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SCIENCE OF THE TOTAL ENVIRONMENT · 2021 · IF 7.963

Enhanced reactivity of zero-valent aluminum/O2 by using Fe-bearing clays in 4-chlorophenol oxidation

Ran Yang,Jun Cai,Hu Yang

Zero-valent aluminum (ZVAl) is a promising reductant because of its relatively low redox potential , which can efficiently activate molecular oxygen to generate reactive oxygen species . However, its long-term performance is limited by the intrinsic dense oxide layer and the passivation effect of the accumulative Al-(hydr)oxide on its surface during the reaction. In this study, four clay minerals with different compositions were mixed with ZVAl by ball milling to obtain four composites of ZVAl and clay (ZVAl-Clay), which were used to degrade a high concentration of 4-chlorophenol (4-CP) under ambient conditions. The oxidation efficiencies of different ZVAl-Clays were strongly relevant to Fe contained in the clay minerals. The Fe-free ZVAl-Clay presented poor oxidation performance, whereas the reaction efficiencies of those ZVAl composites with Fe-bearing clays exhibited varying degrees of improvement. In comparison with the original ZVAl, the highest oxidation rate increased by 23 times, the maximum increased OH production was approximately 8 times, and the corresponding mineralization efficiency improved by 38.7%. However, the levels of improved oxidation performance of various ZVAl-Clays were not positively correlated with their actual total Fe contents, and their degradation efficiencies might also be affected by other physical and/or chemical properties of different clays. The synergistic mechanism revealed by various characterizations was that electron transfer might occur from ZVAl to the structural Fe(III) of the clay through the basal plane or edge of clays triggered by ball milling. Thus, the partially produced Fe(II) on the clay surface promoted the Fenton-like reaction to decompose H 2 O 2 into OH for efficient oxidation of 4-CP. In short, the ZVAl composites with Fe-bearing clays deserved further exploration as potential materials for efficient degradation of organic matters in wastewater samples.

研究领域: 环境科学 · 材料科学
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JOURNAL OF THE ELECTROCHEMICAL SOCIETY · 2017 ·Vol. 164 ·期 6 ·A1321 · IF 3.259

Enhanced Electrochemical Performance of Non-Aqueous Li-O2 Batteries with Triethylene Glycol Dimethyl Ether-Based Electrolyte

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
✓ 已验证 DOI 高影响因子
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JOURNAL OF ALLOYS AND COMPOUNDS · 2024 · IF 5.8

Ensemble effect in porous bimetallic N/C nanocage-grafted CNTs for improved Li-O2 battery cathodes

Tie Liu

The geometric design of atomically dispersed 'framework-active sites' grafted with carbonaceous materials to establish a well-connected three-dimensional network represents a compelling strategy for enhancing the performance of lithium-oxygen batteries, particularly in terms of cyclability. This paper introduces a simple approach that utilizes self-assembly heterogeneous nucleation to fabricate discrete bimetallic (Co, Ni) micron lattices grafted onto CNTs, exhibiting commendable surface properties. This intriguing hierarchical structure optimally harnesses the profound structural effects of CNTs weaving matrix, thereby imparting essential properties to the cathode, including high catalytic activity, intrinsically accessible active sites, and continuous porosity to accommodate discharge products. And such binary metal-nitride grafted configuration is significant in mitigating the embarrassing presence of nitrides (low conductivity) and carbon material (inferior activity). Consequently, cell measurement results indicate that a comparable capacity of 8599.7 mA h g⁻¹ and cyclic performance exceeding 200 cycles are achieved in a semi-solid state battery, outperforming commercially available RuC catalysts. And the DFT calculations further demonstrate the strong electronic coupling transfer and exceptional bifunctional activity observed in this binary metal-nitride sample. Therefore, this work exemplifies both steerable preparation techniques and the considerable potential inherent in geometric design for bimetallic sites grafted with carbonaceous material-based catalysts as they transition from Li-O 2 to Li-air batteries.

研究领域: 材料科学 · 电化学 · 纳米技术
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ELECTROCHIMICA ACTA · 2022 · IF 7.336

A hybrid bioelectrochemical device based on glucose/O2 enzymatic biofuel cell for energy conversion and storage

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 · 生物医学工程
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Advanced Materials Interfaces · 2017 ·Vol. 4 ·期 23 ·1700693 · IF 4.279

A Rational Design of High-Performance Sandwich-Structured Quasisolid State Li–O2 Battery with Redox Mediator

Kailiang Liu,Hongguang Sun,Shanmu Dong,Chenglong Lu,Yang Li,Junmei Cheng,Jianjun Zhang,Xiaogang Wang,Xiao Chen,Guanglei Cui

The increasing interest in Li–O 2 battery arises from its unparalleled theoretical energy density. Nevertheless, the poor reversibility of cathode reaction and unstable characteristic of Li anode hinder its further application. To address these issues, a high-performance sandwich-structured quasisolid polymer electrolyte (QSPE) is designed to meet the requirement of both cathode and anode. For the first time, lithiated Nafion ionomer (Li-Nafion) is introduced into Li–O 2 cell to separate “catholyte” and “anolyte.” Redox mediator (RM) is introduced into gel-like catholyte, based on polymethymethacrylate, to achieve high capacity and reversibility. Polypropylene carbonate is chosen as solid-state anolyte for enhancing interface stability of lithium anode. It is demonstrated that the QSPE exhibits excellent permselectivity to block RM shuttling, as well as good ionic conductivity and high electrochemical window. A solution mechanism formation of discharge product is demonstrated in the Li–O 2 cell with QSPE and the RM works well for cycles at room temperature. This sandwich-structured design strategy will provide a new pathway to promote the properties of Li–O 2 battery.

研究领域: 储能 · 电化学 · 材料科学 · 电池技术
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MATERIALS RESEARCH BULLETIN · 2015 · IF 2.288

Discharging temperature dependence of Li2O2 formation and its effect on charging polarization for Li–O2 Battery

Ming Song,Xihua Du,Yan Chen,Lei Zhang,Ding Zhu,Yungui Chen

Among all the factors that restrict the application of Li–air battery, large charging polarization, due to the poor bulk charge transport ability of discharge product Li 2 O 2 , comes first. In this paper, we adopt the method of controlling discharging temperature to reduce the charging polarization during the first cycle of Li 2 O 2 based on the fact that controlling discharging temperature can reduce Li 2 O 2 bulk charge transport path since finer Li 2 O 2 particles can be observed at higher temperature. The mechanism of reducing charging polarization simply through increasing the discharging test temperature has also been researched in this paper.

CAS / MDL: 33454-82-9 143-24-8
研究领域: 材料科学 · 电化学
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JOURNAL OF SOLID STATE ELECTROCHEMISTRY · 2015 ·Vol. 19 ·期 8 ·2421-2429 · IF 2.446

The investigation of water vapor on the Li–O2 battery using a solid-state air cathode

Wang Xiaofei,Cai Shengrong,Zhu Ding,Mu Shijia,Chen Yungui

A lithium (Li)–oxygen (O 2 ) battery based on an inorganic solid-state air cathode was fabricated, and the influence of water vapor (key component in the air) on the electrochemical behavior of the proposed Li–O 2 battery was deeply investigated. Excluding the negative influence of the corrosion of Li anode that existed in organic-based electrolyte Li–O 2 battery when operated in wet environment, our results showed that water vapor has a positive effect on the discharge and cycling performances of the Li–O 2 battery using a solid-state air cathode. The discharge capacity reached 11734 mA h g −1 (7.8 mA h cm −2 ) in wet O 2 , which was not markedly different with that in dry O 2 (11956 mA h g −1 (8.0 mA h cm −2 )). However, the discharge voltage in wet O 2 was about 110 mV higher than that in dry O 2 . Although the formation of LiOH increased the charge overpotential, the formed LiOH in turn minimized the decomposition of carbon to form Li 2 CO 3 , and enhanced the cycling performance to a certain extent. In addition, we showed that the polarization involved by water vapor could also be largely decreased by slightly increasing the operating temperature; the charge voltage plateau decreased from 4.04 to 3.3 V when the temperature increased from 25 to 50 °C. These results suggest that the Li–O 2 battery using a solid-state air cathode is promising for practical application, especially in wet environment.

CAS / MDL: 90076-65-6 143-24-8
研究领域: 材料科学 · 电化学
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JOURNAL OF ALLOYS AND COMPOUNDS · 2023 · IF 6.2

Band engineering of α-Fe2O3/SnO2 heterojunction photocathode enables highly efficient and stable Li−O2 batteries

Weixue Yang,Jiaqi Zhao,Zhen Li,Jiayu Xin,Fei Li,Yu Wang

Introducing light energy into the charging/discharging process is an effective strategy to reduce the overpotential of Li−O 2 battery, which leads that the battery has higher energy conversion efficiency and better battery performance. However, the development has been hampered by the lack of suitable photocatalysts and cathode structure to accommodate the insoluble Li 2 O 2 . In order to overcome the aforementioned difficulties, a bifunctional photocatalyst α-Fe 2 O 3 /SnO 2 (FS) heterojunction was designed as the cathode to improve the charging/discharging overpotentials simultaneously. The photogenerated electrons and holes from FS participated in the oxygen reduction reaction (ORR) and oxygen revolution reaction (OER) under illumination, giving rise to an ultra-low charging/discharging overpotential of 0.01 V (energy efficiency up to 99.7%), which improved the electrochemical reaction kinetics of the Li−O 2 battery strikingly. In addition, the FS cathode exhibited excellent cycle stability under light (the battery energy efficiency can still maintain 80% after 252 cycles). The bifunctional catalyst designed in this paper has profoundly proved that the band engineering strategy can effectively utilize solar energy and provide important insights for understanding the mechanism of photo-assisted Li−O 2 battery.

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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

Biomimetic chlorophyll derivatives-based photocatalytic fabric for highly efficient O2 production via CO2 and H2O photoreaction

Shuzhen Yu,Yongchun Hou,Qijie Jin,Liangliang Zhu,Su Chen

As global warming and greenhouse gas emissions intensify, the scientific community is continuingly seeking effective solutions. One promising strategy known as artificial photosynthesis is proposed utilizing H 2 O as a reducing agent to transfer CO 2 into fuel. However, low O 2 production and conversion efficiency have hindered this approach in matching with natural photosynthesis. In this work, we propose a novel biomimetic photocatalyst design approach to improve the catalytic efficiency by slow photon mechanism. Our design is mainly inspired by two factors: 1) Chlorophyll, an abundant natural photosynthetic pigment, can efficiently and selectively reduce carbon dioxide and plays a key role in photosynthesis; 2) The iridoplast with a biological photonic crystal structure can significantly improve the efficiency of photosynthesis. Specifically, we couple photonic crystals and photocatalyst of sodium copper chlorophyllin (ChlCu), and binder of PVA through microfluidic blowing-spinning (MBS) to spray a composite photocatalytic film that can convert carbon dioxide and water into carbon monoxide and oxygen. By optimizing the content of ChlCu and the slow photon effect related to the bandgap position, the final CLPPs 300 -0.52% has two slow photon edges overlapping with the catalyst absorption spectrum, thus generating the maximum photon capture capability and achieving a high oxygen catalytic yield of up to 7.8 mmol g -1 h −1 . The spraying property of this material enable it to be coated on the external surfaces of other materials. This opens new possibilities of photocatalytic fabric preparation for CO 2 converting, providing new ideas of greenhouse gas capture and utilization to solve environmental problems.

✓ 已验证 产品关联 DOI 高影响因子
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Materials Today Sustainability · 2023 · IF 7.8

Enhanced direct degradation of photogenerated holes induced by dissolved O2 chemisorbed on oxygen-deficient nano-TiO2

A. Shan,Y. Lu,L. Cheng,Z. Hou,D. Xili,Y. Li,J. Liu,H. Ma,J. Yang

Due to the high electronegativity , dissolved O 2 molecules can form strong chemisorption on oxygen-deficient nano-TiO 2 , which can alter the photocatalytic degradation process . Regarding this point, there is a lack of sufficient investigation so far, although there have been many reports on oxygen-deficient nano-TiO 2 . Here, we make the dissolved O 2 adsorbed on the oxygen-deficient nano-TiO 2 by simply stirring for a long time. The characterization and theoretical calculation results show that the chemisorption of O 2 significantly enhances the surface hydrogen bonding and results in a substantial increase in the co-adsorbed H 2 O molecules and –OH groups. The co-chemisorbed oxygen species promote the separation of electron-hole pairs, meanwhile accelerate the migration and accumulation of holes to the surface, which effectively enhances the direct oxidation of photogenerated holes. The findings of this work suggest that for long continuous reactions, the role of chemisorbed dissolved O 2 molecules on the photocatalytic degradation activity of oxygen-deficient nano-TiO 2 has to be considered.

CAS / MDL: 123334-00-9
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Nanoscale · 2019 ·Vol. 11 ·期 24 ·11513-11520 · IF 6.97

Stabilizing electrochemical Li–O2 batteries with a metal-based cathode of PdNi on Ni nonwoven fabric

Huan-Feng Wang,Jun-Feng Li,Xue-Xi Sun,Ji-Jing Xu

The design of a nanoporous cathode for Li–O2 batteries that can achieve high chemical stability and superior electrochemical performance remains a formidable challenge. A novel approach for the fabrication of nanoengineered PdNi alloys directly coated onto Ni nonwoven fabric (PdNi/NiNF) obtained through electrospinning has been proposed. On the basis of the contributions of the porous structure, the prepared metal-based cathodes can exhibit high chemical and mechanical stabilities, high catalytic activity, and high conductivity. In this design, the major side reactions were excluded when compared with popularly used carbon cathodes, and excellent cycling stability (266 cycles) could be achieved. The proposed cathode exhibited a high discharge capacity of 15 700 mA h g−1 at 500 mA g−1, which was 5 times higher than those reported for carbon-free cathodes.

✓ 已验证 产品关联 DOI PubMed 高影响因子
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Nanoscale · 2019 ·Vol. 11 ·期 12 ·5285-5294 · IF 6.97

Metal–organic framework-derived hierarchical Co3O4@MnCo2O4.5 nanocubes with enhanced electrocatalytic activity for Na–O2 batteries

Yunzhao Liu,Xiaowei Chi,Qi Han,Yuexiu Du,Jiaqi Huang,Xinghao Lin,Yu Liu

The Na–O2 battery system is attracting increasing attention due to its superiority in specific capacity and cost. However, its practical implementation is hindered by many issues, such as high charge–discharge overpotential, limited cycling life, and poor reversibility, all of which result from the mediocre O2 electrode. Herein, to surmount these critical challenges, hierarchical Co3O4@MnCo2O4.5 nanocubes (h-Co3O4@MnCo2O4.5 Ns) with a yolk–shell structure are designed for the first time as the novel O2 electrode. h-Co3O4@MnCo2O4.5 Ns are synthesized from a metal–organic framework via a template-assisted method, which is demonstrated to be helpful in creating a high specific surface area of 130.4 m2 g−1, a hierarchical macro- and mesoporous structure, and synergistic yolk-shelled Co3O4@MnCo2O4.5 active sites. These unique structural properties endow h-Co3O4@MnCo2O4.5 Ns with remarkably enhanced electrocatalytic activity towards both the ORR and OER. The Na–O2 battery based on h-Co3O4@MnCo2O4.5 Ns displays an ultrahigh initial discharge capacity of 8400 mA h g−1, ultralow charge–discharge overpotential of 0.45 V, long cycling life of 135 cycles, and excellent rate capability.

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