CATALYSIS TODAY
·
2018
·
IF 4.667
Miao Lai,Jie Zhao,Qingcai Chen,Shuaijun Feng,Yujie Bai,Yingxuan Li,Chuanyi Wang
In the photocatalytic volatile organic compounds (VOCs) degradation, the accumulation of intermediate products on the surface of catalysts could cause a decrease in activity through retarding reactant (e.g. O 2 ) supply to surface active sites. Herein, Bi decorated TiO 2 photocatalysts (Bi/TiO 2 ) for photocatalytic toluene degradation were prepared and systematically studied. It is found that metallic Bi modification improves the ability of photocatalysts to capture O 2 . As a result, the activities of the Bi/TiO 2 photocatalysts are obviously higher than that of the TiO 2 for photocatalytic toluene degradation, and the productions of photogenerated reactive oxygen species ( O 2 − and H 2 O 2 ) over the Bi/TiO 2 photocatalysts are almost equal to that over the TiO 2 despite the fact that the separation efficiency of photoinduced charge carriers is decreased after the addition of Bi. Adsorbed benzaldehyde is the main surface intermediate on the surface of the Bi/TiO 2 photocatalysts, whereas plenty of more readily oxidized aliphatic carboxylate species was monitored on the surface of the TiO 2 , which can be attributed to insufficient O 2 supply to the TiO 2 surface. This further indicates the positive role of the promoted O 2 supply by Bi in the photocatalytic toluene degradation. The present work offers a new window for addressing the catalyst deactivation in the photocatalytic VOCs degradation.
研究领域:
环境催化
·
大气污染控制
·
材料化学
·
表面科学
·
光化学
✓ 已验证
DOI
高影响因子
ChemSusChem
·
2017
·Vol. 10
·期 7
·1385-1389
·
IF 7.226
Hao Wan,Ya Mao,Zixuan Liu,Qingyou Bai,Zhe Peng,Jingjing Bao,Gang Wu,Yang Liu,Deyu Wang,Jingying Xie
As the first step during discharge, the mass transfer of oxygen should play a crucial role in Li–air batteries to tailor the growth of discharge products, however, not enough attention has been paid to this issue. Herein, we introduce an oxygen-enriching cosolvent, 1,2-(1,1,2,2-tetrafluoroethoxy) ethane (FE1), into the electrolyte, and investigate its influence on the discharge performance. The incorporation of this novel cosolvent consistently enhances the oxygen solubility of the electrolyte, and improves the oxygen diffusivity following a volcano-shape trend peaking at 50 % FE1. It is interesting that the discharge capacities obtained with the investigated electrolytes share the similar volcano trends as the oxygen transport under 50 mA g carbon −1 and higher current densities. The improved oxygen diffusion could benefit the volumetric utilization of the air cathode, especially at the separator side, probably owing to the fast oxygen transport to moderate its concentration gradient. Our results demonstrate the importance of oxygen provision, which easily becomes the capacity-determining factor. Graphical Got Oxygen? The enhancement of oxygen provision is achieved by incorporating 1,2-(1,1,2,2-tetrafluoroethoxy) ethane as the cosolvent in the electrolyte. The oxygen's diffusivity, rather than solubility, exerts the principal effect on discharge performance of the Li–air battery, especially at higher current density, owing to the ameliorated oxygen's accessibility, which improves the utilization ratio of the whole air cathode.
研究领域:
电化学
·
能源材料
·
电池技术
·
纳米材料
·
物理化学
·
先进储能系统
✓ 已验证
DOI
高影响因子
ACS ES&T Engineering
·
2026
·
IF 6.3
Yao Chen,Tianle Hu,Jianwei Ai,Quansheng Zhou,Xinyi Su,Yuchen Zhang,Hanchen Zhang,Shuhui Guan,Zhenfeng Bian,Hiromi Yamashita
Photocatalytic dissolution of precious metals (PMs) relies critically on the generation of specific reactive intermediates; however, the rational control of radical species in visible light remains challenging. Herein, we introduced the cyano (−CN) group into g-C3N4 (denoted as g-C3N4–CN), achieving a remarkable enhancement in the dissolution efficiency of precious metals under visible light. The −CN group not only promotes the visible-light absorption of g-C3N4–CN, but also facilitates the separation of photogenerated charges. The electron paramagnetic resonance (EPR) spectroscopy further demonstrates that g-C3N4–CN instantaneously generates superoxide radicals (O2•–) via efficient oxygen reduction while simultaneously promoting the rapid production of alkyl radicals (R•) through solvent oxidation. In contrast, pristine g-C3N4 exhibits a sluggish generation of all radical species. The distinct radical generation kinetics of g-C3N4–CN is identified as the key driver for its superior dissolution efficiency, enabling precious-metal recovery rates by 2–4 times and establishing a radical-targeted strategy for sustainable photocatalysis.
✓ 已验证
DOI
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
·
2021
·
IF 7.963
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
✓ 已验证
DOI
PubMed
高影响因子
Journal of Materials Chemistry A
·
2016
·Vol. 5
·期 2
·544-553
·
IF 8.262
Qin Zhao,Caixia Wu,Lina Cong,Yuhang Zhang,Guiru Sun,Haiming Xie,Liqun Sun,Jia Liu
Controlling the geometric morphology and distributive location of discharge products play an important role in the reversibility and efficiency of Li–O2 batteries. This work presents novel Co2CrO4 nanospheres (CCO) prepared via a facile method, which are applied as the electrocatalysts for Li–O2 batteries. The as-prepared CCO was characterized by XRD, XPS, SEM, TEM, BET, and TG measurements. The CCO exhibited a yolk–shell microstructure, which could facilitate fast Li+ and O2 diffusion as well as possessing enough space for the discharge product deposition. In comparison to the performance of the cell without catalyst, the overpotential of the cell with CCO was apparently reduced and the cyclability significantly enhanced. Based on the experimental results and DFT calculations, direct evidence of the CCO employment being linked to the Li2O2 morphology was provided. In addition, a catalytic mechanism was proposed. Furthermore, fundamental information about the key factors and steps involved in the Li2O2 formation and decomposition was revealed. We expect that this study gives insight into the development of electrocatalysts, the selection of O2 electrode materials, and the design of O2 electrodes for Li–O2 batteries, as well as advancing our understanding of the catalytic mechanism.
研究领域:
材料科学
·
电化学
·
能源存储与转换
✓ 已验证
DOI
高影响因子
WATER ENVIRONMENT RESEARCH
·
2019
·Vol. 91
·期 8
·770-779
·
IF 1.24
Jinhong Fan,Hehe Qin,Yunfei Zhang,Simin Jiang
In this study, Fe/Cu bimetal composite was prepared by high-energy ball milling (BM) method for the removal of refractory organics. The BM Fe/Cu bimetal was characterized by SEM-EDS, XRD, and XPS. Evenly distributed Fe and Cu was observed in the EDS mapping. In contrasting experiments, the removal rate of 4-chlorophenol (4-CP) by BM Fe/Cu materials was about 10-fold faster than that by chemical substitution deposition (CSD) of Fe/Cu material. Complete 4-CP removal and 66.7% of total organic carbon (TOC) mineralization in the BM Fe/Cu–O 2 system were achieved. Dissolved oxygen plays a crucial role for 4-CP degradation through the in situ generation of reactive oxygen species (ROS) such as H 2 O 2 , ·OH, and via oxygen activation reactions. The predominant reactive radicals were identified to be and ·OH through ESR technique and inhibition experiments. The coexistence of oxidation and reduction of 4-CP in the BM Fe/Cu-O 2 system was proposed. Practitioner points 4-CP removal rate by BM Fe/Cu is 10-fold faster than that by CSD Fe/Cu at the same conditions. Complete 4-CP removal and 66.7% of TOC reduction were achieved. All three ROS including ·OH, , and H 2 O 2 coexisted in the BM Fe/Cu-O 2 system. A harmonious coexistence of oxidation and reduction mechanism was proposed.
研究领域:
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nanoscale
·
2019
·Vol. 11
·期 24
·11513-11520
·
IF 6.97
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.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Di Zhang,Zhongju Ye,Lin Wei,Haibin Luo,Lehui Xiao
Photodynamic therapy (PDT) has attracted great attention as an alternative tumor treatment method. Unfortunately, it suffers from some limitations like poor targeting capability and insufficient therapeutic efficiency caused by tumor hypoxia. In this work, we introduce a novel O2-evolving PDT nanoparticle for homologous cancer cell targeting as well as dual-mode imaging [i.e., magnetic resonance imaging (MRI) and fluorescence imaging]. Specifically, the nanostructure consists of a MnO2 nanosheet-coated metal–organic framework core and cancer cell membrane shell (defined as CM-MMNPs). The MnO2 layer displays H+ and H2O2 responsiveness, which can produce O2 to enhance O2-mediated singlet oxygen (1O2) generation for PDT. Moreover, the resulted Mn2+ can also be used as an optimal MRI contrast agent. The introduction of cell membrane and membrane proteins endow the CM-MMNPs with good stability and integrity in the process of cellular endocytosis, as well as strong homologous cell-targeting ability. This multifunctional nanoparticle has the potential to overcome the hypoxia of cancer cells in PDT, and provides a new paradigm for tumor targeting, detection, and therapy, which is promising for biomedical applications in the future.
研究领域:
生物医学工程
·
癌症研究
·
纳米技术
·
诊疗学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF ENERGY RESEARCH
·
2020
·Vol. 45
·期 5
·7120-7128
·
IF 3.741
Menglu He,Jia Jia,Qing Sun,Weixin Zhang
SUMMARY Li-O 2 battery has attracted much attention due to its ultra-high theoretical energy density in the field of electrochemical energy storage. The introduction of efficient electrocatalyst can effectively accelerate the reaction rate of ORR and OER, so as to improve the coulomb efficiency and poor cycle stability of Li-O 2 battery. In this work, a novel hollow N-doped carbon sphere is prepared by using MOF and polystyrene as template, and act as highly efficient oxygen electrocatalyst for rechargeable Li-O 2 batteries. The hollow structure can provide enough oxygen diffusion channel, deposition and decomposition space for reduction products. N doping into the hollow carbon structure can increase the charge density of adjacent carbon atoms and enhance its catalytic activity of ORR/OER. As a result, the Li-O 2 battery using the hollow N-doped carbon sphere as air cathode exhibited an high specific capacity of 18 762 mAh/g (at a current density of 500 mA/g) and remarkable cycling stability of 212 cycles (at a current density of 500 mA/g and limited capacity of 1000 mAh/g), outperforming the carbon material with common structure. This work highlights the importance of air cathode structure and efficient catalyst, provides a new idea for the design of air cathode of Li-O 2 battery, and expands the scope of future research.
研究领域:
材料科学
·
电化学能源存储
✓ 已验证
产品关联
DOI
高影响因子
Nanoscale
·
2019
·Vol. 11
·期 12
·5285-5294
·
IF 6.97
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.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Materials Today Sustainability
·
2023
·
IF 7.8
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.
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
·
IF 5.816
Shaolong Wang,Dingding Ye,Hao Liu,Xun Zhu,Zhenfei Liu,Rong Chen,Qiang Liao,Yang Yang
The in-situ H 2 O 2 electrosynthesis by two-electron oxygen reduction reaction employing renewable electricity is a promising alternative to traditional anthraquinone process due to its security, environmental friendliness and excellent cost effectiveness, which requires high-performance, cost-effective and environmental-friendly electrocatalysts . A bamboo-derived O-doped rocky electrocatalyst is developed by facile pyrolysis and acid treatment for high-efficiency electroreduction of O 2 to H 2 O 2 . Three-dimensional interconnected hierarchical pores in rocky electrocatalysts expose abundant electroactive sites and facilitate mass transfer of reaction species. From the results of rotating ring-disk electrode test, a H 2 O 2 selectivity up to 80% and superior electrocatalytic activity of the prepared electrocatalyst are achieved by surface oxygen functionalization induced by acid treatment. At the optimal catalyst loading of 2 mg cm −2 , prominent H 2 O 2 productivity of 1037 mmol g c a t a l y s t − 1 h − 1 with high current efficiency up to 74.1% is achieved at 30 mA cm −2 by air-breathing cathode. Higher H 2 O 2 productivity (1525 mmol g c a t a l y s t − 1 h − 1 ) is yielded by further raising the current density to 50 mA cm −2 . Moreover, the durability test of the cathode through ten consecutive runs demonstrates its great stability for electrocatalytic generation of H 2 O 2 . This work inspires the development of promising biomass-derived electrocatalysts for green and sustainable on-site H 2 O 2 electrosynthesis.
研究领域:
材料科学
·
环境科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）