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Green Energy & Environment · 2020 · IF 6.395

Efficient hydrogen production through the chemical looping redox cycle of YSZ supported iron oxides

Li Ma,Yu Qiu,Min Li,Dongxu Cui,Shuai Zhang,Dewang Zeng,Rui Xiao

The chemical looping process, where an oxygen carrier is reduced and oxidized in a cyclic manner, offers a promising option for hydrogen production through splitting water because of the much higher water splitting efficiency than solar electrocatalytic and photocatalytic process. A typical oxygen carrier has to comprise a significant amount of inert support, to maintain stability in multiple redox cycles, thereby resulting in a trade-off between the reaction reactivity and stability. Herein, we proposed the use of ion-conductive yttria-stabilized zirconia (YSZ) support Fe 2 O 3 to prepare oxygen carriers materials. The obtained Fe 2 O 3 /YSZ composites showed high reactivity and stability. Particularly, Fe 2 O 3 /YSZ-20 (oxygen storage capacity, 24.13%) exhibited high hydrogen yield of ∼10.30 mmol g −1 and hydrogen production rate of ∼0.66 mmol g −1 min −1 which was twice as high as that of Fe 2 O 3 /Al 2 O 3 . Further, the transient pulse test indicated that active oxygen diffusion was the rate-limiting step during the redox process. The electrochemical impedance spectroscopy (EIS) measurement revealed that the YSZ support addition facilitated oxygen diffusion of materials, which contributed to the improved hydrogen production performance. The support effect obtained in this work provides a potentially efficient route for the modification of oxygen carrier materials.

CAS / MDL: 1345-25-1
研究领域: 化学工程 · 材料科学
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CERAMICS INTERNATIONAL · 2024 · IF 5.1

Preparation and thermophysical properties of medium-entropy fluorite-structured oxide of (Y0·25Zr0.25Hf0.25Ce0.25)O2−δ

Xinyu Ping,Bin Meng,Xiaohua Yu,Qingqing Yang,Zhiyuan Ma,Xiaoyu Pan

A medium-entropy fluorite-structured ceramic of (Y 0·25 Zr 0.25 Hf 0.25 Ce 0.25 )O 2−δ was prepared using a solid state reaction method combined with conventional sintering at 1600  ° C for 10 h. This ceramic has uniform elemental distribution without impurity and segregation. The annealing experiment results show a reversible transformation between single phase and double phases in (Y 0·25 Zr 0.25 Hf 0.25 Ce 0.25 )O 2−δ in 800–1600 °C. The reversible phase transformation does not display any obvious influence on the thermal expansion of this sample. The thermal expansion coefficient of (Y 0·25 Zr 0.25 Hf 0.25 Ce 0.25 )O 2−δ is 12.4 × 10 −6  K −1 in 100–1500 °C, higher than that of 8 wt% yttria-stabilized zirconia (8 YSZ). Furthermore, (Y 0·25 Zr 0.25 Hf 0.25 Ce 0.25 )O 2−δ possesses a lower thermal conductivity (1.51 W m −1  K −1 at 900  ° C) and higher oxygen barrier property compared with 8 YSZ at high temperature. The Vickers' hardness, Young's modulus and fracture toughness of (Y 0·25 Zr 0.25 Hf 0.25 Ce 0.25 )O 2−δ are 10.0 GPa, 193.9 GPa and 1.93 MPa m 1/2 , respectively. These results demonstrate that (Y 0·25 Zr 0.25 Hf 0.25 Ce 0.25 )O 2−δ can be used as a promising candidate ceramic of thermal barrier coatings.

研究领域: 材料科学 · 热物理性质 · 陶瓷材料
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JOURNAL OF THE EUROPEAN CERAMIC SOCIETY · 2023 · IF 5.7

Microstructure and thermophysical properties of bixbyite-structured high-entropy oxides with nine-principal cations

Xinyu Ping,Bin Meng,Xiaohua Yu,Qingqing Yang,Zhiyuan Ma,Xiaoyu Pan

A new nine-principal cation high-entropy oxide of (Y 1/9 La 1/9 Nd 1/9 Sm 1/9 Yb 1/9 Lu 1/9 Eu 1/9 Gd 1/9 Ce 1/9 ) 2 O 3 (9HEO) was synthesized by co-precipitation method combined with conventional sintering at 1600 °C for 10 h. Two samples of 9HEO-(Ce 3+ ) and 9HEO-(Ce 4+ ) were obtained by adjusting the valence state of Ce element in 9HEO. The ratio of Ce 3+ to Ce 4+ in 9HEO-(Ce 3+ ) and 9HEO-(Ce 4+ ) is approximately 2:1 and 14:15, respectively. These two samples have the same bixbyite structure and similar microscopic morphology. Their relative density, thermal expansion coefficient, hardness and Young’s modulus are close. The higher ratio of Ce 3+ /Ce 4+ in 9HEO-(Ce 3+ ) leads to the expansion of its lattice volume and the decrease of thermal conductivity (κ) compared with 9HEO-(Ce 4+ ). In addition, the κ values of these two samples are lower than those of Y 2 O 3 and (Eu 0.2 Er 0.2 Lu 0.2 Y 0.2 Yb 0.2 ) 2 O 3 , which have a bixbyite structure and lower entropy. 9HEO-(Ce 3+ ) and 9HEO-(Ce 4+ ) show higher oxygen barrier property compared with Y 2 O 3 -stabilised ZrO 2 .

研究领域: 材料科学 · 热物理性能
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JOURNAL OF THE EUROPEAN CERAMIC SOCIETY · 2023 · IF 5.7

Preparation, mechanical and ablation properties of a C/C-TaB2-SiC composite

Zhenxiao Tang,Maozhong Yi,Zhe Zhou,Huang Wu,Yuanming Zhou,Ke Peng

A C/C-TaB 2 -SiC composite was successfully prepared by high-solid-loading slurry impregnation combined with polymer infiltration and pyrolysis. The composite had a density of 3.46 g/cm 3 and consisted of pyrolyzed carbon, carbon fibers, TaB 2 particles, and precursor-derived SiC with their mass fractions of 7.8 %, 13.0 %, 58.6 %, and 20.6 %, respectively. The C/C-TaB 2 -SiC composite possessed a flexural strength of 248.2 ± 16.8 MPa and a fracture toughness of 13.7 ± 1.6 MPa·m 1/2 , and demonstrated a non-brittle fracture behavior . After exposure to oxyacetylene flame with a heat flux of 4.18 MW/m 2 for 120 s, the ablation temperature of the sample surface reached a maximum of 2263 °C, and the mass and line ablation rates were 2.24 mg/s and 12.92 µm/s, respectively. The ablation resistance mainly comes from the hindrance of oxygen diffusion by the oxide layer composed of tantalum oxide and a small amount of SiO 2 .

CAS / MDL: 9002-98-6
研究领域: 材料科学 · 航空航天工程
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JOURNAL OF ALLOYS AND COMPOUNDS · 2023 · IF 6.2

Structural, thermophysical, mechanical and electrical properties of equimolar five-principal element fluorite-structured high-entropy oxides

Xinyu Ping,Qingqing Yang,Bin Meng,Zhiyuan Ma,Xiaoyu Pan

Four kinds of high-entropy oxides (HEOs) with compositions of Y 0.2 Zr 0.2 Hf 0.2 Ce 0.2 X 0.2 O 2−δ (X = La, Nd, Gd, Dy, abbreviated as HEO-La, Nd, Gd, Dy, respectively) are synthesized by solid-state-reaction method combined with conventional sintering in air atmosphere at 1600 °C for 10 h. These HEOs have a fluorite-structured phase with homogeneous element distribution. The thermal conductivity ( κ ) of these four samples is in 1.68–2.18 W m −1 K −1 in 25–900 °C. At 800 °C and 900 °C, the κ value of HEO-Gd is lower than those of the HEO-La, Nd, Dy, yttria-stabilized zirconia (YSZ) and some other HEOs with various crystal structures ((Gd 0.2 Dy 0.2 Ho 0.2 Er 0.2 Tm 0.2 )Ta 3 O 9 , (La 0.25 Eu 0.25 Gd 0.25 Yb 0.25 ) 2 Zr 2 O 7 , (Sm 0.2 Dy 0.2 Ho 0.2 Er 0.2 Yb 0.2 )NbO 4 , Hf 0.25 Zr 0.25 Ce 0.25 Gd 0.125 Ca 0.125 O 2-δ and Sr(Y 0.2 Sm 0.2 Gd 0.2 Dy 0.2 Yb 0.2 ) 2 O 4 ). The sample of HEO-Gd has the highest thermal expansion coefficient (CTE) (12.1 × 10 −6 K −1 ) and fracture toughness ( K IC ) (2.5 MPa m 1/2 ) among HEO-La, Nd, Gd, Dy. Its K IC value is higher than those of other HEOs mentioned above. In addition, HEO-Gd exhibits a better oxygen barrier property compared with YSZ in 450–700 °C. These results indicate that HEO-Gd is a promising candidate as high-temperature thermal insulation ceramic.

研究领域: 材料科学 · 无机非金属材料 · 高温陶瓷 · 热障涂层 · 固态离子学
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CORROSION SCIENCE · 2019 · IF 6.355

High-temperature oxidation resistance of dense amorphous boron-rich SiBCN monoliths

Daxin Li,Zhihua Yang,Dechang Jia,Xiaoming Duan,Delong Cai,Shengjin Wang,Jingkun Yuan,Yu Zhou,Dongli Yu,Yongjun Tian

High-temperature oxidation behavior of dense amorphous boron-rich Si 2 B 1-4 C 2 N monoliths in flowing air was studied in detail. The oxidation products are those of amorphous silica and cristobalite that control the diffusion of oxygen inward. Oxygen diffusion leads to a dense and passivating scale, which acts as a barrier to oxygen. Amorphous boron-rich monoliths oxidize through a classical parabolic manner. The amorphous nature, three-layers structure of oxide scale and varying chemical bonds are primarily responsible for the oxidation resistance with respect to the nano monoliths. The increase in boron content is revealed to weaken the oxidation resistance of the amorphous Si 2 B 1-4 C 2 N monoliths.

研究领域: 材料科学 · 无机非金属材料 · 高温功能材料 · 陶瓷基复合材料 · 表面与界面化学
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Nano Research · 2023 · IF 9.9

Suppressing the lattice oxygen diffusion via high-entropy oxide construction towards stabilized acidic water oxidation

Ni Jing,Shi Zhaoping,Wang Yibo,Yang Jiahao,Wu Hongxiang,Wang Pengbo,Li Kai,Xiao Meiling,Liu Changpeng,Xing Wei

The scale-up deployment of ruthenium (Ru)-based oxygen evolution reaction (OER) electrocatalysts in proton exchange membrane water electrolysis (PEMWE) is greatly restricted by the poor stability. As the lattice-oxygen-mediated mechanism (LOM) has been identified as the major contributor to the fast performance degradation, impeding lattice oxygen diffusion to inhibit lattice oxygen participation is imperative, yet remains challenging due to the lack of efficient approaches. Herein, we strategically regulate the bonding nature of Ru-O towards suppressed LOM via Ru-based high-entropy oxide (HEO) construction. The lattice disorder in HEOs is believed to increase migration energy barrier of lattice oxygen. As a result, the screened Ti 23 Nb 9 Hf 13 W 12 Ru 43 O x exhibits 11.7 times slower lattice oxygen diffusion rate, 84% reduction in LOM ratio, and 29 times lifespan extension compared with the state-of-the-art RuO 2 catalyst. Our work opens up a feasible avenue to constructing stabilized Ru-based OER catalysts towards scalable application.

研究领域: 材料科学 · 电化学 · 催化 · 能源材料
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Journal of Materials Chemistry A · 2020 ·Vol. 8 ·期 28 ·14162-14170 · IF 11.301

A SmBaCo2O5+δ double perovskite with epitaxially grown Sm0.2Ce0.8O2−δ nanoparticles as a promising cathode for solid oxide fuel cells

Zhihong Du,Keyun Li,Hailei Zhao,Xu Dong,Yang Zhang,Konrad Świerczek

Modified by Sm0.2Ce0.8O2−δ (SDC) nanoparticles (NPs), SmBaCo2O5+δ (SBCO) double perovskite oxide is evaluated as a promising cathode material for intermediate temperature solid oxide fuel cells. The SDC NPs are epitaxially grown on the surface of SBCO with (220) planes of SDC aligning smoothly to (020) or (100) planes of SBCO, forming a tight, coherent connection at the interface. The influence of this modification on thermal expansion, oxygen diffusion, electrical conductivity and electrochemical properties is investigated thoroughly in this work. The designed SBCO–SDC cathode material demonstrates a lower thermal expansion coefficient (TEC), ∼16.4 × 10−6 K−1, than that of the unmodified SBCO, ∼20.9 × 10−6 K−1. While SDC coating results in a decreased total electrical conductivity, it facilitates oxygen bulk diffusion and improves the surface exchange reaction kinetics. Coating with SDC NPs can accelerate the rate-determining process of dissociation of the absorbed molecular oxygen, especially at intermediate temperatures. Accordingly, the constructed symmetrical cell with the La0.8Sr0.2Ga0.8Mg0.2O3−δ (LSGM) electrolyte shows lower polarization resistance values, if the SBCO–SDC cathode is utilized. Also, the LSGM electrolyte-supported (300 μm) full cell is found to deliver a high power density of 800 mW cm−2 at 800 °C. Owing to the strong and coherent interfacial connection, the developed cathode demonstrates a relatively steady electrochemical performance.

研究领域: 材料科学 · 能源化学 · 电化学 · 无机功能材料 · 燃料电池技术
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ACS Sustainable Chemistry & Engineering · 2025 · IF 7.3

Enhanced Oxygen Reduction Reaction Kinetics of Li-Containing Oxide as a High-Performance Cathode for Solid Oxide Fuel Cells Through Synergistic Li Volatilization and Anion Doping

Zhe Zhang,Chuangang Yao,Haixia Zhang,Yuxi Sun,Baixi Xia,Wanning Liu,Jingyi Ding,Li Zhang,Xiaoshi Lang,Kedi Cai

LiCoO2 is widely used in lithium-ion batteries. Innovatively, this study reveals that by employing a synergistic strategy of Li volatilization and anion doping, LiCoO2-based materials demonstrate exceptional performance as solid oxide fuel cell (SOFC) cathodes. At high temperatures, Li volatilization forms a Co3O4 phase. Concurrently, anionic doping is achieved by substituting F ions for O ions. The synergy of these two strategies increases the concentration of oxygen vacancies and the formation of heterogeneous interfaces, effectively enhancing the adsorption, dissociation, and diffusion rates of oxygen, thereby significantly improving the oxygen reduction reaction (ORR) of LiCoO2 (LCO). LCOF1 (LiCoO1.9F0.1+Co3O4) exhibits an oxygen diffusion coefficient (Dchem) and surface exchange coefficient (Kchem) of 8.85 × 10–5 cm2 s–1 and 7.61 × 10–3 cm s–1, respectively, which are 45% and 26% higher than those of undoped LCO. Furthermore, at 800 °C, LCOF1 achieves a PPD of 0.86 W cm–2 and an Rp as low as 0.012 Ω cm2, representing improvements of 110% in PPD and a reduction of 78.6% in Rp compared to LCO. These findings indicate that the synergistic effect of Li volatilization and F doping is an effective strategy for enhancing the performance of Li-containing cathodes, offering valuable perspectives for the development of high-performance SOFC cathodes.

研究领域: 材料科学 · 电化学 · 能源材料 · 燃料电池 · 陶瓷
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ENVIRONMENT INTERNATIONAL · 2022 · IF 13.352

Synchronous removal of pharmaceutical contaminants and inactivation of pathogenic microorganisms in real hospital wastewater by electro-peroxone process

Yahan Yu,Zhaokun Xiong,Bingkun Huang,Xinhao Wang,Ye Du,Chuanshu He,Yang Liu,Gang Yao,Bo Lai

Herein, a highly efficient electro-peroxone (E-peroxone) process with graphite felt as ozone diffusion electrode (ODE) was developed for the synchronous removal of pharmaceutical contaminants and inactivation of pathogenic microorganisms in real hospital wastewater. Under optimal conditions, the total organic carbon (TOC) removal rate of real hospital wastewater could reach 93.9%. Importantly, 126 pharmaceutical compounds (antibiotics, antivirals, analgesics, antiepileptics, hormones, and others) were determined in hospital wastewater by using ultra performance liquid chromatography combined with quadrupole time-of-flight mass spectrometry (UPLC-Q-TOF-MS/MS). 110 pharmaceutical compounds could be efficiently degraded in E-peroxone system. Concurrently, the microbial community analysis through high-throughput sequencing showed that E-peroxone process exhibited an excellent disinfection effect in real hospital wastewater. Escherichia coli as a bacterial indicator could be completely inactivated in E-peroxone process·H 2 O 2 and hydroxyl radical ( OH) were found in E-peroxone system based on the results of chemical probe experiments and electron paramagnetic resonance (EPR) analysis. The in-situ generation of H 2 O 2 from cathodic oxygen reduction in ODE can react with ozone to produce OH, and realize high efficiencies for the elimination of pharmaceutical and sterilization. This work established a green and effective way without extra addition of chemical reagents for high-efficiency treatment of real hospital wastewater.

研究领域: 环境工程 · 水处理 · 化学工程 · 微生物学
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