RARE METALS
·
2023
·Vol. 42
·期 6
·1969-1982
·
IF 8.8
Liao Jia-Lin,Zhang Shuai,Bai Tian-Sheng,Ji Feng-Jun,Li De-Ping,Cheng Jun,Zhang Hong-Qiang,Lu Jing-Yu,Gao Quan,Ci Li-Jie
Lithium metal batteries (LMBs) with a high theoretical capacity are seen as a type of the most potential energy storage system. Unfortunately, the growth of lithium dendrite, the irreversible side reactions, and the infinite volume alteration still curb the practical utilization of lithium metal anodes, resulting in low Coulombic efficiency (CE) and safety problems, etc. Herein, we synthesize a lithiophilic 3D copper foam host with uniformly distributed nano-flower-like ZnO particles (CuF/ZnO) and obtain the composite lithium metal anode containing the Li 2 O, LiZn alloy, and pure Li by the infusion of molten Li (CuF/Li 2 O-LiZn@Li). Benefitting from the advantages of the 3D structure of copper foam and the lithiophilicity of ZnO sites, the composite lithium metal anode can restrain the volume alternation and regulate the uniform deposition of lithium. The symmetrical cells of the composite lithium metal anode have a 1600 h long cycle life with a low polarization voltage of 15 mV, and the Coulombic efficiency can maintain about 97.8% at 1.0 mA·cm −2 , 1.0 mAh·cm −2 . Graphical abstract
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Catalysts
·
2023
·Vol. 13
·期 3
·577
·
IF 3.9
Lu Zou,Weilin Kong,Linfeng Peng,Fang Wang
The development of Li-CO2/O2battery with high energy density and long-term stability is urgently needed to fulfill the carbon neutralization and pollution-free environment targets. The biomass-derived heteroatom-doped carbon catalyst with the combination of high-efficiency catalytic activity and sustainable supply is a promising cathode catalyst in Li-CO2/O2battery. Specifically, the unique morphology and mesopore structure can promote the transfer of CO2, O2, and Li+. Abundant channel pores can provide discharge products accommodation to the largest extent. Nitrogen dopant, the commonly recognized active sites in carbon, can improve the electron conductivity and accelerate the sluggish kinetic reaction. Therefore, utilizing the louts leaves as the precursor, we successfully prepare the cellular-like nitrogen-doped activated carbon nanosheets (N-CNs) through the appropriate pyrolysis carbonization method. The as-synthesized carbon nanosheets display a three-dimensional interconnecting pore structure and abundant N-dopant actives, which dramatically improve the electrochemical catalytic activity of N-CNs. The Li-CO2/O2battery with the N-CNs cathode delivers a high discharge capacity of 9825 mAh g−1, low overpotential of 1.21 V, and stable cycling performance of 95 cycles. Thus, we carry out a facile method for N-doped carbon nanosheets preparation derived from the cheap natural biomass, which can be the effective cathode catalyst for environmental-friendly Li-CO2/O2battery.Keywords:biomass-derived carbon;carbon nanosheets;nitrogen defects;cathode catalyst;Li-CO2/O2battery
研究领域:
材料科学
·
环境科学
·
能源科学
✓ 已验证
DOI
高影响因子
Journal of Energy Storage
·
2022
·
IF 8.907
De-Ming Zhu,Fan Bai,Yi-Nan Zhang,Ya-Nan Yang,Zhuang Sun,Jun-Wen Deng,Tao Zhang
Solid-state Li-O 2 batteries (SSLOBs) have been denoted as the holy grail in next-generation Li metal batteries for their high theoretical energy density , manipulation of ambient air to energy storage as well as high safety. However, the solid rigid interfaces both at the cathode and anode side introduce ultra-high resistances in the battery system and impede its operation under ambient temperature. Moreover, the high-reductive Li anode and semi-open cathode would cause severe side reactions during cycling which further degrade battery performance. To manage the above-mentioned issues, a rationally designed SSLOBs based on plastic crystal electrolyte is proposed in this study to enable SSLOBs operation at ambient temperature and in full charge-discharge mode. The brand-new Li-O 2 battery has been improved mainly from two aspects. First, we propose a polyacrylonitrile (PAN) modified succinonitrile (SN) electrolyte (PAN-SN) to retard the polymerization of SN and meanwhile suppress the degradation of Li ionic conductivity. Second, we propose an alternative mixed electron/ion complex conductor (MEIC) cathode to coordinate with plastic crystal electrolyte with an expanded Li-O 2 reactive zone and improved interfacial charge transfer during the charge-discharge process. The fabricated flexible SSLOBs based on PAN-SN electrolyte and MEIC cathode could be successfully fully charged-discharged (cutoff 2.0–4.5 V) for tens of cycles at ambient temperature under simulated air condition (20 vol% oxygen), with high-capacity retention of around 85 %.
研究领域:
能源存储
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电池技术
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材料科学
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电化学
✓ 已验证
DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2018
·
IF 6.653
Yuan Chen,Xu Zhang,Shixiang Feng
Contributions of excited triplet state of humic acid (3HA*) and superoxide radical anion (O2•–), which is mainly generated via the reaction of O2 with HA-derived reducing intermediates (HA•–), to phenol transformation were revealed using acetaminophen, 2,4,6-trimethylphenol and tyrosine as probe molecules. Phenol transformation was initiated by 3HA*, leading to the formation of the phenoxyl radical (PhO•), but the distribution of transformation intermediates was codetermined by 3HA* and HA•–. The influence of HA•– essentially resulted from the production of O2•–, which affected the fate of PhO•. PhO• could undergo dimerization, or react with O2•–, leading to either phenol peroxide formation (radical addition) or phenol regeneration (electron transfer). In addition, PhO• could bind to HA or react with HA radicals, particularly in the absence of O2 and O2•–. These PhO• reactions were dependent on the reduction potential and structure of PhO•. This study also proved that the reaction of phenol with 1O2 and the reaction of PhO• with O2•– lead to the same oxidation product. The contributions of 3HA* and its generated 1O2, HA•– and its generated O2•– to phenol transformation were pH-dependent.
研究领域:
环境化学
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物理化学
·
分析化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 18
·53355-53369
·
IF 5.8
Ding Chunsheng,Lei Jia,Cai Zhiyue,Gao Mengying,Zou Zhaozheng,Li Yuanfeng,Deng Jing
In this research, FeCo 2 O 4 nanomaterial was successfully synthesized by a typical sol–gel method and conducted as an effective agent for peroxymonosulfate (PMS) activation to eliminate antibiotics flurbiprofen (FLU), a strong nonsteroidal drug. FeCo 2 O 4 nanomaterial was characterized by XRD, TEM, SEM, and XPS. Various characterization results proved that FeCo 2 O 4 held stable spinel structure. The interfering factors including initial pH, PMS concentration, catalyst dosage, inorganic anions, and humic acid on FLU removal were also discussed. The conclusion was that the removal efficiency of FLU reached 98.2% within 120 min after adding FeCo 2 O 4 (0.4 g L −1 ) and PMS (3 mM). The optimal pH for FLU degradation was the initial pH of 6.5; too acidic or alkaline was not conductive to the degradation. The existence of HA and Cl − restrained the degradation of FLU, and HCO 3 − promoted the removal, while the influence of NO 3 − and SO 4 2− could not be considered. The radical scavenging experiment confirmed that • OH, O 2 •− , and SO 4 •− participated in FLU removal and SO 4 •− functioned a leading role. FeCo 2 O 4 showed high efficiency for PMS activation in pH range of 3.0 to 10.0. After the fourth cycle operation, the FLU removal rate exceeded 76.9%, and the Co leaching rate was low during the catalytic reaction. This study shows that FeCo 2 O 4 nanomaterial is an efficient and environment-friendly catalyst, which can be applied for PMS activation to remove organic pollutants in water.
研究领域:
环境科学
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化学
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材料科学
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水处理
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2023
·Vol. 34
·期 2
·2305470
·
IF 19
Hangyu Lu,Shiyong Chu,Jiaming Tian,Qi Wang,Chuanchao Sheng,Chen Cheng,Rixin Liu,Anita M. D'Angelo,Wei Kong Pang,Liang Zhang,Haoshen Zhou,Shaohua Guo
Lattice-oxygen redox in layered metal oxide cathodes offers a promising way to exploit high-energy density sodium-ion batteries. However, oxidation and reduction of lattice-oxygen are always asymmetric, showing poor reversibility upon charging and discharging due to the activated oxygen loss and subsequent structural rearrangement. Here, a layered Na 0.7 [Li 0.2 Mn 0.7 Co 0.1 ]O 2 (NLMCO) is developed by balancing lattice-oxygen activity and reversibility, which can deliver a record energy density of 729.7 Wh kg −1 , further exceeding the state-of-the-art Na 0.75 [Li 0.25 Mn 0.75 ]O 2 (NLMO, 638.4 Wh kg −1 ). In light of electron paramagnetic resonance spectroscopy, in situ differential electrochemical mass spectroscopy, and electrochemical testing results, the highly activated lattice-oxygen is effectively stabilized in NLMCO without oxygen molecule release while obvious oxygen release is detected in the highly activated NLMO. Benefiting from the enhanced transition metal-oxygen covalency and reduced band energy gap, the NLMCO electrode demonstrates simultaneously high lattice-oxygen activity and reversibility, thus resulting in excellent rate and cycling performance, as well as ultra-high energy density. The findings highlight the critical association of energy density and lattice-oxygen redox reversibility, which will inspire more interest in anionic redox-based high-energy batteries.
研究领域:
材料科学
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电池技术
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2023
·
IF 5.2
Geng Li,Zhuoyu Cai,Kun Su,Yuxin Zhao,Ying Zhu,Jiangang Han,Yuwei Pan,Weinan Xing,Guangyu Wu
In recent years, advanced oxidation technologies employ peroxynitrite activation have exhibited exceptional effectiveness in eliminating various emerging contaminants. In this study, different calcination temperatures were used to derive Co 3 O 4 nanospheres with varying surface morphologies . This method effectively addresses the issue of high cost associated with high-performance catalyst synthesis or poor catalytic performance of low-cost catalysts. The active species like O 2 •− , •OH, SO 4 •− , 1 O 2 played significant role in TC degradation and 1 O 2 was the dominant reactive oxygen species (ROS). The study also proposed possible degradation pathways based on the 15 intermediates identified through HPLC-MS. Furthermore, the developmental toxicity of the identified intermediates was evaluated using a quantitative conformational relationship prediction method. This paper delves into the reaction mechanism of Co 3 O 4 nanospheres in the activation of PMS and examines the impact of surface morphology on their catalytic performance, providing a new approach to developing a persulfate catalyst that is cost-effective and has high catalytic performance, with a simple synthesis step.
研究领域:
环境科学
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化学工程
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材料科学
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高级氧化技术
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催化
✓ 已验证
产品关联
DOI
高影响因子
Catalysis Science & Technology
·
2025
·
IF 4.2
Yu-Le Wang,Songhai Wu,Yu-Zhen Xu,Yu-Dong Shan,Yong Liu,Xu Han
The selective oxidation of cyclohexene (Cy) to cyclohexene oxide (Cy-ep) using O2 remains challenging due to low epoxidation selectivity. In this work, a series of Mo-doped TS-1 (Mo-TS-1) catalysts were successfully synthesized for the epoxidation of Cy under solvent- and initiator-free conditions with O2 as the oxidant. Among them, 5Mo-TS-1 exhibited high catalytic performance, achieving 43.5% Cy conversion and 50.6% selectivity toward Cy-ep. Additionally, valuable byproducts such as 2-cyclohexen-1-ol (Cy-ol) and 2-cyclohexen-1-one (Cy-one) were obtained with yields of 28.0% and 21.4%, respectively. Since both Cy-ol and Cy-one are valuable intermediates in fragrance synthesis, over 43.5% of Cy was effectively converted into high-value products. Quenching experiments and Raman spectroscopy revealed that surface oxygen vacancies (Ov) facilitate the activation of O2 to form ≡Ov‑superoxo species, which abstract hydrogen from the allylic C-H bond of Cy to generate 3-cyclohexenyl radicals (Cy•). These radicals subsequently react with O2 to form Cy-OO•, followed by hydrogen abstraction from another Cy molecule to yield 2-cyclohexene-1-hydroperoxide (Cy-OOH). A positive correlation between Cy-OOH and Cy-ep formation underscores the critical role of Cy-OOH in the epoxidation process. Furthermore, Raman spectroscopy confirmed the presence of ≡Mo-(η2-O2) peroxo species on the catalyst surface, which preferentially attack the C=C bond of Cy to form Cy-ep. DFT calculations elucidated two distinct O2 activation pathways: In Pathway I, O2 is activated at Ov sites to form ≡Ov‑superoxo, which subsequently reacts with Cy to generate ≡Ov‑peroxo, Cy-OOH, and Cy•. In Pathway II, Mo(V/VI) sites either directly activate O2 or react with peroxo intermediates (≡Ov‑peroxo or Cy-OOH) to form ≡Mo-(η2-O2). This species selectively epoxidizes the alkene bond in Cy to Cy-ep. Notably, the direct activation of O2 at Mo(V/VI) sites bypasses the allylic oxidation route, thereby enhancing the epoxidation selectivity beyond the theoretical limit of 50.0%. This study provides new insight on the importance of surface superoxo and peroxo mediated by Ov and Mo(V/VI) in the epoxidation processes.
研究领域:
催化化学
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材料化学
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绿色化学
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多相催化
·
氧化反应
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Yang Zhan,Shun-zhi Yu,Shao-hua Luo,Jian Feng,Qing Wang
Transition-metal sulfides (TMS) are one of the most promising cathode catalysts for Li–O2 batteries (LOBs) owing to their excellent stabilities and inherent metallicity. In this work, a highly efficient mode has been used to synthesize Co@CNTs [pyrolysis products of metal–organic frameworks (MOFs)]-derived CoS2(CoS)@NC. Benefiting from the special yolk–shell hierarchical porous morphology, the existence of Co–N bonds, and dual-function catalytic activity (ORR/OER) of the open metal sites contributed by MOFs, the CoS2@NC-400/AB electrode illustrated excellent charge–discharge cycling for up to nearly 100 times at a current density of 0.1 mA cm–2 under a limited capacity of 500 mA h g–1 (based on the total weight of CoS2@NC and AB) with a high discharge voltage plateau and a low charge cut-off voltage. Meanwhile, the average transferred electron number (n) is around 3.7 per O2 molecule for CoS2@NC-400, which is the chief approach for a four-electron pathway of the ORR under alkaline media. Therefore, we believe that the novel CoS2@NC-400/AB electrode could serve as an excellent catalyst in the LOBs.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
PubMed
高影响因子
ACS Applied Energy Materials
·
2021
·
IF 6.024
Ziling Wang,Xianzhu Peng,Shuai Guo,Mingjie Sun,Junfang Cheng,Lu Zou,Bo Chi,Jian Pu
Catalysts with high oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) performances are crucial to the development of lithium-oxygen batteries (LOBs), which aim to promote Li2O2 deposition and decomposition and then avoid the active site passivation. Considering the metallic Ag possessing good electrical conductivity and excellent catalytic activity and perovskite oxides exhibiting high abundance, an easily tunable structure, and excellent intrinsically catalytic activity, we adopt the ultraviolet light to realize the deposition of Ag nanoparticles on the La0.6Sr0.4Fe0.9Mn0.1O3 (LSFM) substrate as a high-performance cathode for LOBs. The results confirm that the synergetic effect of Ag nanoparticle decoration and the La0.6Sr0.4Fe0.9Mn0.1O3 substrate could dramatically improve the electronic conductivity and ORR/OER kinetics of the nanohybrids. Ag@LSFM hybrids with abundant active sites and considerable electronic conductivity promote the deposition of a thinner discharge product film, and the corresponding LOBs deliver high discharge capacity (12 477 mAh g–1), a small gap between charge and discharge potentials (∼1.3 V), and high cycling stability (147 cycles). Overall, the study suggests that such a bifunctional catalyst is a promising candidate in LOBs.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
Catalysis Science & Technology
·
2020
·Vol. 10
·期 24
·8445-8457
·
IF 5.721
Kun Liu,Yichen Zhao,Jiale Wang,Qingsong Xue,Guofeng Zhao
The fabrication of qualified catalysts is a key issue to implement gas-phase aerobic alcohol oxidation but necessarily requires understanding the structures of catalytic active sites and the supply of active oxygen species. Herein, we present one example of the Ag–CoO/Ti- powder catalyst for gas-phase benzyl alcohol aerobic oxidation. The first interesting observation is that the Ag–Co3O4 ensembles on the fresh catalyst could be transformed into Ag–CoO due to the presence of reductive benzyl alcohol. The preferred catalyst with 3 wt% Ag and 3 wt% CoO exhibits 93% benzyl alcohol conversion and 99% benzaldehyde selectivity at a weight hourly space velocity of 20 h−1 and a temperature of 240 °C. The structures of Ag–CoO ensembles and oxygen species supply were probed and identified by electron microscopy and other spectroscopy techniques in combination with temperature-programmed thermal analyses, pulse experiments, and kinetic studies. In nature, the oxygen species is generated at the Ag–CoO interfacial sites in the form of atomic oxygen with appropriate chemisorption strength on these sites to achieve a high oxidation activity of benzyl alcohol. Moreover, the Co3O4 ↔ CoO cycle is promoted by Ag at low temperature such as 240 °C to endow the Ag–CoO ensembles with excellent catalytic performance.
研究领域:
催化化学
·
材料科学
·
物理化学
✓ 已验证
DOI
高影响因子
Frontiers in Chemistry
·
2019
·
IF 3.782
Song Hongbing,Liu Zong,Gai Hengjun,Wang Yongjie,Qiao Lin,Zhong Caiyun,Yin Xiangyang,Xiao Meng
Introducing electron-rich nitrogen atoms to ordered mesoporous carbons (OMC) as supports for noble metal catalysts, not only improves the hydrophilic properties of a mesoporous carbon surface, but also enhances the coordination and binding abilities of metal ion. In the present work, nitrogen-doped ordered mesoporous carbons (NOMCs) were successfully fabricated via a facile hydrothermal self-assembly. The prepared NOMCs were characterized through powder X-ray diffraction (XRD), Raman spectroscopy, transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), and nitrogen adsorption-desorption isotherm. The analyses demonstrated that the NOMCs prepared at a pyrolysis temperature of 750°C possessed an ordered 2D hexagonal mesoporous structure, a high graphitization degree, large surface area, and a well-distributed pore size. In particular, NOMCs could anchor Pd nanoparticles uniformly because of the introducing N atoms with strong electronegativity, which were selected as efficient catalysts for the partial oxidation of benzyl alcohol to benzaldehyde. Approximately 24.63% conversion with 85.71% selectivity to benzaldehyde was obtained without using any solvent by molecular O2 oxidation. Most importantly, the TOF value of the catalyst in the reaction system was up to 8698 h−1. After five runs reaction, TOF and selectivity of the catalyst remained essentially same. Hence, the proposed catalyst has a potential engineering application value.
研究领域:
材料科学
·
催化化学
✓ 已验证
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）