at inhibiting the irreversible P2–O2 phase transition of conventional P2-type cathode materials at high voltage and enhancing the cycling stability of sodium-ion batteries, in this article, based on a strategy of adjusting the Na + ion occupancy within the crystal structure, Na 0.67 Ni 0.33 Mn 0.67– x Fe x O 2 (NM– x Fe, x = 0.10, 0.15, 0.20) cathode materials were synthesized by high shear mixer (HSM)-assisted co-precipitation method and evaluated the electrochemical performance at high voltage (4.35 V). The optimal sample NM–0.15Fe exhibits an initial discharge capacity of 130.8 mAh/g (0.1 C), with exceptional retention of 95.9% after 100 cycles (1 C). XRD analysis reveals that Fe intercalation promotes the more amount of Nae-similar occupation; the Nae/Naf ratio equals 1.93 for NM–0.15Fe versus 1.62 for NM, which enhances Na + diffusion kinetics, as confirmed by GITT tests. Through characterizations of in situ XRD, XPS, HRTEM, CV, etc., it is illustrated that the Fe 3+ intercalation can effectively disrupt the Na + /vacancy ordering and inhibit the harmful P2–O2 phase transition, and then improve the cycling stability of the cathode. DFT calculations disclose that intercalated Fe can reduce the electron densities of adjacent transition metallic elements, generating more repulsive forces impacted on sodium and consequently appearance of more Nae sites, leading to a lower Na + diffusion energy barrier. Such strategy of modulating Na occupation sites in crystal structure is conducive to the development of low-cost and high-performance layered cathode materials for sodium-ion batteries.
研究领域:
电化学储能
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材料科学
·
固态化学
·
能源材料
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电池技术
·
过渡金属氧化物
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Changshun Deng,Xiaorong Zhu,Jun Yao,Yibo Wang,Chenyang Shen,Bingqing Ge,Chaoxiang Li,Nianhua Xue,Luming Peng,Xuefeng Guo,Yan Zhu,Yafei Li,Weiping Ding
The direct oxidation of toluene by O 2 to benzaldehyde with high efficiency is a bright route for the green production of benzaldehyde but still a significant challenge. In this study, we develop a ligand modification strategy by bonding organophosphonic acid (OPA) to VTiO x /γ-Al 2 O 3 to restructure its interface microenvironment for enhancement of toluene oxidation to benzaldehyde. The as-prepared catalyst exhibits excellent selectivity over 99 % under mild conditions. Results of comprehensive characterizations and calculations reveal that the OPA bonding in bidentate with the V 6-coordinated species causes noticeable phase reconstruction between VO x and TiO 2 , thereby generating nearby new reactive oxygen species, which is responsible for the conversion of toluene to benzaldehyde at temperatures as low as ∼50 °C, much lower than that over VO x /TiO 2 (>130°C). The interface microdomain around the bonding site of OPA helps to significantly weaken the methyl C H bond of toluene molecule in reaction manifested as the significant decrease in apparent activation energy. Hence, the current work reveals a novel mechanism of the typical catalyst VO x /TiO 2 under OPA bonding, which is useful to solve the classic difficult reaction of toluene to benzaldehyde by O 2 oxidation.
研究领域:
催化化学
·
绿色化学
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2017
·Vol. 164
·期 6
·A1321
·
IF 3.259
Chaolumen Wu,Taoran Li,Chenbo Liao,Qingkai Xu,Yuancheng Cao,Lei Li,Jun Yang
Triethylene glycol dimethyl ether (G3) is evaluated as an electrolyte solvent for non-aqueous lithium-oxygen (Li-O2) batteries. A liquid electrolyte of 1 M LiTFSI in G3 shows lower viscosity, higher oxygen solubility and diffusion, higher ionic conductivity and lithium ionic transference number compared to the conventional liquid electrolyte of 1 M LiTFSI in tetraethylene glycol dimethyl ether (G4). Then the Li-O2 battery using the G3-based electrolyte shows better cycling stability and higher rate capability compared to the battery using the G4-based electrolyte. At a higher current density of 2.5 A gcarbon−1, the discharge capacity of the battery using the G3-based electrolyte is about 1472 mAh gcarbon−1, which is about four times higher than that of the battery using the G4-based electrolyte. At current density of 1 A gcarbon−1 with a fixed capacity of 1000 mAh gcarbon−1, the battery using the G3-based electrolyte can be operated stably for 80 cycles, while only 20 cycles are achieved by using the G4-based electrolyte. Therefore, we think the G3-based electrolyte could be a proper alternative electrolyte to the conventional G4-based electrolyte for the development of Li-O2 batteries.
研究领域:
材料科学
·
电化学
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2018
·
IF 11.698
Meichao Gao,Jinxiang Yang,Tao Sun,Zizhong Zhang,Dafeng Zhang,Huijuan Huang,Huaxiang Lin,Yi Fang,Xuxu Wang
The photocatalytic overall conversion of CO 2 with H 2 O to chemical fuel and oxygen mimicking natural photosynthesis is a huge challenge in photocatalysis. This work shows the achievement of the solar-driven photocatalytic overall CO 2 reduction with H 2 O to CO and O 2 over a Persian buttercup-like BiOBr x Cl 1-x solid solution. A CO generation rate of 15.86 μmol g −1 h −1 with the approximate stoichiometric O 2 evolution is yielded on BiOBr 0.6 Cl 0.4 solid solution under simulated solar light irradiation, which was about 7.5 and 10.2 times higher than that of pure BiOCl (2.11 μmol g −1 h −1 ) and BiOBr (1.55 μmol g −1 h −1 ), respectively. The enhanced photoactivity is contributed to the mediate band gap and energy level tuned by the formation of BiOBr x Cl 1-x solid solution to facilitate the separation of photogenerated charges. Besides the unique electron structure, the photoinduced oxygen vacancy (O V ) formed on BiOBr x Cl 1-x solid solution also plays an important role in the CO 2 reduction.
研究领域:
化学
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材料科学
·
环境科学
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2020
·
IF 2.627
Yingfei Hou,Lin Jiang,Yaoyao Zhang,Zhiwen Qin,Chi Jiang,Ming Wang
Lithium-air (also known as lithium-oxygen) batteries have attracted considerable global attention in recent years due to their extremely high energy density (11,140 W·h·kg −1 ). The electrolyte is a key element in lithium-air batteries and the traditional organic electrolyte has great safety risk due to leakage. On the contrary, the polymer electrolyte has the advantages of high safety, high stability and easy processing comparing with the organic liquid electrolytes. In this paper, a new idea was proposed to coat the Nafion membrane on a layer of polymer for blocking the oxidation reduction electric (RM) and Li based on the selective permeability on lithium ion of the Nafion membrane. Self-made thickness-controllable Nafion membrane, polyvinylidene fluoride-hexafluoropropylene copolymer (PVDF-HFP) and 2,2,6,6-tetramethylpiperidinooxy (TEMPO) were used to prepare a quasi solid polymer electrolyte (NSPE). Electrochemical workstation and LAND battery testing system were used to perform a galvanostatic charge/discharge test on Li-O 2 . The ionic conductivity of NSPE was 4.3 × 10 −4 S·cm −1 at room temperature and the discharge platform was 2.6 V and the charging voltage was 3.7 V after 50 cycles with the cut-off capacity of 500 mA·h·g −1 .
研究领域:
材料科学
·
电化学
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ELECTROCHIMICA ACTA
·
2022
·
IF 7.336
Panpan Zhao,He Zhang,Xiaoxuan Sun,Shuai Hao,Shaojun Dong
In this work, combining poly (methylene green)/glucose dehydrogenase (PMG/GDH) bioanode with Prussian blue/glucose oxidase (PB/GOD) biocathode, we developed a hybrid bioelectrochemical device based on glucose/O 2 enzymatic biofuel cell (EBFC) to achieve energy conversion and storage. Depending on the reversible redox behaviors, PMG and PB play roles of dual-functional nanomaterials , not only as mediators to accelerate electrons transport between enzymes and electrodes surface, but also as pseudocapacitive materials to achieve energy storage. As a result, this hybrid device exhibited superior performance towards energy storage with a specific capacitance of 158.5 mF cm −2 at the current density of 1 mA cm −2 . Meanwhile, a maximum output power density of 783.5 μW cm −2 in the pulse mode could be obtained, which had a prominent increment than that of the prototypical EBFC (87.5 μW cm −2 ) in the steady state. Furthermore, this hybrid device also exhibited better operational stability in long-term charge/discharge cycles test, at the current pulse of 1 mA cm −2 . Through the combination of bioelectrocatalysis and capacitive energy storage, this developed hybrid device achieves effective energy conversion and storage, and provides a high output power to address the insufficient power supply of traditional EBFCs, which may enlarge the practical application of EBFCs in self-powered implantable and wearable devices .
研究领域:
生物电化学
·
能量存储
·
材料科学
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生物医学工程
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JOURNAL OF THE AMERICAN CERAMIC SOCIETY
·
2025
·Vol. 109
·期 1
·e70407
·
IF 3.8
Yuwei Zhang,Cuiwei Li,Guangjin Chen,Chenran Zhao,Zhikun Song,Kepi Chen,Haoran Sun,Linghao Wu,Junhui Xiang
A series of (Y, Yb, Zr, Hf, Sn, W)O 2−δ high-entropy ceramics with varying mole fraction of main elements were synthesized for the first time through the solid-state reaction synthesis method. The microstructure, phase composition, and properties of the prepared materials were thoroughly analyzed and tested. The results indicate that the phase composition transformed from a single-phase fluorite structure to a single-phase C-type rare earth sesquioxide structure as the mole fraction of +3 cations increases. The thermal conductivity of the prepared high-entropy ceramics with porosity of 49.8%–50.1% is very low ranging from 0.33 to 0.37 W·m −1 ·K −1 . Among them, the single-phase C-type rare earth sesquioxide with a higher oxygen vacancy concentration was employed as a catalyst in the CO 2 hydrogenation reaction, attaining a high CO 2 conversion rate of 82.0%. The obtained results have deepened understanding of the role of oxygen vacancies and have important guiding significance for the study of high-entropy oxides with fluorite derived structures.
研究领域:
材料科学
·
陶瓷
·
催化
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能源材料
·
固态化学
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ADVANCED FUNCTIONAL MATERIALS
·
2026
·
IF 19.9
Ningchao Zheng,Zhizeng Pan,Shuai Kang,Deqian Zeng,Xiangbiao Yin,Qiang Wu,Yuezhou Wei,Zhuofeng Hu
Hydrogen peroxide (H 2 O 2 ) is regarded as a promising strategy for radioactive uranium removal, due to its eco-friendliness and ability to convert free UO 2 2+ into insoluble studtite. However, the spontaneous and selective production of H 2 O 2 under ambient conditions remains challenging. This study develops a P-Ag for spontaneous O 2 activation and selective H 2 O 2 synthesis under ambient conditions. The H 2 O 2 yields of P-Ag reach 1210 µmol g −1 h −1 in air and 1876.3 µmol g −1 h −1 in O 2 , surpassing most of the recently reported catalytic systems. Importantly, the H 2 O 2 generated in situ by P-Ag achieves a high uranium removal activity (48.5) within 60 min, outperforming 23 known systems. Mechanistic studies indicate that P-Ag follows a two-step single-electron O 2 activation pathway. The electron-donating Ag sites drive the complete catalytic cycle, encompassing H 2 O/O 2 adsorption, H 2 O dissociation, and *OOH/H 2 O 2 formation, while the red phosphorus substrate serves as an electron reservoir to sustain the Ag sites. The H 2 O 2 produced reacts instantaneously with UO 2 2+ to form studtite, enabling efficient uranium removal. This study not only offers new insights into the selective synthesis of H 2 O 2 via spontaneous O 2 activation, but also proposes an eco-friendly route to mitigate environmental risks from radioactive uranium contamination.
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AICHE JOURNAL
·
2026
·
IF 4
Zhiheng Wang,Ningning Wu,Jiali Huang,Tuo Ji,Han Lin,Liwen Mu,Xiaohua Lu,Jiahua Zhu
Direct synthesis of hydrogen peroxide (DSHP) from H 2 and O 2 is indeed a promising sustainable alternative to the conventional anthraquinone oxidation process, yet achieving high H 2 O 2 productivity and selectivity simultaneously remains a significant challenge. Herein, we designed a diode-inspired interfacial microenvironment to address this challenge by synchronizing the kinetic relay of the key transport and reaction steps in DSHP. Specifically, this microenvironment was fabricated by grafting hydrophobic silane molecules onto the carbon surface followed by loading palladium nanoparticles. Results indicate that the interfacial microenvironment enables an efficient relay of H 2 dissociation, H 2 O 2 formation and desorption, shutting down the reverse path of the side reaction. Benefiting from this diode-inspired interfacial design, high H 2 O 2 productivity of 21,647.1 mol kg Pd −1 h −1 and H 2 O 2 selectivity of 93.3% were successfully achieved under ambient conditions. This work demonstrated the critical role of the interfacial microenvironment in regulating the synergy between mass transfer and reaction in heterogeneous reaction.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Yong Liu,Mingjun Han,Jianye Liu,Yaling Huang,Yisi Liu,Wenzhang Li,Yang Liu,Jie Li
The practical implementation of Li-O 2 batteries remains constrained by three persistent challenges: sluggish oxygen redox kinetics, prohibitive costs of noble metal catalysts, and insufficient activity of non-precious alternatives. Herein, we present a novel ultralow Pt (0.25 wt%) single-atom loading Co 3 O 4 nanoneedle array catalyst (Pt 1 -Co 3 O 4 ) grown on carbon cloth via an ionic substitution strategy. This material functions as an advanced self-supporting cathode for aprotic Li-O 2 batteries. Benefiting from the surface self-reconstruction induced by Pt single-atom occupied the tetrahedral central sites of Co 3 O 4 , the electronic structure of Co 3 O 4 is modified, significantly enhancing the kinetics of both the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). As a result, the Pt 1 -Co 3 O 4 cathode demonstrates excellent cycling stability and a remarkably low discharge–charge overpotential of just 0.86 V. Furthermore, the Li-O 2 battery with this cathode exhibits a high discharge-specific capacity (8.20mAh cm −2 ) and long cycling life (220 cycles, >1100 h at 0.1 mA cm −2 ), outperforming all reported Co 3 O 4 -based ORR/OER catalysts, as well as many non-noble metal catalysts, even those with significant noble metal loading. Crucially, the thin-film-like layers of discharge product Li 2 O 2 are uniformly dispersed on the Pt 1 -Co 3 O 4 nanoneedles. This reduces the adsorption energy between LiO 2 /Li 2 O 2 and Pt 1 -Co 3 O 4 compared to Co 3 O 4 , ensuring good structural stability during discharge/charge cycles and facilitating the decomposition of discharge products during recharge, thus reducing overvoltage and enhancing battery efficiency. These findings position Pt 1 -Co 3 O 4 as a promising catalyst for Li-O 2 batteries and open new avenues for the development of oxide-based single-atom catalysis.
研究领域:
材料科学
·
电化学
·
能源存储与转换
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LANGMUIR
·
2025
·
IF 3.9
Yu-Le Wang,Cong Wang,Song-Hai Wu,Yong Liu,Xu Han
Although spontaneous H2O2 accumulation by sacrificial oxidation of metal disulfides (FeS2, NiS2, etc.) under oxic conditions without external electrical/photonic input has been observed, the mechanistic understanding of HCO3– on the production of H2O2 is still not clear. In this study, HCO3– apparently accelerates the production of H2O2 on NiS2, and the produced H2O2 increases from 53.85 to 90.12 μM with increasing concentrations of HCO3– from 0 to 0.5 M at pH 9.0. Electrochemical analyses indicate that HCO3– effectively mediates the 2e reduction of O2 to H2O2 on the surface of NiS2. EPR and Raman analyses rule out the primary contributions of soluble •OH and O2•– to the production of H2O2 and reveal the presence of both ≡Ni–OO• superoxo and ≡Ni–OOH peroxo on NiS2, which are important precursors for H2O2. The presence of CO3•– also indicates that HCO3– is an important H-donor during the reduction of O2 to H2O2. DFT calculations further reveal that it is thermodynamically more favorable for ≡Ni–OO• and ≡Ni–OOH to abstract H from HCO3– than from H2O to produce H2O2, confirming that HCO3– is a better H-donor than H2O to produce H2O2 via the H-abstraction pathway. This study provides insight into the importance of HCO3– on spontaneous H2O2 accumulation by sacrificial oxidation of NiS2 under oxic conditions without external electrical/photonic input.
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