Journal of Materials Chemistry A
·
2022
·Vol. 10
·期 37
·19757-19768
·
IF 14.511
Min Lu,Li An,Jie Yin,Jing Jin,Rui Yang,Bolong Huang,Yang Hu,Yong-Qing Zhao,Pinxian Xi
The electrochemical oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) are key electrochemical processes in metal–air batteries and water splitting devices. Aluminium–air batteries, as an important type of metal–air battery, have been considered to be promising power candidates for flexible electronics. Here, we describe electronically engineered amorphous Fe–Co–S sites embedded in Prussian blue analogue (FeCoSx-PBA) hetero-nanoframes. The experimental results and DFT calculations reveal the critical role of the introduced FeCoSx layer to PBA, which enhances the electron transfer and alleviates the overbinding effect of OH* during the OER. The FeCoSx-PBA hybrid system supplies an optimized electronic structure for the alkaline OER, which is also confirmed by the much-lowered overpotential (266 mV at 10 mA cm−2) for the alkaline OER. Furthermore, a flexible Al–air battery based on an FeCoSx-PBA cathode catalyst exhibits a high peak power density (58.3 mW cm−2) and energy density (1483 W h kgAl−1), and outstanding stability for more than 50 h of operation under bending or stretching conditions, demonstrating its potential in the practical application of flexible electronic devices. Our results may provide a new strategy of modulating the electronic structure of air electrode catalysts to efficiently promote the reactivity of alkaline OER and Al–air battery processes.
研究领域:
材料科学
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电化学
·
能源技术
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DOI
高影响因子
CHEMISTRY OF MATERIALS
·
2020
·
IF 9.567
Huanhuan Jia,Xinmiao Liang,Tao An,Linfeng Peng,Jiwen Feng,Jia Xie
Finding sodium solid electrolytes (SSEs) with good performance is key to building all-solid-state sodium batteries. In the development of solid electrolytes, halogen doping has been shown to be an effective approach. However, it has rarely been applied to chalcogenide-based SSEs, possibly because of strict structure constraints. In this work, the strategy of halogen doping is successfully demonstrated on Na3.67[Sn0.67Si0.33]0.67P0.33S4, a novel SSE with high structural tolerance. The halogen-doped samples formulated as Na3.57[Sn0.67Si0.33]0.67P0.33S3.9X0.1 (X = Cl, Br, and I) exhibit higher ionic conductivities and lower activation energies than the pristine sample. Na3.57[Sn0.67Si0.33]0.67P0.33S3.9I0.1, the I-doped sample, has the highest ambient ionic conductivity of 1.08 mS cm–1 and the lowest activation energy of 0.24 eV. Structure analysis indicates that the high electronegativity of Cl atoms plays an important role in improving the conduction of Na+ ions in Cl-doped samples. The large atomic radius and high polarizability of I are more important factors to accelerate the transportation of Na+ ions in the I-doped counterpart. Furthermore, the all-solid-state sodium batteries assembled with Na3.57[Sn0.67Si0.33]0.67P0.33S3.9I0.1 as solid electrolytes show decent cyclic stability at 30 °C with a current density of 0.15 A g–1. This work systematically manifests the effect of halogen doping in SSEs, providing a versatile method to develop novel SSEs.
研究领域:
材料科学
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电化学
·
能源存储
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DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Yuan Fang,Shiyu Ji,Xin Wu,Jianfeng Zhu
Passive direct liquid fuel cells are promising power generation devices with the advantages of convenient transportation, storage for liquid fuel and high power density. This paper focuses on improving the intrinsic electrocatalytic performance and durability of nitrogen-doped carbon (N-C) cathodic electrocatalysts. Then, lamellar structured Ce-S-NC heterogeneous electrocatalyst was synthesized and used as a highly durable cathode for two types of passive direct liquid fuel cells, i.e. , direct methanol fuel cells (DMFCs) and direct borohydride fuel cells (DBFCs). In this work, the effect of the S/C molar ratio on the microstructure and electrocatalytic performance of the Ce-S-NC electrocatalysts was investigated, and excellent intrinsic oxygen reduction reaction activity was obtained at an S/C molar ratio of 0.15. The peak power densities of Ce-S-NC based DMFCs reached up to 12.5, 23.6 and 41.9 mW·cm −2 at 20, 40 and 60 °C, respectively. The peak power densities of 59.3, 84.6 and 132.6 mW·cm −2 were obtained in Ce-S-NC based DBFCs at 20, 40 and 60 °C, respectively. In the durability tests, both the Ce-S-NC based air-breathing DBFCs and passive DBFCs showed the stable operation than that of N-C and Ce-NC. When the current density increased from 50 to 150 mA·cm −2 , the Ce-S-NC based DBFC can be operated for 882 h, and only 34 and 91 h for that of N-C and Ce-NC. The electrochemical impedance spectroscopy tests proved Ce-S-NC based DBFC showed the faster mass transfer efficiency. The outstanding durability of Ce-S-NC is mainly attributed to the improved defect density and mass transfer.
研究领域:
材料科学
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能源科学
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电化学
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DOI
高影响因子
Cell Reports
·
2023
·
IF 8.8
Xue Wen,Yang Xiao,Haitao Xiao,Xueqin Tan,Beiyi Wu,Zehua Li,Ru Wang,Xuewen Xu,Tao Li
Summary Bisphenol S (BPS) exposure has been implied epidemiologically to increase obesity risk, but the underlying mechanism is unclear. Here, we propose that BPS exposure at an environmentally relevant dose aggravates diet-induced obesity in female mice by inducing brown adipose tissue (BAT) whitening. We explored the underlying mechanism by which KDM5A-associated demethylation of the trimethylation of lysine 4 on histone H3 (H3K4me3) in thermogenic genes is overactivated in BAT upon BPS exposure, leading to the reduced expression of thermogenic genes. Further studies have suggested that BPS activates KDM5A transcription in BAT by binding to glucocorticoid receptor (GR) in an estrogen-dependent manner. Estrogen-estrogen receptors facilitate the accessibility of the KDM5A gene promoter to BPS-activated GR by recruiting the activator protein 1 (AP-1) complex. These results indicate that BAT is another important target of BPS and that targeting KDM5A-related signals may serve as an approach to counteract the BPS-induced susceptivity to obesity.
研究领域:
内分泌学
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分子生物学
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肥胖研究
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表观遗传学
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DOI
PubMed
高影响因子
ORGANIC PROCESS RESEARCH & DEVELOPMENT
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2020
·
IF 3.023
Zeyu Yang,Wenjie Ye,Youyu Xie,Qinghai Liu,Rong Chen,Hualei Wang,Dongzhi Wei
Bioreductions catalyzed by alcohol dehydrogenases (ADHs) play an important role in the synthesis of chiral alcohols. However, the synthesis of ethyl (S)-4-chloro-3-hydroxybutyrate [(S)-CHBE], an important drug intermediate, has significant challenges concerning high substrate or product inhibition toward ADHs, which complicates its production. Herein, we evaluated a novel ADH, SmADH31, obtained from the Stenotrophomonas maltophilia genome, which can tolerate extremely high concentrations (6 M) of both substrate and product. The coexpression of SmADH31 and glucose dehydrogenase from Bacillus subtilis in Escherichia coli meant that as much as 660 g L–1 (4.0 M) ethyl 4-chloroacetoacetate was completely converted into (S)-CHBE in a monophasic aqueous system with a >99.9% ee value and a high space-time yield (2664 g L–1 d–1). Molecular dynamics simulation shed light on the high activity and stereoselectivity of SmADH31. Moreover, five other optically pure chiral alcohols were synthesized at high concentrations (100–462 g L–1) as a result of the broad substrate spectrum of SmADH31. All these compounds act as important drug intermediates, demonstrating the industrial potential of SmADH31-mediated bioreductions.
研究领域:
生物化学
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药物化学
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酶工程
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DOI
高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2021
·
IF 6.953
Wenyu Wang,Huan Sheng,Daihong Cao,Fenglian Zhang,Weifen Zhang,Fang Yan,Dejun Ding,Ni Cheng
Nitric oxide (NO) has aroused wide interest in the treating infected wounds due to its characteristic functionalities. However, its utilization is limited due to its volatile properties, high reactivity, direct potential toxicity, and byproducts of NO donors limited its application. Herein, endogenously NO donor S-nitrosoglutathione (GSNO) was connected covalently to polydopamine nanoparticles (PDA-GSNO NPs) to minimize the loss of NO in aqueous medium. Meanwhile, near-infrared (NIR)-controlled NO release and photothermal therapy (PTT) was obtained through the photothermal conversion by PDA. Then chitosan (CS)/gelatin (GE) biocomposite hydrogel films with preferable biocompatibility, surface hydrophilicity, hydroabsorptivity, and mechanical adhesive properties were constructed. By embedding PDA-GSNO NPs into the films, a multifunctional wound dressing was fabricated. Under NIR light irradiation, the combination of PTT, NO-releasing, and CS antibacterial agents can strengthen the in vitro antimicrobial efficacy and in vivo wound healing activities. Meanwhile, the obtained wound dressing presented good biocompatibility. This work outlines an approach for combating bacterial infections and demonstrating the possibility for synergistic NO-releasing wound healing.
研究领域:
生物医学工程
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材料科学
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药理学
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DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2022
·
IF 14.224
Lijun Chen,Chenguang Wang,Guozhao Liu,Guanwen Su,Kairu Ye,Wanping He,Huiru Li,Hongyuan Wei,Leping Dang
Reasonable regulation of the micro-morphology of material can significantly enhance the related performance. Herein, bismuth tungstate (Bi 2 WO 6 , simplified as BWO) porous hollow spheres with flower-like surface were prepared successfully, and this unique morphology endowed BWO with improved photocatalytic performance by reflecting and absorbing the light multiple times inside the cavity. To inhibit the rapid recombination of photogenerated e - -h + pairs within BWO itself, black phosphorous quantum dots (BPQDs) were anchored onto the nanosheets of BWO sphere closely by a facile self-assembly process, which will not shade the pores of BWO owing to the small size of BPQDs, but the BP nanosheets have the chance to do that. The band gap of BPQDs expanded much after exfoliation due to the quantum confinement effects, which matched the energy band of BWO well to form S-scheme heterojunction , achieving more efficient separation of photogenerated charges. As a result, the BPQDs/BWO exhibited attractive photocatalytic performance in the degradation of amoxicillin (AMX) and other antibiotics. Besides, the operation conditions were optimized, specifically, 94.5 % of AMX (20 mg/L, 200 mL) can be removed in 60 min when 50 mg of 2BPQDs/BWO was used as catalyst with solution pH = 11. Moreover, a possible degradation pathway of AMX was proposed based on the detected intermediates.
研究领域:
材料科学
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环境科学
·
化学工程
✓ 已验证
DOI
PubMed
高影响因子
iScience
·
2025
·
IF 4.1
Zhiwei Meng,Zirui Peng,Yupeng Yan,Qin Zhang,Yang Li
Photocatalytic technology is currently one of the most effective methods for removing tetracycline (TC) from the environment; however, the underlying photocatalytic mechanism remains unclear. In this study, zinc oxide quantum dots (ZnO-QDs)/hollow-sphere g-C 3 N 4 (CNHS) S-scheme heterojunction photocatalysts were synthesized for the photocatalytic degradation of tetracycline. Experimental results showed that the 7% ZnO-QDs/CNHS photocatalyst exhibited excellent TC degradation efficiency, with a removal rate of 80.2% within 15 min. Through free radical conversion pathway analysis, singlet oxygen ( 1 O 2 ) was identified as the primary active species responsible for tetracycline degradation. Further calculations indicated that the combination of holes (h + ) and superoxide radicals (O 2 − ) produces 1 O 2 , accounting for 83.28% of the total contribution. These findings provide theoretical support for 1 O 2 as the primary active species in pollutant degradation.
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产品关联
DOI
PubMed
高影响因子
ACS Sustainable Chemistry & Engineering
·
2017
·
IF 5.951
Qiang Liu,Qinze Liu,Zhuotong Wu,Yang Wu,Tingting Gao,Jinshui Yao
We report a novel composite absorbent prepared by the simple method that catechol-amine resin coats the hydrocellulose based on the adhesion property like polydopamine. The composite which contains many chelating groups on its surface was characterized by scanning electron microscopy (SEM), infrared spectroscopy (FT-IR), X-ray photoelectron spectroscopy (XPS), etc. The obtained adsorbents were investigated to remove Methyl Orange (MO) and Alizarin Red S (AR) from pH-unregulated aqueous system by batch experiments, including the affected factors of adsorbent dosage, contact time, initial concentration, and temperature. Results showed the adsorption processes belonged to the chemisorption and exhibited a spontaneous and endothermic nature. Besides, the removal performances fitted with the Langmuir isotherm model and pseudo-second order kinetic model very well. The maximum adsorption amounts of MO and AR were 189.39 and 284.09 mg/g at 303 K, respectively. The difference about adsorption amounts may be caused by the strong effect of π–π conjugation and hydrogen bonding between adsorbent and AR. Furthermore, the adsorption processes exhibited a spontaneous and endothermic nature. The recycling test indicated that the adsorbent stayed stable for the removal of both dyes by desorbed three times. Accordingly, the adsorbent with high adsorption capacity and rapid removal rate should be a promising material for the removal of anionic dyes from sewage.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
CHEMICAL PHYSICS LETTERS
·
2025
·
IF 3.1
Shihui Zhang,Xu Zhang,Wanting Shi,Weiyan He,Caihong Li,Xiaojing Wang
Slow charge transfer and a weak built-in electric field (BIEF) at the heterojunction interface critically hinder the construction of efficient S-scheme heterojunctions. Secondary calcination and ultrasonic treatment of g-C 3 N 4 enhance interfacial contact with MIL-101, shortening carrier migration paths. P and Mn doping increases the Fermi-level difference between g-C 3 N 4(C,S) and MIL-101, strengthening the BIEF to drive directional carrier migration. This facilitates the recombination of carriers with low-redox-potential at the heterojunction interface while spatially separating carriers with high-redox-potential, successfully constructing an S-scheme P-Mn-MCN (C,S) heterojunction. The optimized system delivers remarkable photocatalytic performance, achieving 98 % tetracycline hydrochloride degradation under visible light within 60 min.
研究领域:
材料科学
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环境科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF APPLIED ELECTROCHEMISTRY
·
2024
·
IF 2.4
Li Jingzhe,Zhang Jiaxin,Ling Yikai,Long Min,Tian Rui,Liang Ti,Nong Guangzai
Pt counter electrodes are essential components of dye-sensitized solar cells (DSSCs). However, their high cost and poor stability limit the development of these cells. In the quest for alternative materials to replace Pt, this study utilized sodium lignosulfonate as the primary raw material and successfully prepared N, S co-doped hierarchical porous carbon by adjusting the ratio of thiourea. This carbon was then fabricated into a counter electrode to replace Pt. The results showed that the N, S co-doped hierarchical porous carbon exhibited superior electrochemical performance compared to single-atom doped carbon. When used as the counter electrode in DSSCs, it achieved a power conversion efficiency of 8.62%, which is higher than the 7.98% efficiency of Pt. Furthermore, it demonstrated greater stability than Pt in stability tests. These findings confirm that N, S co-doped hierarchical porous carbon could replace Pt, thereby advancing the scientific understanding of DSSCs and promoting their application and development. Graphical Abstract
研究领域:
材料科学
·
能源材料
·
太阳能电池
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DOI
高影响因子
Catalysts
·
2021
·Vol. 11
·期 12
·1550
·
IF 4.146
Hongzhou Dong,Yingjie Chen,Chong Gong,Lina Sui,Qiong Sun,Kangle Lv,Lifeng Dong
Due to slow kinetics of oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) during discharging and charging processes, it is essential to rationally design and synthesize non-precious metal bifunctional electrocatalysts with good performance for metal-air batteries. Herein, Ag-MnFe2O4heterojunction nanoparticles supported on N, S, P-codoped graphene (NSPG) are developed with enhanced ORR and OER bifunctional electrocatalytic activities and stability. In contrast, S, P-doped graphene (SPG) and N, P-doped graphene (NPG) show less stabilization for the heterojunction particles. For example, under alkaline conditions, the ORR half-wave potential of Ag-MnFe2O4/NSPG can reach 0.831 V, and the over potential for OER is 0.56 V at the current density 10 mA·cm−2. Furthermore, Ag-MnFe2O4/NSPG shows better methanol resistance and durability than Pt/C catalysts.
研究领域:
材料科学
·
电化学
·
能源存储
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）