CERAMICS INTERNATIONAL
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2024
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IF 5.1
Jianjian Wang,Yue Yu,Zhiqiang Li,Hualin Wang,Shimin Liu,Tingting Yao,Weiwei Jiang,Nan Wang,Chaoqian Liu,Wanyu Ding,Zhihua Zhang,Chuang Dong
Multi-component high entropy oxides (HEOs) have attracted enormous attention due to their unique structures and potential applications. The conventional selection strategy to obtain HEOs is to search for equimolar cationic systems to maximize configurational entropy and avoid phase separation. We previously explored non-equimolar cationic rocksalt structure Mg–Co–Ni–Cu–Zn–O HEOs using cluster-plus-glue-atom model. In this paper, the mixing entropy, enthalpy and Gibbs free energy of constructed superclusters were numerically calculated and compared with the correlated crystal structure based on recent studies. It indicated the Gibbs free energy rather than mixing entropy agrees well with the phase stability of HEOs. Mg 28 Co 17 Ni 19 Cu 16 Zn 16 O 96 shows the optimal phase stability which is related to the lowest Gibbs free energy, reflecting a regular octahedral environment preferred by the cation composition in the system. Enthalpy and entropy are among important design criteria in determining the phase stability of HEOs but the function of enthalpy is obviously higher than that of entropy. This study provides a comprehensive way to access HEOs which is undoubtedly very important for the development of other non-equimolar cationic high entropy materials such as carbides , silicides , borides or nitrides .
研究领域:
材料科学
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热力学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
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2021
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IF 6.707
Hardy Shuwanto,Hairus Abdullah,Dong-Hau Kuo,Noto Susanto Gultom
Y-doped Zn(O,S) nanocatalysts with different Y amounts have been fabricated, characterized, and applied for photocatalytic hydrogen evolution reaction (HER) and hydrogenation reaction (PHR) to reduce nitro groups and to cleave azo (N N) bond. The oxysulfide formation was confirmed by XRD, SAED, and DRS analyses. The best Y-doped Zn(O,S) could evolve hydrogen by 3,946 μmol g −1 h −1 in aqueous solution with ethanol as a hole scavenger reagent. The PHR of 5% Y-doped Zn(O,S) could hydrogenate 4-nitrophenol to 4-aminophenol and nitrobenzene to aniline in 120 and 90 min, respectively in a low-power UV light illuminated condition (16 W) as confirmed with UV–Vis spectroscopy. Besides of that, a sluggish cleavage of N N bond in azobenzene could be totally done to yield aniline within 30 min. Lastly, the detail mechanisms of HER and PHR including their molecular chemisorption phenomena were proposed and described with the steps of solvation , adsorption, pinning, and surface hydrogenation reactions.
研究领域:
材料化学
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光催化
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纳米催化
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环境化学
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能源化学
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2021
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IF 5.816
Hairus Abdullah,Riski Titian Ginting,Refi Ikhtiari,Noto Susanto Gultom,Hardy Shuwanto,Dong-Hau Kuo
Configurational entropy composites of In-doped Zn(O,S)/Zn-doped In(OH) 3-x S x has been synthesized with a one-step hydrothermal method and carefully characterized with XRD , XPS , SEM, TEM, DRS , PL , EIS , TPC , CV , and MS analyses. The composites were prepared with different sulfur amounts to obtain the optimum performance of visible-light photocatalytic HER . The primary phases of ZnS and In(OH) 3 were formed after the hydrothermal process. However, the results indicated In and O were doped into ZnS lattice and induced lower bandgap values (~2.71–2.84 eV) which are active in visible-light illumination. Simultaneously, the excess Zn and S were also doped to In(OH) 3 with lower bandgap values (~3.38–4.63 eV). The variation of bandgap values is due to the hybridization of In 5s5p to Zn 4s4p and O 2p to S 3p orbitals. As a result, In-doped Zn(O,S) and Zn-doped In(OH) 3-x S x will be a visible-light active material for photoreaction and a favorable phase for electron transfer , respectively. Furthermore, it is also related to a possible antisite-defect formation with I n Z n + to help the electron trapping and enhance the photocarrier separation, leading to an efficient photocatalytic activity . ZI-S1 with additional 5-mmol thioacetamide was found as the catalyst with the highest HER performance which achieved 730 μmol/g·h under visible-light illumination. A plausible photocatalytic HER mechanism is discussed and proposed in this work.
研究领域:
材料科学
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化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF SOLID STATE CHEMISTRY
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2024
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IF 3.2
Hao Sun,Jingyi Yu,Cong Zheng,Sumei Wu,Tingting Yao,Zhiqiang Li,Nan Wang,Cunlei Zou,Weiwei Jiang,Hualin Wang,Shimin Liu,Chaoqian Liu,Wanyu Ding,Jiliang Zhang,Chuang Dong
Mg–Co–Ni–Cu–Zn–O is the firstly reported high entropy oxide (HEO) which has great promise in optoelectrical applications. However, the multicomponent and decreased configurational entropy by extracting one element from (Mg, Co, Ni, Cu, Zn) makes it difficult to synthesize single-phase medium entropy oxides (MEOs) especially when the cations are non-equimolar. In this paper, we synthesized different compositional-type of non-equimolar Co–Ni–Cu–Zn–O MEOs possessing single-phase rocksalt structure guided by the cluster-plus-glue-atom model. Interestingly, Co 21 Ni 43 Cu 16 Zn 16 O 96 and Co 17 Ni 47 Cu 16 Zn 16 O 96 have the lowest single-phase formation temperature (850 °C) when the total cation content is kept unchanged. Further increase or decrease of Co/Ni content (none, little, more) will increase the difficulty of single-phase formation ability and temperature (900–1200 °C). It is suggested the single-phase formation ability of Co–Ni–Cu–Zn–O MEOs is closely related to the Gibbs free energy ( ΔG ) and average cation-size difference ( δ ). The linear decrease of Co content and increase of Ni content can monotonously enlarge the energy band gap ( E g ) from 1.52 eV to 1.93 eV and increase the electrical impedance with five orders of magnitude (∼10 3 Ω–∼10 8 Ω), which may be valuable in the fields of optoelectrical devices.
研究领域:
材料科学
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凝聚态物理
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Wei Deng,Kun Xiong,Nina Ge,Miao Yu,Lin Chen,Jun Wang
For efficient removal of the residual tetracycline (TC) in the aquatic environment, a novel cobalt (Co) and titanium (Ti) co-doped zinc ferrite (CoTiZFO) film was prepared via the Langmuir-Blodgett (LB) method in this study. With the co-doping of Co and Ti, the interfacial photoelectrocatalytic (PEC) activities for degradation of TC by the LB-assembled CoTiZFO (LB-CoTiZFO) films were significantly improved. As the applied voltage was 0.6 V in a two-electrode system, the five-layered LB-CoTiZFO (LB-CoTiZFO-5) films exhibited the optimal TC degradation rate and mineralization rate, which were accordingly 92.85% ± 1.45% and 81.92% ± 0.26%. In the same case, the kinetic rate constant ( k ) for PEC degradation of TC by the LB-CoTiZFO-5 films is equivalent to 3.3-fold of that by the films without the co-doping of Co and Ti. Under the PEC circumstances, the Co 3+ and Ti 4+ in the LB-CoTiZFO-5 film would be reduced to Co 2+ and Ti 3+ , while the Fe 2+ was oxidized to Fe 3+ , which results in the surface rearrangement of the LB-CoTiZFO-5 film. In addition, the Density Functional Theory (DFT) calculation results manifest the covalency competition in the Zn-O-Fe backbone can lead to the Fe-O bond breakage, the bare Fe metals with unpaired valence electrons will diffuse to the Helmholtz layer and serve as active sites, which endows the LB-CoTiZFO-5 films with boosted interfacial PEC activities. Therefore, the LB-CoTiZFO-5 film photoanode shows great prospective in efficient PEC degradation of TC.
研究领域:
环境科学
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材料科学
✓ 已验证
DOI
高影响因子
Journal of Energy Storage
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2023
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IF 9.4
Di Zhang,Mengmeng Zhang,Yingsong Yu,Shuting Liang,Yi Hu
Composite electrolyte membranes with 3D nanofiber network structure, which can adjust internal stress to achieve cyclic stability, has been proved to play an important role in the cycle process of lithium metal batteries . However, its application is greatly impeded by the inherent instability interface. Here, we have created an excellent ion transport system through simple interface engineering design. The system weakens the interaction between PEO and Li + via a direct interfacial driving mechanism that establishes the ion bonds (Li-O/Zn-O) between LLZO/ZnO and PEO respectively, thereby achieving stable ion transport. As a result, Li | LPZ-5 CSE | Li battery displays highly stable Li plating/stripping cycling for over 1000 h at 0.1 mA cm −2 . In addition, lithium metal batteries (LMBs) based on LiFePO 4 cathode can stably cycle for 250 cycles with a specific capacity of 151.9 mAh g −1 (50 °C, 0.2 C). This work provides a straightforward and effective strategy that employs the stable ion transfer process at molecular-level to construct a self-supported membrane, which is positive to the development of long-cycle-life LMBs.
研究领域:
材料科学
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电化学
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电池技术
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纳米技术
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）